water

Article
Enhancing the Efficiency of Banana Peel Bio-Coagulant in
Turbid and River Water Treatment Applications
Abdassalam A. Azamzam 1 , Mohd Rafatullah 1, * , Esam Bashir Yahya 1 , Mardiana Idayu Ahmad 1 ,
Japareng Lalung 1 , Mahboob Alam 2 and Masoom Raza Siddiqui 3

1 School of Industrial Technology, Universiti Sains Malaysia, Penang 11800, Malaysia

2 Division of Chemistry and Biotechnology, Dongguk University, 123, Dongdaero, Gyeongju-si 780714, Korea
3 Chemistry Department, College of Science, King Saud University, Riyadh 11451, Saudi Arabia
* Correspondence: [email protected]; Tel.: +60-46532111; Fax: +60-4656375

Abstract: The aim of the present work is to investigate the potential use of banana peel waste as a
natural coagulant and to enhance its coagulation performance using a green modification approach
for the removal of synthetic water turbidity and river water treatment. Here, the regular banana peel
powder had an average particle size and diameter of 978 ± 37 nm and 602 ± 13 nm, respectively, while
the modified powder possessed 571 ± 41 nm and 360 ± 19 nm particle size and diameter, respectively.
The coagulation performance was investigated at different pH levels, doses, sedimentation times,
and NaCl quantities. The optimum dose was found to be 0.4 g/L for modified banana peel with
turbidity removal of up to 90%. NaCl slightly enhanced the coagulation performance at low quantities
of less than 0.4 g/L, but the activity was reduced at higher concentrations even in the modified
powder. Banana peel powder had a weaker turbidity reduction of 76 and 84% for non-modified and
modified powders in river water, respectively, in addition to significant reduction in water color, total
dissolved and suspended solids, and chemical and biochemical oxygen demand. SEM and FT-IR
characterization were performed to investigate and confirm the coagulation mechanism. Such a green
Citation: Azamzam, A.A.; Rafatullah,
modification of banana peel powder can be an alternative with significantly potential as a low cost
M.; Yahya, E.B.; Ahmad, M.I.; Lalung,
and easily available bio-coagulant, which can certainly contribute to the waste reduction.
J.; Alam, M.; Siddiqui, M.R.
Enhancing the Efficiency of Banana
Peel Bio-Coagulant in Turbid and
Keywords: banana peel powder; modification; coagulant; turbidity; water treatment; enhancement
River Water Treatment Applications.
Water 2022, 14, 2473. https://doi.org
/10.3390/w14162473
1. Introduction
Academic Editor: Tushar Kanti Sen
The consumption and usability of water worldwide have significantly increased in the
Received: 28 June 2022 past few years due to the surge in population [1,2]. Water bodies contain huge amounts
Accepted: 8 August 2022 of microscopic particles and dissolved impurities, making them unfavorable for human
Published: 11 August 2022 use, especially in tropical countries [3]. These impurities include organic and inorganic
Publisher’s Note: MDPI stays neutral compounds, in addition to minerals, which significantly change the physico-chemical and
with regard to jurisdictional claims in biological characteristics of water [4,5]. Thus, surface water must undergo treatment and
published maps and institutional affil- purification, which vary depending on the nature and characteristics of the water to be
iations. treated, and finally meet the standard limits for human use [6,7]. Coagulation is one of the
water treatment approaches that depends on using plant or non-plant-based coagulants,
which are substances used to remove water impurities such as color and turbidity from
raw water, by forming large agglomerates that will eventually settle at the bottom of the
Copyright: © 2022 by the authors. container and can be removed [8].
Licensee MDPI, Basel, Switzerland. Many chemical (non-plant)-based coagulants have been used in water treatment appli-
This article is an open access article
cations, such as iron and aluminium salts, in addition to some polymeric polysaccharides [9].
distributed under the terms and
Aluminium-based salts (such as aluminum sulfate and chloride) and ferric-based salts
conditions of the Creative Commons
(such as ferrous sulphate and ferric chloride) are the most widely used metal saltwater treat-
Attribution (CC BY) license (https://
ment coagulants [10]. Ferric chloride and aluminium sulphate are the most widely used
creativecommons.org/licenses/by/
metal-based coagulants that are characterized by their excellent performance in wastewater
4.0/).

Water 2022, 14, 2473. https://doi.org/10.3390/w14162473 https://www.mdpi.com/journal/water

