water

Review
Could Plant-Based Flocculants Substitute the Conventional
Synthetic Chemicals in the Sludge Dewatering Process?
Yosra Hadj Mansour 1,2 , Bouthaina Othmani 1 , Faouzi Ben Rebah 3, * , Wissem Mnif 4 , Mongi Saoudi 2
and Moncef Khadhraoui 1

1 Laboratory for Environmental Engineering and Ecotechnology, ENIS, University of Sfax,

P.O. Box 1173, Sfax 3038, Tunisia; [email protected] (Y.H.M.);
[email protected] (B.O.); [email protected] (M.K.)
2 LR22ES01 Laboratory of Biomathematics, Faculty of Sciences of Sfax, Department of Mathematics,
P.O. Box 1171, Sfax 3000, Tunisia; [email protected]
3 Higher Institute of Biotechnology of Sfax (ISBS), University of Sfax, P.O. Box 263, Sfax 3000, Tunisia
4 Department of Chemistry, Faculty of Sciences at Bisha, University of Bisha, P.O. Box 199,
Bisha 61922, Saudi Arabia; [email protected]
* Correspondence: [email protected]

Abstract: Due its high water content, sewage sludge dewatering is not just a simple operation; rather,
it is a challenging process and a costly management task. Its final handling is usually preceded by
several dewatering steps, and among them is the conditioning process known as the flocculation
stage, which is carried out using synthetic chemical reagents. Despite the abilities of these additives to
reduce sludge volume and extract its bound waters, they are suspected to cause serious environmental
and health threats. Their substitution by natural and efficient additives originating from plant extracts
could thus be a safe and an eco-friendly alternative, overcoming ecosystem damages. It is within this
context that the present review paper critically investigates the efficacy and feasibility of plant-based
flocculants, aiming to enhance sludge dewatering and dispense with environmental burdens. To
do so, the types of the conventional chemical flocculants, their drawbacks, and their impacts on
the ecosystem and human health were addressed. In parallel, the potential dewatering efficiency
Citation: Hadj Mansour, Y.; Othmani, of plant extracts toward sludge treatment was compiled, and their mechanistic dewatering paths
B.; Ben Rebah, F.; Mnif, W.; Saoudi,
performances were thoroughly discussed. The challenges associated with dewatered sludge and its
M.; Khadhraoui, M. Could
potential exploitation were also highlighted to motivate scientific communities to further explore
Plant-Based Flocculants Substitute
green resources for sludge processing. It is suggested that green resources such as Moringa, Cactus,
the Conventional Synthetic
Aloe, and Okra could be used as green flocculants instead of chemical ones, which would provide a
Chemicals in the Sludge Dewatering
Process? Water 2023, 15, 2602. promising and eco-sustainable approach to sludge dewatering and might represent a path towards
https://doi.org/10.3390/w15142602 an environmentally friendly and clean technology.

Academic Editors: Sílvia Santos

Keywords: sludge; dewatering; conditioning; chemical flocculants; plant-based flocculants
and Xufei Yang

Received: 13 June 2023

Revised: 7 July 2023
Accepted: 11 July 2023 1. Introduction
Published: 18 July 2023
With the aim of protecting ecosystems and ensuring the continuity of human life, great
efforts have been devoted to wastewater remediation and its related technologies. Yet,
despite the well-established paths therein and the effectiveness of conventionally applied
wastewater treatment processes, it is believed that their associated sludge is one of the
Copyright: © 2023 by the authors.
Licensee MDPI, Basel, Switzerland.
detrimental causes behind environmental and human health degradation, primarily if
This article is an open access article
they are disposed of without efficient treatment means [1]. Furthermore, in addition to its
distributed under the terms and unpleasant odor and high quantity of suspended solids (SS) content, the presence of large
conditions of the Creative Commons amounts of water therein renders its management more challenging, and its transport to
Attribution (CC BY) license (https:// the final drying beds is very costly. Its dewatering is hence a crucial step towards ensuring
creativecommons.org/licenses/by/ successful solid–liquid separation, reducing its volume, and alleviating its handling charge.
4.0/). To do so, the sludge is usually conditioned in advance to promote its associated water

Water 2023, 15, 2602. https://doi.org/10.3390/w15142602 https://www.mdpi.com/journal/water

