Article Not peer-reviewed version

Banana Peel Powder Biosorbent

for Removal of Hazardous Organic

Pollutants from Wastewater

Kelly C. S. Farias , Rita C. A. Guimarães , Karla Oliveira , Carlos E. D. Nazario , Julio A. P. Ferencz ,

*
Heberton Wender

Posted Date: 4 July 2023

doi: 10.20944/preprints202307.0154.v1

Keywords: Adsorption; biomass; glyphosate; atrazine; pesticides; dye

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Article
Banana Peel Powder Biosorbent for Removal of
Hazardous Organic Pollutants from Wastewater
Kelly C. S. Farias 1, Rita C. A. Guimarães 2, Karla R. W. Oliveira 3, Carlos E. D. Nazário 3,
Julio A. P. Ferencz 1,4 and Heberton Wender 1,*
1 Nano&Photon Research Group, Laboratory of Nanomaterials and Applied Nanotechnology (LNNA),
Institute of Physics, Federal University of Mato Grosso do Sul, Campo Grande, Mato Grosso do Sul, 79070-
900, Brazil
2 Graduate Program in Health and Development in the Midwest Region, Medical School, Federal University

of Mato Grosso do Sul, Campo Grande 79070-900, Brazil

3 Institute of Chemistry, Federal University of Mato Grosso do Sul, 79070-900, Campo Grande, MS, Brazil

4 Faculty of Engineering, Architecture, Urbanism, and Geography, Federal University of Mato Grosso do

Sul, 79070-900, Campo Grande, MS, Brazil

* Correspondence: author: heberton.wender@ufms.br

Abstract: Disposing pollutants into water sources has posed risks to human health and the environment, and
biosorption has emerged as an eco-friendly, cost-effective, and green alternative for wastewater treatment. This
work shows banana peel powder (BPP) biosorbents for efficient sorption of methylene blue (MB), atrazine, and
glyphosate pollutants. The biosorbent highlights several surface chemical functional groups and morphology
containing agglomerated microsized particles and microporous structures. BPP showed 66% elimination of MB
in 60 min, with an adsorption capacity (qe) of ~33 mg g-1, where a combination of film diffusion and
chemisorption governed the sorption process. Besides, the biosorbent removed 91% and 97% of atrazine and
glyphosate pesticides after 120 min, with qe of 3.26 and 3.02 mg g-1, respectively. The glyphosate and atrazine
uptake best followed the Elovich and pseudo-first-order kinetic, respectively, revealing different sorption
mechanisms. Our results suggest that BPP are low-cost biomaterials for green and environmentally friendly
wastewater treatment.

Keywords: adsorption; biomass; glyphosate; atrazine; pesticides; dye

1. Introduction
Pesticides are essential in modern agriculture, as they increase food production and reduce
weeds and pests in plantations [1]. However, overuse does pose severe risks to human health and the
environment. The water resources contaminated with these pollutants are a severe problem that
originates from their indiscriminate use in agricultural areas or accidental spills [2]. The existence of
toxic chemicals such as pesticides, pharmaceuticals, heavy metals, dyes, and microorganisms, even
in low or trace concentrations, has been advertised in the scientific community since they are very
hazardous to the environment, aquatic ecosystems, and human health [3].
Despite the abovementioned concerns, using pesticides on a large scale will likely persist for a
long time due to their great importance in agribusiness. Contamination caused by these compounds
in aqueous media is recurrent and conventional treatments are ineffective in removing them,
encouraging new treatment technologies to reduce or eliminate their adverse effects [4]. Methods
such as adsorption, electrochemical oxidation, advanced oxidation processes, chlorination,
bioremediation, ultra-filtration, photocatalysis, and reverse osmosis, have been adopted for
removing hazardous inorganic/organic pollutants from wastewater [5,6]. Among them, adsorption
is a feasible method due to its simplicity, ease of operation, and high removal efficiency [7]. Besides,
as it is not a destructive method, adsorption allows the recovery of the adsorbent. Activated carbon,
for example, has been extensively studied as an adsorbent, but its high cost limits its large-scale
application [6,8].

© 2023 by the author(s). Distributed under a Creative Commons CC BY license.

Preprints (www.preprints.org) | NOT PEER-REVIEWED | Posted: 4 July 2023 doi:10.20944/preprints202307.0154.v1