Water 2022, 14, 2473 2 of 15

treatment; however, their use has the limitation of reducing the water pH to become close
to acidic. In addition, they have been reported to cause some health issues to humans
after the consumption of water, such as presenile dementia and Alzheimer’s disease [11].
Another limitation of using metal salts as coagulant agents is the resulting large volume
of sludge and the relative high coagulant cost [12]. Thus, plant-based coagulants are the
suitable and safer alternatives for these chemicals.
Various plant-based coagulants have been used for water treatment applications, in-
cluding Moringa oleifera [13], Cicer arietinum [14], and Dolichos lablab [15]. These materials
have been found to contain several effective proteins that are responsible for coagulation
processes, in which they chemically destabilize water suspended matters, making them
come together to form bigger agglomerates known as flocs [16]. Coagulants from natural
sources are often seen to be safe for human health [12]. Some natural coagulants have been
studied and are known to have the following advantages: the sludge produced is usually
biodegradable, virtually toxin-free, relatively cheap to obtain, and locally available [17]. A
significant number of synthetic materials have been used in water treatment applications,
such as cationic polymers [18], titania nanoparticle [19], and manganese ferrite nanopar-
ticles [20], but these materials are potentially toxic and non-ecofriendly. However, some
natural coagulants are valuable, expensive, and not highly available, which limit their
usage. Ribeiro et al. [21] evaluated the efficiency of Moringa oleifera seeds as a natural
coagulant and reported a high removal performance of turbidity and apparent color from
wastewater. Kristianto et al. [22] investigated the potential of papaya seeds for the same
purpose and reported a direct relationship between the coagulant dose and removal perfor-
mance. Plant seeds may not be available in high quantities and they could be utilized for
other purposes. In this study, we chose another form of plant waste consisting of banana
peel waste as a natural coagulant.
The banana tree has been reported to produce from 3 to 20 fruits in a cluster only once
a lifetime, and after the fruit has been consumed, different parts of the banana tree are not
utilized, such as banana peels and stems, which are thus considered as waste [23]. This
waste has a high quantity of many useful organic compounds, including cellulose, lignin,
pectin substances, pigments, and chlorophyll, etc., in addition to low molecular weight
organic compounds [24]. Worldwide, following the consumption of bananas, million tons
of peels are mostly discarded and are rarely utilized. In Malaysia, banana is ranked as the
second most widely cultivated fruit, and it can be utilised either ripe or unripe. The ripe
banana is used for preparing fried banana and unripe banana is used for making chips [25].
Chip and juice factories consume huge amounts of banana and generate tons of banana
peel waste every year. Banana peels, which account for approximately 40% of the total
weight of fresh bananas, are normally dumped in landfills and result in environmental
problems. Recent investigations have shown that the composition of banana peels mainly
consists of several biopolymers, including pectin, cellulose, lignin, and hemicellulose, in
addition to other chemical substances that contain a large amount of hydroxyl and carboxyl
functional groups [26]. These active functional groups in banana peels are able to combine
with contaminants via complexing, chelating, coordinating, hydrogen bonding, and/or
other effects [27]. Thus, banana peel has gradually become a research hotspot as a highly
available natural coagulant in water treatment applications. Several attempts have been
made to enhance the coagulation performance of banana peels by either mixing them with
other coagulants or conducting chemical modifications to the peels. Fu et al. [28] used
chemical modification to produce oxidized banana peel in order to enhance the coagulation
activity. Chemical modification may lead to chemical leaching in treated water and cause
further issues. In this study, we used a facile and affordable preparation approach to
enhance the coagulation performance of banana peel as a natural coagulant. This approach
consists of multiple microwave radiation treatments followed by multiple grinding to
reduce the particle size and modify the surfaces of the particles. The novelty of this research
is to prove our hypothesis that the coagulation efficiency of the natural coagulant can be
further enhanced without the need for any chemical reactions. Modified and non-modified
Water 2022, 14, 2473 3 of 15

banana peels were evaluated at different doses, different pH values, different sedimentation
times, and different NaCl quantities. The coagulation mechanism of banana peel powder
was also investigated by comparing the effect of the particle size and the solution of banana
peels in a turbid water treatment.

2. Material and Methods

2.1. Materials
Matured and dry banana fruit (Musa cavendish) were obtained from a local market and
were classified by a botanist to ensure the species. Kaolin clay was purchased from Kaolin
Malaysia Sdn Bhd, Malaysia, while NaCl was obtained from Merck, Darmstadt, Germany.

2.2. Preparation and Modification of Banana Peel Powder

The banana fruits were peeled, carefully washed, cut into small pieces, and then air
dried (At room temperature) for several days. After full drying, the peels were ground into a
fine powder using a mortar and pestle to obtain the regular banana peel powder. Modified
banana peel powder was prepared using a green approach, consisting of microwave
treatment (Panasonic microwave oven-NN-CT254B, New Delhi, India). The powder was
first prepared following the same mentioned steps in addition to multiple microwave
treatments at a power of 800 W for 0.5 min, and then cooling and grinding after each
treatment to reduce the particle size and modify the surface morphology of the particles.

2.3. Preparation of Banana Peel Solution

Ten grams of each banana peel powder were measured and added separately to one
liter of distilled water to form the banana peel powder suspension. The suspension was
stirred for 1 h with a magnetic stirrer to ensure all of the protein and active compounds were
fully dissolved, and it was then left to settle for 30 min. The filtrate was finally collected
and concentrations of 1 to 10 wt.% were prepared.

2.4. Characterization of Nano-Banana Peel Powder

The morphological characteristics of the modified and non-modified banana peel pow-
der were examined using a Field Emission Scanning Electron Microscope (FE-SEM) model
Leo Supra, 50 VP (Carl Zeiss, SMT, Frankfurt, Germany). The particle size distribution
was investigated using a laser diffraction analyzer (Nano-ZS90, Malvern, UK). A 1 nm to
100 µm size range was used for a suspension of 0.01% consistency of each powder, which
was dispersed for 15 min with ultrasound at 100% power. The surface functional groups of
the banana peel powder were investigated using FT-IR spectroscopy (Thermo Scientific
model Nicolet I S10 spectrometer, Thermo Fisher Scientific, Waltham, MA, USA).

2.5. Preparation and Standardization of Turbid Water

To ensure a constant turbidity value for all of the experiments, synthetic turbid water
was prepared and used for all of the coagulation experiments. First, 10 g of kaolin clay
particles was added to 1 L of deionized water to obtain the stock solution [29]. The turbidity
was then standardized at 110 NTU by diluting the stock solution using deionized water.
River water was obtained from Penang River on 22 January, and the sampling process
was done following the process described in [30] and samples were directly sent to the
laboratory for characterization.

2.6. Coagulation Experiment

The coagulation experiment was done using the jar test experiment. Water samples
were added to 500 mL jars and the coagulants were added to the jars. Different types,
doses, pH, and NaCl concentrations were used, and the time and stirring speed were
fixed at 200 rpm for 2 min followed by 10 min of slow mixing at 20 rpm and then 30 min
of settling [4]. A constant volume of 50 mL of each concentration of prepared banana
Water 2022, 14, 2473 4 of 15

peel solution was used. Each experiment was repeated three times and the average value
was taken.

