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Adsorption of methyl orange: A review on adsorbent performance

Kingsley O. Iwuozor, Joshua O. Ighalo, Ebuka Chizitere Emenike, Lawal Adewale


Ogunfowora, Chinenye Adaobi Igwegbe

PII: S2666-0865(21)00126-0
DOI: https://doi.org/10.1016/j.crgsc.2021.100179
Reference: CRGSC 100179

To appear in: Current Research in Green and Sustainable Chemistry

Received Date: 29 July 2021


Revised Date: 7 September 2021
Accepted Date: 18 September 2021

Please cite this article as: K.O. Iwuozor, J.O. Ighalo, E.C. Emenike, L.A. Ogunfowora, C.A. Igwegbe,
Adsorption of methyl orange: A review on adsorbent performance, Current Research in Green and
Sustainable Chemistry (2021), doi: https://doi.org/10.1016/j.crgsc.2021.100179.

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Adsorption of Methyl Orange: A Review on Adsorbent Performance

Kingsley O. Iwuozor1, 2*, Joshua O. Ighalo3, 4**, Ebuka Chizitere Emenike2, Lawal

Adewale Ogunfowora5, Chinenye Adaobi Igwegbe3


1
Department of Chemistry, University of Lagos, P. M. B. 1029, Lagos, Nigeria.
2
Department of Pure and Industrial Chemistry, Nnamdi Azikiwe University, P. M. B. 5025,

Awka, Nigeria.
3
Department of Chemical Engineering, Nnamdi Azikiwe University, P. M. B. 5025, Awka,

Nigeria

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4
Department of Chemical Engineering, University of Ilorin, P. M. B. 1515, Ilorin, Nigeria

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5
Department of Chemical Engineering, Federal University of Technology, Minna, Nigeria
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Corresponding author, Email address: kingsleyiwuozor5@gmail.com
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**
Corresponding author, Email address: oshea.ighalo@yahoo.com
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ORCID
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Kingsley O. Iwuozor, https://orcid.org/0000-0002-1161-2147

Joshua O. Ighalo, https://orcid.org/0000-0002-8709-100X


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Ebuka Chizitere Emenike, https://orcid.org/0000-0001-7117-3265

Lawal Adewale Ogunfowora, https://orcid.org/0000-0002-2104-3582

Chinenye Adaobi Igwegbe, https://orcid.org/0000-0002-5766-7047

Highlights

 The performance of various adsorbent groups for MO adsorption was reviewed.

 Composites were the most frequently used (>40%) adsorbent group for MO adsorption

 Nanoparticles and polymers were the most frequently used constituents in the composite

 Nanoparticles were the best adsorbents for MO uptake

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 Clays and minerals had the greatest proportion of adsorbents with >1000 mg/g capacity

Graphical abstract

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Abstract
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Adsorption as a technique is preferred to these other methods in the mitigation of


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methyl orange (MO) because of its simplicity in design and operation, indifferent sensitivity
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towards toxicants and low operational cost. This study is aimed at evaluating the performance

of various adsorbent groups in the mitigation of MO from aqueous solutions. It will help reduce

the arbitrary choice of adsorbent types for MO adsorption leading to a reduction in the amount

of published literature with little/incremental contributions to the field. The study was based

on an analysis of over 240 published works of literature on the subject within the last 5 years.

The adsorbents were classified into the following seven groups based on their chemical

composition; biosorbents, activated carbon, biochar, clays and minerals, polymers and resins,

nanoparticles, and composites. In terms of frequency of utilisation of adsorbent group,

composites were the most frequently used (>40%). It was observed that nanoparticles and

polymers were the most frequently used constituents in the manufacture of composite

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adsorbents for MO. The choice of nanoparticles in composite adsorbents could be due to their

flexibility in going into the matrices of other material types due to their small sizes. Polymers

also act as good matrices for immobilising other composite constituents. Nanoparticles was the

best adsorbent group for MO uptake. Clays and minerals had the greatest proportion of

adsorbents with MO uptake capacity greater than the 1000 mg/g threshold.

Keywords: Adsorption; Biochar; Methyl orange; Nanoparticles; Water pollution

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1. Introduction

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The importance of water in the sustenance of life cannot be overstated as it is present

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in high amounts in all biomass [1-3]. Unfortunately, the contribution of man’s activities has/is
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decreasing the supply of clean water through the introduction of pollutants into water bodies
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[4-6]. Water pollution is caused by several pollutants such as resource mining, oil spills,
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agricultural practices, nuclear waste leakages and wastes from industries [7-9]. One such
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industry is the textile industry that utilises a great deal of water for its processes especially for
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wet processing of materials and also releases a large volume of effluent into the environment
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[10, 11]. The treatment of the industrial effluent is a great concern for the industry in a bid to

make their process environmentally friendly [12-15]. Being the largest consumer of colourants,

the effluent from this industry contain large quantities of dyes (which are toxic, carcinogenic,

mutagenic and pose great threat to humans) used during the process and researchers have spent

a great deal of time in its mitigation from water bodies to make the water less hazardous to the

environment [16-20].

