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https://doi.org/10.1007/s11356-018-3850-9
Abstract
In this study, aqueous extracts of Musa paradisica (banana) peels and Dolichos lablab (Indian beans) seeds were prepared and
tested as natural coagulants for turbidity removal from simulated turbid water. Effects of extraction time (15, 30, and 45 min),
dosage (0.2 to 1.0 mL/L), and water pH on turbidity removals by the natural coagulants were evaluated. In both cases, the
extraction time of 45 min for the preparation of aqueous extract and dosage of 0.6 mL/L gave the best results in terms of turbidity
removal. Natural coagulants from M. paradisica peels powder could efficiently remove turbidity (> 83%) at all tested pH values
(3.0 to 12.0) with maximum turbidity removal of 98.14% at pH 11. In the case of D. lablab seeds, low turbidity removal (71–
74%) was observed at pH between 5.0 and 9.0. The maximum turbidity removal (98.84%) was obtained at pH 11. The scanning
electron microscopy (SEM) analysis of the settled flocs revealed that more compact flocs formed using M. paradisica peels
extract than those developed using D. lablab seeds extract. The chemical analysis and Fourier transform infrared (FTIR)
spectroscopy of the extracts revealed that polymeric substances (carbohydrate and proteins) having functional groups –OH,
C–N, C–C, –COOH, and N–H might be responsible for the coagulation activity. The zeta potential measurements of natural
coagulants revealed that the possible coagulation mechanism would be adsorption and bridging between particles. This study
demonstrated the potential use of aqueous extracts of M. paradisica peels and D. lablab seeds as low-cost natural coagulants for
turbidity removal.
Keywords Natural coagulants . Banana peels . Dolichos lablab . Sustainable water treatment . Turbidity removal
sludge handling cost make natural coagulants as logical, sus- allowed to cool down to room temperature, and the developed
tainable choice for turbidity removal (Renault et al. 2009; color intensity was measured at 620 nm.
Nharingo and Moyo 2016; Bouaouine et al. 2018; Choy et al. The protein contents in the aqueous extracts were analyzed
2014). Various plant-based natural coagulants such as vegeta- by the standard Bradford assay using bovine serum albumin
bles, grains, and legumes have been studied for the turbidity standard (Bradford 1976). In brief, 10 μL of the sample (aque-
removal from water and wastewater (Choy et al. 2016; Kukić ous extract) was mixed with 1 mL of Bradford reagent, incu-
et al. 2015; Mohamed et al. 2015; Muthuraman and Sasikala bated for 5 min before taking absorbance at 595 nm. Fourier
2014; Ramavandi 2014). Some renewable materials such as transform infrared spectra (FTIR) of the powdered samples
orange peel, banana peel, banana pith, papaya seeds, and neem were obtained as KBr pallet with FTIR spectrometer (Perkin
leaf have also been tested (Maurya and Daverey 2018; Kakoi Elmer®, Spectrum Two). FTIR of the aqueous extracts was
et al. 2016). However, difficulties in preparation and/or pro- obtained as KBr pallet with Thermo Nikolet Nexus FTIR
cessing of natural coagulants possess a major hurdle to be ad- spectrometer. The zeta potential of aqueous extracts was mea-
dressed before their successful commercialization. Therefore, sured at different pH (3.0–12.0) using water as solvent by
exploration and extrapolation of simple preparation/extract Zetasizer (Nano-ZS, Malvern, UK).
methods for natural coagulants are highly desirable.
The aims of this study were to prepare natural coagulants Preparation of simulated turbid water
from Musa paradisica (banana) peels and seeds of Dolichos
lablab (Indian bean) by simple method, characterize the pre- Simulated turbid water, to test the potential of the prepared
pared natural coagulant, and evaluate the effects of process natural coagulants, was prepared in the laboratory as reported
parameters (extraction time of natural coagulant, water pH, co- by Kukić et al. (2015). In brief, kaolin powder (1% w/v) was
agulant dosage, and settling time of flocs) on turbidity removal. suspended in tap water and stirred for 2 h in a magnetic stirrer.
To the best of our knowledge, this is the first report on testing The suspension was kept undisturbed for 24 h to achieve
the aqueous extract of M. paradisica peels as natural coagulant. complete hydration of kaolin. This kaolin suspension was kept
in a refrigerator until use. Simulated turbid water was prepared
by 5× dilution of kaolin suspension in tap water. The turbidity
Materials and methods of this simulated turbid water, prepared just before the jar test,
was ~ 62 NTU.