2.7. Characterization of River Water

Water temperature was measured using a regular digital thermometer in the field
during sample collection, and it was held for 1 min in each water sample. The water color
was observed with naked eye using different colored backgrounds. The pH was measured
using automatic waterproof meters from Wagtech International Ltd. (Nairobi, Kenya), and
the total dissolved and suspended solid was measured with a waterproof TDScan Low
from Eutech Instruments (St. Louis, MO, USA), as described in [31]. The chemical oxygen
demand (COD) and biochemical oxygen demand (BOD) were measured using a DR2800
spectrophotometer and dissolved oxygen meter, following the methodology described by
Shan et al. [32].

3. Results
3.1. Characterization of Nano-Banana Peel Powder
Figure 1 presents the FE-SEM images of the modified and non-modified banana
peel powder. The surfaces of the non-modified powder seemed smoother and had no
signs of any fractions (Figure 1a). On the other hand, the modified powder seemed more
homogeneous with rough and sticky surfaces. Multiple microwave treatments of the
banana peel powder produced mild heating, which induced fractions in the particles, as
highlighted with the arrows in Figure 1b, which also reduced the size of the particles. Eng
Water 2022, 14, x FOR PEERand Loo reported that the microwave-assisted extraction of the banana peel
REVIEW 5 of bio-flocculant
16
was found to be better than conventional heating extraction [33].

Figure 1. Morphological analysis of modified and non-modified banana peel powder; (a)
1. Morphological
Figurenon-modified analysissmoother
powder exhibiting of modified
surfacesand
and non-modified banana
(b) modified powder peel sticky
exhibiting powder; (a) non-
surfaces,
modified powderwith exhibiting
clear fractionssmoother
as the arrows indicate.and (b) modified powder exhibiting sticky surfaces,
surfaces
with clear fractions as the arrows indicate.
The regular banana peel powder had an average particle size of 978 ± 37 nm and
average diameter of 602 ± 13 nm, as presented in Figure 2a, compared with modified
banana peel powder, which showed an average particle size of only 360 nm and average
diameter of 543 nm (Figure 2b). Microwave treatment did not significantly affect the
particles diameters, and a huge reduction in particle size could be confirmed compared
with the diameter. Many functional groups can be seen in the FITR spectra (Figure 2c),
Water 2022, 14, 2473 5 of 15

The regular banana peel powder had an average particle size of 978 ± 37 nm and
average diameter of 602 ± 13 nm, as presented in Figure 2a, compared with modified
banana peel powder, which showed an average particle size of only 360 nm and average
diameter of 543 nm (Figure 2b). Microwave treatment did not significantly affect the
particles diameters, and a huge reduction in particle size could be confirmed compared
with the diameter. Many functional groups can be seen in the FITR spectra (Figure 2c),
with a broad peak at 3421.57 cm−1 attributed to the hydroxyl groups. The sharp peak at
2923.06 cm−1 was due to CH stretching vibrations, including CH, CH2 , and CH3 groups [34].
Another two interesting peaks, 1637.65 cm−1 and 1054.40 cm−1 are characteristics of C=O
in aromatics rings and C-O stretching [35]. However, the FT-IR spectra did not show any
Water 2022, 14, x FOR PEER REVIEWsignificant difference between modified and non-modified banana peel function groups,
6 of 16
and the particle size analysis and surface morphology confirmed the effect of treatment.

Figure
Figure 2.
2. Particle
Particlesize analysis
size and
analysis FT-IR
and of modified
FT-IR andand
of modified non-modified banana
non-modified peel powder;
banana (a,b)
peel powder;
average particle size of non-modified and modified banana peel powder, respectively, and (c)
(a,b) average particle size of non-modified and modified banana peel powder, respectively, and
FT-IR spectra.
(c) FT-IR spectra.

3.2.
3.2. Coagulation
Coagulation Experiment
Experiment
3.2.1.
3.2.1. Effect
Effect of
of Dose
Dose on
on the
the Coagulation Performance
Coagulation Performance
Figure
Figure 33presents
presents
the the
effecteffect of changing
of changing the dosethe dosetheofmodified
of both both theandmodified and
non-modified
non-modified bananaon
banana peel powder peel
thepowder on the
coagulation coagulation It
performance. performance. It canthat
can be observed be the
observed
effect
that the increased
steadily effect steadily
with increased
increasingwith increasing
the dose the doseinconcentration
concentration in a in
a similar manner similar
both
manner in The
materials. bothhighest
materials. The highest
removal removal
dose differed dose differed
between between
the modified the modified
banana peel powderba-
nana peel powder (0.4 g/L) and non-modified powder (0.6 g/L). Higher doses led to a
reduced removal efficiency, which could be attributed to the slight dissolving of poly-
saccharides and other materials in the banana peel powder, which led to a slight decrease
in the removal activity. Our results were better than those obtained by Parvatham et al.
Water 2022, 14, 2473 6 of 15

(0.4 g/L) and non-modified powder (0.6 g/L). Higher doses led to a reduced removal
efficiency, which could be attributed to the slight dissolving of polysaccharides and other
materials in the banana peel powder, which led to a slight decrease in the removal activity.
Our results were better than those obtained by Parvatham et al. [27], who used a lower
turbidity of only 44 NTU and reported that the optimum dose of banana peel was 5 g/L.
Banana peels contain several bio-flocculants [36], and the smaller size and sticky edges
of the modified powder helped in releasing such materials, placing them in contact with
Water 2022, 14, x FOR PEER REVIEWturbid water. Thus, a smaller dose (0.4 g/L) in modified powder was enough to achieve7 of w
16
removal of 90% for the overall water turbidity.