Generally, one can subdivide the adsorption process into chemical adsorption (or
chemisorption) and physical adsorption (or physisorption). Chemical adsorption is an irreversible
and localized process (which can only occur at active sites) that involves the formation of strong
bonds between the molecules and ions of the adsorbate on the surface of the adsorbent [9]. In contrast,
physical adsorption is a reversible and non-localized process (occurring on the entire surface of the
adsorbent), characterized by weak van der Waals forces, π-π and dipole-dipole interactions, and
electrostatic forces [7], where the adsorbed substance does not penetrate the solid but remains on its
surface.
When the adsorbent is a biological source material, it is called a biosorbent. Biosorption using
biomass materials is of considerable interest since it is low-cost, environmentally friendly,
biodegradable, and presents interesting physicochemical properties for the adsorption of metals or
organic compounds. In some cases, plant biomass has a high surface area and efficiently allows
contaminants removal by physical-chemical mechanisms similar to activated carbon sorbents [3]. The
usefulness of several biosorbent materials comes from a wide variety of organic groups in their
surface composition, such as carboxylic acids, phenols, amines, and amides, that can retain metal ions
or pollutant molecules through different mechanisms (chelation, ion exchange, and physical
adsorption) [10,11]. Besides, materials derived from biomass are fibrous, allowing more significant
contact between ions in solution with the active sites of the material.
Given their abundance and low cost, the banana peel comes with an alternative for generating
new biosorbents [12–14]. The banana is the world’s fourth most cultivated fruit, and its peel waste is
readily available, underutilized, and can be harnessed for commercial applications [15]. Therefore,
reusing this material to remove organic pollutants from contaminated water is a process of high
commercial interest. The use of dried banana peel powder (BPP) as a biosorbent material has been
explored for the decontamination of wastewater, mainly in the removal of textile dyes [16–19], heavy
metals [20–22], crude oil [23], phenolic compounds [24], pharmaceuticals [25,26], and pesticides [26–
28], as well documented in two relatively recent article reviews [15,29].
BPP was recently evaluated as a biosorbent for atrazine and ametryne removal from water [26].
The authors observed high adsorption capacities for both pesticides without chemical modifications
on the peel surface or pH adjustment. In another study, plantain banana peels (Musa paradisíaca L.)
were employed as biosorbents for removing the pesticide metribuzin from an aqueous solution,
showing a maximum adsorption capacity of 167 mg g-1 [27]. Besides, atrazine removal from water
using treated banana peels as biosorbent showed both pH and temperature dependent. In an
optimized condition (60 °C, 100 mL of atrazine @250 ppm, and 1.5 g of BPP pre-treated with H3PO4),
the biosorbent showed a maximum adsorption capacity of 14 mg g−1, and both external mass transfer
and intraparticle diffusion played essential roles in the adsorption mechanisms [28]. However, works
regarding the efficacy of banana peel at different maturation stages as biosorbents for removing
pesticides in water are scarce. To our knowledge, adsorption capacity and mechanisms have not been
reported in glyphosate pesticides.
Herein, we report Musa Paradisiaca L. BPP biosorbents prepared at three stages of maturation
to remove the hazardous pollutants MB, glyphosate, and atrazine from water, including a deep
discussion of the biosorbent adsorption capacity at equilibrium, the kinetic mechanisms, and aqueous
organic pollutants uptake efficiency. The readily available banana peels were specially processed to
obtain a powdered and low-cost adsorbent without any chemical treatment, ending in a completely
chemical-free, green, and environmentally friendly material. The biosorbent proposed in this study
is relatively simple, cost-effective, and easy to scale up for a practical application regarding removing
recalcitrant pesticides and other organic pollutants from water bodies.

2. Experimental
2.1. Materials
Methylene blue (MB, molecular formula: C16H18N3ClS) was purchased from Merck and used as
a model water-soluble cationic azo dye. Atrazine (molecular formula: C8H14ClN5), 99% pure, was
purchased from Sigma-Aldrich Brazil, and the commercial glyphosate product (C3H8NO5P) used was
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the Roundup® Transorb from Monsanto (a soluble concentrate containing 480 g L-1 glyphosate,
present as 588 g L-1 (43.8%ww) of the potassium salt of glyphosate). All the reagents were of analytical
grade and used without any further purification. All aqueous solutions in this study were prepared
using distilled water.

2.2. Banana Peel Powder Preparation

The banana peel samples were obtained from the Mato Grosso do Sul Supply Center (CEASA)
in Campo Grande – MS/Brazil. The fruits were cleaned with running water, immersed in a
hypochlorite solution (10 mL L-1) for 10 min, and manually peeled with a stainless-steel knife. The
banana peels at three stages of ripening (green, semi-ripe, and ripe) were dehydrated in a forced air
oven at 40 °C until the mass stabilized; crushed in a mill to obtain the powders (BPP); sieved through
a 40 mesh granulometric sieve, and finally, vacuum packed in polypropylene plastic bags.

2.3. Characterization of the Biosorbent

The BPP’s scanning electron microscopy (SEM) images were acquired by dispersing the powder
on a double-sided carbon tape fixed to the stub, covered by a thin layer of gold by sputtering (300
seconds under 0.2 Torr pressure in a Desk III model Denton Vacuum evaporator). The images were
obtained using an SEM microscope (JEOL, model JSM-6380 LV) under the following condition:
accelerating voltage of 15 kV, work distance of ~8 mm, and a secondary electron detector. Fourier-
transformed infrared spectroscopy (FTIR) measurements were performed in the attenuated total
reflectance (ATR) mode, with 20 sweeps for each sample, in the range of 4000 to 500 cm-1, using a
Spectrum 100 (PerkinElmer) equipment. Thermogravimetric analysis (TG-DTG) and differential
scanning calorimetry (DSC) were performed under an N2 atmosphere using a simultaneous thermal
analyzer Netzsch STA 449 F3 Jupiter®, in the temperature range of 25 – 600 °C, and with a scan rate
of 5 °C/min.