Preparation of natural coagulants
Turbidity removal by natural coagulants
The peels of M. paradisica were collected from the Doon
University Hostel Mess, while the seeds of D. lablab were Experiments on turbidity removal by aqueous extracts of M.
purchased from local market, Dehradun, India. The natural paradisica peels and D. lablab seeds were performed using a
coagulants from the samples were extracted in distilled water six-paddle laboratory scale jar test apparatus (Microteknik,
as described by Kukić et al. (2015), with minor modifications. India). All the experiments were conducted in 1000 mL beakers
The banana peel was sun-dried for a week, followed by oven using 500 mL of simulated turbid water with a predefined dos-
drying at 60 °C for 20 min, before ground to fine powder age of aqueous extracts of M. paradisica peels and D. lablab
using a mortar pestle. The powder (1 g) was suspended in seeds. The suspension was rapidly stirred for 2 min at 150 rpm,
100 mL of distilled water, stirred for 15–45 min on a magnetic followed by a gentle agitation at ~ 80 rpm for 20 min to promote
stirrer at room temperature, and then filtered to obtain aqueous the flocs formation. The mixing was stopped and after 60 min of
extracts of M. paradisica peels. The seeds of D. lablab were settling time (if not specified), the supernatant was collected and
ground to fine powder, and the aqueous extract was prepared its turbidity was measured. The settled flocs were also collected
in a manner similar to that of M. paradisica. Both the extracts and characterized under a scanning electron microscope.
were stored in a refrigerator until use. All the experiments were performed in duplicate and con-
ducted at room temperature. Three sets of experiments (in
Characterization of natural coagulants duplicates) were performed for each coagulant. In the first
set of experiments, effects of extraction time (15, 30, and
The pH and turbidity of the prepared aqueous extracts were 45 min) of active coagulant and dosage (0.2 to 1.0 mL/L) on
analyzed by pH meter and turbidity meter, respectively. The the turbidity removal were evaluated. Effects of initial pH (3.0
total carbohydrate content was analyzed by the anthrone to 12.0) of simulated turbid water and flocs setting time (15 to
method using a glucose standard (Scott and Melvin 1953). 60 min) during jar test on turbidity removals were studied in
In brief, 1 mL sample was taken in a test tube and 4 mL the second and third sets of experiments, respectively. An
anthrone reagent (ice cold) was mixed with it. The mixture extraction time of 45 min and 0.6 mL/L of coagulant dosage
was boiled for 15 min at 100 °C in a water bath. Samples were were kept on hold in the second and third sets of experiments.
Environ Sci Pollut Res
Table 1 Characteristics of
prepared natural coagulants Parameter Aqueous extract of M. paradisica peels Aqueous extract of D. lablab seeds
Fig. 2 Zeta potential of natural coagulants from M. paradisica peels and Fig. 4 Effect of initial pH of water on turbidity removal efficiency of
D. lablab seeds as a function of pH selected natural coagulants
of chemical analysis indicating the presence of carbohydrates Zeta potential of natural coagulants and their possible
and proteins in the extracts. mechanism
Fig. 3 Effect of extraction time and dosage on turbidity removal using Fig. 5 Effect of flocs settling time in jar test experiments on the turbidity
aqueous extracts of a M. paradisica (banana) peels and b D. lablab seeds removal efficiency of selected natural coagulants
Environ Sci Pollut Res
bridging between particles would be the most probable coag- experiments. Other natural coagulants (banana peels powder,
ulation mechanism of natural coagulants from M. paradisica papaya seed powder, neem leaf powder, banana stem juice,
peel and D. lablab seed. Similar zeta potentials and mecha- fava beans extracts, conventional starch) also showed negative
nism were reported in literature for the natural coagulants effects of high dosage (above optimum level) on turbidity
from Opuntia ficus-indica (Bouaouine et al. 2018). removal (Maurya and Daverey 2018; Kukić et al. 2015;
However, this is contradictory to the most widely used Choy et al. 2016).
coagulants—proteins from the seeds of Moringa oleifera
(Ndabigengesere et al. 1995) and alum (Subramonian et al. Effect of pH on turbidity removal
2014), whose coagulation mechanism is based on charge
neutralization. The pH is an important parameter in the coagulation process
as it can change the surface charge of the coagulant and/or
Effect of extraction time and dosage on turbidity pollutant (Kukić et al. 2015). Therefore, the effect of water pH
removal (3.0 to 12.0) on turbidity removals by aqueous extracts of M.
