energies

Review
A Review of Modelling of the FCC Unit—Part II:
The Regenerator
Thabang W. Selalame, Raj Patel, Iqbal M. Mujtaba and Yakubu M. John *

Department of Chemical Engineering, Faculty of Engineering and Informatics, University of Bradford,

Bradford BD7 1DP, UK; [email protected] (T.W.S.); [email protected] (R.P.);
[email protected] (I.M.M.)
* Correspondence: [email protected]

Abstract: Heavy petroleum industries, including the Fluid Catalytic Cracking (FCC) unit, are among
some of the biggest contributors to global greenhouse gas (GHG) emissions. The FCC unit’s regenera-
tor is where these emissions originate mostly, meaning the operation of FCC regenerators has come
under scrutiny in recent years due to the global mitigation efforts against climate change, affecting
both current operations and the future of the FCC unit. As a result, it is more important than ever to
develop models that are accurate and reliable at predicting emissions of various greenhouse gases to
keep up with new reporting guidelines that will help optimise the unit for increased coke conversion
and lower operating costs. Part 1 of this paper was dedicated to reviewing the riser section of the FCC
unit. Part 2 reviews traditional modelling methodologies used in modelling and simulating the FCC
regenerator. Hydrodynamics and kinetics of the regenerator are discussed in terms of experimental
data and modelling. Modelling of constitutive parts that are important to the FCC unit, such as
gas–solid cyclones and catalyst transport lines, are also considered. This review then identifies areas
where the current generation of models of the regenerator can be improved for the future. Parts 1



and 2 are such that a comprehensive review of the literature on modelling the FCC unit is presented,


showing the guidance and framework followed in building models for the unit.
Citation: Selalame, T.W.; Patel, R.;
Mujtaba, I.M.; John, Y.M. A Review of
Keywords: fluid catalytic cracking; regenerator; hydrodynamics; kinetics; modelling; coke combustion
Modelling of the FCC Unit—Part II:
The Regenerator. Energies 2022, 15,
388. https://doi.org/10.3390/
en15010388
1. Introduction
Academic Editor: Dmitri A.
Process modelling and simulation have been widely used in a vast number of indus-
Bulushev
tries to analyse, control and optimise the behaviour of different processes. The fundamental
Received: 21 October 2021 requirement for a model is that it be efficient and accurate at making the predictions that
Accepted: 28 December 2021 the end user is interested in. The deactivated catalyst is sent to the regenerator, where the
Published: 5 January 2022 coke on the catalyst is burned off. It has two main functions: (i) to burn off the coke on the
Publisher’s Note: MDPI stays neutral catalyst to regain the catalyst’s activity; (ii) to provide the heat needed to drive the endother-
with regard to jurisdictional claims in mic cracking reactions in the riser-reactor via the exothermic combustion reactions [1]. The
published maps and institutional affil- FCC regenerator is a complex fluidised bed reactor that is used for air combustions of
iations. catalytic coke deposited on catalyst during catalytic cracking of gas oil feedstock. The
regenerator operates in the bubbling/turbulent regime of fluidisation, which results in
complex hydrodynamics in terms of mass, momentum and energy transport phenomena,
making it a difficult process to model [2,3]. The FCC regeneration process also results in
Copyright: © 2022 by the authors. the production of GHG emissions, mainly carbon dioxide, which makes it a significant
Licensee MDPI, Basel, Switzerland. contributor to climate change [4]. The recent global effort, through the Paris Agreement [5]
This article is an open access article
and global treaties on the combat of climate change [6,7], mean it is more important than
distributed under the terms and
ever to build models of units such as the FCC regenerator that can accurately predict the
conditions of the Creative Commons
emissions of GHGs. Such models allow for the optimisation of the unit so that emissions of
Attribution (CC BY) license (https://
various GHGs are minimised.
creativecommons.org/licenses/by/
4.0/).

Energies 2022, 15, 388. https://doi.org/10.3390/en15010388 https://www.mdpi.com/journal/energies

Energies 2022, 15, 388 2 of 38

In Part 1 of this paper, we reviewed the literature on the modelling of the FCC riser;
the current paper will present a similar analysis for the regenerator. The normal operating
conditions of the regenerator are shown in Table 1.

Table 1. Dimensions and Operating conditions of FCC unit [8–12].

Regenerator Dimensions
Height 30–40 m
Diameter 1–2 m
Operating Conditions
Gas oil inlet T 150–300 ◦ C
Catalyst inlet T 675–750 ◦ C
Catalyst exit T 500–550 ◦ C
Coke entering 0.5–1.5 wt%
Coke leaving 0.15–0.35 wt%
Pressure 200–400 KPa
Solid Residence ∼≤ 1 h

The literature on modelling the regenerator is vast and extensive. Because of the sheer
complexity of the unit, many papers published on the topic have taken different approaches
and to varying degrees of detail. Since much of the complexity in the system is a result
of the hydrodynamics, models of the unit have usually benefitted from advancements
in the modelling of cold flow bubbling and turbulent beds. Early work in this field was
aimed at understanding such beds, such as developments of two-phase theory by Toomey
and Johnstone [13]. This was followed by extensions to include the cloud and wake
phase and incorporation of downflow of solids at the wall of the bed through back-mixing
models [14–17]. These models were extensively used by various workers to model the
regenerator hydrodynamics [1,10,18–20]. The reaction kinetics of the chemical reactions
taking place in the regenerator has also been well studied and documented. Early work
in this field dates back to Arthur [21], who studied the rates of combustion of uninhibited
carbon in the form of graphite in air, establishing the existence of a temperature-dependent
ratio of carbon monoxide (CO) to carbon dioxide (CO2 ) produced when carbon burns in the
air. Subsequent work studied the rates of combustion of catalytic coke deposited in porous
alumina–silica particles, which were used as FCC catalysts in the 1960s [22–25]. Post-1970,
there was a change in FCC catalyst that saw the replacement of alumina–silica catalyst
by zeolitic catalysts. Subsequently, more kinetic studies using spent zeolite were published
measuring the rates of the combustion reactions in these then-new catalysts [26–28]. Both sets
of studies reported that the presence of some metals in the catalyst tended to affect the rates
of oxidation reported catalytically. Workers have routinely coupled the hydrodynamics
and the kinetics to produce regenerator models that can predict the conversion of coke and
emissions of gases from the system. Post-2000, driven by the increase in computational
power available to researchers and the need to understand the flow patterns involved in
the gas–solid flow of the regenerator, saw the explosion in the number of papers using
computational fluid dynamics (CFD) to simulate the regenerator [29–31]. These CFD
models seem to represent the highest conceivable amount of rigor that is possible for any
FCC regenerator model [18]. However, this current review is not concerned with CFD
models, but only the classical models that average flow over the reactor cross section to
produce one-dimensional (1D) or two-dimensional models (2D) is discussed here.
In Part 1 of this paper, we showed that there are already a few reviews of the FCC
modelling literature; however, a comprehensive review of traditional FCC unit modelling
approaches was found to be lacking in the literature. Of note was the lack of reviews
that link experimental findings of operations of FCC unit to the traditional modelling
Energies 2022, 15, 388 3 of 38

approaches and the simulation results obtained from said models. The current study
presents a review of the modelling of the regenerator and analysing the experimental data
that has led to the assumptions made in modelling. The modelling was divided in terms of
kinetics, where treatments of reaction rate equations, rate constants and orders of reactions
are considered, and in terms of hydrodynamics, where gas–solid mixing behaviour, flow,
heat and mass transfer in the reactor are considered. Phase description is explained in
the regenerator, and the issue of bubbles in the bed is also explained. In the end, the
deficiencies of current regenerator models are identified, and recommendations for further
work are made.

2. FCC Regenerator
2.1. Regenerator Kinetics
A review of the literature on the combustion of coke on the catalyst in a regenerator
reactor finds that there are generally four levels of complexity or considerations, i.e.,
(i) definition/composition of coke, (ii) rates and orders of reactions, (iii) the issue of
conversion of CO to CO2 and (iv) action from transition metals. All of these are discussed
below. The main aim of the regenerator is to burn off the coke-on-catalyst in order to regain
the activity of the spent catalyst. Additionally, the heat produced from these combustion
reactions is used to power the endothermic cracking reactions in the riser. Kinetic studies
in the regenerator are much simpler compared to that of the riser because, except for
coke, the reacting species are generally known, and therefore, it is easier to generate the
stoichiometric equations for the reactions taking place. This greatly simplifies the analysis in
kinetic studies. During normal operation of the regenerator, two main combustion reactions
occur: the combustion of coke and combustion of carbon monoxide that is produced via
incomplete combustion of coke [25,27,28].
It has been long known that coke formed during catalytic cracking reactions in an FCC
riser-reactor is a complex mixture of various chemical compounds, including hydrocarbons,
sulphuric and nitrogenous compounds [10,32]. The exact nature and composition of coke
have historically been difficult to ascertain, mainly because [33] (i) coke components are
largely involatile and complex in nature, (ii) components are strongly adsorbed to the
surface of the catalyst, and difficult to separate by conventional methods and (iii) coke
concentration on the catalyst is very low (< 1%), which leads to sensitivity issues during
characterisations. Nevertheless, several experimental techniques, such as elemental analy-
sis, temperature-programmed oxidation (TPO), Fourier transform infrared spectroscopy
(FT/IR), X-ray photoelectron spectroscopy (XPS), Thermogravimetric analysis, carbon-13
nuclear magnetic resonance (13 C NMR), supercritical fluid extraction (SFE) and mass spec-
trometry and Raman spectroscopy, have been used by researchers to understand the nature
and composition of coke better. Qian et al. [33] found chemical shift data in 13 C NMR
that distinguished between two types of carbon atoms in coke, namely aromatic (which
makes up 70–90% of the coke) and aliphatic carbons. They also found, after deconvolu-
tion of the C1s profiles in their XPS analysis, that carbon in the coke is primarily bonded
to hydrogen, and that the existence of nitrogen is in both polar and no-polar functional
groups. Nitrogen is typically present in the form of substituted polyaromatic compounds
such as pyrroles (= C–NH2 ), pyridines (–C–NC =) or anilines (= C–NH2 ). Elemental
analysis of Luan et al. [34] found that sulphur, present in the form of thiophene and thiols,
is also a major component of coke. All these studies confirmed the complexity of coke
in terms of structure and composition. However, for the purposes of modelling, in order
to predict the evolution of gases released from coke combustion in the regenerator, the
exact nature of the components of coke is not required as such an undertaking would be
greatly tedious but to very little utility. Generally, only the elemental composition of coke
is required. The relative elemental composition of coke is known to depend on the type
of gas oil feed used for cracking and the cracking catalyst; therefore, these compositions
are expected to vary depending on the specific operating parameters at a refinery [35]. It
is also common practice that nitrogen and sulphur are considered negligible since their
Energies 2022, 15, 388 4 of 38

molar composition is small compared to both hydrogen and carbon [1,32,36,37]. However,
recent results from FT/IR elemental analysis by Luan et al. [34] may question the validity
of this assumption as they have found spent catalyst to have a composition of 0.82 wt%
carbon, 0.32% nitrogen, 0.71 wt% hydrogen and 0.76% sulphur, from analysis of flue gas
emissions of the regenerator. These emission results show that both sulphur and nitrogen
may be significant for some feeds and need to be included in the model description of coke.
Another common assumption is the neglect of hydrogen so that coke is simplified to be
equivalent to carbon. Bai et al. [37] argued that the hydrogen reaction’s contribution to
combustion in the regenerator should not be ignored as the burning rate of hydrogen can
be up to two times that of carbon, and since the temperature is an important part of the
FCC unit, it is, therefore, necessary to include hydrogen in the coke. Hence, most models
of FCC units will model coke as CHn , where n is the molar ratio of hydrogen to carbon in
the coke. TPO studies of commercial spent equilibrium FCC catalysts by Bayraktar and
Kugler [38] showed that n ranges from 0.45 to 0.96 (depending on the catalyst used and
method of spent catalyst pre-treatment) for cracking of sour gas oil. This range is consistent
with the range of 0.4–2.0 given by Hashimoto et al. [39].
The coke combustion inside an FCC regenerator can typically be described using a
simple reaction scheme consisting of the following reactions in Equations (1)–(3):
 
β+2 n β 1 n
CHn + + O2 → CO + CO2 + H2 O (1)
2( β + 1) 4 β+1 β+1 2

1 homogeneous
CO + O2 → CO2 (2)
2
1 heterogeneous
CO + O2 → CO2 (3)
2
where n is the molar ratio of hydrogen to carbon in the coke and β is the molar ratio of CO
to CO2 . The subsequent oxidation of carbon monoxide is assumed to occur both on the
surface of the catalyst (heterogeneous) and in the gaseous phase (homogeneous), with the
reactions having different rates and hence the separate chemical reaction equations. Some
studies noted the independent oxidation of carbon and hydrogen in the coke, allowing for
the coke combustion equation to be split into two with separate equations for the oxidation
of hydrogen and carbon [25]. Furthermore, several workers only consider carbon in coke
and assume that the hydrogen is negligible [22,27,40]. Rate equations for the reactions are
developed using the simple power law, where the rate of the reaction is a product of the
kinetic parameter (given by the Arrhenius equation) and the concentrations (or partial
pressures) of the reacting species raised to some order, n. The purpose of the kinetic studies
is to determine kinetic parameter, which includes the frequency factor and activation energy
of the reaction and the orders of the reactions, which are all determined empirically from
fitting reaction model to experimental data. However, it was noticed early on by Weisz
and Goodwin that kinetic studies on the combustion of coke in porous catalyst particles
encountered some mass transfer effects that affected the apparent rates of reaction. Weisz
and Goodwin, in a series of publications [22–24], presented some significant work in the
combustion of coke in porous silica-alumina catalysts. Their work essentially defines two
modes, determined by temperature and the size of the porous particle, that control the rate
of combustion of the coke: (1) intrinsic chemical kinetics-controlled region and (2) diffusion
or mass transfer limited region. They report that for any sized particle, there exists a
temperature beyond which the rate of combustion is limited by how quickly oxygen can
diffuse to the reaction site. This is the type 2 combustion region. Below that temperature, the
reaction can be assumed to be in region 1. In this mode, the ‘true’ temperature-dependent
rate of reaction can be determined in the abundance of reactants. In order to achieve higher
conversions of coke in the regenerator, it is desirable that operating conditions are such
that no mass transfer limitations are present, which is the fundamental assumption made
by most researchers modelling the regenerator.
Energies 2022, 15, 388 5 of 38

Some of the early work on the combustion of carbonaceous deposits in the air was
made by Arthur [21]. This paper by Arthur presented yet another important factor in the
kinetic studies of combustion of the carbonaceous particle using analysis of evolved gas,
which is the difference between the global CO/CO2 ratio and the local ratio. The former
measures the ratio of the gases at the outlet, while the latter is concerned with the ratio
at the surface of the particle. At the surface of the combusting material, CO and CO2 are
produced via the reaction in Equation (1) at a certain β ratio, and subsequently, β decreases
due to the effect of reactions in Equations (1) and (2). Arthur [21] carried out combustion
experiments on two uninhibited carbon sources (artificial graphite and coal char) and used
Phosphoryl Chloride (POCl) to inhibit any further oxidation of carbon monoxide in order
to capture the local β ratio. They found that rate combustion was independent of the mass
of carbon present but proportional to the partial pressure of oxygen raised to a power less
than unity. They also concluded that the β ratio at the surface of combustion seems to be
uniquely determined only by temperature, provided the combustion has no mass transfer
limitations. The β they determined in their work is shown in Table 2. Although their work
was performed on uninhibited carbon, which is far from the combustion of coke trapped in
porous cracking catalyst, their results were nevertheless important to understanding the
intrinsic rates of oxidation of carbon in the air.
In the intrinsic chemical kinetics mode, Weisz and Goodwin [23] found that the
combustion of coke (i.e., carbon) in the porous alumina–silica catalyst was first order in
carbon. They found that there is only a single reproducible rate constant for this reaction
for any given temperature that was independent of the catalyst or source of the coke
used and that this relation followed Arrhenius type relationship with temperature. They
also reported that the coke combustion on Si–Al catalyst was similar to that of burning
behaviour of uninhibited graphite previously reported by Arthur [21], which they believed
suggested the existence of a basic, un-catalysed rate of combustion of carbonaceous deposit
in porous solids. Tone et al. [25] looked at the combustion of carbon and hydrogen in coke
separately and confirmed the first-order kinetics with respect to both, and to oxygen partial
pressure, for the combustion of coke on Si–Al catalyst. With the switch to zeolitic catalysts
in the FCC unit in the 1970s, some new combustions kinetics studies were carried out on
these then-new catalysts. These workers [27,28,41] confirmed the first-order kinetics of
combustions in terms of both carbon and hydrogen for coke on zeolite catalyst. The order of
reaction with respect to oxygen partial pressure (or concentration) is generally reported as
being first-order [25,26,28,41]. However, contrary to this, Arthur [21] reported that the rate
of combustion of graphite showed proportionality with oxygen partial pressure but raised
to a power less than unity. Although, as noted before, the worker in that study used POCl
to inhibit the subsequent oxidation of carbon monoxide due to incomplete combustion and
conceded that the POCl also has some inhibition effects on the carbon combustion reaction,
hence this may account for the discrepancy in the reaction order for oxygen.
Energies 2022, 15, 388 6 of 38