Water 2023, 15, 2602 2 of 14

removal and extend the life of the mechanical devices used for dewatering (plate and
membrane filter presses), which are precious and energy-consuming [2].
This latter task is usually performed via the supply of synthetic flocculants, also
called synthetic conditioners, such as aluminum sulphate, poly-aluminum chloride, ferrous
chloride, and polyacrylamide [3,4]. The key role of these chemicals is to agglomerate the
suspended matter into large and settleable flocs and free them from the water to which
they are bound. Consequently, the sludge volume will be reduced upon the release of the
trapped water into solid particles, thus leading to an increase in its settling velocity and
compactness [5]. However, in spite of their efficiency in facilitating solid–liquid separation,
the effective application of these chemicals is doubtful, as it is reported to cause serious
environmental burdens; thus, it is a growing human health concern [6].
In fact, due to their nonbiodegradability, metal salts and organic polymer residues may
accumulate in the treated sludge and thus hinder its usage. Further, if valorized in agricul-
ture, those residues may leach out into soil and groundwater, endangering fauna, flora, and
human health [7]. Likewise, it is accepted that severe diseases such as Alzheimer’s disease
and neurotoxic and carcinogenic illnesses have been ascribed to the extensive application
of these chemicals in wastewater treatment and sludge dewatering [8,9]. Additionally, the
high cost and non-availability of such chemicals, especially in developing countries, could
represent the main hurdles to their supply. Taking these drawbacks and limitations into
consideration, in sludge conditioning, replacing chemical flocculants with natural ones
derived from plant extracts is both worth considering and deemed to be a safe and environ-
mentally friendly option. In this vein, although some prior studies have highlighted the
uses of some plant-based flocculants (such as Moringa [10], Cactus [11], and Okra [12]) as
surrogates for their chemical equivalents, and although they have been evaluated for their
sludge-dewatering performance, the application of green conditioners in this field, com-
pared to the conventional synthetic flocculants that are extensively exploited in wastewater
treatment plants, is still in its infancy, [13–16]. In order to persuade environmentalists and
stakeholders to invest in the replacement of chemical flocculants with safe and green ones,
additional works exploring natural flocculants in the dewatering process are required.
Thus, the present review paper sheds light on the feasibility of using plant-based floc-
culants for sludge dewatering and offers a comparison of their performance with those of
their chemical equivalents. Although previous reviews and studies mention other biofloccu-
lants derived from animals, plants, or microorganisms, the majority of these works focused
on sludge composition, conditioning, and dewatering methods [17–19]. It is also worth
noting that flocculants originating from animals or microorganisms are difficult to acquire
and require sophisticated technology and substantial precautions. Furthermore, most of the
recent review articles presented a holistic summary of the coagulation/flocculation process
in sludge dewatering [20], i.e., they reviewed the commonly used chemical and natural
flocculants without comparing their dewatering capabilities. Few reviews have discussed
and assessed the potential use of plant-based flocculants instead of chemical ones for sludge
treatment [21]. As a result, and as has already been indicated, this paper offers a thorough
analysis of the viability of replacing the notorious chemical flocculants with those derived
from plants. An overview of the sludge’s physicochemical properties, its conditioning
techniques, and, in particular, the flocculation process is presented. In the present review,
the use of chemical flocculants as conditioners and their impact on the environment and
human health are highlighted with the aim of drawing the attention of environmentalists
and wastewater stakeholders to the necessity of considering green surrogates. Thus, also in
this paper, the performances of the plant-based flocculants that are most widely used in
sludge dewatering are compared to those of their chemical equivalents. Challenges to and
the future the prospects of their application are addressed in the hopes that it will help to
establish an effective, green, and environmentally friendly dewatering process.
Water 2023, 15, 2602 3 of 14

2. Sludge Properties and the Necessity for Dewatering

Sludge is a suspension of thick semi-solid deposits (slurry, organic matters, trace
metals and nutrients, etc.) and microorganisms, which form more than 96% of the sludge’s
weight and volume [22]. This high water content can be classified into free and bound
water. Free water is easily separated from the sludge by simple filtration or sedimentation.
However, bound water, which consists of vicinal, interstitial, and internal water, is difficult
to separate. According to its position in the sludge matrix, the vicinal water is held on the
solids’ surface, the interstitial one is captured in the interstices, and the internal water is
chemically bound to the solids [23]. This kind of water is deemed to be the main barrier
for dewatering because it is tightly attached to the sludge’s constituents (microorganisms
and organic and inorganic matter) and binds them together. As a result, sludge porosity
decreases, thus preventing water withdrawal.
Otherwise, microorganisms and organic polymers, namely the extracellular polymeric
substances (EPS), are considered to be the prime factors to maintain the sludge’s moisture
due to their ability to trap water. Thus, based on the water distribution within, the EPS can
be classified into three types, namely the soluble (S-EPS) and the loosely bound (LB-EPS)
and tightly bound extracellular polymeric substances (TB-EPS) [24]. Despite its high bound
water content, the EPS forms stable and viscous gel networks due to the prevalence of
proteins and polysaccharides in their composition [25]. The ionization of these biopolymers
imparts a negative surface charge to the sludge particles and leads to the aggregation of
organic matter and microbial cells [26]. Consequently, important water volume is retained,
and flexible flocs with low settleability are produced, resulting in dewatering difficulties.
Considering the complex structure of sludge, dewatering is necessary to promote the
further treatment, transportation, and disposal of sludge and to elucidate the causes of
its exploitation.
Generally, sludge dewatering is carried out by conventional mechanical means using
different pieces of equipment and methods, such as centrifuging, belt filter presses, plate
and frame filters, etc. [27]. Although, the efficacy of these methods in eliminating free water,
as well as a small portion of bound water and the dry solids produced after dewatering,
does not exceed 40% [28]. Therefore, the sludge is typically subjected to a pretreatment stage
by different conditioning technologies involving biological (enzyme treatment), physical
(ultrasonic, thermal, and microwave treatments, filter aid applications), and chemical
(acid or alkali, oxidation, and flocculation treatment) methods [29–31]. To elucidate their
efficiency in aiding sludge dewatering, the principles behind each conditioning method, as
well as their limitations, are briefly described in Table 1.