2.4. Adsorption Experiments

2.4.1. Biosorption of the Methylene Blue Azo Dye
Initially, we selected MB as a pollutant organic compound model for the preliminary study of
the adsorption capacity of biosorbents. In the tests, 50 mg of BPP was added to 50 mL of a solution
containing MB dye in an initial concentration of 50 mg L-1. The kinetic tests were performed for 60
min, under vigorous agitation, with the collection of 500 µL aliquots at predetermined time intervals.
After collection, the samples were centrifuged for 10 min to remove the biosorbent, and the
supernatant was analyzed by UV-Vis absorption spectrophotometry through monitoring MB
maximum peak at 664 nm. All experiments were carried out in triplicate, and the percentage of
removal of the dye, the amount of dye adsorbed at time t, 𝑞𝑞𝑡𝑡 (mg g-1), and the adsorption capacity at
equilibrium, 𝑞𝑞𝑒𝑒 (mg g-1), were respectively calculated by the following equations:
C0 − C𝑡𝑡
%𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅𝑅 = � � × 100 (1)
𝐶𝐶0
C0 − C𝑡𝑡
𝑞𝑞𝑡𝑡 = � � × 𝑉𝑉 (2)
𝑅𝑅
C0 − C𝑒𝑒
𝑞𝑞𝑒𝑒 = � � × 𝑉𝑉 (3)
𝑅𝑅
where C0 , C𝑒𝑒 and C𝑡𝑡 (mg L-1) is the initial dye concentration, dye concentration at equilibrium, and
at time t, respectively; V (L) is the volume of the dye solution, and 𝑅𝑅 (g) is the mass of the adsorbent.

2.4.2. Biosorption of the Glyphosate and Atrazine Pesticides

The adsorption properties of the biosorbents were also evaluated against the glyphosate and
atrazine pesticides in batch experiments, where an aqueous solution of atrazine (or glyphosate) at a
concentration of 20 mg L-1 was separately prepared (pH ~5.5). In each experiment, a certain amount
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of the biosorbent (10, 30, 50, and 60 mg) was added to 10 mL of the pesticide solution in 50 mL beakers.
The mixture was vigorously stirred for 12 h to achieve equilibrium under dark conditions. Kinetic
studies were performed for 120 min for both pesticides using 60 mg of the BPP in the semi-ripe
maturation stage, with the collection of 500 µL aliquots at predetermined time intervals. For pesticide
quantification, the solutions were immediately filtered through a 0.45 µm membrane filter connected
to a syringe and analyzed using a Shimadzu HPLC equipment model prominence 20A, equipped
with a quaternary pump, automatic sampler, and a DAD detector. The chromatographic method was
developed and optimized for each pesticide. For atrazine, the conditions obtained as ideal were
methanol/water pH 3.0 (90:10 v/v) as the mobile phase; Eclipse C18 150 cm x 4.6 mm chromatographic
column; 4.5 µm and wavelength of 240 nm; the flow of 0.6 mL min-1; oven temperature of 35 ºC;
analysis time of 6 min; and injection volume of 20 µL. For glyphosate, the parameters were the same,
except 70:30 v/v as the mobile phase, the wavelength of 230 nm, the flow of 0.8 mL min-1, and the
analysis time of 3 min.

2.4.3. Kinetic Models of Adsorption

The dye and pesticide adsorption processes were evaluated using the Avrami fractional-order,
pseudo-first-order, pseudo-second-order, pseudo-general-order, Elovich, and intraparticle diffusion
models to investigate the adsorption mechanism and the main adsorption process steps. The kinetic
models were fitted using nonlinear fitting. table 1. presents the equation related to each model, where
𝑘𝑘𝑓𝑓 (min-1), 𝑘𝑘𝑠𝑠 (g mg-1 min-1) and 𝑘𝑘𝐺𝐺 (min-1) are the rate constants of the pseudo-first, pseudo-second,
and pseudo-general order models, respectively, 𝑡𝑡 is time in min, 𝑞𝑞𝑡𝑡 is the amount of adsorbate
adsorbed at time 𝑡𝑡 (mg g-1) and ℎ0 (mg g-1min-1) is the initial sorption rate of the. For the pseudo-
general model, 𝑛𝑛 represents the kinetic order of adsorption. In the case of the fractional-order
(Avrami) model, 𝑘𝑘𝐴𝐴𝐴𝐴 (min-1) and 𝑛𝑛𝐴𝐴𝐴𝐴 are the rate constant and the fractional adsorption order,
respectively. In the Elovich chemisorption model, 𝛼𝛼 is the initial sorption rate (mg g-1 min-1), and 𝛽𝛽
(g mg-1) is the desorption constant related to the magnitude of surface coverage and activation energy.
𝑘𝑘𝑖𝑖𝑖𝑖(1,2,3) (mg g-1 min1/2) represents the rate constant of intraparticle transport, and C (mg g-1) is the
boundary layer (film diffusion). Detailed information regarding these kinetic models can be found in
the literature [30–34].

Table 1. Kinetic adsorption models and their respective nonlinear equations.

Equation
Kinetic model Nonlinear equation
number
Pseudo-first-order 𝑞𝑞𝑡𝑡 = 𝑞𝑞𝑒𝑒 {1 − exp(−𝑘𝑘𝑓𝑓 𝑡𝑡)} 1
Pseudo-second- 𝑘𝑘𝑠𝑠 𝑞𝑞𝑒𝑒2 𝑡𝑡
𝑞𝑞𝑡𝑡 = 2
order 1 + 𝑞𝑞𝑒𝑒 𝑘𝑘𝑠𝑠 𝑡𝑡
ℎ0 = 𝑘𝑘𝑠𝑠 𝑞𝑞𝑒𝑒2 3
Pseudo-general- 𝑞𝑞𝑒𝑒
𝑞𝑞𝑡𝑡 = 𝑞𝑞𝑒𝑒 − 4
order (𝑘𝑘𝐺𝐺 (𝑞𝑞𝑒𝑒 )𝑛𝑛−1 𝑡𝑡(𝑛𝑛 − 1) + 1)1/(1−𝑛𝑛)
Avrami Fractional-
𝑞𝑞𝑡𝑡 = 𝑞𝑞𝑒𝑒 {1 − exp [−(𝑘𝑘𝐴𝐴𝐴𝐴 𝑡𝑡)]𝑛𝑛𝐴𝐴𝐴𝐴 } 5
order
1 1
Elovich 𝑞𝑞𝑡𝑡 = 𝑅𝑅𝑛𝑛(𝛼𝛼𝛽𝛽) + 𝑅𝑅𝑛𝑛(𝑡𝑡) 6
𝛽𝛽 𝛽𝛽
Intraparticle
𝑞𝑞𝑡𝑡 = 𝑘𝑘𝑖𝑖𝑖𝑖(1,2,3) √𝑡𝑡 + 𝐶𝐶 7
diffusion

