energies

Article
Thermodynamic Analysis of CNG Fast Filling Process of
Composite Cylinder Type IV
Adam Saferna 1 , Piotr Saferna 1 , Szymon Kuczyński 1,2, * , Mariusz Łaciak 2 , Adam Szurlej 2
and Tomasz Włodek 1,2

1 Techplast Sp. z o.o., Krakowska 83 P, 34-120 Andrychów, Poland; [email protected] (A.S.);

[email protected] (P.S.); [email protected] (T.W.)
2 Gas Engineering Department, Drilling, Oil and Gas Faculty, AGH University of Science and Technology,
Mickiewicza 30 Av., 30-059 Kraków, Poland; [email protected] (M.Ł.); [email protected] (A.S.)
* Correspondence: [email protected]

Abstract: Due to ecological and economic advantages, natural gas is used as an alternative fuel in the
transportation sector in the form of compressed natural gas (CNG) and liquefied natural gas (LNG).
Development of infrastructure is necessary to popularize vehicles that use alternative fuels. Selected
positive factors from EU countries supporting the development of the CNG market were discussed.
The process of natural gas vehicle (NGV) fast filling is related to thermodynamic phenomena
occurring in a tank. In this study, the first law of thermodynamics and continuity equations were
applied to develop a theoretical model to investigate the effects of natural gas composition on the
filling process and the final in-cylinder conditions of NGV on-board composite cylinder (type IV).
Peng–Robinson equation of state (P-R EOS) was applied, and a lightweight composite tank (type





 IV) was considered as an adiabatic system. The authors have devised a model to determine the
influence of natural gas composition on the selected thermodynamic parameters during fast filling:
Citation: Saferna, A.; Saferna, P.;
Kuczyński, S.; Łaciak, M.; Szurlej, A.;
Joule–Thomson (J-T) coefficient, in-cylinder gas temperature, mass flow rate profiles, in-cylinder
Włodek, T. Thermodynamic Analysis mass increase, natural gas density change, ambient temperature on the final natural gas temperature,
of CNG Fast Filling Process of influence of an ambient temperature on the amount of refueled natural gas mass. Results emphasize
Composite Cylinder Type IV. Energies the importance of natural gas composition as an important parameter for the filling process of the
2021, 14, 5568. https://doi.org/ NGV on-board composite tank (type IV).
10.3390/en14175568
Keywords: compressed natural gas; alternative fuels; CNG tank; composite cylinder fast filling;
Academic Editor: Muhammad composite tank (type IV), energy storage
Abdul Qyyum

Received: 21 June 2021

Accepted: 30 August 2021
1. Introduction
Published: 6 September 2021
Natural gas is widely used in industry, energy sector, and residential. Due to ecological
Publisher’s Note: MDPI stays neutral
and economic advantages, natural gas is also increasingly used as an alternative fuel in the
with regard to jurisdictional claims in
transportation sector in the form of compressed natural gas (CNG) and liquefied natural
published maps and institutional affil- gas (LNG). The history of gaseous fuels used in internal combustion engines begins in
iations. 1860s when the French inventor Etienne Lenoir constructed the first two-stroke engine
powered by a mixture of town gas and air [1]. Since then, gaseous fuels have been used to
power vehicles, and they were the most popular in times of crisis related to the shortage of
conventional fuels [2,3]. A dynamic increase in the number of natural gas vehicles (NGV)
Copyright: © 2021 by the authors.
has been observed. In 2020, there were over 28.5 million vehicles. The world leader in the
Licensee MDPI, Basel, Switzerland.
use of CNG in transport is China, with over 6.7 million NGV vehicles, the next place Iran
This article is an open access article
4.9 million, and India with 3.3 million NGVs. The EU leaders are Italy with 1.1 million
distributed under the terms and NGV, Germany with 98,200 NGV, and Bulgaria with 69,800 NGV [4].
conditions of the Creative Commons Changes in the global natural gas market have been observed in recent years, including
Attribution (CC BY) license (https:// a significant increase in unconventional natural gas production, as well as the importance of
creativecommons.org/licenses/by/ LNG technology in international natural gas trading, which caused a decrease in natural gas
4.0/). prices [5–7]. In Poland, significant projects are planned, ongoing, or have been completed

Energies 2021, 14, 5568. https://doi.org/10.3390/en14175568 https://www.mdpi.com/journal/energies