Table 1. Conditioning methods for improving sludge dewatering.

Conditioning Methods Principle Limitations

Lysis of EPS and microbial cells to release the bound water in the - Long processing time.
Biological methods - Difficult microorganism cultivation.
sludge through the addition of enzyme or microbial leachate [32].

Modification of the structural properties of the sludge to increase

its filterability and settle ability via the addition of solid and - Energy-consuming.
Physical methods
porous material (skeleton builder) or through thermal treatment - Voluminous sludge cake.
(freeze-thawing, thermal, and microwave treatment) [33].
Modification of the physicochemical properties of the sludge via
the addition of chemical reagents conducive to either solids
- Careful pH monitoring.
degradation to ease bound water release as a result of pH
Chemical methods - Questionable safety of the
alteration (alkali or acid treatment) or by the consolidation of
used chemicals.
solids to increase its permeability and promote solid/liquid
separation (coagulation/flocculation) [34,35].

As presented in Table 1, it is worth mentioning that long processing times and high
energy requirements impede the real application of biological and physical conditioning
methods on an industrial scale. So, for economic reasons, among all of the chemical
Water 2023, 15, 2602 4 of 14

conditioning approaches, coagulation/flocculation is the most applied one for sludge

dewatering due to its rapidity, cost-effectiveness, and efficacy in separating water from solid
particles [36]. Coagulation/flocculation is based on the addition of chemicals to aggregate
the (SS) into large and compacted flocs, enabling the removal of the bound water of sludge
and improving its settleability. Likewise, regarding wastewater treatment, the efficiency of
the coagulation/flocculation process to assist in sludge dewatering depends on the nature
and physicochemical properties of the used chemical coagulants/flocculants, which are
generally aluminum salts, iron salts, and acrylamide-based synthetic polymers [37,38].

3. Chemical Flocculants for Improving Sludge Dewatering: Efficiency and Effects on

the Environment and Human Health
The conventional synthetic flocculants, such as aluminum sulphate (Al2 (SO4 )3 , alu-
minum chloride (AlCl3 ), polyaluminium chloride (PACl), ferric sulphate (Fe2 (SO4 )3 , and
ferric chloride (FeCl3 ), as well as cationic and anionic polyacrylamides (PAM), have been
applied in sludge dewatering for a long time [14,39,40]. The efficacy of these chemicals
has been assessed in several research works. For instance, in a study conducted by Masihi
and Gholikandi [41], the dewatering performances of aluminum (Al2 (SO4 )3 and AlCl3 )
and iron (Fe2 (SO4 )3 and FeCl3 ) salts were evaluated with respect to their specific resistance
to filtration (SRF), capillary suction time (CST), time to filter (TTF), and moisture content
(MC) in treating an anaerobically digested sludge. As listed in Table 2, significant SRF
reductions of 95% and 93% were found using 150 mg/g of AlCl3 and FeCl3 , respectively,
while the higher dosages of 300 mg/g for Al2 (SO4 )3 and Fe2 (SO4 )3 lessened the SRF by
more than 80%. Even the addition of these metal salts to the sludge also minimized the
CST, TTF, and MC, thus improving its dewatering. Moreover, a notable SRF decrease from
11.30 × 1012 m/kg to 3.90 × 1012 m/kg was achieved using PACl as a flocculant to treat a
biological sludge [42]. Interestingly, comparing the dewatering efficacy of PACl with that
of FeCl3 , Niu et al. [43] revealed that the best decrease in SRF (from 1.72 × 1012 m/kg to
0.07 × 1012 m/kg) was gained using FeCl3 . In this study, the investigators demonstrated
that inorganic salts enhance sludge dewatering by neutralizing the charge of particles or
through compression in the double layers of the EPS, which is carried out by trivalent
cations (Al3+ or Fe3+ ) [43]. As a result, the aggregation of sludge colloids and the seepage
of bound water renders the sludge amenable to dewatering.
Otherwise, synthetic polymers, namely PAMs, have been commonly used in sludge
conditioning to enhance its dewatering [44,45]. On account of their long chain and high
charge density, polyacrylamide-based flocculants bridge the small solids together to form
large and settleable flocs. Consequently, the separation of solids from water content in
the sludge may occur, enabling efficient dewatering. In fact, as displayed in Table 2, the
application of PAM led to important decreases in the dewatering properties (SRF, CST, and
MC) of sewage sludge [46]. Likewise, in treating a waste-activated sludge, Wu et al. [47]
found that prominent reductions in SRF (from 14.20 × 1012 m/kg to 0.40 × 1012 m/kg) and
CST (from 225 s to 19.70 s) were achieved by a cationic PAM.
Water 2023, 15, 2602 5 of 14

Table 2. Efficiency of chemical flocculants for sludge dewatering.