3. Results and Discussion

3.1. Characterization of the Biosorbents
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Figure 1a shows the optical images obtained from the fruits and the obtained BPP at the three
ripening stages studied in this work. According to the literature, the maturation stages were classified
as green, semi-ripe, and ripe [35]. The powders showed different colors after drying and crushing the
banana peels, changing from brown to dark brown as the ripening degree increased, Figure 1a. The
calculated yield based on the kilogram of the peel was 11.3, 12.8, and 17.9% for green, semi-ripe, and
ripe BPP, respectively. Figure 1b shows the FTIR spectra of the BPP for the three ripening stages. The
band at around 3277 cm-1 can be attributed to the axial stretching vibration of the O–H of the hydroxyl
groups characteristic of lignin, cellulose, hemicellulose, and adsorbed water, and the band at 2919
and 2850 cm-1 to the symmetrical and asymmetrical C–H stretching of methoxy groups in lignin,
cellulose, and hemicellulose [19,36]. The band around 1736 cm-1 is a signature of C=O stretching in
carbonyl or carboxyl groups [19,37]. The band around 1588 cm-1 is due to C–O or C=C vibrations. The
bands in the 1320-1375 cm-1 spectra interval correspond to the phenols’ angular C–O–H deformations
and the C–O stretching vibrations in carboxylate groups (alkanes and alkyl groups) [19]. For the
spectral interval 950-1100 cm−1, the observed absorption band may indicate the presence of O–H
deformation vibration, C–O stretching vibration of alcoholic groups, aliphatic ethers, and β-
glycosidic bond present both in cellulose and hemicellulose [19]. Therefore, the FTIR spectra analysis
suggests that the as-prepared BPP has elevated potential to conduct the biosorption of cationic
organics molecules due to the presence of many functional groups in the sample composition [15,38].

Figure 1. Optical images of the banana fruits and the obtained BPP at the different ripeness stages (A)
and FTIR spectra of the BPP samples (B).

We investigated the morphological properties of the BPP samples for the three chosen ripening
stages through SEM images, Figures 2a-c. The images show an irregular morphology evidencing the
presence of agglomerated and microsized particles with smooth surfaces, as well as microporous
structures. The BPP showed more agglomerated particles in the ripe stage than in the green and semi-
ripe maturation stages, which presented similar morphological features.
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Figure 2. SEM images of green (A), semi-ripe (B), and ripe (C) BPP. Scale bars correspond to 10 µm.

Figure 3 shows BPP samples’ TG, DTG, and DSC curves obtained at different ripening stages.
Typical characteristics of thermal degradation of biomass-based materials are observed, which
correspond to the release of adsorbed water from moisture up to 100 ºC, the release of structural
water, and the decomposition of several constituents in the range of 150 to 450 ºC, such as
hemicellulose, cellulose, lignin, pectin, glucose, starch and protolignin [39,40]. For this temperature
interval, all volatile and non-volatile gases (H2, CO2, CO, CH4) are expected to be eliminated from the
biomass [41]. The total mass loss at 600 °C was ~70% for all samples. The DTG made it possible to
identify the temperature at which the mass losses occurred with greater precision. Notably, TG/DTG
curves at all maturation stages show the release of adsorbed water at 60 °C and remarkable features
of mass loss in the 150 - 450 °C interval. For the green BPP (Figure 3a), three peaks are observed
between 150 and 450 °C, i.e., the main peak centered near 275 °C and two small shoulders near 220
and 355 °C. This last minor feature at 355 °C is present in all ripening stages and slowly intensifies as
the ripening process proceeds. However, the peak at 220 °C divides into two peaks for semi-ripe BPP
(Figure 3b), which are centered at 150 and 180 °C and become more pronounced and sharper for the
ripe BPP (Figure 3c). Therefore, the samples showed distinct mass loss processes for the different
ripening stages studied, with more defined and less-overlapped steps for the ripe BPP. It is important
to note that TG/DTG curves have shown to be an analytical tool able to separate and distinguish
banana ripeness. Besides, all these observed mass losses follow the events in the DSC curves, where
it is possible to highlight an endothermic peak between 23 and 75 °C, corresponding to the release of
water and characteristic exothermic signs of the thermal decomposition of the biosorbents.
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Figure 3. TG, DTG, and DSC curves of the green (a), semi-ripe (b), and ripe (c) BPP biosorbents. The
measurements were performed under an N2 atmosphere with a 5 °C/min heating rate. The DTG scale
was normalized and omitted for easy visualization of the superposed graphs.