Figure 3.3.Coagulation
Figure Coagulationactivity
activityof of
thethe modified
modified andand non-modified
non-modified banana
banana peel powder
peel powder at different
at different doses.
doses.
3.2.2. Effect of pH on the Coagulation Performance
3.2.2.AEffect
betterofcoagulation
pH on the performance
Coagulation Performance
was found in neutral conditions with a pH value of
6 to 8.AFigure
better4coagulation
presents theperformance was found inofneutral
coagulation performance bananaconditions
peel powderswithinawhich
pH value
can
of 6 to 8. Figure 4 presents the coagulation performance of banana peel powders in which
be clearly seen that it affected both of them in a similar manner, despite the superior activity
can
of be clearly
modified seen that
banana peel itpowder.
affectedUsing
both the
of them in a similar
optimum dose ofmanner,
modifieddespite the superior
and non-modified
activity of modified banana peel powder. Using the optimum dose become
banana peel powder, the turbidity removal was reduced when the pH of modified
acidic,and
at
non-modified
(pH = 2) 57 andbanana
55 % forpeel powder, and
the modified the non-modified
turbidity removalbananawas reduced
peel powder, when the pH
respectively.
become acidic,
However, at (pH = pH
at an alkaline 2) 57
(pHand 55 %the
= 11), forturbidity
the modified andwas
removal non-modified
reduced bybanana peel
78 and 62%
for modified and non-modified banana peel powder, respectively. A
powder, respectively. However, at an alkaline pH (pH = 11), the turbidity removal was previous study a
showed similar finding, that banana peel had the best turbidity
reduced by 78 and 62% for modified and non-modified banana peel powder, respec-removal in natural and
slightly
tively. Aalkaline
previouspHstudy
(pH 8.0) [37]. Atsimilar
a showed natural and slight
finding, thatalkaline
banana pH,
peel the
hadcoagulant cationic
the best turbidity
charged banana peel particles were equal to the clay particles (anionic suspension),
removal in natural and slightly alkaline pH (pH 8.0) [37]. At natural and slight alkaline and
thus destabilized them all through the coagulation mechanism. In a previous
pH, the coagulant cationic charged banana peel particles were equal to the clay particles study by
Chong and Kiew, the authors achieved turbidity removal in alkaline (93.4%)
(anionic suspension), and thus destabilized them all through the coagulation mechanism. and acidic
(81.4%) conditions, and reported a significant decrease in the coagulation performance
In a previous study by Chong and Kiew, the authors achieved turbidity removal in alka-
when the pH of the solution was increased (from 4–8), while this increased drastically
line (93.4%) and acidic (81.4%) conditions, and reported a significant decrease in the co-
beyond pH 8 [38]. This can be explained by the complex structure of the banana peel
agulation performance when the pH of the solution was increased (from 4–8), while this
material, which may contain amphoteric ions. As reported in a previous study, the removal
increased drastically beyond pH 8 [38]. This can be explained by the complex structure of
mechanism of banana peel involves both coagulants and flocculants, which mean the action
the banana peel material, which may contain amphoteric ions. As reported in a previous
of more than one mechanism at the same time [39].
study, the removal mechanism of banana peel involves both coagulants and flocculants,
which mean the action of more than one mechanism at the same time [39].
Water2022,
Water 14,2473
2022,14, x FOR PEER REVIEW 87 of 16
of 15

Water 2022, 14, x FOR PEER REVIEW 8 of 16

Figure 4.
Figure 4. Coagulation
Coagulationactivity
activityofofmodified
modifiedand
andnon-modified banana
non-modified peel
banana powder
peel at different
powder pH
at different
levels.
pH levels.
Figure 4. Coagulation activity of modified and non-modified banana peel powder at different pH
levels.
3.2.3. Effect
3.2.3. Effect of
of Sedimentation
Sedimentation Time
Time on
on the
theCoagulation
CoagulationPerformance
Performance
In
3.2.3.In thisof
Effect
this study, sedimentation
Sedimentation
study, Time on
sedimentation time seemed
the seemed
time toto
Coagulation not have a significant
Performance
not have a significant effect
effect on the
on the co-
coagu-
agulation
lation this performance.
Inperformance. Similar
Similar
study, sedimentation resultsresults
time werewere
seemed reported
reported
to not after
have after
30 min 30 of
a significant min ofon sedimentation
sedimentation
effect the co- in both in
both samples,
samples,
agulation as canasbe
performance.can be
seen seen from
fromresults
Similar Figure Figure
5. The
were 5. The powder
powder
reported 30 requires
afterrequires
min of some sometimetime
sedimentation toinsedimen-
to sedimentate,
tate, samples,
both
only only
the theasflocs
huge huge flocs
can were
be seen were directly
from Figure
directly sedimented
5. The
sedimented powder after
min, 10
after 10requires min,time
insome
which inthe
which
toturbiditythe turbidity
sedimen- removal
tate,
was only
removal
76 andthe64%
was huge
76for flocs
and werefor
64%
modified directly
modified
and sedimented after
and non-modified
non-modified banana 10 min, in whichpeel
peel banana
powder, the turbidity
powder, Similar
respectively. respec-
removal
results was
were 76 and
obtained 64%by for modified
Mahmudabadi and etnon-modified
al. [40], who banana
tively. Similar results were obtained by Mahmudabadi et al. [40], who reported that the
reported peel
thatpowder,
the respec-
removal efficiency
tively.
removal
of Similar
the coagulant results
efficiency were
of
remainedtheobtained
coagulant
constant by after
Mahmudabadi
remained et al. [40],
constant
a sedimentation after who
time ofreported
a sedimentation
100 min. thatInthe
time of 100
our study,
removal efficiency of the coagulant remained constant after ato
sedimentation time of 100turbidity
min. In our study, only 30 min was needed to sedimentate all the flocs and to achieve the
only 30 min was needed to sedimentate all the flocs and achieve the optimum
min. In ourAnother
study, only 30 min
usedwas needed to sedimentate all the flocs andand to achieve theresults of
optimum turbidity
removal. removal.
study Another
the aqueous study usedofthe
extract aqueous
Moringa extract
oleifera of Moringa
showed oleifera
optimum turbidity removal. Another study used the aqueous extract of Moringa oleifera
and showed
turbidity results
removal with of turbidity
sedimentation removal
timewith sedimentation
similar to ours [41]. time
and showed results of turbidity removal with sedimentation time similar to ours [41].
However, similar to
although ours [41].
there
were significant
However,although
althoughdifferences
there in
were the particle
significant sizes in our
differences study, modified particles were able
However, there were significant differences in the in the particle
particle sizes in sizes in our study,
our study,
to form large
modified
modified
flocs
particles
particles were
and
were sedimentate
ableable to form
to form
in flocs
a similar
largelarge flocs time as theinlarger
and sedimentate
and sedimentate in
a similar
non-modified
a time
similar time
as the
banana
as the
peel
largerpowder.
largernon-modified
non-modified banana
banana peelpeel powder.
powder.