Dewatered Sludge Parameters

Raw Sludge Chemical Flocculant References
SRF × 1012 (m/kg) CST (s) TTF (s) DS (%) MC (%)
Al2 (SO4 )3
51.94 57 140 _ 89
Optimal dose = 300 mg/g
Anaerobically digested
Fe2 (SO4 )3
sludge 43.99 51 137 _ 88
Optimal dose = 300 mg/g
SRF = 265 × 1012 m/kg [41]
CST = 283 s AlCl3
TTF = 600 s 18.29 35 118 _ 87
Optimal dose = 150 mg/g
MC = 97.80%
FeCl3
13.25 32 129 _ 86
Optimal dose = 150 mg/g
Biological sludge
SRF = 11.30 × 1012 m/kg
PACl
DS = 12% 3.90 55 _ 22.50 80.80 [42]
Optimal dose = 10%
MC = 98.50%
CST = 132 s
FeCl3
0.07 _ _ _ _
Sewage sludge Optimal dose = 10%
[43]
SRF = 1.72 × 1012 m/kg
PACl Optimal dose = 10% 0.50 _ _ _ _
Sewage sludge
MC = 98% Cationic PAM
1.07 9.77 _ _ 74.70 [46]
SRF = 2.19 × 1012 m/kg Optimal dose = 2 g/kg
CST = 150 s
Waste-activated sludge
PAM
SRF = 14.20 × 1012 m/kg 0.40 19.70 _ _ _ [47]
Optimal dose = 3 mg/g
CST = 225 s

Based on all of this information, it can be concluded that synthetic flocculants certainly
improve sludge dewatering. However, due to their chemical nature, the application of these
flocculants requires many precautions as it can harm both the environment and human
health [48,49]. In fact, as reported in the literature, the enhancement of sludge dewatering
using metal salts or PAM as flocculants generally requires carefully controlled pH and
a specific dosage to ensure the aggregation of solids and rule out the re-stabilization of
sludge flocs [43]. Furthermore, admittedly, sludge treated by such chemicals is voluminous
and acidic, thus impeding its transport and disposal [24]. Additionally, dewatering devices
may be damaged as a result of the intensive use of corrosive ferric salts [50]. Moreover,
due to their non-biodegradability, chemical residuals ascribed from synthetic flocculants
may remain embedded in the dewatered sludge matrix, subsequently leading to secondary
pollution and limiting the use of this sludge [51]. Consequently, sludge handling becomes
much more costly as further treatment is required. Generally, serious environmental
pollution is associated with with the use of these synthetic polymers. For example, the
resulting alum sludge is a source of toxic aluminum that is harmful to both human and
marine life. Aluminium may be associated with Alzheimer’s disease, and its toxicity
towards fish has previously been reported [7,52]. However, obtaining an exact estimation
of the toxic sludge produced in a region is difficult as various factors may control its
production (the polymer type, water characteristics, sludge characteristics, the process
used, etc.) [53].
Generally, the mechanisms of coagulation/flocculation include charge neutralization
and the bridging effect, which are appropriate for sludge dewatering. The used polymers
can efficiently destroy the relative stability of the charged particles and allow them to
agglomerate into large flocs prior to sedimentation and mechanical dewatering. In the
dewatering process, the resulting charge neutralization reduces the thickness of the hy-
drated shell of sludge particles and allows for the enhancement of free water content by
compressing the electric double layer and weakening the sludge water surface tension. In
deep dewatering, chemicals weaken the water-trapping capability of sludge by destroying
the network structure of sludge. Moreover, the bridging effect is also essential in sludge
dewatering [54–56].
Water 2023, 15, 2602 6 of 14

Considering all of these adverse effects and limitations associated with the application
of chemical flocculants as conditioners for sludge dewatering, looking for natural, efficient,
and harmless surrogates has become the primary focus of environmentalists, not only to
comply with the standard regulations but also to provide safe and costless sludge treatment,
transport, and disposal. Thus, natural flocculants derived mainly from plant extracts have
been evaluated as possible alternatives to enhance the dewatering process.

4. Plant-Based Flocculants for Sludge Dewatering: Efficiency and Comparison with

Chemical Flocculants
Over the last few years, more than 57 plants have been identified as natural coagu-
lants/flocculants for the treatment of various wastewaters [57]. Despite efforts to prove
their efficiency in removing various water pollutants, the exploration of plant-based floccu-
lants for sludge dewatering is still limited to only a few plants, such as Moringa, Cactus,
Aloe, and Okra, which are believed to be the most effective sludge conditioners due to
their active agent content [11,12,58,59]. Indeed, the application of these popular plants as
green flocculants could be attributed to their reliable ability to aggregate sludge’s colloidal
particles into big flocs, allowing for easy sedimentation and separation from the treated
water [13,60,61]. Thus, this flocculating activity has piqued the interest of scholars and has
spurred on many in the scientific community to exploit them in sludge dewatering and ap-
ply them as surrogates for chemical conditioners. The following section sheds light on the
most extensively studied plants in the context of sludge dewatering. Later on, a comparison
will be made between the plant-based flocculants and synthetic chemical flocculants.