3.2. Adsorption Efficiency Evaluation

3.2.1. BPP as Biosorbent for Methylene Blue Removal
The BPP biosorbent efficiency for MB removal was evaluated at a fixed pH = 5.5 and ambient
temperature (23 °C). We first assessed the effect of the contact time of the pollutant with the
biosorbent and then the dynamic process of sorption. Figures 4a and 4b show MB’s removal
Preprints (www.preprints.org) | NOT PEER-REVIEWED | Posted: 4 July 2023 doi:10.20944/preprints202307.0154.v1

percentage and adsorption capacity. The BPP biosorbents showed similar adsorption properties for
all stages of maturation studied; however, on average, a minor trend is present with a higher
adsorption ability for the semi-ripe BPP, reaching approximately 66% of MB removal after 60 min.
The MB adsorption process proved fast, and about half of the initial concentration disappeared from
the solution in the first 10 min of contact with the BPP biosorbents. The semi-ripe BPP biosorbent
showed the highest adsorption capacity by removing approximately 33 mg g-1 of the dye. It is
essential to highlight that even close, the equilibrium seems not ultimately achieved after 60 min.

Figure 4. Removal (%) of methylene blue dye (a) and adsorption capacity of the BPP biosorbents
obtained at different ripening stages (b). Conditions: 50 mg of BPP; 50 mL MB dye solution at C0 = 50
mg L-1.

We confronted different kinetic models to the obtained data to explore more valuable
information regarding the mechanism of sorption and the potential rate-controlling steps, such as
mass transport and chemical reaction processes. The calculated parameters from each model and the
corresponding fit curves can be seen in Table 2 and Figure S1 of the supplementary material,
respectively. Considering the entire contact time, the best fitting was the pseudo-second-order since
2
it presented the highest correlation coefficient 𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 compared to pseudo-first. The pseudo-general-
2
order resulted in 𝑛𝑛~2 and similar 𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 (Table 2), which corroborates the previous finding. The
calculated maximum uptake capacities were 28.9, 31.2, and 30.6 mg g-1 for green, semi-ripe, and ripe
BPP, respectively. These values are very close to the respective experimental 𝑞𝑞𝑒𝑒 of 30.08, 33.09, and
31.86 mg g-1, and, therefore, it is possible to infer that the primary sorption mechanism of MB sorbate
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is chemisorption. Hence, the fast MB removal is due to the binding between the dye and functional
groups on the biosorbent surface [6]. The initial adsorption rate ℎ0 from the pseudo-second-order
model at ambient temperature was near 24 mg g-1 min-1 for green and semi-ripe BPP biosorbents and
diminished to almost 18 mg g-1 min-1 when the ripening process was completed.

Table 2. Kinetic parameters for MB removal using green, semi-ripe, and ripe banana peel powders as
biosorbents.

Ripeness stage
Parameters
Green Semi-ripe Ripe
Fractional-order
𝑘𝑘𝐴𝐴𝐴𝐴 (𝑅𝑅𝑚𝑚𝑛𝑛−1 ) 0.2463 0.2446 0.2171
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 ) 27.24 29.15 28.53
𝑛𝑛𝐴𝐴𝐴𝐴 1.847 1.834 1.628
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.87933 0.87933 0.88390
Residual sum of squares 10.08664 10.08664 11.18622

Pseudo-first-order
𝑘𝑘𝑓𝑓 (𝑅𝑅𝑚𝑚𝑛𝑛−1 ) 0.4546 0.4485 0.3536
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 ) 27.24 29.15 28.53
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.8914 0.8526 0.8955
Residual sum of squares 9.07798 14.41271 10.0676

Pseudo-second-order
𝑘𝑘𝑆𝑆 (𝑚𝑚 𝑅𝑅𝑚𝑚−1 𝑅𝑅𝑚𝑚𝑛𝑛−1 ) 0.02883 0.02479 0.01948
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 ) 28.91587 31.17221 30.62174
ℎ0 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 𝑅𝑅𝑚𝑚𝑛𝑛−1 ) 24.11 24.09 18.27
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.93429 0.91524 0.94816
Residual sum of squares 5.49249 8.28495 4.99531

Pseudo-general-order
𝑘𝑘𝐺𝐺 (𝑅𝑅𝑚𝑚𝑛𝑛−1 ) 0.0274 0.0248 0.0195
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 ) 28.95 31.17 30.43
𝑛𝑛 2.019 2.019 2.026
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9347 0.9233 0.9485
Residual sum of squares 5.45624 7.49779 4.96548

Elovich
𝛼𝛼(𝑅𝑅𝑚𝑚 𝑚𝑚−1 ) 798.53 735.74 373.85
𝛽𝛽(𝑚𝑚 𝑅𝑅𝑚𝑚−1 ) 0.32 0.29 0.28
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9982 0.9969 0.9983
Residual sum of squares 0.15103 0.30636 0.15982

Intraparticle diffusion
𝑘𝑘𝑖𝑖𝑖𝑖1 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 𝑅𝑅𝑚𝑚𝑛𝑛−0.5 ) 11.80 13.64 12.37
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C1 (𝑅𝑅𝑚𝑚 𝑚𝑚−1) 2.43 2.49 1.68

2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.8349 0.8687 0.9249
Residual sum of squares 14.46599 15.10262 6.89282
𝑘𝑘𝑖𝑖𝑖𝑖2 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 𝑅𝑅𝑚𝑚𝑛𝑛−0.5 ) 4.09 2.42 2.82
C2 (𝑅𝑅𝑚𝑚 𝑚𝑚−1) 13.14 17.86 15.40
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9647 0.9910 0.9828
Residual sum of squares 0.44689 0.23652 0.61859
𝑘𝑘𝑖𝑖𝑖𝑖3 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 𝑅𝑅𝑚𝑚𝑛𝑛−0.5 ) 1.20 1.35 1.29
C3 (𝑅𝑅𝑚𝑚 𝑚𝑚−1) 20.91 22.48 21.80
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9948 0.9935 0.9879
Residual sum of squares 0.13581 0.06013 0.10017