Table 2. Kinetic studies of FCC regenerator reactions.

homo het
Authors C + O2 →CO + CO2 H + O2 →H2 O CO + O2 → CO2 CO + O2 →CO2 Conditions and Fuels Burned Model/Correlation
Artificial graphite, coal char granules  
[21] 3
460–900 ◦ C
CO
CO2 = 103.4 × exp − 51,900
RT

−r4 = k4 PCO , −r3 = k3 nC PO2

−r2 = k2 nC PO2 , −r1 = k1 nC PO2
 
k1 = 1.63 × 106 exp − 152,900
RT (kPa−1 s−1 )
Coked silica–alumina catalyst   
[25] 3 3 3
467–560 ◦ C k2 = 424 exp − 107,000
RT kPa−1 s−1
  
k3 = 10.8 exp − 76,190
RT kPa−1 s−1
  
−1 −1 −1
k4 = 6.58 × 10−7 exp − 57,600
RT kmolkPa s gcat

d[CO] 0.5 0.5

− dt = k[CO ][O2 ][ H2 O ]
[42] 3 N/A 
k= 1.3 × 1011 exp − 125,000
RT m3 kmol−1 s−1

Coked Zeolite CDY, Alkaline ex-change

zeolites ( MgY, AlY ), Transition metal − dC = kPO2 C
 dt
[26] 3
 
exchanged zeolite (CrY, CoY, CuY ) k = 2.96 exp − 109,600 m3 kPa−1 s−1
RT
400–500 ◦ C
d(CO+CO2 )
dt = kCPO2
Coked Zeolites CRC-1, Y-7, Y-9
[27] 3  
600–800 ◦ C k= 2.75 × 103 exp − 161,000
RT m3 kPa−1 s−1
k C C
−rC = C Mr
C O2

Coked Zeolite catalyst C

[41] 3 3   
650–700 ◦ C k C = 1.4 × 108 exp − −125,000
RT m 3 kmol−1
Energies 2022, 15, 388 7 of 38

Table 2. Cont.

homo het
Authors C + O2 →CO + CO2 H + O2 →H2 O CO + O2 → CO2 CO + O2 →CO2 Conditions and Fuels Burned Model/Correlation
−rC = k C CC PO2
−rCO = 2k CO PO2 PCO
  
−1 −1
Coked OCTYDINE 1169 BR catalyst k C = 4.71 × 102 exp − 109,600
RT kPa s
[28] 3 3 3
620–720 ◦ C   
k CO 16
= 3.81 × 10 exp − RT 232,200
kmolm−3 kPa−2 s−1
 
β = 2.66 × 104 exp − 61,500
RT

1.3–6.1 kPa O2 partial pressure −0.64

 
[43] 3
Charcoal, graphite, coked FCC catalyst
CO
CO2 = 102.2 xO2
exp − 4000T±600
0.58±0.02
rCO = k CO Cc CO 2
0.68±0.02
rCO2 = k CO2 CC CO 2
Coked catalyst  
[44] 3 k CO = (1.1 ± 0.2) × 10 exp − 146,000
6
320–730 ◦ C RT
 
k CO2 = (3.0 ± 0.4) × 103 exp − 112,000
RT

Components: C—coke as carbon, H—coke as hydrogen, CO—Carbon monoxide, CO2 —carbon dioxide, H2 O—water vapour. Units: P—kPa, T—K, Activation energy—kJ.kmol−1 ,
x (mole fraction)—(-). Reactions: 1—C to CO2 —C to CO2 , 3—H to H2 O, 4—CO to CO2.
Energies 2022, 15, 388 8 of 38

The understanding of the oxidation of carbon monoxide to carbon dioxide is far less
straightforward, mostly because it is difficult to measure the concentrations of gaseous
products at the surface of the catalyst in the catalyst pores. It is generally accepted that this
oxidation occurs both heterogeneously (on the surface of the catalyst) and homogenously
(in the gas phase in the intra particle spaces or pores, and in the bulk gas phase); however, to
what extent each of these reactions is significant is not entirely clear. Early workers [45–49]
carried out studies towards the development of a global carbon monoxide burnout rate
in the gaseous form, in the temperature range 770–2400 K using a variety of fuels such as
propane and methane. Although their experiments are not directly on FCC regeneration,
they still present a good understanding of the homogenous carbon monoxide oxidation
reaction. Experiments were based on combustions of different types of fuel and in vastly
different conditions (temperature and pressure ranges), some experiments in the presence
of water vapour [49] and others in dry conditions [45,46]. There is general agreement in
this literature that oxidation is first order in carbon monoxide. Data across the literature
suggest there is some dependency on the temperature in the order with respect to water
vapour, with work in the region 770–1500 K [45] seeming to be in support of a half order
with respect to water vapour, and those in the range 1500–2400 K reporting lower orders of
zero or close to it. There is little agreement in the order of oxygen; Ghazal [50] reported
a value of 0.75. Other workers reported different values for the order of oxygen; 0.5 [45]
and 0.2 or 1 [49]. Howard et al. [42] collated data from various authors in order to define
a global carbon monoxide burning rate, and their results are reported in Table 2. They
note that their choices for orders for carbon monoxide and water are because these agree
with some of the previously published work. However, they also note that the value for
the oxygen order is only chosen because it performs no better or worse than any of the
other values reported in the literature. Nevertheless, Howard et al. [42] had confidence
in their kinetic rate equation because the data used to produce it were representative of
different types of burners, reactors, fuels, equivalence ratios, pressures and temperatures.
For the problem of ‘afterburn’ in the FCC unit, data collated by Howard and co seem
to suggest their rate equation is sufficient in describing the homogenous oxidation of
carbon monoxide. This is because significant deviations from this rate equations were only
observed beyond the 1500 K temperature mark, which is beyond the operating temperature
for modern FCC regenerators. In this regard, Howard proposed that the mechanism for this
reaction can be thought of as an equilibrium reaction involving free radicals of hydroxyl,
oxygen and hydrogen. On the other hand, studies conducted to measure this homogenous
condition under FCC regeneration conditions [25,41] reported that the overall contribution
of this homogenous reaction to the overall carbon monoxide oxidation in the regenerator is
negligible. In fact, Tone et al. [25] reported that they found no evidence for this reaction
when the reactor is operated at the same temperature and pressure while running carbon
monoxide and oxygen stream through the reactor in the absence of the catalyst.
Regarding the catalytic oxidation of carbon monoxide, Tone et al. [25] proposed a
reaction mechanism for the regeneration of coked Si–Al cracking catalyst involving the
parallel oxidation of carbon in the coke to both carbon oxides, followed by the oxidation
of carbon monoxide to carbon dioxide on the surface of the catalyst. They essentially
assume that the homogenous oxidation of carbon monoxide is negligible after it was
found that the concentration of carbon dioxide in the affluent gas stayed the same when
the combustion reactions are conducted without the catalyst present in the reactor. This
observation suggested that significant oxidation of CO only occurred in the presence of
catalysts particles, meaning only the heterogeneous oxidation is significant to the kinetic
study. This result is consistent with the work from Morley and de Lasa [51] which found
that of the two oxidations of carbon monoxide, the homogenous reaction was negligible
compared to the heterogeneous version. Tone et al. [25] reported the heterogeneous reaction
to be first-order in carbon monoxide partial pressure and independent of oxygen partial
pressure in the range 0.05–0.15 atm. On the other hand, Arandes et al. [28] also reported
rates for this reaction and confirmed that the reaction is first order in carbon monoxide;
Energies 2022, 15, 388 9 of 38

however, they reported an order of one with respect to oxygen partial pressure. It is worth
noting that the two workers reported similar values for the activation energy of the carbon
monoxide reaction, 57.6 kJ/mol [25] and 51.5 ± 0.5 kJ/mol [28]. The small difference is
likely due to the variations in the catalyst structure and transition metal composition. It was
demonstrated that oxides of transition metals such as copper and nickel promote catalytic
carbon monoxide oxidation [25]. This variability brought about by transition metal oxides
inevitably means that the rate equations and kinetic constants for this reaction will vary
across different studies, and therefore, it is difficult to produce a universal rate equation
for the FCC regeneration as FCC catalysts are widely different in their transition metal
content. The same problem is encountered when dealing with the rate equations for coke
combustion, as it was also shown that transition metals on the catalyst or in the coke could
catalyse the reaction to varying degrees [26].
Thus far, the kinetic studies discussed only involved models that describe the overall
conversion of coke to gaseous oxides without regard for the mechanism involved in the
conversions or the reaction intermediates. Several workers studied the rate of combustion
of unsaturated coke on FCC catalyst by explicitly including the carbon oxide complexes
formed on the catalyst surface in the reaction mechanism. These ‘surface complexes’ can
then transform to produce CO or CO2 . Generally, two types of such studies exist in the
literature [44]: the first is such that direct conversion of coke and oxygen to form surface
complexes, and the second uses the Langmuir-type model for dissociative adsorption. The
type of model used determines the forms of the rate equations. In the first case, the chemical
and rate equations (shown in Equations (4)–(6) may be written as follows [44]:
 
1 E0
C + O2 → C (O)∗ ; r0 = k0 exp − S∗ [O2 ]n0 (4)
2 RT
 
E
C (O)∗ → CO; r1 = k1 exp − 1 S∗ [O2 ]n1 (5)
RT
 
∗ 1 E2
C (O) + O2 → CO2 ; r2 = k2 exp − S∗ [O2 ]n2 (6)
2 RT
where S∗ is the molar amount of surface intermediate complex, C (O)∗ , and n is the reac-
tion order with respect to oxygen concentration. Equations (4)–(6) show one suggested
mechanism for oxidation; however, the exact mechanism has been debated for years in
the literature. Some of the main issues of contention are the formation, or lack thereof,
of C (O2 )∗ complex and whether or not the carbon oxides (CO and CO2 ) are formed as
primary products of coke combustion [43]. As a result, many workers developed kinetic
models that show alternative mechanisms for this coke oxidation reaction [43,52,53]. In the
Langmuir-type model, Equation (4) to form the carbon oxide complex is replaced by an
equilibrium reaction shown Equation (7), while the other reactions remain unchanged [44]:

2C + O2 ↔ 2C (O)∗ (7)

r1 and r2 (Equations (8) and (9), respectively), which are the rate equations for the
formation of CO and CO2 , respectively, can be written in the following forms [44]:
 h   i1
E1
k0 exp − ∆H
2
k1 exp − RT RT [O2 ]
r1 = h   i1 S∗ (8)
1 + k0 exp − ∆H
2
RT [O2 ]

 h   i1
k0 exp − ∆H
E2 2
k2 exp − RT RT [O 2 ]
r2 = h   i1 S∗ [O2 ]n (9)
1 + k0 exp − ∆H
2
RT [O2 ]
Energies 2022, 15, 388 10 of 38

where ∆H is the adsorption enthalpy, and everything else is as defined previously. These
two models described here have the advantage of incorporating the effect of adsorption
explicitly at the surface to the rate of oxidation, but this comes at the cost of an increase
in the number of parameters being estimated from experimental data. Kanervo et al. [44]
applied all three models described here to kinetic studies of spent FCC catalyst regeneration.
They found that all three models adequately described the coke oxidation experimental data
well, meaning no considerable advantage is gained from explicitly including the surface
complexes into the reaction scheme. This result also meant it was difficult to ascertain
which mechanism accurately described the system definitively; hence, this remains an open
question. However, for the purposes of FCC regenerator modelling, researchers seldom
use kinetic models that describe the formation of surface complexes, opting instead for the
simpler model described in Equations (1)–(3), which capture all the necessary information
without losing much accuracy.
Table 2 summarises some kinetic studies that are relevant to the modelling of the FCC
unit regenerator. In conclusion, the literature of kinetic studies related to the regenerator
is vast, and the main reactions occurring in the unit are well known. Generally, coke is
understood to be a complex mixture of carbon and hydrogen, based on its hydrocarbon
origins, with varying H/C ratios depending on feed. The coke combustion reaction is
generally believed to follow simple first-order kinetics with respect to both carbon and
hydrogen and with respect to oxygen. Carbon monoxide formed proceeds to be oxidised
to carbon dioxide both homogeneously and heterogeneously, but there is some debate over
which of the two carbon monoxide reactions is more important to the conversions of the
unit. Therefore, for completeness, both reactions can be used in the model. It is difficult to
compare various kinetic studies on regenerator reactions because some metals may catalyse
the reactions, and their varied composition in FCC catalysts results in varied kinetic
parameters. The rich literature in this area means that researchers are spoilt for choice when
it comes to choosing a kinetic scheme and kinetic parameters for their regenerator model.
However, it is important that the choice be based on the range of operating conditions in
which the kinetic model is valid and on the type of catalysts that are used in the study since
how well kinetic parameters extrapolate beyond their range of validity is not known, and
the effect of catalyst variations was already described.

2.2. Hydrodynamics of the Regenerator

2.2.1. Axial Profiles
Experimental data of axial profiles of solid holdup in an FCC regenerator from Kim
and Kim [3] are shown in Figure 1. The profile resembles an ‘S-shape’ profile with three
visible regions: (a) the region near the distributor which has a high volume of solid, (b) the
region at the top which has a small volume of solid, and (c) the short transition region in
between. The difference in the solid holdup between the top and the bottom of the bed
creates two discernible regions in the bed. The dense bed, region (a), consists of most of the
solids and gases, and the freeboard (or lean phase), region (b), consists of the gas leaving
the bed and the small fraction of solid particles entrained in that gas. Gases and particles
leaving the freeboard region are separated in the cycles at the top of the regenerator, where
catalysts are returned to the dense bed while the gas can leave the regenerator chamber.
Since the dense bed region is the region containing most of the solids and gas, it is generally
accepted that this is where most of the combustion of coke on catalyst takes place. For
modelling purposes, an understanding of the mixing and flow behaviour inside the dense
bed is required.
Energies 2022, 15, 388 11 of 38

Figure 1. Axial solid profile in FCC regenerator (redrawn from [3]).