Energies 2021, 14, 5568 2 of 19

to diversify natural gas supplies, including the LNG terminal in Świnoujście [8–10]. Thus,
it can be assumed that the use of natural gas as an alternative fuel in transport will be one
of the prospective segments of the Polish natural gas market.
To mitigate the environmental impact of transport, infrastructure development is
necessary to popularize vehicles that use electricity and other alternative fuels. Directive
2014/94/EU of the European Parliament and of the Council on alternative fuels infras-
tructure obliges Member States to deploy electricity charging infrastructure, refueling
stations for hydrogen and refueling stations for natural gas, including biomethane (RNG),
in gaseous form (CNG) and liquefied form (LNG) [11]. In terms of other alternative fuels
(biofuels, synthetic fuels), it remains up to the Member States. Natural gas infrastructure
should be deployed along the Trans-European Transport Network (TEN-T) by 2025 and in
urban and suburban areas [12]. The European Green Deal, published in December 2019,
presents the need to accelerate the shift towards sustainable and smart transport and the
use of alternative transport fuels [13]. NGVs require durable, lightweight, and safe tanks
to maintain regular vehicle size, weight, and driving range.
Natural gas as a transportation fuel has the potential to reduce emissions, and it is
justified to use compressed natural gas for transport purposes [14,15]. Development of tank
design can contribute to vehicle weight reduction and thus fuel consumption reduction.
High pressure cylinder design for the on-board storage of natural gas as fuel for vehicles
includes: (i) type I, which are made of metallic materials; (ii) type II, which has a metal
liner and hoop-wrapped composite reinforcement; (iii) type III, which has a metal liner
and a full wrapped composite reinforcement, and (iv) type IV, which have a non-metallic,
non-load sharing liner and a composite reinforcement on both the cylindrical part and
dome ends [16]. The advantage of using materials such polymers and fiber composites
for alternative fuel tanks is that they are light while offering high shock resistance and
long life.
The process of vehicle tank fast refueling lasts approx. 5 min. The standard service
pressure of the tank in the vehicle is 200 bar (the maximum pressure should not exceed
260 bar). The tanks are designed and tested to be refueled 1000 times a year during its
operation in the temperature range from −40 ◦ C to 65 ◦ C with the possibility of temporary
temperature increase to 82 ◦ C [16–18].
A few researchers have addressed the problem of modelling and thermodynamic
analysis of the filling process of cylinders with compressed natural gas. Kuntz modeled
the fast filling process of the tank with compressed natural gas based on the first law of
thermodynamics [19]. Farzaneh-Gord et al. studied the temperature effects on natural gas
in NGV cylinder during the fast filling process. The ideal and real gas were compared using
the Peng–Robinson equation of state (PR EOS), for the one-component system-methane,
which is the main component of natural gas [20,21]. Deymi-Dashtebayaz et al. modeled
a dynamic fast filling process of compressed natural gas to the vehicle’s cylinder using
PR EOS for methane. They investigated the influence of the initial pressure of the storage
reservoir on methane parameters in NGV cylinder at target pressure [22]. In another
manuscript, Farzaneh-Gord et al. presents the analysis of the reservoirs pressures and
temperatures on the performance of the cascade fueling station and compares these effects
between one-component systems: methane and hydrogen [23,24]. In 2014, Nahavandi and
Farzaneh-Gord investigated the flow and heat transfer during filling in natural gas vehicle’s
onboard cylinder type III. They employed Redlich–Kwong equation of state to determine
the thermodynamic properties of methane [25]. Deymi-Dashtebayaz et al. determined heat
transfer rate between in-cylinder flow and inner surface of cylinder wall and developed
a thermodynamic method to predict gas pressure and temperature variations inside the
cylinder and cylinder wall temperature during the refueling. On-board storage cylinders
types I and III were considered [26]. In their carefully designed study, Farzaneh-Gord et al.
provided a detailed theoretical analysis of the natural gas composition effects on the filling
process of an onboard natural gas vehicle cylinder for methane and selected Iran natural
gas compositions. Calculations were performed with AGA8 EOS [27]. Khamforoush
Energies 2021, 14, 5568 3 of 19

et al. developed the model of compression process of real natural gas and compared with
real data from CNG filling station. The polytropic work of a three-stage compressor was
considered [28]. Ramoutar offers a comprehensive thermodynamic analysis of Natural Gas
Vehicle cylinder refueling from a cascade reservoir using chilled natural gas and studied the
temperature effects on cylinder fill ratio [29]. There is a limited number of researchers and
research groups in the field of cylinder filling process modelling. Other research groups,
i.e., Zhang et al., studied the fast refill of compressed natural gas with active heat removal
and Taccani et al. performed analysis of the loading and unloading system of a CNG carrier,
equipped with lightweight cylinders [30,31].
Despite the interest in the modelling of cylinder filling with compressed natural gas,
there are also studies which have considered thermodynamic parameters during hydrogen
fast filling to cylinders (types III and IV) [32–42].
In this study, the main objective is to investigate the effects of natural gas composition
on an NGV on-board cylinder during the fast filling process. It was assumed that, during
filling, a lightweight cylinder (type IV) is connected to one reservoir tank. The theoretical
model was developed based on the mass and energy balance. Thermodynamic properties
of natural gas in the cylinder were calculated for selected time steps during the filling
process. The thermodynamic properties of natural gas mixtures are computed based on P-R
EOS and thermodynamics relationships. The influence of selected natural gas compositions
that occur in Polish gas transmission and distribution systems, has been analyzed for its
impact on the fast filling process.