Figure 5.
Figure 5. Coagulation
Coagulationactivity of modified
activity and non-modified
of modified bananabanana
and non-modified peel powder at different
peel powder at different
sedimentation times.
sedimentation times.
Figure 5. Coagulation activity of modified and non-modified banana peel powder at different
sedimentation times.
Water 2022, 14, x FOR PEER REVIEW 9 of 16
Water 2022, 14, 2473 8 of 15

3.2.4. Effect of NaCl Quantity on the Coagulation Performance

3.2.4.The effect
Effect of different
of NaCl Quantity quantities of NaCl onPerformance
on the Coagulation the coagulation performance of modi-
fied The
and effect
non-modified banana peel powders is presented
of different quantities of NaCl on the coagulation in Figure 6. It can be
performance seen that
of modified
NaCl in small amounts of less than 0.4 g/dm 3 showed enhancement in the coagulation
and non-modified banana peel powders is presented in Figure 6. It can be seen that NaCl in
performance
small amountsby of2%
less(from 90%
than 0.4 to 92%).
g/dm A larger
3 showed quantity induced
enhancement a dramaticperformance
in the coagulation drop in the
activity.
by NaCl
2% (from 90%was toused
92%).toAincrease the solubility
larger quantity induced of banana
a dramaticpeeldrop
proteins
in thebyactivity.
the salting-in
NaCl
effect,
was usedwhich enhanced
to increase thethe breaking
solubility of of protein
banana peelassociations,
proteins byleading to increased
the salting-in effect,protein
which
solubility the
enhanced [42].breaking
NaCl worked in a similar
of protein manner
associations, for both
leading the modified
to increased and solubility
protein non-modified[42].
banana
NaCl peel powders,
worked which
in a similar couldfor
manner be both
due to the
the ion exchange
modified that occurred banana
and non-modified betweenpeelthe
clays and which
powders, Na ions,
+ andbe
could theduecoagulation
to the ionefficiency
exchangeof banana
that occurredpeel between
did not depend
the claysonand
the
protein
Na contents. This exchange led to increasing the negativity of the surface charge in
+ ions, and the coagulation efficiency of banana peel did not depend on the protein

the clay and

contents. enhancingled
This exchange theto coagulation
increasing theperformance, while
negativity of the a larger
surface charge amount of NaCl
in the clay and
caused alterations
enhancing in the coagulant
the coagulation performance, charges,
while leading to limiting
a larger amount its coagulation
of NaCl perfor-
caused alterations
mance.
in A previous
the coagulant study
charges, done to
leading bylimiting
Eskibalci
its and co-workers
coagulation reported A
performance. theprevious
same results,
study
where large quantities of NaCl increased the turbidity values and reduced the coagula-
done by Eskibalci and co-workers reported the same results, where large quantities of NaCl
tion activity [43]. Although NaCl is not harmful to humans and the environment, adding
increased the turbidity values and reduced the coagulation activity [43]. Although NaCl
it not
is to drinking
harmfulwater could and
to humans raisethe another issue of changing
environment, adding it the water taste
to drinking andcould
water it thus be-
raise
come unacceptable
another issue of changingfor drinking.
the water taste and it thus become unacceptable for drinking.

Figure 6.
Figure 6. Coagulation
Coagulationactivity
activityofof
modified andand
modified non-modified banana
non-modified peelpeel
banana powder at different
powder NaCl
at different
quantities.
NaCl quantities.