4.1. Moringa
Moringa, and chiefly the Moringa oleifera (MO) species, is the most investigated plant
in the field of sludge dewatering. The MO seeds allow for the congregation of sludge’s solid
particles into dense and settleable flocs. In other words, this natural flocculant enhances
sludge dewatering due to its ability to strengthen solids by reducing its compressibility
and improving its permeability to facilitate bound water release. To gain more insight into
Moringa’s capacity to aid sludge dewatering, see Table 3, which compiles the previous
research works that have assessed the variations in dewatering properties (such as the
SRF and the CST) that occur when using Moringa as a flocculant. In fact, Rabea et al. [62]
found that the powder of MO seeds decreased the SRF by up to 70%. This result denotes
that filterability becomes greater via powder supplementation, hence promoting sludge
water removal.

Table 3. Sludge dewatering performance when using Moringa as an alternative to chemical flocculants.

Raw Sludge. Flocculant Sludge Dewatering Performance References

Sewage sludge MO powder
SRF = 3.43 × 1015 m/kg [62]
SRF = 1.22 × 1016 m/kg Optimal dose = 6 g/L
Waste-activated sludge MO powder
SRF = 2.50 × 1012 m/kg [63]
SRF = 4.50 × 1012 m/kg Optimal dose = 4 g/L
MO powder
SRF = 3.30 × 1010 m/kg
Sewage sludge Optimal dose = 2 g/L (for SRF)
CST = 5.60 s
SRF = 8.00 × 1010 m/kg Optimal dose = 3 g/L (for CST) [64]
CST = 6.8 s Chemical polymer (Zetag 7653) SRF = 3.30 × 1010 m/kg
Optimal dose = 0.05 g/L CST = 3.60 s
Sewage sludge
MO water extract SRF = 1.22 × 1011 m/kg
SRF = 4.45 × 1011 m/kg [65]
Optimal dose = 4.69 g/L CST = 4.50 s
CST = 6.90 s
Water 2023, 15, 2602 7 of 14

Table 3. Cont.

Raw Sludge. Flocculant Sludge Dewatering Performance References

MO water extract
SRF = 3.64 × 1011 m/kg
Optimal dose = 3 g/L (for SRF)
Sewage sludge CST = 7.10 s
Optimal dose = 5 g/L (for CST)
SRF = 0.90 × 1012 m/kg [66]
CST = 9 s Chemical polymer (Zetag 8140) SRF = 1.48 × 1011 m/kg
Optimal dose = 13 mg/L CST = 5.50 s
MO salt extract
SRF = 1.10 × 1011 m/kg
Optimal dose = 235.58 mg/L
Synthetic Kaolin sludge
[67]
SRF = 3.90 × 1011 m/kg Alum
SRF = 0.80 × 1011 m/kg
Optimal dose = 212.02 mg/L
MO salt extract SRF = 12.10 × 1012 m/kg
Water treatment sludge Optimal dose = 40 mL/L CST = 59.70 s
SRF = 35.10 × 1012 m/kg [68]
Alum SRF = 6.64 × 1012 m/kg
CST = 175.4 s
Optimal dose = 40 mL/L CST = 42.20 s
Moringa Pergerina SRF = 1.21 × 1013 m/kg
Water treatment sludge Optimal dose = 100 mL/L CST = 19 s
SRF = 1.61 × 1013 m/kg [69]
Ferric chloride SRF = 0.97 × 1013 m/kg
CST = 44 s
Optimal dose = 100 mL/L CST = 9 s

Furthermore, the effects of the extraction methods of MO-based flocculants on sludge

dewaterability have been within the scope of interest of many different investigations.
In this respect, Muyibi et al. [63] appraised the flocculating efficacy of MO dry powder
used directly and dissolved in water or salt solution as conditioning agents to treat waste-
activated sludge. Both the dry powder and its water extract exhibited better dewatering
performance than the salted MO seed solution. As shown in Table 3, the MO powder
decreased the SRF from 4.50 × 1012 m/kg to 2.50 × 1012 m/kg. Additionally, the treated
sludge showed the smallest volume and the most notable settling rate of 66.70% compared
to 48% using the salted solution. The results of this study are in accordance with those
reported by Wai et al. [64]. The three MO forms—powder, water, and NaCl-aqueous
extracts—disclosed comparable CST variations of around 5 s, while the lowest SRF value
was registered using the powdered MO form. The latter allowed for a decline in the
SRF from 8.00 × 1010 m/kg to 3.30 × 1010 m/kg (Table 3). In comparison to a cationic
polyacrylamide (Zetag 7653, a commercial flocculant) and in the context of sewage sludge
dewatering, Wai et al. [64] reported that the efficiency of MO powder to reduce the SRF
was as good as that of Zetag 7653. As depicted in Table 3, similar SRF decreases from
8.00 × 1010 m/kg to 3.30 × 1010 m/kg were achieved using 2 g/L of MO and 0.05 g/L of
Zetag 7653. Even though a high natural flocculant dosage was required, the availability,
biodegradability, and safety features of MO as a conditioning agent make it an alternative
eco-sustainable solution to mitigate all of the threats associated with the use of chemical
flocculants.
The significant dewatering performance of MO powder compared to MO water and
salt extracts could be ascribed to the capacity of this powder to, once dissolved in the
sludge matrix, release the cationic proteins that are responsible for its flocculating ability.
Due to its low molecular weight and positive charge density, the cationic MO proteins
neutralize the negatively charged solids to generate dense and compacted flocs that are
readily settleable via gravitational decantation. On the other hand, the un-dissolved MO
powder serves as an adsorbent to collect sludge solids and assist in its dewatering. In fact,
it may produce rigid and porous solids of low compressibility and good permeability to
enhance water removal.
Regarding MO water and salt extracts, researchers assume that their effectiveness is due
to the total solubility of proteins as active agents. Along this line, Tat et al. [65] revealed that
MO water extract was better than dry powder and salt (NaCl) extracts with respect to reducing
SRF and CST. Also, in dewatering a sewage sludge using this natural flocculant, Mohammad
Water 2023, 15, 2602 8 of 14