2. Natural Gas Composition

Natural gas is a mixture of components with different properties, and therefore, the
thermodynamic properties of natural gas depend on their individual components. To know
the detailed natural gas properties during cylinder filling, the influence of its composition
should be considered. For this purpose, the Peng–Robinson equation of state (PR EOS)
was applied.
Presented in Table 1, the gas samples are similar in composition to the real natural
gas which occurs in the Polish natural gas transmission system. Natural gas in Poland
has different compositions which results from the genesis of natural gas. The natural gas
produced in the southern part of Poland (high-methane gas) has a different composition in
comparison to the gas supplied by the LNG terminal located in Świnoujście—northwest of
Poland (natural gas with a high content of ethane). In addition, nitrogen-rich natural gas
composition (Gas sample 5) which occurs in western Poland, is different due to production
from nitrogen-rich natural gas reservoirs located in the western part of Poland. Therefore,
CNG refueling stations, feed from various outlet points of the transmission/distribution
system, located in different places in Poland may differ slightly in composition (except for
nitrogen-rich gas). In addition, a hypothetical composition with the use of 3% hydrogen in
a mixture with methane was also considered (Gas sample 6) due to the development of
hydrogen technology and the recognition of hydrogen as one of the main energy carriers
in the future. To compare the calculation results with other studies, pure methane (Gas
sample 1) was also investigated. Gas sample 4 is an example of natural gas with heavier
additives (propane and butanes).
Selected for this research, real natural gas mixtures (Gas samples 2, 3, 5) may be
available at the refueling stations, which can be filled at the fast-refueling stations to
composite tanks (type IV) installed in NGV.t
Energies 2021, 14, 5568 4 of 19

Table 1. Mole fraction of natural gas from various outlet points of the transmission system in Poland
(Gas samples 2,3,5) and other gas samples.

Gas Sample No.

Chemical
Component 1 2 3 4 5 6
Formula
Concentration, [% Mol]
methane CH4 100 96.2 93.3 90 80.3 97
ethane C2 H6 - 2.6 6.3 6.5 0.3 -
propane C3 H8 - 1.1 0.3 2.5 - -
butane n-C4 H10 - - - 0.5 - -
isobutane i-C4 H10 - - - 0.5 - -
nitrogen N2 - 0.1 0.1 - 19.4 -
hydrogen H2 - - - - - 3

3. CNG Filling Station

There are two types of CNG infrastructure: time-fill and fast-fill. The main differences
between those two systems are: (i) available storage capacity and (ii) size of the compressor.
These factors determine the amount of fuel dispensed and the time it takes for CNG to be
fueled. The problem of long-time filling was solved by the infrastructure that allows filling
the NGV tank in time like vehicle refueling with gasoline or diesel (filling time less than
300 s). The filling time of an NGV tank in less than 300 s can be described as fast fill.
Fast filling process of a composite cylinder (type IV) with compressed natural gas.
To increase the utilization of compressor and reservoir tanks, CNG fast filling stations
operates in a buffer or cascade storage system and the reservoir tanks are arranged to
increase the pressure [43,44]. Figure 1 shows a schematic diagram of a cascade CNG fast
filling system. During the fast-filling process of a composite tank (type IV) installed in an
NGV, it is connected to a low-pressure reservoir tank. When the gas flow rate reaches a
predetermined rate, the system switches to the medium pressure tank and finally to the
high-pressure tank to complete filling. As a result, the high-pressure storage tank always
operates at a maximum pressure, ensuring that NGVs are always filled with the maximum
available gas flow rate. For calculation purposes, it was assumed that the pressure in
the reservoir tank is not changing during the fast-filling process of the composite tank
(type IV).

Figure 1. Scheme of the fast-filling process (cascade storage) of the composite tank (type IV).
Energies 2021, 14, 5568 5 of 19

4. Thermodynamic Analysis of a CNG Composite Tank (Type IV) Fast Filling Process
To perform calculations and to develop a thermodynamic model of the composite tank
(type IV) fast filling process, it was assumed that a composite CNG tank (type IV), installed
in an NGV, is considered as an open thermodynamic system that goes through a quasi-
static filling process. To determine the selected thermodynamic parameters, the continuity
equation and the first law of thermodynamics were applied. Another assumption was to
assume a constant volume of the composite tank (type IV) which has only one entry point
(inlet). Based on the above assumptions, the continuity equation (conservation of mass
principle) can be written in the form of Equation (1):

. dmc
mi = (1)
dt
.
In Equation (1), mi is the inlet mass flow rate which can be calculated as natural gas
expansion in the orifice (cylinder inlet) [19,27].