3.2.5. Effect
3.2.5. Effect of
of Powder
Powder Solution
Solution onon the
the Coagulation
Coagulation Performance
Performance
The solution
The solution of of banana
banana peels
peels had
had aa weaker
weaker coagulation
coagulation effect
effect compared
compared with with the the
powder (Figure
powder (Figure7).7).The
Themodified
modified banana
banana peel
peel solution
solution generally
generally had had a stronger
a stronger effecteffect
than
than
the the non-modified
non-modified bananabanana peel solution,
peel solution, and theand the coagulation
coagulation effect ofeffect of both solutions
both solutions steadily
steadily increased with the increase in their concentration. At the lowest concentrationthe
increased with the increase in their concentration. At the lowest concentration of 1 wt.%, of
1 wt.%, the
turbidity turbidity
removal wasremoval was almost
almost similar similar and
for modified for modified
non-modifiedand non-modified banana
banana peel solutions
peel
at 35 solutions at 35 and 33%,
and 33%, respectively. respectively.
However, at the However,
maximum at the maximum
tested concentrationtested
(10 concentra-
wt.%), the
tion (10 wt.%),
turbidity removal theincreased
turbiditytoremoval
81 and 72%,increased to 81 and
respectively. 72%, respectively.
Microwave Microwave
treatment helped with
treatment helped with the extraction of active compounds from banana peel [44], which
the extraction of active compounds from banana peel [44], which explained the enhanced
explained
effect of thethe enhanced
modified effectpeel
banana of the modified
solution, bananaatpeel
although the solution, although at The
same concentration. the same
SEM
figures show the fractions in the particle surfaces that allowed the particles
concentration. The SEM figures show the fractions in the particle surfaces that allowed to be fully
hydrated, allowing the active compounds to be released from them.
the particles to be fully hydrated, allowing the active compounds to be released from Pathak et al. [45]
reported
them. Pathakthat the surface
et al. of their banana
[45] reported that thepeel became
surface rough
of their and porous
banana after microwave
peel became rough and
treatment, which confirmed the efficiency when releasing the active compounds. Similarly,
Water 2022, 14, x FOR PEER REVIEW 10 of 16

Water 2022, 14, 2473 9 of 15

porous after microwave treatment, which confirmed the efficiency when releasing the
active compounds. Similarly, Vu et al. [46] found that microwave treatment assisted the
extraction
Vu et al. [46]offound
phenolic compoundstreatment
that microwave from banana peels
assisted by inducing
the extraction porous and
of phenolic surface
compounds
fraction.
from Although
banana the
peels by optimum
inducing solution
porous in banana
and surface peel was
fraction. found the
Although to be the strongest,
optimum solutionit
still
in considered
banana weaker
peel was found than thethe
to be powder. Mokhtar
strongest, it stilletconsidered
al. [36] used NaOH
weaker to enhance
than the
the powder.
extraction of active compounds from banana peels and reported that only 0.1 g/L was
Mokhtar et al. [36] used NaOH to enhance the extraction of active compounds from banana
enough
peels andtoreported
achieve that
88% only
turbidity
0.1 g/Lremoval. Our findings
was enough to achieve could
88%have been less
turbidity than that,
removal. Our
but using NaOH will end up with the addition of another drawback, as further processes
findings could have been less than that, but using NaOH will end up with the addition of
will be required
another drawback, to as
remove it from
further the water.
processes will be required to remove it from the water.

Figure 7.
Figure 7. Coagulation
Coagulation activity
activity of
of different
different concentrations
concentrations of
of modified
modified and
and non-modified
non-modified banana
banana
peel solutions.
peel solutions.

3.3. Effect
3.3. Effect of
of Modified
Modified Banana
Banana Peel
Peel Powder
Powder onon River
River Water
Water Treatment
Treatment
Modified and non-modified banana peel powders were
Modified and non-modified banana peel powders were appliedapplied for actual
for actual river
river water
water
at at the optimized
the optimized conditions
conditions to investigate
to investigate theirineffect
their effect other in other
water water treatment
treatment parameters.pa-
rameters.
Table Table 1the
1 presents presents the physico-chemical
physico-chemical parameters parameters
of the river of water
the river water
before and before
after and
the
after the treatment.
treatment. It can be observed
It can be observed that the reduction
that the reduction in river
in river water water was
turbidity turbidity wasthat
less than less
than
in the that in the
synthetic synthetic
turbid water,turbid
which water,
was 76 which
and 84% was
for 76 and 84% for
non-modified and non-modified
modified banana and
modified
peel powder,banana peel powder,
respectively. respectively.
However, this couldHowever,
be due tothis could turbidity
the initial be due tolevelthe (36%)
initial
turbidity level (36%) and/or turbidity of river water, which could be due other chemical
and/or turbidity of river water, which could be due other chemical or microorganisms in
or microorganisms in which banana peels have limited coagulation action in [28]. Re-
which banana peels have limited coagulation action in [28]. Recently, Yimer, and Dame
cently, Yimer,
reported and Dame
that coliform reported
bacteria that coliform
can highly bacteria
affect the can highly
initial river affect water
and surface the initial river
turbidity,
which were significantly increased when increasing the dose of the natural
and surface water turbidity, which were significantly increased when increasing the dose coagulant up to
certain dosage stage [47]. Banana peel biomasses contain various chemical
of the natural coagulant up to certain dosage stage [47]. Banana peel biomasses contain groups such
as carboxylic
various chemicalacid,groups
phosphate,
such asand hydroxylacid,
carboxylic groups, which also
phosphate, act as active
and hydroxyl centers
groups, for
which
the adsorption of water color, TDS, TSS, and COD [48]. Microwave treatment
also act as active centers for the adsorption of water color, TDS, TSS, and COD [48]. Mi- of banana
peels
crowaveincreases theirofadsorption
treatment banana peelscapacity, which
increases explains
their the enhanced
adsorption capacity,removal of river
which explains
water pollutants after modified banana peel treatment. Modified
the enhanced removal of river water pollutants after modified banana peel treatment. banana peel powder
significantly increased the adsorption capacity of river water pollutants, which may be
Modified banana peel powder significantly increased the adsorption capacity of river
accredited to the superior ion exchange capacity and favorable microprecipitation on the
water pollutants, which may be accredited to the superior ion exchange capacity and
surfaces due to the presence of a high porosity in the modified particles compared with the
favorable microprecipitation on the surfaces due to the presence of a high porosity in the
non-modified ones, as reported by Li [49].
modified particles compared with the non-modified ones, as reported by Li [49].
Water 2022, 14, 2473 10 of 15

Table 1. Effect of modified and non-modified banana peel powder in river water treatment.