et al. [66] found significant decreases in SRF (from 0.90 × 1012 m/kg to 3.64 × 1011 m/kg)
and CST (from 9 s to 7.10 s). Nonetheless slightly better SRF (1.48 × 1011 m/kg) and CST
(5.50 s) declines were observed using a synthetic cationic polyacrylamide (Zetag 8140).
Likewise, the MO seeds extracted by NaCl salt exhibited a comparable SRF reduction
(72%) to that found using alum (79%) in a sludge dewatering process based on a drinking
water treatment method [67]. These results are in agreement with those reported by
Ghebremichael and Hultman [68].
Interestingly, with the increase in awareness about the necessity to look for natural
resources as alternatives to chemical flocculants for sludge dewatering, another species of
Moringa, Moringa peregrina (MP), was explored for the first time by Mazaheri et al. [69] to
dewater a sewage sludge. Similarly, to MO, the MP was prepared by dissolving its seeds
powder in NaCl solution. A significant decline in CST from 44 s to 19 s was achieved using
100 mL/L of MP. Similarly, the SRF value dropped from 1.61 × 1013 m/kgto 1.21 × 1013
m/kg, whereas larger reductions in CST (9 s) and SRF (0.97 × 1013 m/kg) were found
using 100 mL/L of FeCl3 . From an environmental point of view, due to its efficiency, safety,
biodegradability, and sustainability, the application of MP as a bioflocculant instead of
FeCl3 as a synthetic flocculant is favorable.

4.2. Cactus and Aloe

In contrast to Moringa, a few studies have addressed sludge dewatering using Cactus
and Aloe. To the best of our knowledge, only two research works have investigated the
efficiency of these plants in assisting in the sludge dewatering process. For instance, in a
study related to the application of Cactus (Opuntia ficus indica), Betatache et al. [11] reported
that replacing a chemical flocculant with cactus juice for sewage sludge dewatering is
feasible. In comparison with a few tested synthetic organic cationic (Chimfloc C4346),
anionic (Sedipur AF 400), and non-ionic (Sedipur NF 102) polymers, as well as metal
salts—namely alum (Al2 SO4 ) and iron chloride (FeCl3 )—the cactus juice showed the best
dewatering performance. In fact, as presented in Table 4, the SRF value obtained using
the cactus juice (SRF = 0.17 × 1012 m/kg) was slightly less than those obtained using the
cationic polymer (SRF = 0.3 × 1012 m/kg), the non-ionic polymer (SRF = 4 × 1012 m/kg),
and alum (SRF = 1.3 × 1012 m/kg). This result implies that cactus-derived flocculants have
the capacity to enhance sludge dewatering.

Table 4. Application of Cactus and Aloe vera as natural flocculants in sludge dewatering.

Raw Sludge Flocculant Sludge Dewatering Performance References

Cactus juice
SFR = 0.17 × 1012 m/kg
Optimal dose = 0.4 g/kg
Cationic polyacrylamide
(Chimfloc C4346) SFR = 0.3 × 1012 m/kg
Optimal dose = 6 g/kg
Non-ionic polyacrylamide
Sewage sludge (Sedipur NF 102) SFR = 4 × 1012 m/kg [11]
SRF = 1.03 × 1013 m/kg Optimal dose = 6 g/kg
Alum
SFR = 1.3 × 1012 m/kg
Optimal dose = 40 g/kg
FeCl3
SFR = 1.3 × 1012 m/kg
Optimal dose = 80 g/kg
Municipal wastewater sludge Aloe vera gel
Settling rate = 67.50% [59]
Settling rate = 55% Optimal dose = 3 mL/L

On the other hand, regarding the use of Aloe vera, Jaouadi et al. [59] appraised the
efficiency of aloe gel as a flocculant to treat sewage sludge. They noticed that the addition
of this natural flocculant as a conditioner promotes the raw sludge’s settleability, and an
Water 2023, 15, 2602 9 of 14

enhanced settling rate of 67.50% was achieved using 3 mL/L as a result of the aggregation
of flocs. Moreover, it can be deduced that this improvement in particle strength allowed for
the removal of the trapped bound water, hence facilitating solid–liquid separation.
Based on these promising findings, cactus and aloe vera have the potential to be
bioflocculants for sludge dewatering, and their polysaccharide content and specifically
their polygalacturonic acid content are regarded as the main agents responsible for their
flocculating abilities [60]. Due to its long polymeric chains, polygalacturonic acid provides a
bridge to adsorb the suspended sludge solids and binds them together in order to produce
strong and dense aggregates. Consequently, the compressed solids enable the smooth
withdrawal of bound water, facilitating sludge dewatering.