 1/γ (  "  γ − 1/γ #)1/2

. P 2γ PR PC
mi = Cd ·ρ R · Aori f ice · C · 1− (2)
PR γ−1 ρR PR

if: γ/γ − 1
PC 2
≤
PRγ+1
 γ + 1/2(γ − 1)
. p 2γ
mi = Cd γPR ρ R Aori f ice (3)
γ−1
if: γ
 
PC 2 γ −1
>
PR γ+1
Equation (2) is valid for subsonic flow, while Equation (3) is for sonic conditions. The
discharge coefficient Cd was introduced to account the irreversibility of the flow through
the orifice. The first law of thermodynamics for a specific volume of a composite tank can
be written in general form as the following Equation (4):
! !
Vi2 Vi2 V2
  
. . . d .
Qcv + ∑ mi hi + + gzi = ∑ me he + + gze + m u+ + gz + W cv (4)
2 2 dt 2 cv

The work in the filling process is equal to zeroandtherefore the potential energy and
V2
kinetic energy change in the NGV composite tank 2 can be neglected. The equation
cv
can be simplified as shown below:
!
dUC . . V2
= Q + mi hi + i (5)
dt 2

By applying the energy balance equation for the reservoir tank, it was obtained
V2
hi + 2i = h R . In this case, it is assumed that the conditions of the reservoir tank do not
change, so h R remains constant during the filling process. By substituting h R into Equation
(5), the following equation was obtained:

dUC . .
= Q + mi h R (6)
dt
The heat loss from the NGV composite tank to the environment can be written as:
.
Q = −UHC AC ( TC − Tamb ) (7)
Energies 2021, 14, 5568 6 of 19

Heat transfer coefficient of the composite tank UHC represents the heat exchange rate
between natural gas in the cylinder and the environment. A higher UHC value means a
lower final in-cylinder condition. Combining Equations (1), (6), and (7), the following
equation was obtained:

d (mC uC ) dmC
= −UHC AC ( TC − Tamb ) + hR (8)
dt dt
or after transformation:
d (mC uC ) d
− (mC h R ) = −UHC AC ( TC − Tamb ) (9)
dt dt
The above equation can be transformed to the following form:

d(mC uC − mC h R ) = −UHC AC ( TC − Tamb )dt (10)

Equation (10) was integrated within the limits from the start of the integration process
“s” to the next time step of the filling process “r”, as shown in Equation (11):

Zr Zt
d (mC uC − mC h R ) = − UHC AC ( TC − Tamb )dt (11)
s 0

The result of integration for one reservoir tank of the fast-filling station is shown below:

mCr (uC − h R ) − mCs (uC − h R ) = −UHC AC · Tav t (12)

where
mCr —the mass of natural gas filled for the “last/recent” step;
mCs —the mass of natural gas filled at the “start” of the filling process;
The average temperature difference between the composite tank and the environment
∆Tav is defined as:
Zt
1
∆Tav = ( TC − Tamb )dt (13)
t
0

Finally, the first law of thermodynamics for the filling of a composite tank installed in
NGV can be written in the form of Equation (14):

UHC AC ∆Tav t mCs

uC = h R − + (m − h R ) (14)
mCr mCr Cs

Equations (2), (3), and (14) can be applied to calculate the thermodynamic properties
of natural gas (density and internal energy) in a composite tank at any time during the
filling process. In the case of an adiabatic system, Equation (14) can be simplified and
written as:
mCs
uC = h R + (U − h R ) (15)
mCr Cs
If mCs = 0, the following relationship is valid at any time during the composite tank
filling process:
uC = h R (16)

5. Calculation of Natural Gas Thermodynamic Properties

As mentioned in the previous chapter of this study, it is necessary to determine several
thermodynamic parameters of natural gas to analyze the filling process of the composite
tank. These parameters are i.e., density (or specific volume) and internal energy. This
Energies 2021, 14, 5568 7 of 19

chapter explains how these properties were calculated. Detailed methods for calculating
most of the thermodynamic parameters of natural gas can be found in [26,27,45,46].

5.1. Peng–Robinson Equation of State

The Peng–Robinson equation of state (PR EOS) is one of the most popular equations
for describing the PVT (Pressure-Volume-Temperature) behavior of real pure substances
and their mixtures. This equation has the following form as seen in Equation (17) [47]:

RT am
p= − (17)
v − bm v ( v + bm ) + bm ( v − bm )

Parameters am and bm are defined by classical mixing rules:

am = ∑ ∑ zi z j ami,j (18)
i j

bm = ∑ z i bi (19)
i

Other parameters of the PR EOS are defined as:

p
ami,j = 1 − δij · ai αi a j α j (20)
" s !#2
T
αi = 1 + κi 1 − (21)
Tcri

where
κi = 0, 379642 + 148503ωi − 0, 164423ωi 2 + 0, 016666ωi 3 (22)
R2 Tcri 2
ai = 0, 45724· (23)
pcri
RTcri
bi = 0, 07780· (24)
pcri
In the PR EOS, the compressibility factor Z is defined as:
   
Z3 + ( B − 1) Z2 + A − 3B2 − 2B Z + B3 + B2 − AB = 0 (25)

where PR EOS dimensionless coefficients are determined according to the following formula:
am p
A= (26)
R2 T 2
bm p
B= (27)
RT
From the general form of the real gas equation of state, the molar density can be deter-
mined:
p
ρm = (28)
ZRT