Generally, chemisorption is described by pseudo-second-order and Elovich models. The former

model embodies covalent forces and ion exchange by the sharing/exchange of electrons between
adsorbate and adsorbent; the latter is indicated for sorbent materials that contain a heterogeneous
surface [42]. Both models are indistinguishable under certain conditions and are frequently used to
describe the kinetic of chemisorption [43]. The Elovich model was applied to our data and could
better describe the obtained MB chemisorption kinetics compared to the pseudo-second-order. The
initial sorption rate 𝛼𝛼 was higher for BPP in the green stage and decreased as the ripening process
proceeded; however, with similar desorption constants 𝛽𝛽. It is important to note that desorption
constant is exceedingly small compared to the initial sorption rate.
It is well-established that the sorption process may involve several steps, including (i) transport
of the solute molecules from the bulk aqueous phase to the surface of the solid particles (film
diffusion); (ii) diffusion of the solute into the interior of the sorbent pores where the adsorption
becomes intraparticle controlled, which is usually a slow process [30]; and (iii) surface chemical
reaction or complex formation, where the interaction of molecules of adsorbate with the surface
functional groups of adsorbent takes place [42]. The intraparticle diffusion model was used to
evaluate these stages. The results could be divided into three parts, with a satisfactory correlation
factor, indicating that three steps are present in the kinetics of the biosorption process (Figure S1,
supplementary material). In the first step, which relates to the external mass transfer (film diffusion)
of dye to the biosorbent surface [44], the semi-ripe BPP presented a higher 𝑘𝑘𝑖𝑖𝑖𝑖1 and, therefore, a
faster film diffusion process. However, the 𝑘𝑘𝑖𝑖𝑖𝑖2 was higher for the green BPP, showing that the mass
transfer inside the biosorbent through intraparticle or pore diffusion is significantly more efficient for
the green BPP as compared to the other maturation stages. Finally, the third step when adsorption
approaches the equilibrium, that corresponds to diffusion processes related to chemical reactions or
complex formation, shows no considerable differences, and means the kinetic goes similar for the
BPP in three studied maturations stages.
For all the BPP maturation stages, the diffusion rate was high in the initial steps and decreased
as time preceded, which shows that the adsorption rate is mainly governed by film diffusion at the
early stage of removal of MB dye. Comparing the y-intercept values (C1-C3) of BPP biosorbent for the
three maturation stages, one can see that higher values were obtained for semi-ripe BPP, validating
the more significant boundary layer effect and an enhanced film diffusion for BPP at this maturation
stage [31,45]. Interestingly, at all studied maturation stages, the linear plots do not pass through the
origin, which means the intraparticle diffusion is not the only rate-limiting step [31]. Therefore, one
hypothesis is that sorption combines film diffusion and chemisorption. The diffusion-chemisorption
model was also evaluated to validate this hypothesis [42]. This model considers that chemisorption
and film diffusion control the adsorption process, where KDC is the diffusion-chemisorption rate
constant, as expressed in Eq. 7.
𝑡𝑡 0.5� = 1� 1 0.5
𝑞𝑞𝑡𝑡 𝐾𝐾𝐷𝐷𝐷𝐷 + � �𝑞𝑞𝑒𝑒 �𝑡𝑡 (Eq. 7)
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Figure S2 and Table S1 of the supplementary material present the fitted curves and the calculated
parameters for MB adsorption at the BPP biosorbents for the three maturation stages. A more than
99% correlation coefficient was obtained for all BPP maturation stages, with KDC values of 32.76, 31.40,
and 26.25 for green, semi-ripe, and ripe BPP, respectively. Moreover, the calculated 𝑞𝑞𝑒𝑒 are
remarkably close to the experimental results. Therefore, by confronting the best-fitted kinetic models
evaluated in this work, it is possible to infer that the overall mechanism of adsorption of the MB dye
onto BPP is a multi-step process that includes both physisorption and chemisorption.

3.2.2. Biosorption of Atrazine and Glyphosate

Figures 5a-b show the total removal percentage of atrazine and glyphosate adsorbed at
equilibrium for different BPP biosorbent dosages. It is possible to verify that the adsorption efficiency
follows the order semi-ripe > ripe > green for both pesticides. Besides, the adsorption efficiency
improved with the increase in the biosorbent mass, which can be attributed to the increased number
of active sites. In addition, the total removal is higher for glyphosate than atrazine, where 98% and
93% removal efficiencies were achieved using 60 mg of biosorbent, respectively.

Figure 5. Total removal of atrazine (a) and glyphosate (b) for different biosorbent dosages after 12
hours at the following conditions: 10 mL of pesticide at 20 mg.L-1 and in contact with 10, 30, 50, and
60 mg of BPP. Percentual removal (left, black) and amount adsorbed at time t (right, red) of atrazine
(c) and glyphosate (d) pesticides at the following conditions: 60 mg of semi-ripe BPP and 10 mL of
pesticide at 20 mg.L-1.