4.3. Okra
Like Cactus and Aloe, Okra (Abelmoschus esculentus) is a common polysaccharide-
based flocculant widely applied for wastewater treatment [61,70]. However, its application
in sludge treatment is still limited. To fill this gap, Lee’s group has explored the dewater-
ing efficiency and feasibility of using Okra in lieu of conventional synthetic flocculants
for sludge dewatering [12,71,72]. Scholars have paid great attention to assessing how
the methods used to extract bioflocculants (conventional hydrothermal and microwave-
assisted extraction) affect their dewatering abilities. In a preliminary study conducted by
Lee et al. [12], Okra water extract and its oven-dried powder (acquired after conventional
hydrothermal extraction) were evaluated in terms of their efficiency in dewatering synthetic
kaolin sludge. Both natural flocculants showed significant SS removal and water recov-
ery rates exceeding 98% and 68%, respectively (Table 5). Further improvements in these
dewatering properties were observed using microwave-extracted powder as salient SS re-
moval (99%) and water recovery (75%) rates were attained [72]. The prominent dewatering
capabilities of okra-based flocculants are merely attributed to the high solubility of their
polysaccharides with the increase in extraction temperature when using microwave ex-
traction. Likewise, compared to conventional synthetic flocculants (Table 5), Okra showed
higher SS removal and water recovery rates than a cationic and anionic PAM. According
to these interesting findings recorded by Lee et al. [12,71,72], the dewatering efficiency
of Okra, and specifically its microwave-extracted powder, as a bioflocculant makes it a
relevant candidate to replace the commonly used chemical flocculants.

Table 5. Sludge dewatering using Okra as natural flocculant.

Raw Sludge Flocculant Sludge Dewatering Performance References

Okra water extract SS removal ≥ 98%
Optimal dose = 175 mg/L Water recovery ≥ 68%
Okra oven-dried powder SS removal ≥ 98%
Optimal dose = 150 mg/L Water recovery ≥ 68%
Okra microwave-extracted
SS removal ≥ 99%
powder
Water recovery ≥ 75%
Synthetic Kaolin sludge Optimal dose = 30 mg/L [12,71,72]
Cationic polyacrylamide
SS removal ≥ 98%
(FO 4400 SH)
Water recovery ≥ 65%
Optimal dose = 70 mg/L
Anionic polyacrylamide
SS removal ≥ 95%
(AN 934 SH)
Water recovery ≥ 60%
Optimal dose = 50 mg/L

5. Potential Dewatering Flocculants: Synthetic or Plant-Based Ones

Overall, in spite of the paucity of research studies on the application of plant-based
flocculants for sludge dewatering, the aforementioned results obtained using Moringa,
Cactus, Aloe, and Okra have elucidated their ability to separate water from the solids
Water 2023, 15, 2602 10 of 14

of sludge, implying that their use in sludge dewatering is apt. For all of these plants,
researchers have made efforts to optimize their extraction conditions (solvent concentration,
extraction with water or salt, oven-drying, microwave-assisted extraction, temperature)
to produce suitable bioflocculants with efficient dewatering activities. Considering the
time and costs associated with their extraction procedures, the aforementioned plants are
deemed to be effective biomaterials capable of enhancing sludge dewaterability.
Furthermore, as depicted in Tables 3–5, it can be seen that the SRF and CST are
the most appraised dewatering parameters. Dry matter content, time to filter, sludge
volume index, volume of filtrate, and water recovery rate were also assessed in some
investigations [4,59,71]. Compared to the raw sludge, all of the discussed plant extracts
exhibited outstanding SRF and CST decreases. The reduction in these two parameters
reflects their potential to modify the physicochemical properties of sludge. As a matter
of fact, the decrease in SRF values denotes an improvement in sludge filterability as a
result of an increase in the porosity of its solids. Consequently, the sludge cake becomes
more permeable to allow for the release of the bound water stuck in the EPS. In parallel,
the compressibility of its solids decreases, allowing for water content to quickly decrease
during filtration.
Moreover, as shown in Tables 3–5, it can be said that the dewatering performance of
bioflocculants is comparable (in case of Moringa) and even superior (in the cases of Cactus
and Okra) to PAM. However, it is worth noting that, in spite of the fact that higher plant
extract dosages were required to compete with their chemical counterparts, these natural
products are beneficial for sludge dewatering as they may help the process become rid
of the detrimental environmental damage and human health risks associated with it [73].
They are also highly biodegradable, abundant, locally available, and can be cultivated and
derived from renewable resources [74]. Hence, the application of these natural flocculants to
dewater sludge is regarded as economically feasible in terms of raw materials procurement.
Moreover, using these innocuous bioflocculants in dewatering processes would be
easier compared to using chemicals because neither pH adjustments nor health precautions
are required to reduce sludge volume. This volume was found to be three times smaller
when Moringa was used instead of alum [75]. Consequently, this notable reduction could
definitely minimize the cost of sludge handling, transport, and disposal.
Furthermore, due to the fact that plant-based flocculants are natural, the dewatered
sludge treated using natural flocculants can be relatively free from chemicals depending on
the type of the raw effluent. Taking into consideration their antimicrobial activity, the use
of plants as flocculants also ensures the removal of pathogens and unpleasant odors from
the sludge, further demonstrating their utility in protecting the environment and human
health [59,76]. Moreover, the dewatered sludge is deemed to be a nontoxic byproduct
suitable for applications in agriculture as a soil conditioner or fertilizer due to its high
nutrient content. This sustainable strategy fits well with the concept of “waste to wealth”.
Thus, alongside their promising activity to aid the dewatering process, the application of
plant-based flocculants instead of chemical ones opens up profitable opportunities to reuse
the produced sludge, which may, in turn, alleviate the economic burdens related to the
management, disposal, cost, and safety of sludge.