2.2.2. Bubbling Behaviour

The FCC regenerator at normal operation with modern FCC catalyst particles is known
to occur in the bubbling/turbulent regime of solid–gas fluidisation [3]. The fluidisation
behaviour is known to be dependent on the physical properties of the solid particles, such
as size and density. Geldart and co-workers [54,55] provided a classification of particles
based on their fluidisation behaviour; this classification is the most widely used in the
field of gas–solid fluidisation. The FCC catalyst is classified as Group A particles [11,56].
This classification means that these particles are characterised by relatively small particle
size (30 ≤ dp ≤ 150 µm). These particles easily form bubbles that rise at velocities higher
than the emulsion gas velocity when fluidised. For group A particles, two velocities are
of significance in the bubbling bed region: Um f , the minimum fluidisation velocity, and
Umb , the minimum bubbling velocity. Determination of minimum fluidisation is generally
trivial, starting from a fixed bed of particles in a vessel with a porous base to allow the
fluidising gas to be pumped through the bed; the velocity of the gas is then increased
until incipient fluidisation occurs. The literature on the derivation of correlations for
minimum fluidisation velocity is vast [57–64]. Usually, correlations of Um f are derived
by dimensional analysis involving fluid dynamics dimensionless numbers such as drag
coefficient, Reynold’s number, Galilei number, Archimedes number related by to flow and
particle properties such as densities and particle size. The Um f literature is reviewed and
summarised elsewhere [65,66]. Several authors also provided correlations to describe the
transition of Group A powders at the minimum bubbling velocity [55,67–70]. The study of
the behaviour of bubbles formed in fluidised bed (beyond Umb ) has been of great interest
to many researchers. These studies produced great insights into gas–solid flow in FCC
regenerators during normal operation.
Additionally, evidence of the formation of bubbles in the dense bed in the regime
beyond Umb is seen from the X-ray studies [71–75]. Bubbles here refer to the voids or
pockets of air that are observed rising through the surrounding gas–solid emulsion. Stud-
ies that focus on the movement of isolated bubbles are usually the starting point in the
Energies 2022, 15, 388 12 of 38

understanding of bubble motion in the dense bed. These studies are divided into two:
(i) two-dimensional beds (formed from two thinly separated parallel-sided transparent
plates) and three-dimensional beds. Bubbles in two-dimensional beds were observed to
be shaped liked spherical caps, while bubbles in three-dimensional beds appear spherical
with indented bases [56]. Both studies show bubbles rising through the emulsion before
eventually erupting at the surface of the dense bed. This observation is important for mod-
elling because it establishes the inherent heterogeneity that is found in the dense bed for a
freely bubbling bed operating beyond Umb , so that this dense bed region can be thought of
as being made up of two distinct phases. Consequently, the famous two-phase theory by
Toomey and Johnstone [13] of fluidisation was developed to describe this observed flow
behavior, and it postulated that the two regions are the emulsion, which is the continuous
phase where the solid particles are found, and the bubble phase, which is essentially a
solid free void containing gas. According to this theory, the emulsion is static at incipient
fluidisation conditions while any gas in excess of that required for minimum fluidisation
travels through the bed in the form of bubbles. The theory provided a framework for
mathematically describing the flow in bubbling/turbulent beds and has been widely used
in the modelling of gas–solid beds in this regime, including the FCC regenerator. Further-
more, the tracer experiments of Rowe [76] provided great insights into the flow around
the rising bubble phase, showing a region of penetration of bubble gas into the emulsion;
this region is seen around the rising bubble and is clearly discernible from the bubble and
the emulsion phases. The distinct nature of this region meant it was hydrodynamically
different from the two phases described by the two-phase theory. This region was termed
the cloud. Additionally, these tracer experiments also showed that the indented base of the
bubbles is filled with a cluster or conglomerate of particles that are drawn by the bubbles
as they rise to the surface. This mechanism of particles being drawn by rising bubbles, as is
described later, has been identified as the prime mechanism for solid mixing in the bed [65].
This leads to the conclusion that an extra phase can be identified (i.e., the cloud and wake
phase) between the emulsion and the bubble, an observation that led to the bubbling bed
model by Kunii and Levenspiel [15]. Unlike in gas–liquid systems where the interphase
is a continuous film surrounding the bubble, no such film exists in gas–solid systems.
Bubbles are prevented from collapsing by pressure exerted on the particles by enclosed
gas; however, the interphase is permeable to gas [56]. The significance of this observation
for heterogeneous systems such as combustion of coke on the catalyst in the regenerator is
that gas in the bubble is not in contact with the solid or catalyst particles meaning bubbles
may lead to a significant bypass of gas. The transport of gas such as oxygen from within
the bubbles to the emulsion encounters resistance through the cloud–wake region on both
sides, i.e., at the interphase with the emulsion and with the bubble. Therefore, under certain
conditions, such as high superficial gas velocity, bypass is a likely phenomenon [56].
The velocity and size of the rising bubble are important parameters when modelling
the dense bed because, as was explained above, the large velocity of bubbles may result in
poor gas–solid contact and bypassing. Photographic studies of rising bubbles are quite clear
that bubbles are seen rising, and their size changes as they rise [77]. Two processes, which
occur in parallel for any freely bubbling bed, are responsible for the change in the size of
bubbles as they rise: (i) coalescence and (ii) bubble splitting. Coalescence is identified as the
main reason for bubble growth, the other being that the decrease in hydrostatic pressure
with height above the base of the dense bed; however, the effect of hydrostatic pressure is
assumed insignificant compared to coalescence [78]. Coalescence is a nucleation process
that occurs when two bubbles merge with one another to produce a bigger bubble, and it
was observed in two-dimensional beds. Evidence of coalescence in freely bubbling beds
is seen through the existence of two different bubble profiles at the top and bottom of the
dense bed; the top consists of a small number of relatively large bubbles, whereas at the
bottom of the dense bed, a large number of small bubbles is observed [56]. This suggests
that bubbles merge and grow as they rise. From this observation, several studies were
carried to correlate the size of the bubble to some operating parameters, such as the height
Energies 2022, 15, 388 13 of 38

of the bed above the distributor plate [71,77,79–85]. On the other hand, Rowe [86] observed
rising bubbles developing cusps on the roof and then subsequently splitting to form two
smaller bubbles. Usually, the smaller of the two bubbles are seen being reabsorbed, but
in some instances, especially for fine particles (diameter < 45 µm), the two bubbles then
continue to rise separately [11]. As a result of both the growth and splitting of bubbles
occurring simultaneously in the bed, Davidson and Harrison [87,88] theorised that there
must exist a limit on the size of the growing bubbles inside the bed. Basically, for a given
bed and flow conditions, bubbles rising in the bed will not grow past a particular size.
This theory is based on the assumption that as a bubble rises, the drag exerted by particles
moving downward relative to the bubble (in the surrounding cloud and emulsion phases)
sets in motion internal circulation currents of the gas within the bubble, and that velocity of
said circulation, Uc , approximates the bubble rise velocity, Ub . As Uc (∼ Ub ) increases, due
to coalescence, such that Uc > Ut (where Ut is the terminal fall velocity of the particles in
the bed), then the solids in the wake are drawn up inside the bubble resulting in splitting.
Therefore, the limit on the bubble size is reached when db corresponding to bubble rise
velocity equal to Ut is reached. An alternative theory to bubble splitting states that the
breakage of bubbles is primarily a result of the development of instabilities at the roof of
the bubble, allowing particles ahead of the bubble to fall through the void and divide it into
two [89–91]. It is not exactly clear in the literature which of these theories is correct, but it is
deductible that the likely reason for splitting is the entry of solid particles into the bubble
and that the best predictor of whether or not this occurs is the velocity of the rising bubble.
Since Ub is connected to db [92], these two properties of the bubble have been correlated in
experiments [72,73] so that bubble splitting can be predicted from bubble rise velocity.
Davidson and Harrison [88] drew similarities in the rise of air bubbles in liquid systems
to that of gas bubbles in gas–solid systems. They found that the famous [93] correlation in
Equation (10) for rising air bubbles in gas–liquid fluid beds predicted the Ub of an isolated
bubble in gas–solid systems reasonably well. The reason why this equation is valid for
solid systems is not clear. p
Ub = 0.711 gdb (10)
Sit and Grace [94] studied oxygen gas bubbles in two-dimensional beds and found that
bubbles in proximity affect each other’s rise velocities. They found that during the process
of coalescence, the trailing bubble in a pair accelerates towards the leading bubble until
the encroachment period. It is clear from this that the rise velocity of a swarm of bubbles
in a freely bubbling bed will be different from that given by Equation (10). Davidson
and Harrison [88] then proposed a theory that the average velocity of a bubble in a freely
bubbling bed is the sum of the velocity the bubble would have rising in isolation, see
Equation (10), plus the upward velocity of the particulate phase between the bubbles. This
is summarised in Equation (11).
q  
Ub = 0.711 gd p + U − Um f (11)

Equation (11) is widely used in reactor modelling and design [11]; however, its validity
has been questioned [84]. Other similar equations for bubble velocity in freely bubbling
beds were proposed by various workers [95–97]; however, there is little agreement between
them [56]. As a result, it is usually sufficient, at least in the initial stages of design, to
use Equation (11) for bubble rise velocity. Where a correlation for bubble size with bed
height is available, Equation (11) then gives the variation in the velocity of the bubbles in a
swarm with the height of the bed. Equations (10) and (11) show that the rise velocity of the
bubbles, either in isolation or in a freely bubbling bed, is correlated to the size of the bubble,
hence the multitudes of studies that have been devoted to producing these correlations for
different process conditions [92].
The issue of solid and gas mixing in the dense bed is also of significance, especially
for the purposes of modelling. Rowe [86] in Figure 2 showed the displacement caused
by the passage of a single bubble. Originally the bed contained two differently coloured
Energies 2022, 15, 388 14 of 38

materials of equal size and density profiles; the coloured substance originally occupied only
the bottom of the bed, with the white particles occupying the top. Rowe [86] reported that
the bed became fully mixed after the passage of 50 bubbles. Rowe and Partridge [72,73,76]
described two mechanisms as being responsible for this solid mixing behaviour in the
dense bed. Firstly, solids are carried in the wake of the bubble and subsequently ejected
at the surface of the bed and replaced by emulsion solids. Secondly, the drift mechanism
of bubbles draws up solids as they rise, leaving behind a finger of underlying material
(as seen in Figure 2). These two-mechanism are described as being the main mechanisms
in which particles move large distances in the dense bed and therefore inducing mixing.
Several other workers [98–102] all reported similar behaviour, with particles seen to be
moving upwards in areas of rising bubbles and downwards in areas of low bubbling.
Stein et al. [100] used positron emission particle tracing and a three-dimensional bed to
observe particle trajectories. They observed that particles move upward in the central region
of the bed (where most bubbling occurs) and downwards near the wall. This is consistent
with the radial bubble flow profiles reported by Werther and Molerus [103] that showed
high bubble flow in the central area of the bed and none at or near the walls. As a result
of this motion, good axial mixing of solids can be assumed. In contrast, evidence of poor
lateral mixing of solids was presented by Callcott et al. [104] using a rectangular bed. Poor
lateral/radial mixing of solids was also demonstrated through small lateral/radial solid
dispersion coefficients compared to the axial direction [105–108]. Callcott et al. [104] found
that solid tracers could be completely mixed vertically in 75 s at a fluidisation velocity of
3Umf , but complete mixing over the horizontal direction required about 1.5 h. The upward
motion in the centre and downward motion at the walls result in a circulation pattern that
is often referred to as a ‘Gulf Stream’ circulation. This ‘Gulf stream’ circulation of particles
can be influenced by flow nonuniformity at the distributor plate [109]. Differences in gas
distribution systems of industrial units mean that each unit can have its own preferred
flow paths, and therefore its own solid circulation and mixing characteristics. In summary,
for solids in the dense bed, axial mixing of solids is usually good enough that well-mixed
assumption in this direction is reasonable. However, this assumption may break down
when considering mixing in the lateral direction. The significance of this is that poor lateral
mixing may result in the creation of hotspots in the reactor along the radial direction.
Because most models that are 1-D are essentially averaged across the reactor area, they are
unable to predict these hotspots and therefore may lead to inaccurate predictions.

Figure 2. Displacement caused by a single rising bubble through a three-dimensional bed [86].
Energies 2022, 15, 388 15 of 38

2.3. Reactor Models for Bubbling Beds

Grace [110] emphasised the importance of the hydrodynamic factors (such as gas
distribution, bubble size, residence time distribution, phase division and interphase ex-
change, etc.) and kinetic factors (such as stoichiometry, reaction orders and kinetic con-
stants, etc.) to modelling of reactors. In order to predict the contact and flow inside the
FCC regenerator, the development of a model to describe the flow is required. Several
classifications for hydrodynamic models of fluidised beds exist in the literature. The famous
classification is by Harris and Davidson [111], who classify models into three categories, i.e.,
(i) models that predict the radial variation in solid suspension but not axial, (ii) models that
predict axial solid suspension but not radial and (iii) models that employ fundamental fluid
dynamic equations for two-phase gas–solid flow. Yates [56] classified models as (i) simple
or arbitrary models based on empirical correlations obtained from small-scale experiments
and (ii) models based on bubble dynamics that describe reactor behaviour in terms of
the known physics and hydrodynamics of fluid beds. Ultimately model classification is
difficult because the objectives of the classifications differ, and there is so much overlap
that it becomes a strenuous task to group them. For the present work, the classification
by Yang [78] based on phase description is employed. This is chosen here because this
classification is straightforward as balance equations are developed for each phase without
having to worry about what happens within the same phase. Phase description allows
mass, energy and momentum balances for each phase assumed present in the reactor to
be carried out, and therefore, the behaviour of properties of each phase can be predicted.
By this classification, three classes of models are identified; (i) homogeneous models, two-
phase models and three-phase/bubbling bed models. An extra class is discussed where the
phases in some regions cannot be assumed to be consistent with phases in the rest of the
dense bed.
The primary postulate of two-phase models is their treatment of gas division among
the two phases. As mentioned before, traditionally, it was assumed that all gas in excess
of that required for minimum fluidisation passed through the bed in the form of bubbles.
However, several investigators found that this assumption greatly overestimates the so-
called visible gas flow (or flow through the bed in bubble form) and underestimates the
flow of gas in the emulsion [71,112–114]. Rowe [115] showed that higher conversion
is achieved than predicted by conventional two-phase theory as a result of higher than
predicted interstitial gas flow. As a result, corrections are usually employed to account for
this deviation from the ideal two-phase flow. The commonly used corrections are in the
form [112] as seen in Equations (12) and (13):
 
ε b Ub = Y U − Um f (12)

Ub = (U − Ub )(1 + kε b ) (13)
where Y and k represent the deviation from the ideal two-phase flow. The primary differ-
ence between bubble velocity predicted by Equations (12) and (13) to that predicted by
correlations such as that shown in Equation (11) is that the former only predicts bubble
velocity using Um f and makes no reference to bubble size. It is reasonable to assume that
the latter would be more representative of the real system as they are capable of predicting
acceleration caused by bubble growth. Nevertheless, both types of correlations have been
used in modelling bubbling beds in the literature.
One of the earliest two-phase models was by Davidson and Harrison [88]. It made
the following assumptions: (a) gas in emulsion at Um f and is either well mixed or plug
flow, (b) bubbles exist through the bed with uniform size and (c) interphase gas exchange
is by diffusion and through flow between emulsion and bubbles. Although this model
agreed well with some experimental data, it has been criticised for its simplistic definition
of the gas–solid bubble and was later updated by other workers [56,116] to account for
bubble growth in beds of fine particles. Since then, more work has been published using
this model to account for axial gas dispersion.
Energies 2022, 15, 388 16 of 38

Kunii and Levenspiel’s [15] bubbling bed model is one of the earliest incorporations of
the cloud and wake region. The assumptions of this model are: (a) most reactant gas travels
up the bed in uniform size bubbles surrounded by cloud and wake, and interstitial gas
flow is negligibly small in comparison, (b) plug flow in bubble phase, and (c) interchange
between emulsion and bubble phase is through the cloud and wake, through two resistances
to transport. As with the previous model, many variations in the bubbling bed model now
exist in the literature to account for such things as the gas flow through the emulsion, the
growth of bubbles up the bed and the dispersion of gas up the reactor. Such models include
Stephens et al.’s [16] counter-current back mixing model, which updated the bubbling bed
model by including emulsion phase back mixing, downflow of solids during circulation
and linear increase in bubble diameter. Kato and Wen’s [17] model updated the bubbling
bed model by assuming bubble size growth is given by a correlation and that bubble
and emulsion phases in the bed are represented by a series of well-mixed tanks whose
heights are equal to the bubble diameter corresponding to that vertical position above
the distributor.
Grid enhanced models vary from the above models in that the region near the dis-
tributor is considered to show a different flow pattern to the rest of the bed. It is assumed
gas penetrates the bed in the form of jets [117]. Photographic studies of the grid region
showed that the term ‘jet’ refers to a variety of flow patterns near the gas inlet, such as elon-
gated cavities forming above the orifice and leaving as bubbles [118], plumes developing
necks which divide into a series of bubbles [119], chains of bubbles emanating from the
orifice [120] and permanent flame-like dilute phase regions penetrating into the bed [121].
In their model, Behie and Kehoe [117] made no distinction between these flow patterns
and assumed that these jets could generally be taken as plug flow in the axial direction
and perfectly mixed radially/laterally. The jetting effect is thought to produce enough
turbulence in its vicinity that the phase surrounding the jet is assumed to be a well-mixed
emulsion. Of course, some variations to this jet transport model near the grid exist, for
example, the tubular jet model [122] and the sink and source model [123,124]. The jet
penetration height (referred to as h in Table 3) was also studied in detail and correlations
exists to find it. Davidson et al. [65] reviewed and published some of this literature in
their book.
In the general case, the energy balance for the system (in Equations (14) and (15) could
be written for each phase, assuming a two-phase flow model:
Bubble phase:

∂(ε b hb ) ∂(ε b Ub hb )
ρb + ρb = ∆Qreaction + ∆Qbe + Sb (14)
∂t ∂z
Emulsion phase (for a well-mixed emulsion with thermodynamic equilibrium):

∂(ε e he )
ρb = ∆Qreaction + ∆Qeb + Se (15)
∂t
where the ε b and ε e are volume fractions of the bubble and emulsion, respectively, hb and he
are the specific enthalpies of the bubble and emulsion phases, respectively, ∆Qreaction is the
heat of reaction in the phase which depends on the rates of reactions and their associated
heats of reaction, ∆Qbe and ∆Qeb are the heat exchanges between the bubble and emulsion
phases, respectively, which depend on the heat transfer coefficient between the two phases,
the interphase area and the temperature difference between the phases. Sb and Se are the
energy source/sink terms in the bubble and emulsion phases, respectively.
Energies 2022, 15, 388 17 of 38

Table 3. Classification of reactor hydrodynamic models for FCC regenerator type Fluidised beds.