5.2. Enthalpy and Joule–Thomson Coefficient Calculation

Enthalpy (h) was determined according to Equation (29)

h = hid + hres (29)

Energies 2021, 14, 5568 8 of 19

where hres is the residual enthalpy given by the following formula:

  √  
T da m
− a m
Z+ 1+ 2 B
hres = RT ( Z − 1) + dT√ ·ln  √   (30)
2 2bm Z+ 1− 2 B

and hid is the ideal gas enthalpy calculated from a given polynomial function [47]:
 2  3  4
T T T
T B · 1000 C · 1000 D · 1000 1000· E
hid = A· + + + − + F − H + hid298.15K (31)
1000 2 3 4 T
where
A, B, C, D, E, F, H—empirical coefficients;
T—temperature [K]/1000;
hid298.15K — ideal gas enthalpy in 298.15 K;
Calculated change of the compressibility factor Z during the composite tank (type IV)
filling process with the considered natural gas mixtures and gas samples is presented on
Figure 2.

Figure 2. Change of the compressibility factor Z during the filling process of the composite tank (type IV) for the considered
natural gas mixtures and samples.

Isobaric heat capacity was determined according to Equation (32):

C p = C pid + C pr (32)

where

 √  ∂B

 √
 2
  √  
−
2 − 1 ∂T T d a2m − am
∂Z ∂Z ∂B
+ 1 + 2 ∂T Z+ 1+ 2 B
!
T dam − am
 
∂Z ∂T p p ∂T p p
C pres = R· T +Z−1 + dT√ ·  √  −  √   + dT√ ·ln  √   (33)
∂T p 2 2bm Z+ 1+ 2 B Z− 1− 2 B 2 2bm Z+ 1− 2 B

Ideal gas heat capacity Cpid is calculated from empirical polynomial functions [48]:
   2  3
T T T E
C pid = A + B· + C· + D· + 2 (34)
1000 1000 1000 T
1000
Energies 2021, 14, 5568 9 of 19

Joule–Thomson coefficient is defined with the application of PR EOS according to the

following Equation (35):
  "   # "   !! #
∂T 1 ∂v 1 R ∂Z
µ J-T = = T −v = T T +Z −v (35)
∂P h Cp ∂T p Cp p ∂T p

5.3. Internal Energy Calculation

By assuming that the internal energy is a function of temperature and molar specific
volume, the residual internal energy function is defined by Equation (36) [27]:

Zvm
"   #
∂P
um − umid = T − P dvm (36)
∂T vm
vm,I →∞

where
um —molar internal energy of real gas;
umid —molar internal energy of ideal gas.
By using Equation (28), the partial derivative in Equation (36) can be calculated from
the following equation:
    "   #
∂P ∂P ∂Z
= = Rρm Z + T (37)
∂T vm ∂T ρm ∂T ρm

By substituting Equation (37) in Equation (36) and by replacing the variable vm with
ρm , the equation will be obtained that will enable the calculation of the internal energy [49]:

Zρm 
2 ∂Z dρm
um − umid = − RT (38)
∂T ρm ρm
0

To calculate the molar internal energy of an ideal gas, the following equation was used:

umid = hmid − pvm = hmid − RT (39)

In Equation (39), hmid is the molar enthalpy of an ideal gas, calculated with the
following equation:
n
∑ x j hm,i
j
hmid = (40)
j =0

where
j
hm,i —molar enthalpy for component j in the ideal gas mixture;
Internal energy per mass unit was calculated from Equation (41):
um
u= (41)
M
The procedure for calculating the selected properties of natural gas in a composite
tank (type IV) begins with the indication of the initial conditions (pressure and temper-
ature). The remaining initial thermodynamic properties, including the enthalpy of the
reservoir tank h R = u R + ( pv) R , are calculated using the Peng–Robinson equation of state.
Equation (2) or (3) is used to calculate the inlet mass flow. Equation (1) is used to calculate
the natural gas mass in a composite tank (type IV), and then the specific volume of natural
gas stored in the composite tank is calculated using the gas density. Equation (15) was
solved to calculate the specific internal energy of natural gas in the composite tank in
the new time period. When the specific internal energy and specific volume were deter-
Energies 2021, 14, 5568 10 of 19

mined, the remaining properties (e.g., compressibility factor, gas density, Joule–Thomson
coefficient) were calculated using the P-R equation of state.

6. Results and Discussion

This study analyzes the scenario in which a composite tank was installed in a NGV
and was considered as an adiabatic system. As a result of this assumption, the orifice
diameter and the mass flow rate at the inlet to the composite tank have no effect on the
final in-cylinder temperature and pressure. The orifice diameter and cylinder volume
were assumed to be 1 mm and 50 L, respectively. It was also assumed that the discharge
coefficient of the orifice Cd (at the inlet to the composite tank) is equal to one. The results
are presented for a single reservoir tank as shown in Figure 3.

Figure 3. Thermodynamic scheme of the investigated system (buffer storage).