6. Challenges and Future Prospects in the Application of Plant-Based Flocculants for

Sludge Dewatering
As evidenced by the studies highlighted in this review, the most frequently used plants
to dewater sludge are polysaccharide-based flocculants such as Cactus, Aloe, and Okra.
The use of these natural extracts as green conditioners will likely inspire researchers to
look for other plants that contain polysaccharides to investigate their dewatering perfor-
mance. Further studies should be also conducted to provide a greater understanding of the
efficiency of bioflocculants. To fulfill this research objective, future studies should clarify
the effects of sludge’s physicochemical properties (water content distribution, nature of
EPS, solids content) on its dewaterability. Investigations into its rheological properties are
Water 2023, 15, 2602 11 of 14

also highly recommended because sludge viscosity not only affects sludge’s filterability
(block of water release) but it may also deteriorate the equipment used for dewatering
(e.g., the clogging of filters). Moreover, variations in EPS components and their interactions
with plant-based flocculants during the conditioning stage are still lacking; nevertheless,
most of the previous works in the literature have systematically correlated dewatering
characteristics such as the SRF and CST with the capacity of sludge solids to release the
bound water entrapped in the EPS matrix [12,64]. Hence, scientific evidence regarding this
phenomenon is urgently required (for example, characterization through Scanning Electron
Microscopy (SEM) or assessing a sludge cake via fluorescence spectroscopy). In addition,
the mechanisms of dewatering when using plants as flocculants should be elucidated in
future research studies. Furthermore, with the aim to scale up their application, techno-
economic analyses conducted through the life cycle assessment (LCA) method are greatly
needed to fully describe sludge dewatering processes involving raw sludge collection,
treatment, bioflocculant preparation, and disposal, as well as the environmental impact
associated with each stage of the process.

7. Conclusions
For the sake of environmental and human health preservation, substituting conven-
tional synthetic flocculants in sludge dewatering with safe, clean, and natural ones derived
from plants appears to be an ecofriendly approach. However, despite their biodegradability,
availability, and cost-effectiveness, the potential utility of these natural extracts for use
in the sludge dewatering process has still not been adequately addressed. Unfortunately,
only four plants, namely Moringa, Cactus, Aloe, and Okra, have been investigated in the
literature; however, all have shown efficient dewatering performances that are comparable
and even superior to chemical flocculants. Prominent decreases in sludge SRF and CST
transcending 90% were found for polysaccharide-based flocculants such as Cactus and
Okra. Moreover, their application can be regarded as a profitable and an eco-sustainable
strategy not only to enhance the dewatering process but also to promote environmentally
friendly sludge disposal and reuse, especially in the field of agriculture as sludge with
a high nutrient content can be deployed as a soil conditioner or fertilizer. Thus, on one
hand, extensive studies are needed to fill the knowledge gaps in appraising the dewatering
abilities of other natural resources to facilitate their large-scale application, and on the other
hand, evaluating the reliability of the produced sludge for agriculture use is necessary to
make sludge dewatering, management, and disposal more green and clean.

Author Contributions: Conceptualization, M.K. and F.B.R.; writing—original draft preparation,

Y.H.M.; writing—review and editing, B.O., M.K. and F.B.R.; visualization, M.K. and F.B.R.; supervi-
sion, M.K., F.B.R., W.M. and M.S.; project administration, F.B.R. and W.M.; funding acquisition, F.B.R.
and W.M. All authors have read and agreed to the published version of the manuscript.
Funding: This research was supported by the Deanship of Scientific Research at University of
Bisha-Saudi Arabia through the project number UB-GRP-66-1444.
Data Availability Statement: Not applicable.
Acknowledgments: The authors extend their appreciation to the Deanship of Scientific Research at
the University of Bisha for funding this research through the general research project under grant
number (UB-GRP-66-1444).
Conflicts of Interest: The authors declare no conflict of interest.

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