Based on the results obtained at the equilibrium, the adsorption (removal percentage and 𝑞𝑞𝑡𝑡 ) as
a function of time was only carried out for semi-ripe BPP and using 60 mg of biosorbent, as shown in
Figures 5c-d. The concentration of the pesticides decreased for longer contact times, suggesting the
occurrence of adsorption in the solid phase. Atrazine was adsorbed more slowly in the first 15 min
compared to glyphosate, followed by a sudden increase in the adsorption rate at this time, reaching
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a faster equilibrium at nearly 60 min of reaction (Figure 5c). On the other hand, the uptake of
glyphosate was relatively quick in the initial phase of the adsorption what can be attributed to the
accelerated instantaneous external diffusion, as also described before [28], and gradually decreased
over time as it approached equilibrium at near 90 min (Figure 5d). The amount of dye adsorbed (𝑞𝑞𝑡𝑡 )
increase over time following the same trend as observed for the total removal percentage, with 𝑞𝑞𝑒𝑒
values of 3.02 and 3.26 mg g-1 for atrazine and glyphosate, respectively.
Different models were investigated and adjusted to the experimental data to better understand
kinetic behavior, as presented in Table 3. For atrazine, the Avrami fractional-order showed the
highest correlation coefficient; however, the kinetic order is not a fractional number (𝑛𝑛𝐴𝐴𝐴𝐴 is close to
the unity), and the model converges to the pseudo-first-order model (see Table 1). We then assume
the biosorption kinetics of atrazine to follow the pseudo-first-order in which calculated 𝑞𝑞𝑒𝑒 = 3.46 mg
g-1 best approximated the experimental value of 3.02 mg g-1 with a satisfactory correlation factor of
93.66%. For glyphosate, the pseudo-second-order showed a best fit compared to pseudo-first-order,
with a correlation factor of 97.76%, a calculated 𝑞𝑞𝑒𝑒 = 3.99 mg g-1 close to the experimental value (3.26
mg g-1), and ℎ0 = 0.15 mg g-1 min-1. The general-order ends up with a remarkably similar result of
pseudo-second-order kinetic for the glyphosate case; however, as observed for the MB dye, the
Elovich equation was fitted with a higher correlation coefficient than pseudo-second. Interestingly,
the model’s initial sorption rate and desorption constant are higher than that obtained for atrazine,
showing that glyphosate is initially favored to chemisorb at the BPP particle surfaces. It is noteworthy
that the diffusion-chemisorption model did not fit perfectly in the data as did in the case of the MB
2
dye, with a correlation factor 𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 < 0.7 for both pesticides.

Table 3. Kinect parameters for glyphosate and atrazine removal using semi-ripe banana peel powder
biosorbents.

Pesticide
Model and Parameter
Glyphosate Atrazine
Fractional-order
−1
𝑘𝑘𝐴𝐴𝐴𝐴 (𝑅𝑅𝑚𝑚𝑛𝑛 ) 0.02608 0.02270
−1
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚 ) 3.22 3.46
𝑛𝑛𝐴𝐴𝐴𝐴 1.41 0.99
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9609 0.9446
Residual sum of squares 0.03271 0.08532

Pseudo-first-order
−1
𝑘𝑘𝑓𝑓 (𝑅𝑅𝑚𝑚𝑛𝑛 ) 0.03689 0.02270
−1
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚 ) 3.22 3.46
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9554 0.9366
Residual sum of squares 0.03738 0.09751

Pseudo-second-order
−1 −1
𝑘𝑘𝑆𝑆 (𝑚𝑚 𝑅𝑅𝑚𝑚 𝑅𝑅𝑚𝑚𝑛𝑛 ) 0.00964 0.00332
−1
𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚 ) 3.99 5.01
−1 −1
ℎ0 (𝑅𝑅𝑚𝑚 𝑚𝑚 𝑅𝑅𝑚𝑚𝑛𝑛 ) 0.15 0.08
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9776 0.9197
Residual sum of squares 0.01879 0.12358

Pseudo-general-order
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𝑘𝑘𝐺𝐺 (𝑅𝑅𝑚𝑚𝑛𝑛−1 ) 0.00894 0.00608

𝑞𝑞𝑒𝑒 (𝑅𝑅𝑚𝑚 𝑚𝑚−1 ) 4.03 4.56
𝑛𝑛 2.05 1.72
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9870 0.9394
Residual sum of squares 0.01621 0.10437

Elovich
−1
𝛼𝛼(𝑅𝑅𝑚𝑚 𝑚𝑚 ) 0.37 0.18
𝛽𝛽(𝑚𝑚 𝑅𝑅𝑚𝑚−1 ) 1.20 0.90
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.9845 0.9578
Residual sum of squares 0.01934 0.07265

Intraparticle diffusion
−1 −0.5
𝑘𝑘𝑖𝑖𝑖𝑖1 (𝑅𝑅𝑚𝑚 𝑚𝑚 𝑅𝑅𝑚𝑚𝑛𝑛 ) 0.333 0.556
−1
C1 (𝑅𝑅𝑚𝑚 𝑚𝑚 ) 0.144 -1.357
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 0.99239 0.97753
Residual sum of squares 0.03612 0.12962
−1 −0.5
𝑘𝑘𝑖𝑖𝑖𝑖2 (𝑅𝑅𝑚𝑚 𝑚𝑚 𝑅𝑅𝑚𝑚𝑛𝑛 ) 0.008 0.050
−1
C2 (𝑅𝑅𝑚𝑚 𝑚𝑚 ) 3.173 2.465
2
𝑅𝑅𝑎𝑎𝑖𝑖𝑎𝑎 ---- 0.94987
Residual sum of squares ---- 0.00048