The Joule–Thomson coefficient µ J-T plays an important role during the composite tank
fast filling process. A gas with a positive µ J-T coefficient cools down during the expansion.
The change in temperature with respect to pressure is directly related to the value of the
µ J-T coefficient. It is advisable to determine this coefficient during the filling process of the
composite tank [22,50].
Figure 4 shows the influence of natural gas composition on the µ J-T coefficient in the
cylinder during the filling process under the initial conditions of 300 K and 0.101325 MPa.
Data analysis presented in Figure 4 shows that in the initial stage of composite tank
filling, there occurs an increase of the J-T coefficient. The J-T coefficient is positive through-
out the filling process, so the gas temperature should decrease as the pressure decreases.
Comparing the values of the J-T coefficient for different natural gas compositions, it can
be noticed that µ J-T is higher for mixtures with lower methane content in the composition
(for gas samples 4, 3, 2). For nitrogen-rich gas (Gas sample 5), the J-T coefficient ratio is
the lowest among the analyzed samples. The results obtained are consistent with those
obtained by Farzaneh-Gord et al. 2014 [27]. The maximum value of J-T coefficient for pure
methane is slightly higher—this can be a result of different initial pressure in the reservoir
tank and the use of different EOS.
Figure 5 shows the influence of natural gas composition on the gas temperature
inside the composite tank during the filling process (for the assumed initial conditions of
T = 300 K and p = 0.101325 MPa). The analysis of the results shows that the temperature of
the natural gas in the composite tank decreases at the beginning of the refueling process.
The reason of the natural gas temperature drop at the early stage of composite tank filling
is the Joule–Thomson effect which occurs during the isenthalpic expansion on the orifice
(from the inlet pressure of 21 MPa which is set in the reservoir tank, to the initially low
pressure in the composite tank 0.101325 MPa) [22,49]. During the fast filling process, the
natural gas is injected to the composite tank, mixes with the gas initially contained in
the tank, and compresses it. Since there is low pressure in the tank initially, this causes
Energies 2021, 14, 5568 11 of 19

that the temperature of the natural gas injected into the tank initially decreases due to
isenthalpic expansion.

Figure 4. In-cylinder Joule–Thomson coefficient changes for the considered natural gas mixtures during the composite tank
fast filling process: (a) vs. pressure change in the composite tank; (b) vs. filling time of the composite tank.

The lowest natural gas temperature in the composite tank occurs at the highest calcu-
lated J-T coefficient. When the compression process and the conversion of the supplied
enthalpy to internal energy in the composite tank overcome the cooling effect of the
Joule–Thomson effect (which decreases with the pressure increase in the cylinder), the tem-
perature of the natural gas in the composite tank begins to increase. The gas temperature
increases quickly as the initial quantity of gas in the composite tank is low and increases
rapidly with the fueling process (Figure 5). The natural gas temperature increase in the
composite tank during the fueling process slightly slows down due to the influence of
lower ambient temperature and lower dynamics of the compression process in the final
phase (decrease in mass fueling efficiency).
The analysis of the temperature profiles presented in Figure 5, shows that the lowest
gas temperature during filling corresponds to the natural gas sample with the lowest
methane content in the composition (Gas sample 4, for gas with the highest coefficient µ J-T ),
but it should be noted that this does not apply to nitrogen-rich natural gas (Gas sample 5),
where nitrogen significantly reduces the Joule–Thomson effect. At the end of the refueling
process, a temperature difference of about 11 K occurs for the natural gas sample with
the highest methane content (Gas sample 2) and the natural gas sample with the lowest
methane content (Gas sample 4). It should also be noted that the maximum difference
in the final gas temperature in the tank is higher, considering nitrogen-rich natural gas
sample (Gas sample 5), which is 20 K. Obtained results are consistent with those presented
in different articles [20,22,27]. The decrease of methane temperature at the beginning of the
Energies 2021, 14, 5568 12 of 19

filling process is slightly higher—this can be a result of different cylinder volume and the
use of different EOS.

Figure 5. Temperature changes of the considered natural gas mixtures during the composite tank fast filling process: (a) vs.
pressure change in the composite tank; (b) vs. filling time of the composite tank.

Figure 6 shows the mass flow rate profiles during the composite tank filling process
for selected compositions of natural gas at constant initial conditions: ambient temperature
T = 300 K and pressure p = 0.101325 MPa. Analysis of the results shows that at the early
stage of filling, the mass flow rate is constant due to a chocking effect formed on the tank
orifice (inlet). The highest value of the mass flow rate occurs for the high-methane natural
gas with the lowest content of methane in the composition (Gas sample 4). It is caused due
to the higher density of natural gas with this composition.
Energies 2021, 14, 5568 13 of 19

Figure 6. Mass flow rate change of the considered natural gas mixtures during the composite tank fast filling process: (a) vs.
pressure change in the composite tank; (b) vs. filling time of the composite tank.