Before Treatment After Treatment

Parameter
Result Non-Modified Banana Peel Modified Banana Peel
(Mean ± SD) Powder Powder
Temperature (◦ C) 29 29 29
Turbidity (NTU) 36.1 ± 3.4 8.5 ± 1.2 (76%) 5.76 ± 1.7 (84%)
pH 6.78 ± 0.1 6.92 ± 0.4 6.98 ± 0.6
Color Faint brown Colorless Colorless
Total dissolved solid (mg/L) 43.6 ± 5.1 8.3 ± 1.1 5.7 ± 3.3
Total suspended solid (mg/L) 35.2 ± 1.3 11.8 ± 2.5 9.3 ± 1.4
Chemical oxygen demand (mg/L) 87.2 ± 4.2 61.8 ± 3.9 60.1 ± 2.8
Biochemical oxygen demand (mg/L) 31.7 ± 2.3 26.2 ± 1.8 24.4 ± 1.1

4. Discussion
Several studies used microwave and ultrasonic treatment during the coagulation pro-
cess, without examining the effect of these treatments on the particles themselves [50]. The
significant reduction in particles size could be due to the fragility of the fibers after multiple
microwave treatments. Despite the mild heating in each treatment, microwaves are able
to induce surface fractions on smooth surfaces, leading to their breaking and detachment,
which explains the insignificant reduction in particle diameters [44]. Eng et al. [33] ex-
tracted bio-flocculants from banana peels and used them in pure form, and reported an
optimum turbidity removal performance of only 45.16%. However, the results of this study
were significantly higher than that. Based on our finding, it can be seen that modified
banana peel powder had the best action compared with the non-modified one and their
solutions. Exposing the powder to microwave radiation produces more fractions in the
powder’s particles, which enhances their adsorption and captures the turbidity, leading to
a better performance. The scanning electron micrograph showed the existence of pores fa-
vorable for the sorption mechanism, which explains the reduction in river water pollutants,
besides turbidity reduction. The modified banana peel powder exhibited a coagulation
and sorption mechanism of action; the enhanced removal of river pollutants confirms the
sorption action of the powder. Our findings confirm the results of several studies on the
sorption mechanism of banana peel powder [49,51,52]. Charge neutralization and bridge
formation are the two main known coagulation and flocculation mechanisms for most
natural plant coagulants [53]. At a constant condition, the coagulation performance of
the three materials of banana peels can be compared, as presented in Table 1. The filtrate
of banana peels was considered to be one, as there were no significant different between
the modified and non-modified filtrate at small concentrations, which presented only 38%
removal capacity compared with the modified powder, which was 92% at the same condi-
tions. Although the dose of banana peel was relatively higher than that of the literature,
most previous literature used filtrate rather than raw powder, which increased the costs
and processing time. Table 2 presents a comparison of our findings with other natural
coagulants in different conditions. As shown in the table, different natural coagulants
experimented under different conditions, and the turbidity removal among them ranged
between 54 to 96% for apricot seed extract and moringa seed powder, respectively [54,55].
Our modified banana peel powder recorded a 92% reduction under natural conditions,
which is comparative with other coagulants, considering it as a waste.
Water 2022, 14, 2473 11 of 15

Table 2. Comparison of the coagulation performance of the modified banana peel powder with
previous literature.

Bio-Coagulant Optimal Experimental Conditions Turbidity

Dose (g/L) pH Type of Waste Water Reference
Removal (%)
Banana peel extract 0.1 1 Synthetic domestic wastewater 88 [36]
Moringa seed powder 0.15 6–8 Paper mill effluent 96 [55]
White popinac 0.05 7 Synthetic turbid river water 76 [56]
Iraqi date seed extract 0.06 7 Synthetic turbid water 90 [57]
Apricot seed extract 0.03 7 Raw surface water 54 [54]
Jackfruit peel extract 0.1 2 Sewage synthetic wastewater 70 [58]
Banana peel powder 0.4 7 Kaolin synthetic wastewater 59 [59]
Non-modified banana peel
0.6 6–8 Kaolin synthetic wastewater 81 This study
powder
Modified banana peel powder 0.4 6–8 Kaolin synthetic wastewater 92 This study

Figure 8 presents an illustration of the coagulation mechanisms for the three tested
samples, namely non-modified banana peel powder, modified banana peel powder, and
their solutions (filtrate). The primary purpose of using a coagulant, besides removing
very fine particles from suspensions, is that this process results also in less turbidity of the
water, i.e., clearer water. With the coagulants’ positive charge, the negatively charged parti-
cles in the water are neutralized. Banana peel possesses positively charged proteins and
polysaccharides that interact with opposite (negatively charged) suspended solids, leading
to their neutralization and precipitation. Forming bridges between the particles enhances
the removal efficiency, which could occur in modified banana peel as a result of modifi-
cation. Although regular banana peel particles also possess positive charges, the larger
size of the particles restricts the bridging performance of the particles. Vilardi et al. [60]
reported that banana peel possessed a good adsorption capacity for heavy metals, which is
a different mechanism of banana peels in water treatment. The smaller size of the modified
powder helped to reduce the repulsive forces between the clay particles, resulting in a
higher formation of microflocs and thus a better coagulation performance. Rapid mixing is
normally used to enhance the formation of microflocs and to induce the collision between
the coagulant particle and suspended solids [61]. However, as our study used constant
mixing for the two powders, modified banana peel powder formed more micrflocs in a
faster manner compared with the unmodified one, and this formation of bridge linkages
then promoted the binding effect (due to the surface roughness) among them. This pro-
cess results in the formation of much larger flocs, consisting of small banana peels and
suspended solids in the subsequent flocculation process. In the case of using non-modified
banana peel powder, the large particles may sediment without forming large flocs, thus
producing a lower coagulation performance.
The raw water was faint brown in color, due to the high turbidity, and total dissolved
and suspended solids. After the treatment with both powders, it can be observed that
modified powder had better action in reducing all of the parameters. Although the chemical
oxygen demand of raw water was 87.2 ± 4.2 mg/L, a small reduction occurred even in the
case of modified powder, which reduced to 60.1 ± 2.8 mg/L. River water collected several
types of chemical compounds and minerals, and the action of the banana peel was limited
to the formation of flocs and/or formation of bridge linkages [61]. Not all the chemicals
can be coagulated around the particles, and thus limited action was reported for COD.
This hypothesis can be confirmed with the results of the biochemical oxygen demand,
which reflected the action of microorganisms. It slightly reduced from 31.7 ± 2.3 mg/L
to 26.2 ± 1.8 and 24.4 ± 1.1 mg/L for non-modified and modified banana peel powders,
respectively. Similar findings were reported for BOD, and the authors reported a slight
decrease and reported that the increase in BOD was due to the natural coagulant itself,
especially at high dosage [62]. Based on the results obtained from the present study,
modified banana peel powder has great potential in water treatment applications, and it
could be also used in the adsorption of dyes and other pollutants [60,63].
Water2022,
Water 14,2473
2022,14, x FOR PEER REVIEW 13 16
12 of 15