Model Classification Description Governing Mass Balance Equations

This model was first proposed by Toomey and Johnstone [13]. It
draws from the observations of bubbles rising in bubbling beds and
Two-Phase Flow Models postulates that two phases in the bed exist, i.e., the emulsion and the
bubble phase. According to the original theory from Toomey and
Johnstone, the emulsion phase is at minimum fluidisation conditions
while any gas through the distributor plate in excess of that required For emulsion gas:
for incipient fluidisation passes through the bed in the form of 2
− D Ae ∂ ∂zC2Ae + Ue ∂C∂zAe + Kbe (C Ae − C Ab ) + R Ae = 0;
∂C Ae
bubbles (i.e., the bubble phase). Each phase is represented by a mass ∂t
For bubble phase:
balance equation, and an interchange term is included in each ∂C Ab ∂2 C Ab ∂C Ab
equation for transfer between the phases. If more than one component ∂t − D Ab ∂z2 + Ue ∂z + Kbe (C Ab − C Ae ) + R Ab = 0;
is present in the phase, i.e., a mixture of gas in air bubbles, separate For plug flow D A = 0, and for well-mixed flow D A = ∞, for
equations are written for each phase. dispersion model D A is defined.
Generally, gas flow in the bubbles is assumed to be plug flow, while
gas flow in the emulsion is assumed plug flow or well-mixed [78].
However, non-ideality of flow in dense beds is likely, so models can
replace traditional ideal flow with dispersion models, tanks in series
and residence time distribution models.
Bubbling bed Models or Cloud and Wake Models

These models are an extension of the two-phase models. They were Assuming flow through the bed only in the bubble phase
first proposed by Kunii and Levenspiel [15,125,126] to account for the (reasonable at high gas superficial velocities), mass balance
cloud and wake regions that were seen from X-ray imagining studies equations are as follows [78].
[72,73]. This consideration of the cloud–wake phase adds extra
resistance to mass and heat transfer between the emulsion and the   Bubble phase:
dNAb
− V1b = R Ab + Kbc (C Ab − C Ac );
bubble phase. There is bubble→cloud resistance and cloud → dt
emulsion resistance. These models are usually governed by these Cloud–wake phase:
assumptions: (a) bubbles are uniform in size and evenly distributed, Kbc (C Ab − C Ac ) = R Ac + Kce (C Ac − C Ae );
(b) flow in the vicinity of the bubble follows the Davidson [88] model Emulsion phase:
and (c) emulsion stays at minimum fluidisation velocity. Kce (C Ac − C Ae ) = R Ae ;
Energies 2022, 15, 388 18 of 38

Table 3. Cont.

Model Classification Description Governing Mass Balance Equations

These models differentiate between different regions in the
regenerator dense bed; for example, it was described above that
imaging studies showed that bubbling behaviour in the region near
the gas distributor plate (large number of small bubbles observed) is
different from the behaviour at the top of the dense bed (small number
of large bubbles observed). Furthermore, it was also observed that For the grid region, i.e., 0 ≤ z ≤ h at steady state.
changing only the gas distribution plate in a reaction system leads to Gas in the jets: 
different conversions in the reactor [117,127]. This evidence led Behie ∂C
Uj ∂zAj + K je C Aj − C Ae = 0;
and Kehoe [117] to propose the Grid effect model, which treats the
region of the bed near the distributor plate differently from the rest of GasR in the emulsion: 
h
Multiple Region Models the dense bed. From this proposition, the grid region may be modelled Ue (C Ae0 − C Ae ) + 0 K je C Aj − C Ae dz + R Ae = 0;
differently, while either one of the previous models is used to describe This model predicts that the transfer coefficient K je is 40–60 times
the rest of the bed, with jets assumed to lose momentum and break off the value of the coefficient between bubble and emulsion phase (i.e.,
into bubbles [65]. According to the original model from Behie and Kbe ) [78]. This result is expected since the bubble formation profile
Kehoe, gas enters the bed through the distributor in the form of near the grid is shown to favour more turbulence (and therefore
high-speed jets that penetrate the emulsion to a distance h before better mass transfer) in this region than in the rest of the dense bed.
bubble formation is observed. This region between the distributor and
the part of the bed up to h is considered the grid region. Jets are
assumed to cause turbulent mixing of the emulsion, and hence
emulsion is assumed perfectly mixed, while the jets are assumed
perfectly mixed laterally/radially and plug flow in the axial direction.
Energies 2022, 15, 388 19 of 38

The other class of hydrodynamic reactor models not included in Table 3 are the
pseudo-homogenous models that make no distinction between the emulsion phase and
the bubbles passing through it. These models, therefore, do not have any division of gas
in the dense bed and often employ simple mixing models such as plug flow, well-mixed
tanks, tanks in series and dispersion models for gases and solids mixing in the bed [78].
Ultimately, within this framework of model classes, there is a lot of flexibility in that
simulation engineers have the ability to choose between different alternative assumptions
for (i) phase description in the dense bed (i.e., emulsion–bubble, emulsion–cloud–bubble or
pseudo-homogenous), (ii) mixing characteristics for gases and solids in the bed (i.e., plug
flow or well-mixed or dispersion model) and (iii) the heat and mass transfer resistance
between phases (i.e., direct transfer between emulsion and bubble, or transfer between
emulsion and bubble via cloud phase). This flexibility has inevitably resulted in a wide
variety of unique models for modelling bubbling bed reactors in the industry. Table 4 shows
a review of FCC regenerator models published between 1990 and 2020 in terms of kinetic
modelling and hydrodynamics described in this work. We have attempted to summarise
the variety of model assumptions in Figure 3 based on the review in Table 4. Generally, it
can be seen that the model complexity of bubbling/turbulent beds with significant bubbling
activity is based upon the distinct phases present in the bed. For two-phase models, the
gas division is an important parameter since it determines the flow rate of gas through the
two phases. Clearly, the two-phase model in its original postulates has proven inadequate
in the prediction of gas division, but it is nevertheless a good starting point for most bed
designs. Another consideration for some beds is the existence of different regions in dense
beds, with the region near the distributor having some obvious hydrodynamic differences
from the rest of the bed, hence requiring separate treatment in the model. However, this
effect is usually negligible except in shallow beds. The simplest models will ignore the
existence of different phases and regions in the bed, assuming pseudo-homogeneous flow
in the reactor, although the current literature suggests these models have been phased out
as they fail to predict the heterogeneity that is important to reactor performance.

Figure 3. Summary of Regenerator modelling and key hydrodynamic assumptions.

It is shown in Table 4 that the description of coke used in the FCC regenerator is that of
coke modelled as pure carbon, or coke modelled as a hydrocarbon mixture with empirical
formula CHq , where q is the molar ratio of hydrogen to carbon, ranging from 0.4 to 2.0, as
shown by Hashimoto et al. [39].
Energies 2022, 15, 388 20 of 38

Table 4. Review of FCC Regenerator models.

Dense Bed
Freeboard
Investigators Kinetic Model Description Hydrodynamic Model Description
Coke Definition Reaction Rates Model Class Emulsion Bubble Kinetic Hydrodynamic
Coke burning by Kunii and Perfectly mixed
Bubble phase is plug
[36] C Levenspiel [14]. Two-phase emulsion for both N/A N/A
flow.
No bubble phase reaction. solids and gases.
Complete and Incomplete coke Well-mixed bubble
burning kinetics from de Lasa and Grid effect model with Well-mixed emulsion phase.
[128] CH0.7 N/A N/A
Errazu [129,130]. two-phase dense bed. for solids and gases. Single uniform value of
CO oxidation ignored. bubble size defined.
Complete and incomplete C Grid effect model with a
burning, H burning, homogenous Two-phase bubbling region. Well-mixed emulsion
CHn Plug flow bubble phase.
[131] and heterogeneous oxidation of Grid region has a fully for both solids and N/A N/A
0.83 ≤ n ≤ 1.67 Bubble size not defined.
CO with kinetics from mixed zone and a dead zone gases.
Faltsi-Saravelou and Vasalos [132]. in series.
Coke burning, homogeneous and Well-mixed emulsion
[19] C heterogeneous CO oxidation Two-phase for both solids and Plug flow bubble phase. N/A N/A
kinetics as defined by [41,51]. gases.
Studies [22–24] for coke
Tubular reactor for
combustion. Only
Well-mixed solids. bubble phase.
Study [26] for homogenous CO homogenous Two-phase
[10,18] CHn Two-Phase Tubular reactor for Used [11] correlation for
oxidation. afterburn tubular reactor.
gases. bubble size with axial
[133] for heterogeneous CO considered.
level.
oxidation.
Complete and incomplete coke
All dense bed Plug flow for
CHn burning, homogeneous and Well mixed for both Bubble is well mixed.
[134] Two-phase reactions both solids and
n not defined heterogeneous CO oxidation with solids and gases. Bubble size not defined.
considered. gases.
kinetics as defined by [1].
Energies 2022, 15, 388 21 of 38

Table 4. Cont.

Dense Bed
Freeboard
Investigators Kinetic Model Description Hydrodynamic Model Description
Coke Definition Reaction Rates Model Class Emulsion Bubble Kinetic Hydrodynamic
Carbon burning and CO
heterogeneous combustion Well-mixed tanks for
kinetics by [136]. both solids and gases
[135] CH0.8 Pseudo-homogeneous N/A N/A N/A
Hydrogen burning kinetics by [27]. in each of the R2R
Homogenous CO oxidation regenerators.
kinetics by [137].
Well-mixed emulsion Bubble phase is plug
Coke burning and CO oxidation
[138] C Two-phase for both solids and flow. N/A N/A
kinetics from [41].
gases. Bubble size not defined.
Complete and incomplete coke
burning, homogeneous and Phase is well mixed All dense bed Plug flow for
[139] CH1.18 heterogeneous CO oxidation all Pseudo-homogeneous for solids. N/A reactions both solids and
considered, but kinetics source not Gases in plug flow. considered. gases.
clearly stated.
All dense bed
Reaction scheme as defined by Well mixed for solids. Plug flow for bubble Not defined
[20] CHn Two-phase reactions
[10,18]. Plug flow for gases. phase. explicitly.
considered.
Only Plug flow for
Coke combustion, homogenous Well-mixed phase for
homogenous gases.
[140] C and heterogeneous oxidation as Pseudo-homogenous both solids and N/A
afterburn No catalyst in
defined by [1]. gases.
considered. freeboard.
Energies 2022, 15, 388 22 of 38

Although the homogenous carbon monoxide oxidation was generally found to be

negligible compared to the heterogeneous version, such as in the work of Morley and
de Lasa [51], both reactions were included in models of the FCC regenerators to varying
degrees. This allows models to be subdivided into three categories with respect to CO
oxidation: (1) models that consider only the heterogeneous reaction [138], (ii) models that
consider only the homogenous reaction and (iii) models that consider both reactions [1,10,140].
Models that ignore the post-combustion CO oxidation reactions completely, such as [36],
were generally phased out, which shows the significance of these so-called afterburn
reactions. Ultimately, the level of detail included in the kinetic model depends on the
end-use of the model and the accuracy required. In recent times, with stricter regulations
surrounding emissions, it is advisable to include all the important reactions so that more
accurate predictions of emissions can be made.
Models increase in complexity from homogeneous to two-phase models to grid effect
models. Table 4 shows that the simple pseudo-homogeneous models are seldom used
to model FCC regenerators. One reason for this is that pseudo homogeneity in fluidised
beds is usually observed at a smooth fluidisation regime, and the homogeneity decreases
towards the turbulent regime. In the bubbling/turbulent regime, the bubbles rising through
the bed are seen dispersed in the ‘continuous phase’ or emulsion, indicating that the flow
mixture is highly non-homogeneous. Comparative studies were conducted to compare the
performance of hydrodynamic models of the FCC regenerator. Lee et al. [32] compared
three different models for describing the FCC regenerator, namely the grid effect model,
the two-phase model and the bubbling bed model, and compared the simulation results
to data from a working refinery FCC unit. They found that the bubbling bed model gave
the smallest error in relation to the coke conversion and exit catalyst temperature plant
data when the emulsion is considered perfectly mixed for solids, and the dense bed and the
freeboard are assumed two thermally uniform stages in series for heat balance. However,
they have noted that although the bubbling bed outperformed the two other models, it
still was not an exact description of the regenerator. The work of Lee et al. [32] has given
results that suggest that the grid effect model is generally more suited for shallow beds
(where DL ∼ 1) as it was originally developed for such cases [117]. This is in line with the
review in Table 4 that shows that only a few researchers have used this model to simulate
the regenerator. The more perplexing observation from Table 4, in light of the results
from Lee et al. [32], is the limited adoption of the bubbling bed model as opposed to the
two-phase model, which was outperformed by the former in terms of both coke conversion
and catalyst outlet temperature. One reason for this could be that the two-phase model is
much simpler and less computationally expensive. Another reason is that the complexity of
the model used is very much linked to the purpose of the model. Models used in the initial
design stages are usually shortcut and simple models, whereas control and optimisation
models can generally be more involved.
Another issue of note is the treatment of emulsion phase gas mixing or flow. Grace [141]
noted that no other feature in fluidised bed reactor modelling has been subject to as many
alternative assumptions as the axial mixing of emulsion gas. Table 4 shows that in terms of
modelling the FCC regenerator, the behaviour of emulsion phase gas remains unresolved.
The assumption for gas in emulsion alternates between well mixed and plug flow in the
axial direction. For comparison, Table 4 shows there is some consensus in assuming gas
in the bubble phase is plug flow while particles in the emulsion are assumed well mixed.
This assumption of plug flow in the bubbles is consistent with the experimental evidence
discussed, which suggested that gas starts to deviate from plug flow when solids are intro-
duced to the flow. Because bubbles are assumed to be essentially solid-free, the plug flow
of gas is reasonable. However, the emulsion is different because both gas and solids are
present in the suspension. While both plug flow and well-mixed assumptions have been
used with great utility when describing gas in the emulsion, they are two different flow
patterns and therefore mean the understanding of gas mixing in the emulsion as an open
question. Levenspiel [142] thoroughly reviewed the problem of emulsion phase gas mixing
Energies 2022, 15, 388 23 of 38

in bubbling fluidised beds. They compared results from thirty-nine experiments conducted
on group A-type particles by five different reactor groups in various flow reactors, where
the extent of conversion was measured during the experiments. They conclude that gas
flow in the dense bed cannot be modelled using simple plug flow or well-mixed flow
models, and in some cases, these assumptions can be highly inaccurate. Of interest is
that parameters can be adjusted in the models so that both sets of assumptions produce
results that match measured reactor outlet temperatures, and this is usually sufficient for
industrial purposes. The downside is that conditions such as conversion within the dense
bed cannot be definitively predicted. Nevertheless, it usually does not affect the exit results
which description of emulsion gas is chosen, and until such a time when experiments were
conducted to study gas mixing conclusively, this will remain an unsolved aspect of FCC
regenerator modelling.
Treatment of bubbles in the bed is also poorly addressed in the regenerator, as can
be seen, that many workers of two-phase models have not clearly defined the bubble size
or have provided insufficient information for this detail to be discernible to the reader.
It may be that this parameter was accounted for in their models but not published in
their papers, or it was not treated at all. Workers that properly accounted for bubble size
either used a Davidson theory type assumption with uniform bubble size through the
bed [128,132,143] or used a correlation for bubble size with height to account for bubble
growth through the bed [10,18]. Levenspiel [142] showed that bubble size, for a uniform
bubble description in a bubbling bed model, does affect the conversion through the bed.
This is consistent with the earlier work [132], which studied the effect of bubble size on
oxygen exchange between the emulsion and bubble phase. They reported that smaller
bubbles (in the range 5–10 cm) increased the interchange of oxygen between the emulsion
and bubble phase resulting in more oxygen being carried to the reacting catalyst surface
in the dense bed, while larger bubbles (≥ 20 cm) resulted in lower oxygen interchange
and lower coke conversion. Faltsi-Saravelou et al. [132], however, have not addressed the
issue of bubble growth through the bed. Nevertheless, a proper description of bubble size
needs to be incorporated into dense bed models employing either two-phase or bubbling
bed models.