paradisica peel powder and D. lablab seed powder was stud-
Turbidity removals by the natural coagulants, processed at ied. For a fixed coagulant dosage (0.6 mL/L), maximum tur-
different extraction time (15, 30, and 45 min) from the M. bidity removal by both the aqueous extracts of M. paradisica
paradisica peel powder and D. lablab seed powder, were peel powder (98.14%) and D. lablab seed powder (98.84%)
studied at various dosages. The results, as shown in Fig. 3, was observed at pH 11.0 (Fig. 4). Three distinct phases of pH
clearly suggests a positive effect of extraction time on turbid- dependency on turbidity removal with D. lablab seed powder
ity removal efficiency for both the natural coagulants. It is extract were evident. Appreciable turbidity removal (78–84%)
obvious that with increasing time, the extracts got enriched was noted below pH 5.0 (phase I), followed by low turbidity
with polymeric substances (i.e., carbohydrates and proteins) removal (71–79%) between pH 5.0 and 9.0 (phase II), while
primarily responsible for the turbidity removal (Table 1). excellent turbidity removals (86–98%) were observed in
As expected, the coagulant dosage significantly influenced phase III (pH > 9.0). However, the impact of water pH was
the turbidity removal efficiency (Fig. 3a, b). In case of 45 min not significant in the case of extracts of M. paradisica peel
of extraction time, turbidity removals increased with dosage powder, where turbidity removals were > 80% at all tested pH.
up to 0.6 mL/L. Beyond this dosage, turbidity removals were Contrasting reports of pH dependence have also been reported
slightly diminished in both cases. Therefore, 0.6 mL/L was in the literature. For example, pH dependency on coagulation
used as an optimum coagulant dosage in the rest of the activity was reported for horse chestnut and acorn as natural
coagulants (Šćiban et al. 2009) but not with fava bean (Vicia the other hand, utilization of M. paradisica peels for the prep-
faba L.) seed extracts (Kukić et al. 2015). This indicates that aration of coagulant is beneficial as it is a waste material and
the natural coagulants from M. paradisica peel powder were would have negligible cost towards transportation, drying,
highly stable at a wide range of pH and can be used as a and grinding of peels. It is also important to note that the
coagulant for treating real water and wastewater samples. dosage of commercial coagulant is ~ 16 times higher than
natural coagulants (Table 2). This indicates that the use of
Effect of setting time on turbidity removal natural coagulants will generate ~ 16 times less sludge than
commercial coagulants to treat the same volume of water.
Settling of flocs formed due to the action of coagulants is an Therefore, the sludge handling cost can be lowered by replac-
important and last event of the coagulation-flocculation pro- ing the chemical coagulants with natural coagulants.
cess. A faster settling of flocs is desirable in the coagulation
process and indicates the efficiency of coagulant. Figure 5
shows the effect of settling time on the turbidity removal (co-
agulation efficiency) of aqueous extracts of M. paradisica peel
Conclusion
powder and D. lablab seed powder. As expected, the turbidity
The study revealed that water is a good solvent to extract
removal increased from 73.21 to 87.71% when settling time
active coagulants from M. paradisica peels and D. lablab
increased from 15 to 60 min for D. lablab seed’s coagulant.
seeds. Chemical analysis and FTIR analysis confirmed the
The maximum turbidity removal (95.13% and 87.71% by M.
presence of polymeric substances (carbohydrate and proteins).
paradisica peel powder and D. lablab seed powder, respec-
The functional groups –OH, C–N, C–C, –COOH, and N–H
tively) was observed at 60 min of settling time. The result
might involve in the coagulation process. Extraction time and
indicates that flocs formed by the coagulants from M.
dosage significantly affect the turbidity removal. The best re-
paradisica peel powder were settled faster than D. lablab seed
sults in terms of turbidity removal were obtained at 45 min of
powder.
extraction time and 0.6 mL/L of dosage. Natural coagulants
from M. paradisica peels are highly active at all tested pH (3
Morphology of flocs formed with natural coagulants
to 12). On the other hand, the best water pH for natural coag-
ulants from D. lablab seeds is either < 5 or > 9. The flocs
The surface of flocs formed after the jar test experiment was
formed by the coagulants from M. paradisica peels are denser
observed under the SEM to study their morphology. SEM
than coagulants from the D. lablab seeds. Overall, the study
images of flocs (Fig. 6) formed using M. paradisica peels
confirmed that aqueous extract of M. paradisica peels is better
extract (left) and D. lablab seeds extract (right) were of
coagulant than the aqueous extract of D. lablab seeds.
irregular-shape flakes. However, the flocs formed using M.
paradisica peels extract were more closely and firmly packed
Acknowledgments The authors would like to thank Mr. Ashis Ranjan
compared to that of D. lablab seed extract. The compact flocs Behera for zeta potential analysis.
may be desirable as they are easy to handle and separate. This
could be the reason for the faster settling of flocs formed by Compliance with ethical standards The authors have
the coagulants from M. paradisica peel powder. The morpho- followed the accepted principles of ethical and professional conduct.
logical studies of flocs further confirmed that the natural co- The work did not involve human participants and/or animals.
agulants extracted from M. paradisica peels are better than
Conflict of interest The authors declare that they have no conflict of
coagulants extracted from D. lablab seeds.
interest.
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