It should also be mentioned that nitrogen-rich gas (Gas sample 5) has the highest
molar mass, but the mass flow rate is only slightly higher than in the case of pure methane,
because nitrogen-rich gas has the highest compressibility factor among the selected samples.
Figure 6 presents the effect of the natural gas composition on the mass flow profile during
the composite tank filling process. Obtained results are consistent with those presented
in other works [20,22,27]. The initial mass flow rate for methane is 0.035 kg/s. The time
required to reach the final pressure (20 MPa) in the cylinder is about 220 s. Compared to
other works, the filling time is shorter, due to the adoption of a smaller tank volume for
the calculation.
Figure 7 shows the in-cylinder mass increase during the composite cylinder (type IV)
fast filling process. The mass of gas in the composite tank is expected to be higher for the
natural gas with higher density. The density is higher for a gas with a lower temperature
and lower methane content. The gas temperature in the composite tank is also lower for
low-methane gas (Gas samples 4, 3, 2), with no significant nitrogen content (see Figure 5).
The final mass accumulated in the composite tank (after the filling process is complete) is
slightly higher (0.5 kg) for nitrogen-rich natural gas with the lowest content of methane
(Gas sample 5) compared to pure methane. In the case of high-methane gas with the lowest
methane content (Gas sample 4), the weight of compressed natural gas is about 1.2 kg
more than in the case of pure methane. This relationship shows the significant influence of
natural gas composition on the fast filling process of a composite tank (type IV).
Energies 2021, 14, 5568 14 of 19

Figure 7. In-cylinder mass increase for the considered natural gas mixtures during the fast filling process of the composite
tank (type IV).

Figure 7 shows the effect of natural gas composition on the composite tank filling
time. The analysis shows that there is difference between the time profiles for the different
natural gas compositions. The slight influence of the gas composition on the filling time
results in two opposing effects. The mass flow rate at the inlet of the composite tank for gas
with a lower methane content is higher (Gas sample 4), so the time should be shorter (not
for nitrogen-rich gas). On the other hand, the mass accumulated in the cylinder is greater
for such gas, so it takes more time to fill the composite tank. Obtained results are consistent
with those presented in other works [20,22,27]. The final in-cylinder mass of methane is
about 7 kg, reached after about 220 s. Compared this result with other works, the filling
time is shorter, due to the conjunction with a smaller tank volume for the calculation (50 l
tank in this work vs. 67 l) and thus a lower accumulated mass of methane (7 kg in this
work vs. 8 kg).
Figure 8 shows the profiles of natural gas density changes in the composite tank
during the fueling process. The results for the obtained profiles of density changes are
consistent with the profiles of gas mass increase in the tank (Figure 7).

Figure 8. Density profiles for the considered natural gas mixtures during the fast filling process of the composite tank
(type IV).
Energies 2021, 14, 5568 15 of 19

Figure 9 shows the influence of the ambient temperature on the final natural gas
temperature for the various gas compositions at the end of fast filling process. The analysis
of the results shows that the final gas temperature in the composite tank is the highest
for nitrogen-rich gas (Gas sample 5). Natural gas mixtures with a higher percentage of
methane also exhibit high final temperatures (including methane and methane with 3%
hydrogen blend).

Figure 9. Influence of initial temperature (ambient) on the final in-cylinder temperature for the considered natural
gas mixtures.

Mixtures of natural gas samples 4, 3, and 1 showed the lowest values of the final
gas temperature after the filling process. It is essential that increasing the initial ambient
temperature causes a linear increase of the final gas temperature in the composite tank.
Moreover, other studies [25] showed that the initial gas temperatures in the tank (type III
and type IV) and in the reservoir tank (ambient temperature) have an important impact on
the natural gas properties after composite tank fast filling completion. Obtained results are
consistent with those presented in other works [20,22]. The final in-cylinder temperature
for methane is about 350 K, with the initial gas temperature 300 K. Comparing this result
with the other, it shows that the final in-cylinder temperature is similar.
Figure 10 shows the effect of an ambient temperature (corresponding to the gas
temperature) on the amount of gas mass filled into the composite tank—for different
natural gas compositions. As mentioned earlier, the amount of gas filled into the composite
tank has a direct impact on the range of the NGV and is one of the major problems
associated with the NGV industry.

Figure 10. Influence of the initial (ambient) temperature on the mass of fueled natural gas mixtures and samples.
Energies 2021, 14, 5568 16 of 19

The analysis showed that the mass of the fueled gas decreases with the increase of the
ambient temperature in which the process of the composite tank filling has been carried
out. It can be observed that the difference of the fueled mass for the considered different
natural gas compositions decreases with the ambient temperature increase. As the ambient
temperature decreases, the amount of gas refilled into the composite tank increases, so it
can be concluded that the tanks should be filled at lower ambient temperatures (rather at
night than during the day). The weight of the fueled gas is the highest for the gas mixtures
with the highest density (Gas samples 4, 3, 2). For nitrogen-rich gas, due to the higher
compressibility factor, the mass of the refueled natural gas (Gas sample 5) decreases slower
with the increase of the ambient temperature. Obtained results are consistent with those
presented in other works [22,27]. The final in-cylinder mass of methane (Gas sample 1)
is about 7 kg for the initial gas temperature 300 K. Comparing this result to the other, it
shows that the final in-cylinder mass is higher, due to the conjunction with a smaller tank
volume for the calculation (50 l tank in this work vs. 67 l) and thus a lower accumulated
mass of methane (7 kg in this work vs. 8 kg).