Figure8.8.Schematic
Figure Schematic illustration
illustration of the
of the coagulation
coagulation performance
performance of modified
of modified and non-modified
and non-modified banana
banana peel powder, and banana peel
peel powder, and banana peel filtrate. filtrate.

The raw water was faint brown in color, due to the high turbidity, and total dis-
5. Conclusions
solved
Theand suspended
utilization solids.
of plant After has
wastes the always
treatmentbeenwith both powders,
a golden it can scientists
goal for many be observed to
that modified powder had better action in reducing all of the parameters.
ensure the sustainable utilization of natural material and minimize the use of chemical Although the
chemical
or syntheticoxygen demandThis
substances. of raw water
study was 87.2
confirmed the± 4.2 mg/L,
ability a small
to use green reduction
enhancementoccurredof
even inpeel
banana the case
wasteofinmodified powder,applications.
water treatment which reduced Basedto on
60.1all±the
2.8findings
mg/L. River waterbeen
that have col-
lected several
gathered, it cantypes of chemical
be concluded thatcompounds
banana peels and minerals,
after microwave and modification
the action ofpresented
the banana a
peel coagulation
high was limited performance
to the formation of flocswith
compared and/or formation of
non-modified bridgeThe
powder. linkages
filtrate[61]. Not all
of banana
the chemicals
peel showed a can be coagulated
weaker effect at thearound the particles,
same dose, and thus
and increased withlimited actionthe
increasing was re-
dose.
ported for COD.
Microwave This of
treatment hypothesis
banana peel canpowder
be confirmed
induceswith the results
fractions in theofparticles,
the biochemical
leading
oxygen
to roughdemand, which
and porous reflected
surfaces thatthe action of microorganisms.
significantly It slightly reduced
enhanced the coagulation from
performance.
31.7mild
The ± 2.3 heating
mg/L toof26.2 ± 1.8 and
treatment 24.4
also ± 1.1 mg/L
assesses for non-modified
the grinding and modified
process, resulting banana
in a smaller
peel powders,
particle respectively.
size, which Similar
also enhanced the findings
coagulationwere reported for
performance. TheBOD, and the
significant authors
reduction
reported a slight decrease and reported that the increase in BOD was due to the natural
in river water turbidity, color, total dissolved and suspended solids, and chemical and
coagulant itself, especially at high dosage [62]. Based on the results obtained from the
biochemical oxygen demand demonstrated the potential of modified banana peel powder
present
as study, modified
an alternative solution banana peel powder
to synthetic, chemical,hasor great potential in
even expensive watercoagulants,
natural treatment ap- in
plications,
addition and it value
to added couldtobethealso used inofthe
utilization adsorption
banana of dyes
peel wastes and other pollutants
available.
[60,63].
Author Contributions: Conceptualization, A.A.A., E.B.Y. and M.R.; writing—original draft prepara-
tion, A.A.A. and E.B.Y.; writing—review and editing, M.I.A., J.L., M.A., M.R.S. and M.R.; supervision,
5. Conclusions
M.I.A., J.L. and M.R.; funding acquisition, M.R. and M.R.S. All authors have read and agreed to the
The version
published utilization ofmanuscript.
of the plant wastes has always been a golden goal for many scientists to
ensure the sustainable utilization of natural material and minimize the use of chemical or
Funding: The authors are grateful to the Researchers Supporting Project Number (RSP-2021/326),
synthetic substances. This study confirmed the ability to use green enhancement of ba-
King Saud University, Riyadh, Saudi Arabia.
nana peel waste in water treatment applications. Based on all the findings that have been
gathered, it Review
Institutional can be Board
concluded that banana
Statement: peels after microwave modification presented
Not applicable.
a high coagulation
Informed performance
Consent Statement: compared with non-modified powder. The filtrate of
Not applicable.
banana peel showed a weaker effect at the same dose, and increased with increasing the
Data
dose.Availability
Microwave Statement: Theofdata
treatment that support
banana this studyinduces
peel powder are available in thein
fractions article.
the particles,
leading to rough and
Acknowledgments: porousare
The authors surfaces
gratefulthat significantly
to the Researchers enhanced
Supportingthe coagulation
Project per-
Number (RSP-
formance.King
2021/326), The Saud
mildUniversity,
heating ofRiyadh,
treatment also
Saudi assesses the grinding process, resulting in a
Arabia.
smaller particle size, which also enhanced the coagulation performance. The significant
Water 2022, 14, 2473 13 of 15

Conflicts of Interest: The authors declare no conflict of interest.

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