2.4. FCC Regenerator Performance Predictions

Several studies of FCC regenerator modelling have provided simulation results for
the axial distribution of gas in the regenerator, the temperature in the bed and the coke
conversion. Some of these results are presented in Figure 4 and discussed.

Figure 4. Cont.
Energies 2022, 15, 388 24 of 38

Figure 4. Comparison of predictions from FCC regenerator models in the literature against
plant/experimental data for (a) axial profiles of carbon dioxide, (b) axial profiles of oxygen, (c) axial
profiles of water vapor and (d) axial profiles of temperature, along the regenerator. Predictions
from [18,131,132,134], and plant/experimental data from [19,132,144].
Energies 2022, 15, 388 25 of 38

As can be seen, the plant data used here can be divided into two; one where only
the exit conditions are reported and the other where conditions along the regenerator
are reported (i.e., temperature readings along the regenerator [132]). Figure 4 shows
that the exit gas compositions from simulations generally agree well with plant data.
However, profiles of gas compositions vary along the riser depending on the flow and
mixing pattern assumptions in the dense bed. In Figure 4a,b simulations from Jober
et al. [134] show uniform gas composition in the dense bed while simulations from other
workers [18,131,132] show gas profiles increasing for carbon dioxide and decreasing for
Oxygen with the height of the dense bed. This is because the former has assumed well-
mixed conditions for gases in the dense bed while the latter has assumed plug flow
conditions for gases in the dense bed. For data with plug flow gas conditions in dense
bed, there is a steep increase (for CO2 and H2 O) and decrease (for O2 ) in the initial stages
of the dense bed with the rate decreasing with height. This is because compositions of
oxygen from the inlet air are higher in the initial stages of the dense bed, which promotes
faster combustions reactions in this region, and as oxygen is used up in air reaching the
freeboard, the rates of combustion are lower in this region, and hence only small changes
occur in this region. The data and simulations report matching exit flue gas compositions
of 15–20 mol% carbon dioxide, 0–5 mol% oxygen and 0–0.2 mol% carbon monoxide. There
is a larger discrepancy in plant and simulation results for exit flue gas composition for
water vapour. Simulations appear to overestimate the amount of water vapour released
from the regenerator. The likely cause of this discrepancy lies in the hydrogen composition
in coke (i.e., the moles of hydrogen per mole of carbon in coke). This quantity was proven
to depend on the quality and type of gas oil feed used in the riser reactor, meaning some
feeds produce coke with higher hydrogen content, therefore corresponding to higher water
vapour composition in the regenerator flue gas. The moles of hydrogen per mole of carbon
in coke from catalytic cracking of gas oil were reported to vary between 0.4 and 2.0 [32,39].
Simulations of workers [131,132,134] showed that the CO composition leaving the dense
bed is higher than zero, but this CO is almost always converted into CO2 by the time it
reaches the regenerator cyclones in the freeboard. This ‘afterburn’ reaction demonstrates
the importance of including the freeboard in the FCC regenerator model. de Lasa and
Grace [145] also demonstrated that the freeboard is also important because of the influence
of the recycling of catalyst particles on coke conversion.
Figure 4d shows the variation in temperature with the height of the regenerator
for single regenerator units. Plant data from Faltsi-Saravelou et al. [132] showed that
temperature in the regenerator quickly increases in the first 20% of the unit. The initial low
temperature is from the mixing of the catalyst with cooler lifting air. The steep increase at
the bottom is from combusting reactions releasing exothermic heat that heats up the catalyst
and the air flowing throw the bed. Higher up the bed increase in temperature is very small
because there are reduced reactions in those oxygen lean regions. The temperature in the
dense bed is one of the most important variables in the regenerator because heat from the
‘clean’ catalyst is going to be used to provide energy for the endothermic cracking reactions
in the riser reactor. Some researchers [19,29,144,146] reported commercial regenerator
dense bed temperatures of 907–1040 K. In each case, the difference between dense bed and
freeboard temperature is between 3 and 40 K. These data are consistent with simulations
results shown in Figure 4d [18,134]. The final temperature in the dense bed is determined
by the initial weight fraction of coke on the catalyst, the temperature and flow rate of air
through the bed, the catalyst circulation rate and the height of the bed. It is important
to note that the temperature description so far has not made a distinction between the
temperature of the catalyst and the temperature of the gas; thus far, it was assumed that
the temperature is the same. However, as with mass transfer, a resistance in heat transfer
between the emulsion and the bubble phase exists, which means that at any height above
the distributor plate, the two phases will have different temperatures. Very little data
showing this difference have been reported in the literature and in conversion simulation
studies, such as those discussed in this paper. Similar to the lack of plant/commercial data
Energies 2022, 15, 388 26 of 38

about axial profiles of gas composition in the regenerator, the reason for this is likely linked
to the difficulty of making these measurements during the normal operation of the unit.
However, regenerator models employing computational fluid dynamics (CFD) tackled this
problem correctly [29–31,62,147].

2.5. Shortcomings and Future Recommendations

The following shortcomings were identified from the review of FCC regenerator models:
(a) Axial mixing: Table 4 shows that the mixing of solids and gas in the bed is usually
assumed to be either plug flow or well mixed in the axial direction. Considering the
results from Callcott et al. [104] that showed that tracer solids could be completely
mixed in the axial direction in 75 s, and also noting that the characteristic residence
time for solids in the FCC regenerator is in the range of minutes to an hour (see Table 1),
then it is totally reasonable to assume complete mixing for solids in the axial direction.
However, gas mixing is more complex, as was explained earlier. It has now been
established that the motion of bubbles up the bed causes a rise to circulation patterns
of solids in the bed so that solids are moving up the bed in bubbling regions and
moving down the bed in regions of low bubbling activity. It was suggested by several
workers [16,148] that the regions of downflow of solids drag down the interstitial gas
so that downflow of gas is possible in the bed. Stephens et al. [16] suggested that the
downflow of gas occurs when the downflow velocity of solids exceeds the velocity
of rising emulsion gas. Consequently, this is what has led to back-mixing models
for bubbling fluidised beds. The review in Table 4 shows that back-mixing models
and their applicability to the FCC regenerator has yet to be explored, and since it has
been clear from Levenspiel [142] that plug flow or well-mixed assumptions do not
accurately predict gas mixing in the dense bed, it is worth exploring back-mixing
models for their performance in describing gas flow in FCC dense beds;
(b) Radial mixing: According to Grace [141], knowledge of lateral/axial mixing can be
far more important than axial mixing in predicting the performance of fluidised units.
The FCC regenerator models reviewed in Table 4 are all 1-D models that assume
perfect axial mixing of both solids and gases so that any variation that occurs is only
in the axial direction. It was described [104] that solids mixing is poor in the lateral
(or radial) direction and that complete mixing is only achieved in the time scale in the
order of 1.5 h, which exceeds the normal time scale for the residence time of solids in
the FCC regenerator (see Table 1). Therefore, it seems unreasonable to assume perfect
radial mixing of solids in the regenerator. In order to understand lateral/radial solid
mixing better, a lateral dispersion coefficient was used to encompass all the solids
mixing processes identified by Rowe and other workers [72,73,149] i.e., emulsion drift,
bubble wake lift and bubble eruption scattering. Determination of the dispersion
coefficient was generally performed in two ways; (i) a diffusion-type [101,150], where
experimental data are fitted to a model that is based on the analogy that solid particles
behave similar to gas molecules travelling in a continuous isotropic environment,
and (ii) a stochastic-type model [105,151,152] that assumes a solid particle in a bubble
induced mixing cell can randomly jump between adjacent mixing cells, and that this
jumping is governed by a probability distribution. There has been some success in
using these dispersion models, especially in the fields of bubbling fluidised gasifica-
tion and combustion of coal and biomass, but so far, there is limited literature on their
application for FCC regenerator modelling;
(c) Emissions: in the last three decades, there has been increased scrutiny and regulations
on the anthropogenic emissions of GHGs, such as CO, CO2 , SOx , CH4 and NOx ,
case in point the Kyoto Protocol of 1997 [7] and the Paris Agreement of 2015 [5].
European countries will report their greenhouse gas emissions reductions as per the
approved United Nations Framework Convention on Climate Change (UNFCCC)
transparency framework as well as the Intergovernmental Panel on Climate Change
(IPCC) methodology guidelines [153]. The reason for such global actions is the
Energies 2022, 15, 388 27 of 38

influence of human-made emissions on climate. Fossil Fuel emissions, of which the

emissions from the FCC regenerator are a part of, were reported to account for 87% of
all the carbon (i.e., CO, CO2 , CH4 etc) emissions from anthropogenic sources [154].
Therefore, the ability to predict the emissions of GHGs from the FCC unit is of
importance towards the global goals of mitigation of climate change by a reduction
in anthropogenic emissions. The current generation of FCC regenerator models
(discussed in Table 4) can predict the emissions of carbon-based GHGs because coke
burned in the regenerator unit is described as CHn . However, since other important
elements such as nitrogen and sulphur that are precursors to GHGs ( NOx and SOx ,
respectively) and are present in coke but have been ignored in modelling, which
means the current models are unable to predict these emissions. Hence, considering
the gravity of the climate change problem, it is recommended that future models
include kinetics for the combustion of sulphur and nitrogen so that their emission
gases can be monitored and addressed;
(d) Temperature: A common assumption in modelling is to assume that there is ther-
modynamic equilibrium between the gas and the solids in the emulsion phase. This
treats any resistance to heat transfer at the solid–gas interphase as negligible. Since
the temperature of the catalyst is an important parameter in the FCC regenerator, the
rate of heat transfer between the catalyst particle and the gas plays an important role
in the performance of the unit since it determines the energy balance. For design
purposes, this assumption is usually sufficient [155]. However, since the heat capacity
and thermal conductivity values for the catalyst are usually appreciably higher than
that of the gas, for cases where a more detailed description of the temperature of gas
and catalyst is required, arguably in the case of the FCC regenerator for its influence
on riser thermal balance, the loosening of the thermal equilibrium assumption may
be worth exploring;
(e) Bubble properties: from examining Table 4, it is easy to see that the bubbles rising
through the dense bed of the FCC regenerator have generally been poorly described
in the models. Bubbles affect the gas–solid contact in the bed and therefore control
mass and heat transfer in the bed; hence, their modelling in two-phase or bubbling
beds is of great importance to the prediction of coke conversion and thermal balance
in the regenerator. Although the understanding of bubble size, growth and frequency
is highly empirical, these empirical correlations provide a great understanding of the
bubbling phenomena in the dense bed and should be included in the modelling of the
FCC regenerator.

3. Modelling FCC Unit Constitutive Components

3.1. Cyclones
Cyclones are usually used in both the reactor and the regenerator systems of an FCC
unit. They are the conventional industry equipment used to separate gas–solid two-phase
flow. In the FCC reactor system, the cyclones are used in the disengaging section to separate
entrained catalyst particles from the wet gases going to the main fractionating column.
In the FCC regenerator, the cyclones are used to separate any entrained catalyst particles
escaping at the top of the freeboard from the flue gases leaving the regenerator system. The
most used type of cyclone in these systems is the tangential inlet cyclone that uses turbulent
swirling flow to separate the high-density entrained phase (the catalyst particulate phase)
from the low-density carrier phase (the gas) [156]. The swirling flow pattern usually
consists of a double vortex flow pattern; an outer vortex with downward axial velocity and
an inner vortex with upward axial velocity, shown in Figure 5a. The outer vortex loses
its downward momentum towards the bottom of the cyclone and subsequently changes
direction to flow upwards, resulting in the inner vortex being formed [156]. Because of
the complex nature of the flow inside the cyclone, this flow pattern influences some of
the important operational parameters, such as the separation efficiency and the pressure
drop [156]. For this reason, these parameters are usually estimated using CFD, where
Energies 2022, 15, 388 28 of 38

the anisotropic turbulence and localised flow field at short time and space scales can be
considered [157]. However, because CFD is beyond the scope of the current work, only the
global balances over the cyclone are carried out to model the system.

Figure 5. (a) vortex flow patterns inside a tangential inlet cyclone [158], (b) a basic vortex quick
separation showing a multi-cyclone system for FCC reactor termination [159].

Similar to the disengaging–stripping section, the cyclone model consists of balances

for mass and energy and estimation of pressure drop. Pressure drop and separation
efficiency are the most important performance parameters for the operation of a cy-
clone [156,157,160–163]. Before balances can be made, the current approach requires that
efficiency and pressure drop be quantities that are known (specified) or be quantities that
can be predicted based on the operating conditions. Experimental data from the literature
have shown that these performance indicators are dependent on solid loading, gas and solid
flow rates, gas and solid properties (such as particle size, gas viscosity, etc.), temperature
and entry effects, and cyclone geometry [157,160,162,164–166]. Traditionally, prediction
of the performance indicators is such that a function of the above-mentioned variables
is developed to predict the indicator. Several methods for estimating efficiency are well
established in the literature: time-of-flight correlation, the equilibrium orbit model and
the fractional efficiency method [167–171]. Zhang and Basu [163] developed the following
semi-empirical correlation (Equation (16)) for the collection efficiency of gas–solid cyclones
using equilibrium orbit theory:
!
1.04δ3.9
η = 1 − exp − (16)
0.002Re05 − 0.0102Re03 δ1.3 + 0.416Re00.58 δ3.15

with Re as the Reynolds number based on particle diameter and subscript 0 denotes that
Re is taken at the bottom of the cyclone where the conical radius is r0 . Traditionally,
correlations for η are made such that η = f ( Re, St) where St is the well-known Stokes
number. However, Zhang and Basu [163] chose their correlation such that η = f ( Re, δ) as
they noted that this correlated better compared to the traditional Reynolds–Stokes approach.
In this case, δ (in Equation (17)) is the non-dimensional ratio of the radius of the particle
Energies 2022, 15, 388 29 of 38

orbit in the cyclone to the radius at the exit (i.e., rr0 ). Without much loss of accuracy, the
workers [163] found that:
 1
2πSt 2α
δ= (17)
B2
For:  
1− α

1 R
1− α r0 −1
B= R
(18)
r0 −1
where α is an exponent of the velocity distribution of the free vortex and can be obtained
empirically from different sizes of cyclones. Zhang and Basu found a value of α = −0.65.
Thus, from the above analysis, for known process and stream conditions of the cyclone, the
collection efficiency can be predicted. In both the reactor and the regenerator systems, the
entrained catalyst is separated from the gas phase using a multi-stage cyclone system rather
than just a single cyclone to maximise the separation and the throughput. In order to carry
out the conservation balance equations, it is usually assumed that all cyclones are identical
(both in terms of dimensions and flow conditions) for simplicity, the flow rate through
the cyclone dipleg is controlled by the holdup in the cyclone, no reactions occur in the
cyclone because the flows are considered dilute with small solid loadings and cyclones are
in thermal equilibrium with the disengaging section since this is where they are located [10].
Therefore, only material balances are required in this case for modelling the cyclone systems.
The temperature of flow into and out of the cyclones is therefore constant and is determined
by energy balances in the disengaging section. The thermal equilibrium assumption is
valid because no reactions are assumed to occur in the cyclone, no new streams are present,
and at a steady state, the cyclone body approaches the surrounding (disengaging section)
temperature; hence, it is reasonable to assume that temperature does not change in the
cyclone. Considering the mentioned assumptions, Han and Chung [10] showed that for a
reactor system with NCY cyclones, the pseudo-steady state catalyst balance for the cyclones
under continuous stirred tank assumption is given by Equation (19):
 2
ρb NCY ηCY vcCY wcST ACYi
wcCY = (19)
ACYd k vCY VST

where ACY is the area of the cyclone at the inlet (i) and at the dipleg (d), and vcCY is the
velocity at the inlet of the cyclone, which may be calculated using the Rosin, Rammler and
Intelmann equation in Equation (20) [172]:

9µ g ACYi
vcCY =  w
 (20)
dcm πNCYt ρc − VgST hCYi
gST

where dcm is the minimum particle diameter completely separated by the cyclone system,
and NCYt is the number of 360◦ turns made spirally down the cyclone. For typical industrial
cyclones, NCYt ranges from 1 to 10 and can be estimated from the cyclone geometry by
Equation (21) [173]:  

Lc
1 L b + 2
NCYt =  (21)
H H

where H is the height of the cyclone inlet mouth, and Lb and Lc are heights of the cyclone
body and conical base, respectively. Since the holdup, inlet velocity of the catalyst and
the cyclone separation efficiency are known, the flow rate of catalyst entrained with gas
that is not captured by the cyclone, FcMF , that flows to the main fractionating unit and the
Energies 2022, 15, 388 30 of 38

flow rate gas from the cyclone to the main fractionating unit, FgMF , can be determined by
Equations (22) and (23), respectively [10]:
 
wcCY
FcMF = (1 − ηCY )vcCY ACYi NCY (22)
VST
p
FgMF = KvMF PST − PMF (23)
Note that for flow rates in the regenerator cyclones, the above equations would
calculate the flow rate of catalyst and gas that make up the flue gas stack. Flow rates
through the dipleg can be calculated via simple balances between inlet flow rates into
the cyclone and the flow rates leaving at the top of the cyclone for steady state operation.
As previously stated, a pressure drop is also an important performance indicator for
cyclone operation. Pressure loss in a cyclone is usually divided according to different
contributions [174,175]: head losses at the cyclone inlet, losses in the separation space
due to gas flow and the wall and losses in the vortex finder mainly due to gas reversal
and contraction at the exit. The relative magnitudes of the losses depend on the cyclone
classification as either low-loaded or high-loaded [171,176]. It was already established
that solid loading for the FCC cyclones might be assumed to be small; therefore, it can be
assumed to be low-loaded. For low-loaded conditions, Chen and Shi [175] and Li et al. [177]
showed that the contributions of outlet pressure losses might be ignored. Chen and Shi [175]
developed a ‘universal’ method that predicts the pressure losses of a cyclone, the so-called
C-S method, and this method is now widely used in the literature and was subsequently
improved for better accuracy by Li et al. [177], especially for high-loaded cases. The C-S
model predicts that from Equation (24):

1
∆PCY = ρ g ξCY Ug (24)
2
where Ug is either the inlet or the outlet gas velocity and ξCY is the dimensionless pressure
drop parameter. In the literature, two main methods of determining ξ are usually used [171]:
the first method accounts for effects of cyclone geometry and solid loading on pressure
losses (e.g., ξCY = ξgeometry × ξsolid ) [178], and the second method sums the individual
contributions to pressure loss (e.g., ξCY = ξin + ξbody + ξvortex + ξout ) [170,175]. Chen and
Shi [175] proposed Equation (25) for ξCY for dust-laden flows:
 ∼
2 ∼2
C 2k i b ∼ ∼ ∼−1.5n V 1
ξCY = (1 + i )(1 −  ∼ ∼
 + 1.11 f K A F s V θw d r +  ∼θwn +  ∼2 2 (25)
ρg ∼ ∼2
1 + 1.33 b − d r r c dr K2A d r − r c

where the (∼) indicates a nondimensional variable. Ci is the inlet solid loading (kg of inlet
solid/m3 of inlet gas), k i is a correction coefficient of expansion loss (≈ 0.3) [162], f is the
2
friction coefficient (≈ 0.005 for steel cyclones) [162] and KA is the inlet area ratio (= πD4ab ;
for D cyclone barrel diameter and a, b for cyclone inlet width and height). Non-dimensional
∼ ∼ ∼
b
variables are such that b is dimensional width (= D ), F s dimensionless contact area, r c
∼
rc
is the dimensionless radius of core flow (= R ), d r is the dimensionless cyclone outlet
∼
de Vθw
diameter (= D) and V θw is the dimensionless tangential velocity at radius R (= Ug ). Chen
∼ ∼
and Shi [175] correlated r c with d r in Equation (26):

∼ ∼ ∼2
r c = 0.38 d r + 0.5 d r (26)
Energies 2022, 15, 388 31 of 38

Additionally, the dimensionless tangential velocity at the cyclone wall is given by

Equation (27) [162]:
∼0.16
∼ 1.11K − 0.21
d Re0.06
V θw = A qr (27)
∼ ∼
1 + f Fs K A d r
For
ρ g Ug D
Re = ∼ (28)
µg K A d r
Note that different workers in the literature and no doubt in the industry have devel-
∼
oped alternative equations for ξCY and V θw . Therefore, the choice of expression must be
based on their ranges of applicability, especially in terms of solid loading, which has a great
impact on the pressure drop of a cyclone.

3.2. Catalyst Transport Lines

The transport lines carry catalysts between the reactor and the regenerator systems.
The catalyst circulation rate within the transport lines is controlled by a slide valve that
should be attached to the line [10,18]. In terms of the dynamics of both units, the circulation
rate with the transport lines affects the holdup of catalyst in the regenerator and the
disengaging–stripper section of the reactor; hence, it affects the coupling of the two systems.
This coupling makes the catalyst transport line and associated valves important features for
any model of the FCC unit. By taking the pressure across the slide valve into account, the
flow rate of catalyst through the transport line can be calculated from Equation (29) [10,18]:
√
FcV = k v f v ( xv ) ∆P (29)

where FcV is the catalyst flow rate through the valve, k v is the valve flow rating factor
and f v ( xv ) is the valve flow characteristic function. ∆P is the pressure drop across the
valve, which depends on the direction of catalyst flow; for example, for the spent catalyst
transport line, the ∆P is the pressure difference between the bottom of the stripper and
the regenerator dense bed. In this example, FcV is catalyst flow rate out of the stripper
and the catalyst flow rate into the dense bed. Because the catalyst residence time inside
the transport lines is in the order of a few seconds, its influence on the regenerator, and
therefore the whole FCC unit, is small so that the transport lag may be ignored [10,135].
This assumption therefore leads to negligible energy loss through the transport line so that
catalyst retains the temperature of the vessel it is leaving so that no further energy balance
is required. However, some workers have explicitly described the valve characteristics in
their model but instead provided catalyst circulation rate as a specification based on plant
data [19]. In such cases, models are unsuitable to use to study the effects of changes in
flow conditions on the unit dynamics because the coupling of the pressure drop across the
vessels and valve characteristics with the rest of the unit has been removed, which could
lead to inaccurate predictions. Nevertheless, such studies presented useful results in terms
of conversions in both reactor systems.

4. Conclusions
Overall, modelling of the FCC unit using traditional reaction engineering approaches
has certainly come a long way. The kinetics of the regenerator is now well understood, with
models published able to predict the emissions of carbon monoxide and carbon dioxide
that are produced during the combustion reactions. Additionally, analytical technology
had come a long way since the early 1960s when FCC modelling first began, with tools
now able to characterise coke at the elemental level. This means researchers are now able
to incorporate elements such as sulphur and nitrogen into their kinetic models to predict
greenhouse gas emissions such as SOx and NOx that are also directly produced during the
combustion reactions in the regenerator. Due to the current global action against climate,
Energies 2022, 15, 388 32 of 38

we recommend that future models make necessary changes to incorporate the combustion
of sulphur and nitrogenous compounds, which are also present in the coke. In terms of
hydrodynamics, both the fluidised bed reactor vessels of the FCC unit have significant flow
heterogeneity during their normal operation. In the regenerator, the heterogeneity arises
from bubbles rising through the emulsion, whereas in the riser clusters of catalyst particles
are observed in the suspension. This heterogeneity is important to the conversion in both
vessels and has been modelled to varying degrees by researchers. More recently, the study
of such flow patterns is being conducted via CFD, providing detail that is seldom captured
experimentally or via traditional modelling simulations.

Author Contributions: Conceptualization, T.W.S., R.P., I.M.M. and Y.M.J.; methodology, T.W.S.
and Y.M.J.; software, T.W.S.; validation, T.W.S. and Y.M.J.; formal analysis, T.W.S., R.P., I.M.M.,
Y.M.J.; investi-gation, T.W.S. and Y.M.J.; resources, T.W.S., R.P., I.M.M., Y.M.J.; data curation, T.W.S.;
writing—original draft preparation, T.W.S.; writing—review and editing, T.W.S., R.P., I.M.M., Y.M.J.;
visualization, T.W.S.; supervision, R.P., I.M.M., Y.M.J. All authors have read and agreed to the
published version of the manuscript.
Funding: This research received no external funding.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Acknowledgments: The main author (T.W.S.) would like to acknowledge the Government of
Botswana for funding his Ph.D. research studies.
Conflicts of Interest: There is no conflict of interest regarding the publication of this research.

Nomenclature
Symbol Description Units
C Molar concentration kmolm−3
D Dispersion coefficient m2 .s−1
dp Particle diameter m
dcm Smallest particle diameter separated by cyclone m
F Mass flow rate kg.s−1
g Acceleration due to gravity ms−2
Height of jet penetration through the bed
h mkJ.kg−1
Enthalpy of the phase
Deviation coefficient from ideal two-phase flow
k (−)varied
Reaction rate constant
K Interphase mass transfer coefficient ms−1
Reaction order
n (−)(−)
Molar ratio of hydrogen to Carbon in coke
Molar flux
N kmol.m−2 s−1 (−)
Number of cyclones
NCYt Number of 360◦ turns made spirally down a cyclone (−)
P Pressure kPa
r Reaction rate kmolm−3 s−1 kPa.s−1
Component reaction rate
R kmol.m−3 .s−1 kJ.kmol−1 .K−1
Ideal gas constant
Re Reynolds number (−)
S Energy source term kJ.s−1
T Temperature K
Ub Bubble rise velocity m.s−1
Uc Gas circulation velocity inside rising bubbles m.s−1
Umb Minimum bubbling velocity m.s−1
Um f Minimum fluidisation velocity m.s−1
Ut Terminal velocity of particles in the bed m.s−1
V Volume m3
Energies 2022, 15, 388 33 of 38

w Mass of holdup in reactor or cyclone kg

x Mole fraction (−)
Y Deviation coefficient from ideal two-phase flow (−)
Greek letters and other symbols
ε Volume fraction (−)
α Exponent of velocity distribution in a cyclone vortex (−)
β Molar ratio of CO to CO2 (−)
ρ Density kg.m−3
δ Ratio of particle radius to radius of the cyclone (−)
η Cyclone separation efficiency (−)
ξ Cyclone Pressure drop parameter (−)
∼
V θw Dimensionless tangential velocity at cyclone wall (−)
∆Q Heat of reaction kJ.s−1
∆P Pressure drop kPa
∆H Enthalpy change of reaction kJ.kmol−1
Subscripts
e Emulsion
b Bubble phase
be Bubble to emulsion
eb Emulsion to bubble
CO Carbon monoxide
C Coke
CO2 Carbon dioxide
H2 O Water vapor
c Catalyst
g Gas

References
1. Arbel, A.; Huang, Z.; Rinard, I.H.; Shinnar, R.; Sapre, A.V. Dynamic and Control of Fluidized Catalytic Crackers. 1. Modeling of
the Current Generation of FCC’s. Ind. Eng. Chem. Res. 1995, 34, 1228–1243. [CrossRef]
2. Sadeghbeigi, R. Fluid Catalytic Cracking Handbook: An Expert Guide to the Practical Operation, Design, and Optimization of FCC Units;
Butterworth-Heinemann: Oxford, UK, 2012. [CrossRef]
3. Kim, S.W.; Kim, S.D. Void properties in dense bed of cold-flow fluid catalytic cracking regenerator. Processes 2018, 6, 80. [CrossRef]
4. Wetherald, R.T.; Manabe, S. Sensitivity Studies of Climate Involving Changes in Co2 Concentration. Dev. Atmos. Sci. 1979, 10,
57–64. [CrossRef]
5. UNFCCC. Paris Agreement. Int. Leg. Mater. 2016, 55, 740–755. [CrossRef]
6. UNFCCC. National Inventory Submissions 2020|UNFCCC n.d. Available online: https://unfccc.int/ghg-inventories-annex-i-
parties/2020 (accessed on 28 June 2021).
7. UNFCCC. Kyoto Protocol to the United Nations Framework Convention on Climate Change. Am. J. Int. Law 1998, 92, 315–331.
[CrossRef]
8. Berruti, F.; Pugsley, T.S.; Godfroy, L.; Chaouki, J.; Patience, G.S. Hydrodynamics of circulating fluidized bed risers: A review. Can.
J. Chem. Eng. 1995, 73, 579–602. [CrossRef]
9. Grace, J.R.; Avidan, A.A.; Knowlton, T.M. Circulating Fluidized Beds; Blackie Academic & Professional: London, UK, 1997.
10. Han, I.S.; Chung, C.B. Dynamic modeling and simulation of a fluidized catalytic cracking process. Part I: Process modeling. Chem.
Eng. Sci. 2001, 56, 1951–1971. [CrossRef]
11. Kunii, D.; Levenspiel, O. Fluidization Engineering; Butterworth-Heinemann: Oxford, UK, 1991.
12. Shah, M.; Utikar, R.; Pareek, V.; Evans, G.; Joshi, J. Computational fluid dynamic modelling of FCC riser: A review. Chem. Eng.
Res. Des. 2016, 1, 403–448. [CrossRef]
13. Toomey, R.D.; Johnstone, H.F. Gas Fluidization of Solid Particles. Chem. Eng. Prog. Vol. 1952, 48, 220–226.
14. Kunii, D.; Levenspiel, O. Fluidization Engineering; John Wiley and Sons: New York, NY, USA, 1969.
15. Kunii, D.; Levenspiel, O. Bubbling bed model: Model for the Flow of Gas through a Fluidized Bed. Ind. Eng. Chem. Fundam. 1968,
7, 446–452. [CrossRef]
16. Stephens, G.K.; Sinclair, R.J.; Potter, O.E. Gas exchange between bubbles and dense phase in a fluidised bed. Powder Technol. 1967,
1, 157–166. [CrossRef]
17. Kato, K.; Wen, C.Y. Bubble assemblage model for fluidized bed catalytic reactors. Chem. Eng. Sci. 1969, 24, 1351–1369. [CrossRef]
18. Han, I.S.; Chung, C.B. Dynamic modeling and simulation of a fluidized catalytic cracking process. Part II: Property estimation
and simulation. Chem. Eng. Sci. 2001, 56, 1973–1990. [CrossRef]
Energies 2022, 15, 388 34 of 38