The intraparticle diffusion model was also investigated. Unlike the observed for the MB, the
model could only be satisfactorily divided into two parts, indicating that only two well-defined steps
are present in the adsorption processes of the pesticides (Figure S3 and Table 3). In this case, the
diffusion process showed a higher 𝑘𝑘𝑖𝑖𝑖𝑖1 value for atrazine compared to glyphosate suggesting that
the instantaneous surface sorption step is faster in the former case [44]. Besides, for each of the
pesticides the 𝑘𝑘𝑖𝑖𝑖𝑖1 is far higher than the 𝑘𝑘𝑖𝑖𝑖𝑖2 indicating the film diffusion predominates in the
sorption mechanism, and the mass transfer inside the biosorbent through intraparticle or pore
diffusion is present but less significant. Although being rarely described [34], the y-intercept values
(C1 and C2 in our case) of the intraparticle equation are related to the boundary layer effect and
showed higher values for the glyphosate pesticide, with an initial negative value for atrazine. A
negative value can be explained by the combined effects of film diffusion and surface reaction control
[34,46]. As for MB, the linear plots (Eq. 7) obtained for the pesticides do not pass through the origin,
meaning the intraparticle diffusion is not the only rate-limiting step [31].
Therefore, the kinetic process for the BPP biosorbent has shown to be highly dependent on the
physicochemical properties of the contaminant, and their interactions with the biosorbent differed
between the pesticides studied. It is essential to highlight that the biosorbent could uptake more dye
molecules in comparison to the pesticides since the calculated 𝑞𝑞𝑒𝑒 were about nine times worst for the
latter. However, this is the first report regarding glyphosate removal using BPP as a biosorbent with
an impressive uptake of 3.26 mg g-1 under the studied conditions. For atrazine, two previous studies
have applied banana peels as a biosorbent [26,28]. However, we show that our untreated BPP are
competitive biomaterials and so far deserve attention, especially regarding the low amount of
biosorbent employed in this work and the fact that no pretreatment in acid solution was applied.
Since it is a cheap and relatively abundant material that typically decomposes in nature, we have
shown herein that BPP is a candidate for wastewater treatment for the removal of hazardous dyes,
pesticides, and other organic or inorganic pollutants due to its abundant availability of chemical
functional groups that provide a bridge to sorption of target pollutant molecules.
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4. Conclusions
In three stages of maturation, Banana (Musa Paradisiaca L.) peel powder was evaluated as a
biosorbent for removing MB dye and the glyphosate and atrazine pesticides from water. The BPP
was thoroughly characterized, revealing the presence of many functional groups on the surface and
an irregular morphology encompassing agglomerated and microsized particles with smooth surfaces
(starch) and microporous structures. The BPP showed distinct mass loss processes with more
pronounced and less overlapped steps for the ripe BPP, where TG/DTG curves have shown to be a
precise analytical tool able to separate and distinguish bananas at different ripening stages. The
biosorption properties of BPP were initially evaluated against the MB dye and showed a high
adsorption capacity of ~33 mg g-1 for the semi-ripe stage, with a fast evolution in time where ~50% of
dye was absorbed in 10 min, achieving 66% in 60 min. The kinetics of MB removal was mainly
governed by film diffusion and chemisorption.
Moreover, the BPP biosorbents were evaluated against atrazine and glyphosate, showing
adsorption efficiencies in the following order for both pesticides: semi-ripe > ripe > green. The
pesticide sorption efficiency improved with the increase in the amount of biosorbent, showing higher
total uptake of glyphosate compared to atrazine, with 98% and 93% removal and maximum
adsorption capacity of 3.26 and 3.02 mg g-1, respectively. The biosorption of glyphosate and atrazine
followed Elovich and pseudo-first-order kinetics, respectively. Therefore, without any chemical
treatment, the low-cost biosorbent proposed herein is an entirely chemical-free, green, and
environmentally friendly biomaterial for removing recalcitrant pesticides and other organic
pollutants from water bodies.

Supplementary Information (SI): Kinetic models and intraparticle diffusion fits for MB; Diffusion-
chemisorption model fits for MB; Parameters obtained from diffusion-chemisorption model; Kinetic models and
intraparticle diffusion fits for glyphosate and atrazine.

Author Contributions: Kelly Farias: Methodology, formal analysis, investigation, writing-original draft. Rita
Guimarães: Methodology, supervision. Karla Oliveira: Methodology, formal analysis. Carlos Nazario:
Methodology, formal analysis. Julio Ferencz: Formal analysis, investigation, writing-review & editing.
Heberton Wender: Conceptualization, supervision, resources, writing-review & editing.
Funding: This study was financed in part by the Fundação Universidade Federal de Mato Grosso do Sul –
UFMS/MEC – Brazil, by the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - Brasil (CAPES) -
Finance Code 001 and by the National Council for Scientific and Technological Development (CNPq).
Acknowledgments: This work was partially supported by the National Council for Scientific and Technological
Development (CNPq; processes # 427835/2016-0 and # 313300/2020-8); and The Foundation for Support to the
Development of Teaching, Science, and Technology of the State of Mato Grosso do Sul (FUNDECT, projects #
099/2014, # 106/2016, and # 228/2022).
Ethics approval: Not applicable. This article does not contain any studies with human participants or animals
performed by any of the authors.
Consent to participate: All authors have given consent to their contribution.
Consent for publication: All authors have agreed with the content, and all have given explicit consent to publish.
Competing interests: The authors declare no competing interests.

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