7. Conclusions
In this study, the first law of thermodynamics and continuity equations were applied
to develop a theoretical model to investigate the effects of natural gas composition on the
filling process and the final in-cylinder conditions of NGV on-board composite cylinder
(type IV). Properties of various gas samples were calculated with PR EOS. Samples were
selected based on the composition which occurs in the Polish distribution and transmission
system. The results of this study show that: (i) J-T coefficient is higher for mixtures with
a lower methane content in the composition; (ii) at the end of the refueling process, the
maximum difference in the final gas temperature in the tank is higher, considering nitrogen-
rich gas sample, which is 20 K; (iii) the highest value of the mass flow rate occurs for the
high-methane natural gas with the lowest content of methane in the composition (Gas
sample 4); (iv) for high-methane gas with the lowest methane content (Gas sample 4), the
weight of compressed natural gas is about 1.2 kg more than in the case of pure methane;
(v) increase in the initial ambient temperature causes a linear increase of the final gas
temperature in the composite tank, which in this study is highest for nitrogen-rich natural
gas (Gas sample 5); (vi) analysis of influence of an ambient temperature on the amount of
the refueled natural gas mass showed that the weight of the fueled gas is the highest for
the natural gas mixtures with the highest density (Gas samples 4, 3, 2). For nitrogen-rich
natural gas, due to the higher compressibility factor, the mass of the refueled gas (Gas
sample 5) decreases slower with the increase of the ambient temperature.
Main practical aspects of this research are related to the influence of natural gas
composition on the fast-refueling process. Composition of natural gas has an influence
on the time of fast-filling NGV cylinder and compressor performance due to the filling
process. This process should be as short as possible and during this time the tank should
be filled with as much gas as possible. The temperature of CNG during the filling process
is essential to the final process conditions and process safety standards. Furthermore, the
charged mass is different for each natural gas composition and it has a direct influence on
the driving range.
These results emphasize the importance of natural gas composition as an important
parameter for investigating the filling process of the NGV on-board composite tank (type
IV) as a practical issue.
In the next research step, the authors plan to perform experimental tests on the
developed ultralight composite tanks (type IV) that will allow calibration of the model (i.e.,
measurements of in-cylinder pressure and temperature).
Energies 2021, 14, 5568 17 of 19

Author Contributions: Conceptualization, S.K., T.W. and P.S.; methodology, S.K. and T.W.; validation,
S.K. and T.W.; investigation, S.K.; resources, S.K.; data curation, T.W. and S.K.; writing—original
draft preparation, S.K. and T.W.; writing—review and editing, A.S. (Adam Saferna), P.S., M.Ł. and
A.S. (Adam Szurlej); visualization, T.W. and S.K.; supervision, S.K.; funding acquisition, A.S. (Adam
Saferna) and P.S. All authors have read and agreed to the published version of the manuscript.
Funding: This research was supported by RPO WM, RPMP.01.02.01-IP.01-12-072/18.
Acknowledgments: Special thanks to Piotr Ryba.
Conflicts of Interest: The authors declare no conflict of interest.

Nomenclature

Symbols
A Area (m2 )
A, B dimensionless Peng–Robinson EOS coefficients
ai , bi Peng–Robinson EOS constants
Cd Orifice discharge coefficient
Cp Isobaric heat capacity (kJ/kg·K)
Cv Isochoric heat capacity (kJ/kg·K)
g Gravitational acceleration (m/s2 )
h Specific enthalpy (kJ/kg)
hm Molar enthalpy (kJ/kmol)
.
m Mass flow rate (kg/s)
M Molecular weight (kg/kmol)
p Pressure (bar or Pa)
.
Q Heat transfer rate (kW)
R universal gas constant (kJ/(kmol·K)
t Time (s)
T Temperature (K or ◦ C)
u Internal energy (kJ/kg)
um Molar internal energy
UHC Heat transfer coefficient (W/(m2 K))
v Specific volume (m3 /kg)
vm Molar specific volume (m3 /mol)
V Velocity (m/s)
W Actual work (kJ/kg)
.
W Actual work rate (kW or MW)
z Height (m)
Z Compressibility factor
Greek letters
α Soave alpha function
δij Binary coefficient
ρ Density (kg/m3 )
ρm Molar density (mol/m3 )
ρr Reduce density
γ Isentropic exponent
µJ-T Joule–Thomson coefficient (K/MPa)
ω Acentric factor
Energies 2021, 14, 5568 18 of 19

Subscripts
C NGV onboard cylinder
cr Critical
cv Control volume
R Reservoir tank
id Ideal gas
I Initial or inlet condition
r Recent
res Residual
S Start of filling process
amb Ambient
av Average

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