19. Ali, H.; Rohani, S.; Corriou, J.P. Modelling and control of a riser type fluid catalytic cracking (FCC) unit. Chem. Eng. Res. Des.
1997, 75, 401–412. [CrossRef]
20. Yakubu, J.M.; Patel, R.; Mujtaba, I.M. Optimization of fluidized catalytic cracking unit regenerator to minimize CO2 emissions.
Chem. Eng. Trans. 2017, 57, 1531–1536. [CrossRef]
21. Arthur, J.R. Reactions between Carbon and Oxygen. Trans. Faraday Soc. 1951, 47, 164–178. [CrossRef]
22. Weisz, P.B. Corn bustion of Carbonaceous Deposits within Porous Catalyst Particles III. The CO2 CO Product Ratio. J. Catal. 1966,
6, 425–430. [CrossRef]
23. Weisz, P.B.; Goodwin, R.B. Combustion of Carbonaceous Deposits within Porous Catalyst Particles II. Intrinsic Burning Rate. J.
Catal. 1966, 6, 227–236. [CrossRef]
24. Weisz, P.B.; Goodwin, I.D. Combustion of Carbonaceous Deposits within Porous Catalyst Particles I. Diffusion-Controlled
Kinetics. J. Catal. 1963, 2, 397–404. [CrossRef]
25. Tone, S.; Miura, S.-I.; Otake, T. Kinetics of Oxidation of Coke on Silica-Alumina Catalysts. Bull. Jpn. Pet. Inst. 1972, 14, 76–82.
[CrossRef]
26. Hano, T.; Nakashio, F.; Kusunoki, K. The burning rate of coke deposited on zeolite catalyst. J. Chem. Eng. Jpn. 1975, 8, 127–130.
[CrossRef]
27. Wang, G.X.; Lin, S.X.; Mo, W.J.; Peng, C.L.; Yang, G.H. Kinetics of Combustion of Carbon and Hydrogen in Carbonaceous
Deposits on Zeolite-Type Cracking Catalysts. Ind. Eng. Chem. Process Des. Dev. 1986, 25, 626–630. [CrossRef]
28. Arandes, J.M.; Abajo, I.; Fernández, I.; López, D.; Bilbao, J. Kinetics of gaseous product formation in the coke combustion of a
fluidized catalytic cracking catalyst. Ind. Eng. Chem. Res. 1999, 38, 3255–3260. [CrossRef]
29. Amblard, B.; Singh, R.; Gbordzoe, E.; Raynal, L. CFD modeling of the coke combustion in an industrial FCC regenerator. Chem.
Eng. Sci. 2017, 170, 731–742. [CrossRef]
30. Hosseini, S.H.; Rahimi, R.; Zivdar, M.; Samimi, A. CFD simulation of gas-solid bubbling fluidized bed containing FCC particles.
Korean J. Chem. Eng. 2009, 26, 1405–1413. [CrossRef]
31. Azarnivand, A.; Behjat, Y.; Safekordi, A.A. CFD simulation of gas-solid flow patterns in a downscaled combustor-style FCC
regenerator. Particuology 2018, 39, 96–108. [CrossRef]
32. Lee, L.S.; Yu, S.W.; Cheng, C.T.; Pan, W.Y. Fluidized-bed catalyst cracking regenerator modelling and analysis. Chem. Eng. J. 1989,
40, 71–82. [CrossRef]
33. Qian, K.; Tomczak, D.C.; Rakiewicz, E.F.; Harding, R.H.; Yaluris, G.; Cheng, W.C.; Zhao, X.; Peters, A.W. Coke formation in the
fluid catalytic cracking process by combined analytical techniques. Energy Fuels 1997, 11, 596–600. [CrossRef]
34. Luan, H.; Lin, J.; Xiu, G.; Ju, F.; Ling, H. Study on compositions of FCC flue gas and pollutant precursors from FCC catalysts.
Chemosphere 2020, 245, 125528. [CrossRef]
35. Ibarra, Á.; Veloso, A.; Bilbao, J.; Arandes, J.M.; Castaño, P. Dual coke deactivation pathways during the catalytic cracking of raw
bio-oil and vacuum gasoil in FCC conditions. Appl. Catal. B Environ. 2016, 182, 336–346. [CrossRef]
36. Elshishini, S.S.; Elnashaie, S.S.E.H. Digital simulation of industrial fluid catalytic cracking units: Bifurcation and its implications.
Chem. Eng. Sci. 1990, 45, 553–559. [CrossRef]
37. Bai, D.; Zhu, J.X.; Jin, Y.; Yu, Z. Simulation of FCC catalyst regeneration in a riser regenerator. Chem. Eng. J. 1998, 71, 97–109.
[CrossRef]
38. Bayraktar, O.; Kugler, E.L. Coke content of spent commercial fluid catalytic cracking (FCC) catalysts: Determination by
temperature-programmed oxidation. J. Therm. Anal. Calorim. 2003, 71, 867–874. [CrossRef]
39. Hashimoto, K.; Takatani, K.; Iwasa, H.; Masuda, T. A multiple-reaction model for burning regeneration of coked catalysts. Chem.
Eng. J. 1983, 27, 177–186. [CrossRef]
40. Dimitriadis, V.D.; Lappas, A.A.; Vasalos, I.A. Kinetics of combustion of carbon in carbonaceous deposits on zeolite catalysts
for fluid catalytic cracking units (FCCU). Comparison between Pt and non Pt-containing catalysts. Fuel 1998, 77, 1377–1383.
[CrossRef]
41. Morley, K.; De, L. On the Determination of Regeneration of Kinetic Parameters for the Craclung Catalyst. Can. J. Chem. Eng. 1987,
65, 773–777. [CrossRef]
42. Howard, J.B.; Williams, G.C.; Fine, D.H. Kinetics of Carbon Monoxide Oxidation in Postflame Gases. In Symposium (International)
on Combustion; Elsevier: Amsterdam, The Netherlands, 1973.
43. Li, C.; Brown, T.C. Carbon oxidation kinetics from evolved carbon oxide analysis during temperature-programmed oxidation.
Carbon 2001, 39, 725–732. [CrossRef]
44. Kanervo, J.M.; Krause, A.O.I.; Aittamaa, J.R.; Hagelberg, P.H.; Lipiäinen, K.J.T.; Eilos, I.H.; Hiltunen, J.S.; Niemi, V.M. Kinetics of
the regeneration of a cracking catalyst derived from TPO measurements. Chem. Eng. Sci. 2001, 56, 1221–1227. [CrossRef]
45. Williams, G.C.; Hottel, H.C.; Morgan, A.C. The Combustion of Methane in a Jet-Mixed Reactor. In Symposium (International) on
Combustion; Elsevier: Amsterdam, The Netherlands, 1969; Volume 12, pp. 913–925. [CrossRef]
46. Schneider, G.R. Kinetics of Propane Combustion in a Well Stirred Reactor. Ph.D. Thesis, Massachusetts Institute of Technology,
Department of Nuclear Engineering, Cambridge, MA, USA, 1961.
47. Friedman, R.; Cyphers, J.A. Flame structure studies. III. Gas sampling in a low-pressure propane-air flame. J. Chem. Phys. 1955,
23, 1875–1880. [CrossRef]
Energies 2022, 15, 388 35 of 38

48. Singh, T.; Sawyer, R.F. CO Reactions in the Afterflame Region of Ethylene/Oxygen and Ethane/Oxygen Flames. In Symposium
(International) on Combustion; Elsevier: Amsterdam, The Netherlands, 1971; Volume 13, pp. 403–416. [CrossRef]
49. Sobolev, G.K. High-Temperature Oxidation and Burning of Carbon Monoxide. In Symposium (International) on Combustion;
Elsevier: Amsterdam, The Netherlands, 1958; Volume 7, pp. 386–391. [CrossRef]
50. Ghazal, F.P.H. Kinetics of Carbon Monoxide Oxidation in Combustion Products. Ph.D. Thesis, Massachusetts Institute of
Technology, Cambridge, MA, USA, 1971.
51. Morley, K.; de Lasa, H.I. Regeneration of cracking catalyst influence of the homogeneous CO postcombustion reaction. Can. J.
Chem. Eng. 1988, 66, 428–432. [CrossRef]
52. Ahmed, S.; Back, M.H. The role of the surface complex in the kinetics of the reaction of oxygen with carbon. Carbon 1985, 23,
513–524. [CrossRef]
53. Tucker, B.G.; Mulcahy, M.F.R. Formation and decomposition of surface oxide in carbon combustion. Trans. Faraday Soc. 1969, 65,
274–286. [CrossRef]
54. Geldart, D. Types of gas fluidization. Powder Technol. 1973, 7, 285–292. [CrossRef]
55. Baeyens, J.; Geldart, D. Predictive Calculations of Flow Parameters in Gas Fluidized Beds and Fluidization Behaviour of Various
Powders. In Proceedings the International Symposium Fluidization and Its Applications; Cepadues Edition: Toulouse, France, 1973;
p. 263.
56. Yates, J.G. Fundamentals of Fluidized-Bed Chemical Processes: Butterworths Monographs in Chemical Engineering; Butterworth-
Heinemann: Oxford, UK, 1983.
57. Kumar, A.; sen Gupta, P. Prediction of minimum fluidization velocity for multicomponent mixtures. Indian J. Technol. 1974, 12,
225–227.
58. Mawatari, Y.; Tatemoto, Y.; Noda, K. Prediction of minimum fluidization velocity for vibrated fluidized bed. Powder Technol. 2003,
131, 66–70. [CrossRef]
59. Rowe, P.N.; Nienow, A.W. Minimum fluidisation velocity of multi-component particle mixtures. Chem. Eng. Sci. 1975, 30,
1365–1369. [CrossRef]
60. Asif, M. Predicting minimum fluidization velocities of multi-component solid mixtures. Particuology 2013, 11, 309–316. [CrossRef]
61. Delebarre, A. Revisiting the Wen and Yu equations for minimum fluidization velocity prediction. Chem. Eng. Res. Des. 2004, 82,
587–590. [CrossRef]
62. Amarasinghe, W.S.; Jayarathna, C.K.; Ahangama, B.S.; Tokheim, L.A.; Moldestad, B.M.E. Experimental Study and CFD Modelling
of Minimum Fluidization Velocity for Geldart A, B and D Particles. Int. J. Model. Optim. 2017, 7, 152–156. [CrossRef]
63. Zhang, X.; Zhou, Y.; Zhu, J. Enhanced fluidization of group A particles modulated by group C powder. Powder Technol. 2021, 377,
684–692. [CrossRef]
64. Lee, J.R.; Lee, K.S.; Hasolli, N.; Park, Y.O.; Lee, K.Y.; Kim, Y.H. Fluidization and mixing behaviors of Geldart groups A, B and C
particles assisted by vertical vibration in fluidized bed. Chem. Eng. Process. Process Intensif. 2020, 149, 107856. [CrossRef]
65. Frank, D.J.; Roland, C.; David, H. Fluidization, 2nd ed.; Academic Press Inc.: Cambridge, MA, USA, 1985.
66. Anantharaman, A.; Cocco, R.A.; Chew, J.W. Evaluation of correlations for minimum fluidization velocity (Umf) in gas-solid
fluidization. Powder Technol. 2018, 323, 454–485. [CrossRef]
67. Shaul, S.; Rabinovich, E.; Kalman, H. Generalized flow regime diagram of fluidized beds based on the height to bed diameter
ratio. Powder Technol. 2012, 228, 264–271. [CrossRef]
68. Shaul, S.; Rabinovich, E.; Kalman, H. Typical fluidization characteristics for Geldart’s classification groups. Part. Sci. Technol.
2014, 32, 197–205. [CrossRef]
69. Kong, W.; Tan, T.; Baeyens, J.; Flamant, G.; Zhang, H. Bubbling and Slugging of Geldart Group A Powders in Small Diameter
Columns. Ind. Eng. Chem. Res. 2017, 56, 4136–4144. [CrossRef]
70. Abrahamsen, A.R.; Geldart, D. Behaviour of gas-fluidized beds of fine powders part I. Homogeneous expansion. Powder Technol.
1980, 26, 35–46. [CrossRef]
71. Rowe, P.N.; Yacono, C.X.R. The bubbling behaviour of fine powders when fluidised. Chem. Eng. Sci. 1976, 31, 1179–1192.
[CrossRef]
72. Rowe, P.N.; Partridge, B.A. X-ray study of bubbles in fluidized beds. Process Saf. Environ. Prot. Trans. Inst. Chem. Eng. Part B 1965,
43, 157–175.
73. Rowe, P.N.; Partridge, B.A. An X-ray study of bubbles in fluidised beds. Chem. Eng. Res. Des. 1997, 75, S116–S134. [CrossRef]
74. Rowe, P.N.; Everett, D.J. Fluidised bed bubbles viewed by X-rays. Part I: Experimental details and the interaction of bubbles with
solid surfaces. Trans. Inst. Chem. Eng. 1972, 50, 42–48.
75. Yacono, C.X.R. An X-Ray Study of Bubbles in Gas-Fluidised Beds of Small Particles. Ph.D. Thesis, University College London,
London, UK, 1975.
76. Rowe, P.N. A note on the motion of a bubble rising through a fluidized bed. Chem. Eng. Sci. 1964, 19, 75–77. [CrossRef]
77. Rowe, P.N. Prediction of bubble size in a gas fluidised bed. Chem. Eng. Sci. 1976, 31, 285–288. [CrossRef]
78. Yang, W. Handbook of Fluidization and Fluid-Particle Systems; CRC Press: New York, NY, USA, 2003.
79. Whitehead, A.B.; Gartside, G.; Dent, D.C. Fluidization studies in large gas-solid systems. Part III. The effect of bed depth and
fluidizing velocity on solids circulation patterns. Powder Technol. 1976, 14, 61–70. [CrossRef]
Energies 2022, 15, 388 36 of 38

80. Geldart, D. The size and frequency of bubbles in two- and three-dimensional gas-fluidised beds. Powder Technol. 1970, 4, 41–55.
[CrossRef]
81. Werther, J. Bubble growth in large diameter fluidized beds. Fluid Technol. 1975, 1, 215.
82. Mori, S.; Wen, C.Y. Estimation of bubble diameter in gaseous fluidized beds. AIChE J. 1975, 21, 109–115. [CrossRef]
83. Cai, P.; Schiavetti, M.; de Michele, G.; Grazzini, G.C.; Miccio, M. Quantitative estimation of bubble size in PFBC. Powder Technol.
1994, 80, 99–109. [CrossRef]
84. Darton, R.C.; Nauze, R.; Harrison, D.; Davidson, J. Bubble Growth due to Coalescence in Fluidised Beds. In Chemical Reactor
Theory; Lapidus, I., Amundson, N.R., Eds.; Prentice-Hall: New York, NY, USA, 1977.
85. Horio, M.; Nonaka, A. A generalized bubble diameter correlation for gas-solid fluidized beds. AIChE J. 1987, 33, 1865–1872.
[CrossRef]
86. Rowe, P.N. Experimental Properties of Bubbles. Fluidization; Academic Press: New York, NY, USA, 1971; p. 121.
87. Harrison, D.; Davidson, J.F.; de Kock, J.W. Bubble growth theory in fluidized beds. Chem. Eng. Sci. 1961, 39, 202.
88. Davidson, J.F.; Harrison, D. Fluidized Particles; Cambridge University Press: Cambridge, NY, USA, 1963.
89. Upson, P.C.; Pyle, D.L. The Stability of Bubbles in Fluidized Beds. In Fluidization and its Applications: Proceedings of the International
Symposium; Cepadues Edition: Toulouse, France, 1973; pp. 207–222.
90. Clift, R.; Grace, J.R.; Weber, M.E. Stability of Bubbles in Fluidized Beds. Ind. Eng. Chem. Fundam. 1974, 13, 45–51. [CrossRef]
91. Rice, W.J.; Wilhelm, R.H. Surface dynamics of fluidized beds and quality of fluidization. AIChE J. 1958, 4, 423–429. [CrossRef]
92. Karimipour, S.; Pugsley, T. A critical evaluation of literature correlations for predicting bubble size and velocity in gas–solid
fluidized beds. Powder Technol. 2011, 205, 1–14. [CrossRef]
93. Davies, R.M.; Taylor, G.I. The mechanics of large bubbles rising through extended liquids and through liquids in tubes. Proc. R.
Soc. Lond. Ser. A Math. Phys. Sci. 1950, 200, 375–390. [CrossRef]
94. Sit, S.P.; Grace, J.R. Effect of bubble interaction on interphase mass transfer in gas fluidized beds. Chem. Eng. Sci. 1981, 36, 327–335.
[CrossRef]
95. Chiba, T.; Kobayashi, H. Solid exchange between the bubble wake and the emulsion phase in a gas-fluidised bed. J. Chem. Eng.
Jpn. 1977, 10, 206–210. [CrossRef]
96. Pyle, D.L.; Harrison, D. An experimental investigation of the two-phase theory of fluidization. Chem. Eng. Sci. 1967, 22, 1199–1207.
[CrossRef]
97. Pyle, D.L.; Harrison, D. The rising velocity of bubbles in two-dimensional fluidised beds. Chem. Eng. Sci. 1967, 22, 531–535.
[CrossRef]
98. Marsheck, R.M.; Gomezplata, A. Particle flow patterns in a fluidized bed. AIChE J. 1965, 11, 167–173. [CrossRef]
99. Gabor, J.D. On the mechanics of fluidized particle movement. Chem. Eng. J. 1972, 4, 118–126. [CrossRef]
100. Stein, M.; Ding, Y.L.; Seville, J.P.K.; Parker, D.J. Solids motion in bubbling gas fluidized beds. Chem. Eng. Sci. 2000, 55, 5291–5300.
[CrossRef]
101. Mostoufi, N.; Chaouki, J. Local solid mixing in gas–solid fluidized beds. Powder Technol. 2001, 114, 23–31. [CrossRef]
102. Shabanian, J.; Chaouki, J. Influence of interparticle forces on solids motion in a bubbling gas-solid fluidized bed. Powder Technol.
2016, 299, 98–106. [CrossRef]
103. Werther, J.; Molerus, O. The local structure of gas fluidized beds -II. The spatial distribution of bubbles. Int. J. Multiph. Flow 1973,
1, 123–138. [CrossRef]
104. Callcott, T.G.; Rigby, G.R.; Singh, B. Experiences in the handling of particulate materials. BHP Tech. Bull. 1975, 19, 20.
105. Gabor, J.D. Lateral solids mixing in fludized-packed beds. AIChE J. 1964, 10, 345–350. [CrossRef]
106. Hirama, T.; Ishida, M.; Shirai, T. The Lateral Dispersion of Solid Particles in Fluidized Beds. Kagaku Kogaku Ronbunshu 1975, 1,
272–276. [CrossRef]
107. Mori, Y.; Nakamura, K. Solid Mixing in Fluidised Bed. Chem. Eng. 1965, 29, 868–875. [CrossRef]
108. Fan, L.T.; Shl, Y.F. Lateral Mixing of Solids in Batch Gas-Solids Fluidized Beds. Ind. Eng. Chem. Process Des. Dev. 1984, 23, 337–341.
[CrossRef]
109. Merry, J. Gulf stream circulation in shallow fluidized beds. Trans. Inst. Chem. Eng. 1973, 51, 361–368.
110. Grace, J.R. Processes. In AIChE Symposium Series; McGill Univ.: Montreal, QC, Canada, 1974.
111. Harris, B.J. Modeling options for circulating fluidized beds: A core/annulus deposition model. Circ. Fluid. Bed Technol. 1994,
32–39.
112. Grace, J.R.; Clift, R. On the two-phase theory of fluidization. Chem. Eng. Sci. 1974, 29, 327–334. [CrossRef]
113. Rowe, P.N. A model for chemical reaction in the entry region of a gas fluidised-bed reactor. Chem. Eng. Sci. 1993, 48, 2519–2524.
[CrossRef]
114. Sane, S.U.; Haynes, H.W.; Agarwal, P.K. An experimental and modelling investigation of gas mixing in bubbling fluidized beds.
Chem. Eng. Sci. 1996, 51, 1133–1147. [CrossRef]
115. Rowe, P.N. Two-Phase Theory and Fluidized Bed Reactor Models; ACS Symposium Series; ACS: Houston, TX, USA, 1978; Volume 65,
pp. 436–446. [CrossRef]
116. Darton, R. A Bubble growth theory of fluidised bed reactors. Trans. Inst. Chem. Eng. 1979, 57, 134–138.
117. Behie, L.A.; Kehoe, P. The grid region in a fluidized bed reactor. AIChE J. 1973, 19, 1070–1072. [CrossRef]
Energies 2022, 15, 388 37 of 38

118. Markhevka, V.I.; Basov, V.A.; Melik-Akhnazarov, T.K.; Orochko, D.I. The flow of a gas jet into a fluidized bed. Theor. Found. Chem.
Eng. 1971, 5, 80.
119. Kececioglu, I.; Yang, W.-C.; Keairns, D.L. Fate of solids fed pneumatically through a jet into a fluidized bed. AIChE J. 1984, 30,
99–110. [CrossRef]
120. Rowe, P.N.; MacGillivray, H.J.; Cheesman, D. Gas discharge from an orifice into a gas fluidised bed. Trans. Inst. Chem. Eng. 1979,
57, 194–199.
121. Kozin, V.E.; Baskakov, A.P. A study of the grating region of fluidized bed above bubble-cap-type gas-distributors. Chem. Technol.
Fuels Oils 1967, 3, 544–547. [CrossRef]
122. Baerns, M.; Fetting, F. Quenching of a Hot Gas Stream in a Gas Fluidized Bed. Chem. Eng. Sci. 1964, 20, 273–280. [CrossRef]
123. Merry, J.M.D. Fluid and particle entrainment into vertical jets in fluidized beds. AIChE J. 1976, 22, 315–323. [CrossRef]
124. Merry, J.M.D. Penetration of vertical jets into fluidized beds. AIChE J. 1975, 21, 507–510. [CrossRef]
125. Kunii, D.; Levenspiel, O.; Levenspiel, O. Fluidized Reactor Models. 1. For Bubbling Beds of Fine, Intermediate, and Large
Particles. 2. For the Lean Phase: Freeboard and Fast Fluidization. Ind. Eng. Chem. Res. 1990, 29, 1226–1234. [CrossRef]
126. Levenspiel, O.; Kunii, D.; Fitzgerald, T. The processing of solids of changing size in bubbling fluidized beds. Powder Technol. 1968,
2, 87–96. [CrossRef]
127. Cooke, M.J.; Harris, W.; Highley, J.; Williams, D.F. Kinetics of oxygen consumption in fluidized bed carbonizers. Tripart. Chem.
Eng. Conf. Symp. Fluid. I 1968, 30, 14–20.
128. Kumar, S.; Chadha, A.; Gupta, R.; Sharma, R. CATCRAK: A Process Simulator for an Integrated FCC-Regenerator System. Ind.
Eng. Chem. Res. 1995, 34, 3737–3748. [CrossRef]
129. de Lasa, H.I.; Errazu, A.; Barreiro, E.; Solioz, S. Analysis of fluidized bed catalytic cracking regenerator models in an industrial
scale unit. Can. J. Chem. Eng. 1981, 59, 549–553. [CrossRef]
130. Errazu, A.F.; de Lasa, H.I.; Sarti, F. Fluidized bed catalytic cracking regenerator model: Grid effects. Can. J. Chem. Eng. 1979, 57, 2.
131. Filho, R.M.; Batista, L.M.F.L.; Fusco, M. A fast fluidized bed reactor for industrial FCC regenerator. Chem. Eng. Sci. 1996, 51,
1807–1816. [CrossRef]
132. Faltsi-Saravelou, O.; Vasalos, I.A.; Dimogiorgas, G. FBSim: A model for fluidized bed simulation-II. Simulation of an industrial
fluidized catalytic cracking regenerator. Comput. Chem. Eng. 1991, 15, 647–656. [CrossRef]
133. Krishna, A.S.; Parkin, E.S. Modeling the regenerator in commercial fluid catalytic cracking units. Chem. Eng. Prog. 1985, 81, 55–62.
134. Penteado, J.C.; Rossi, L.F.; Negrão, C.O. Numerical Modelling of a FCC Regenerator. In Proceedings of the 17th International
Congress of Mechanical Engineering (COBEM), Sao Paulo, Brazil, 10–14 November 2003.
135. Fernandes, J.L.; Verstraete, J.J.; Pinheiro, C.I.C.; Oliveira, N.M.C.; Ramôa Ribeiro, F. Dynamic modelling of an industrial R2R FCC
unit. Chem. Eng. Sci. 2007, 62, 1184–1198. [CrossRef]
136. Daly, C.; Tidjani, N.; Martin, G.; Roesler, J. Détermination des Paramétres Cinétiques dans la Régénération des Catalyseurs de FCC;
Technical Report No. 56010; Institut Français du Pétrole (IFP): Paris, France, 2001.
137. Zwinkels, M. FCC Regenerator Simulation Model. Ph.D. Thesis, Institute Francais du Pétrole (IFP), Paris, France, 1997.
138. Shaikh, A.A.; Al-Mutairi, E.M.; Ino, T. Modeling and simulation of a downer-type HS-FCC unit. Ind. Eng. Chem. Res. 2008, 47,
9018–9024. [CrossRef]
139. Dasila, P.K.; Choudhury, I.; Saraf, D.; Chopra, S.; Dalai, A. Parametric Sensitivity Studies in a Commercial FCC Unit. Adv. Chem.
Eng. Sci. 2012, 2, 136–149. [CrossRef]
140. Kim, S.; Urm, J.; Kim, D.S.; Lee, K.; Lee, J.M. Modeling, simulation and structural analysis of a fluid catalytic cracking (FCC)
process. Korean J. Chem. Eng. 2018, 35, 2327–2335. [CrossRef]
141. Grace, J.R. Fluidized Bed Reactor Modeling; ACS Symposium Series; ACS: Washington, DC, USA, 1981; Volume 22, pp. 3–18.
[CrossRef]
142. Levenspiel, O. Difficulties in trying to model and scale-up the Bubbling Fluidized Bed (BFB) reactor. Ind. Eng. Chem. Res. 2008, 47,
273–277. [CrossRef]
143. Faltsi-Saravelou, O.; Vasalos, I.A. FBSim: A model for fluidized bed simulation-I. Dynamic modeling of an adiabatic reacting
system of small gas fluidized particles. Comput. Chem. Eng. 1991, 15, 639–646. [CrossRef]
144. Singh, R.; Gbordzoe, E. Modeling FCC spent catalyst regeneration with computational fluid dynamics. Powder Technol. 2017, 316,
560–568. [CrossRef]
145. de Lasa, H.I.; Grace, J.R. The influence of the freeboard region in a fluidized bed catalytic cracking regenerator. AIChE J. 1979, 25,
984–991. [CrossRef]
146. Cao, B.; Zhang, P.; Zheng, X.; Xu, C.; Gao, J. Numerical simulation of hydrodynamics and coke combustions in FCC regenerator.
Pet. Sci. Technol. 2008, 26, 256–269. [CrossRef]
147. Wu, C.; Cheng, Y.; Ding, Y.; Jin, Y. CFD-DEM simulation of gas-solid reacting flows in fluid catalytic cracking (FCC) process.
Chem. Eng. Sci. 2010, 65, 542–549. [CrossRef]
148. Latham, R.; Potter, O.E. Back-mixing of gas in a 6-in diameter fluidised bed. Chem. Eng. J. 1970, 1, 152–162. [CrossRef]
149. Rowe, P.N.; Partridge, B.A.; Cheney, A.G.; Henwood, G.A.; Lyall, E. Mechanisms of solids mixing in fluidised beds. Trans. Inst.
Chem. Eng. Chem. Eng. 1965, 43, T271.
150. Liu, D.; Chen, X. Lateral solids dispersion coefficient in large-scale fluidized beds. Combust. Flame 2010, 157, 2116–2124. [CrossRef]
Energies 2022, 15, 388 38 of 38

151. Olsson, J.; Pallarès, D.; Johnsson, F. Lateral fuel dispersion in a large-scale bubbling fluidized bed. Chem. Eng. Sci. 2012, 74,
148–159. [CrossRef]
152. Fan, L.T.; Song, J.C.; Yutani, N. Radial particle mixing in gas-solids fluidized beds. Chem. Eng. Sci. 1986, 41, 117–122. [CrossRef]
153. IPCC. Climate Change and Land an IPCC Special Report on Climate Change, Desertification, Land Degradation, Sustainable Land
Management, Food Security, and Greenhouse Gas Fluxes in Terrestrial Ecosystems; IPCC: Geneva, Switzerland, 2019.
154. le Quéré, C.; Andrew, R.M.; Friedlingstein, P.; Sitch, S.; Hauck, J.; Pongratz, J.; Pickers, P.A.; Korsbakken, J.; Peters, G.P.;
Canadell, J.G.; et al. Global Carbon Budget 2018. Earth Syst. Sci. Data 2018, 10, 2141–2194. [CrossRef]
155. Scala, F. Fluidized Bed Technologies for Near-Zero Emission Combustion and Gasification; Woodhead Publishing Limited: Cambridge,
UK, 2013.
156. Nakhaei, M.; Lu, B.; Tian, Y.; Wang, W.; Dam-Johansen, K.; Wu, H. CFD Modeling of Gas–Solid Cyclone Separators at Ambient
and Elevated Temperatures. Processes 2020, 8, 228. [CrossRef]
157. Wang, B.; Xu, D.L.; Chu, K.W.; Yu, A.B. Numerical study of gas–solid flow in a cyclone separator. Appl. Math. Model. 2006, 30,
1326–1342. [CrossRef]
158. Hashemi Shahraki, B. The Development and Validation of New Equations for Prediction of the Performance of Tangential
Cyclones. Int. J. Eng. 2003, 16, 109–124.
159. Lu, C.-X. FCC riser quick separation system: A review. Pet. Sci. 2016, 13, 776–781. [CrossRef]
160. Wei, Q.; Sun, G.; Yang, J. A model for prediction of maximum-efficiency inlet velocity in a gas-solid cyclone separator. Chem. Eng.
Sci. 2019, 204, 287–297. [CrossRef]
161. Chu, K.W.; Wang, B.; Xu, D.L.; Chen, Y.X.; Yu, A.B. CFD–DEM simulation of the gas–solid flow in a cyclone separator. Chem. Eng.
Sci. 2011, 66, 834–847. [CrossRef]
162. Masnadi, M.S.; Grace, J.R.; Elyasi, S.; Bi, X. Distribution of multi-phase gas–solid flow across identical parallel cyclones: Modeling
and experimental study. Sep. Purif. Technol. 2010, 72, 48–55. [CrossRef]
163. Zhang, R.; Basu, P. A simple model for prediction of solid collection efficiency of a gas–solid separator. Powder Technol. 2004, 147,
86–93. [CrossRef]
164. Jiang, Y.; Qiu, G.; Wang, H. Modelling and experimental investigation of the full-loop gas–solid flow in a circulating fluidized bed
with six cyclone separators. Chem. Eng. Sci. 2014, 109, 85–97. [CrossRef]
165. Baltrrnas, P.; Vaitiekūnas, P.; Jakštonienn, I.; Konoverskytt, S. Study of gas-solid flow in a multichannel cyclone. J. Environ. Eng.
Landsc. Manag. 2012, 20, 129–137. [CrossRef]
166. Su, Y.; Mao, Y. Experimental study on the gas–solid suspension flow in a square cyclone separator. Chem. Eng. J. 2006, 121, 51–58.
[CrossRef]
167. Lapple, C.E. Gravity and Centrifugal Separation. Am. Ind. Hyg. Assoc. Q. 1950, 11, 40–48. [CrossRef]
168. Gimbun, J.; Chuah, T.G.; Choong, T.S.Y.; Fakhru’l-Razi, A. A CFD Study on the Prediction of Cyclone Collection Efficiency. Int. J.
Comput. Methods Eng. Sci. Mech. 2006, 6, 161–168. [CrossRef]
169. Dirgo, J.; Leith, D. Aerosol Science and Technology Cyclone Collection Efficiency: Comparison of Experimental Results with
Theoretical Predictions. Exp. Results Theor. Predict. Aerosol Sci. Technol. 2007, 4, 401–415. [CrossRef]
170. Cortés, C.; Gil, A. Modeling the gas and particle flow inside cyclone separators. Prog. Energy Combust. Sci. 2007, 33, 409–452.
[CrossRef]
171. Morin, M.; Raynal, L.; Karri, S.B.R.; Cocco, R. Effect of solid loading and inlet aspect ratio on cyclone efficiency and pressure drop:
Experimental study and CFD simulations. Powder Technol. 2021, 377, 174–185. [CrossRef]
172. Rosin, P.; Rammler, E.; Intelmann, W. Principles and limits of cyclone dust removal. Zeit Ver Dtsch. Ing. 1932, 76, 433–437.
173. Maheshwari, F.; Parmar, A. A Review Study on Gas-Solid Cyclone Separator using Lapple Model. J. Res. 2018, 4, 1–5.
174. Hoffmann, A.C.; Stein, L.E. Computational Fluid Dynamics. Gas Cyclones and Swirl Tubes, Berlin, Heidelberg; Springer:
Berlin/Heidelberg, Germany, 2002; pp. 123–135. [CrossRef]
175. Chen, J.; Shi, M. A universal model to calculate cyclone pressure drop. Powder Technol. 2007, 171, 184–191. [CrossRef]
176. Knowlton, T.; Karri, R.S.B. Differences in cyclone operation at low and high solids loading. In Proceedings of the International
Fluidization South Africa Conference, Johannesburg, South Africa, 19–20 November 2008; pp. 119–160.
177. Li, S.; Yang, H.; Wu, Y.; Zhang, H. Improved cyclone pressure drop model at high inlet solid concentrations. Chem. Eng. Technol.
2011, 34, 1507–1513. [CrossRef]
178. Casal, J.; Martinez-Benet, J.M. A better way to calculate cyclone pressure drop. Chem. Eng. 1983, 90, 99–100.