Various authors have used different treatment approaches based on their strengths and

weaknesses for the mitigation of dyes from the environment [21-23]. Due to the disadvantages

of other remediation approaches, adsorption is preferred for dye removal from aqueous

environments [24]. Precipitation and coagulation use a lot of chemicals and produce toxic

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sludge beds [25, 26], whereas electrodialysis is linked with high running costs and corrosion

[26, 27]. Adsorption is a common method for removing dyes from wastewater. Its benefits over

other treatments include its flexibility, ease of operation and design, low volume sludge and

low cost of set-up [28-34]. However, some of the drawbacks of the adsorption process include

toxicity of wastes from spent adsorbents, the use of chemicals for desorption, and the transfer

of the pollution load rather than its elimination [35].

Methyl Orange (MO) is one of the most common dyes used in the textile industry [36-

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38]. It is also used as a pH indicator for titrations [39-41]. Its chemical structure and properties

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are shown in Figure 1 and Table 1 respectively. Different methods can be utilised for the

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removal of MO dye from solutions, and examples of such techniques include; advanced

oxidation processes [42-44], photocatalytic degradation [45-47], ultra-filtration [48-50],


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electrochemical degradation [51-54], and coagulation-flocculation [55-57]. However, the
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above-listed methods have disadvantages such as complexity, high operational cost and time-
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consuming unit operations as stated above [58]. Adsorption as a technique is preferred to these
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other methods in the mitigation of MO because of its simplicity in design and operation,
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indifferent sensitivity towards toxicants and low operational cost [59, 60].

Table 1. Characteristics of MO [61].

Property Value
IUPAC name Sodium-4-(4-dimethylamino phenyl diazenyl) benzenesulfonate
Molecular formula C14H14N3SO3Na
Molecular weight 327.34 g/mol
pKa 3.4
Colour & form Orange-yellow powder or crystalline scales
Melting point > 300 ℃
Solubility Less than 1 mg/mL at 18 C

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Figure 1. Chemical structure of MO

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From the exhaustive search of the authors’, it was discovered that even though a large

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amount of research has been done on the adsorption of MO, there is yet to be any review on
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the subject matter. The reason for using MO as the adsorbate in this study is due to its popularity
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as a dye and pH indicator [62, 63]. This study is aimed at evaluating the performance of various

adsorbent groups in the mitigation of MO from aqueous solutions. The novelty of this study is
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centred on the study of the different adsorbents that have been used in the removal of MO from
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aqueous solution within the last five years with emphasis on their adsorbent capacity, making
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comparison amongst them and drawing inferences. This study would be able to give more

insight into the adsorption of MO, to better inform future researches. It will also help reduce

the arbitrary choice of adsorbent types for MO adsorption leading to a reduction in the amount

of published literature with little/incremental contributions to the field.

2. Methodology

This study utilised recent articles that have been published on the adsorption of MO

from aqueous solutions. The articles were obtained from the Google Scholar search engine and

the search was restricted to all papers on the subject matter published in the past five years

(2016-2021). Our reason for this was to engage the most recent research and advances that
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have been made on the subject matter. Over 240 published articles were obtained that have

been published within this time frame. The papers were scrutinised to study the performance

of the various adsorbents that have been used for MO uptake. The adsorption capacity was used

as the yardstick for measuring the performance of the various adsorbents. The percentage

removal efficiency was documented from articles where it was reported but it was not used as

the basis or indicator for measuring the performance of the various adsorbents because it is

dependent on the dosage of the adsorbent as well as the adsorbate’s concentration [64]. For

better comparison and analysis, the adsorbents were group into seven different groups based

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on their chemical composition or make-up. The groups are;

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 Group A: Biosorbents

 Group B: Activated carbon


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 Group C: Biochar
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 Group D: Clays and Minerals


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 Group E: Polymers and resins


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Group F: Nanoparticles


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Group G: Composites

Figure 2 shows a summary of the different precursors used for the preparation of the various

adsorbent types considered in this study. Besides polymeric adsorbents and composites, the

preparation of most other adsorbent types are quite simple. With the exception of polymers and

nanoparticles precursors, most of the other precursors are low-cost and readily available. The

availability of precursors from agricultural residues may be limited to the farming/processing

season, or the possibility of cultivation of the original crops in such area based on climatic

limitations.

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Figure 2. Summary of adsorbent types considered in the study and potential precursors for

their synthesis

Besides the stipulation of removal efficiency (RE%) and adsorption capacity (𝑞𝑚𝑎𝑥 ), the

method of determination of the adsorption capacity was reported, the optimum pH and

temperature were also reported for each of the adsorbents as they are process parameters that

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greatly influence the capacity of any given adsorbent. The specific surface area of the adsorbent

was also reported. The 𝑞𝑚𝑎𝑥 was reported in four significant figures in order of decreasing

adsorption capacity. With the aid of the current classification, the adsorbent performance was

analysed and inferences were drawn. A comparison was also made across the various groups

to investigate their performance for MO uptake.

3. Empirical results of the various adsorbent groups

3.1 Group A: Biosorbent

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Biosorbents are materials of biological origin that have been thermo-chemically

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decomposed and is used for the sequestration of pollutants from the environment through
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adsorption [65]. Biosorbents are very popular adsorbents as most of them are cheap and readily
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available [66]. Another reason for this is that it does not form intermediate products and there
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is a large array of materials that can be used as biosorbents [67]. According to El-Sayed and
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El-Sayed [68], biosorbents can be classified into four major classes and which have been

utilised in the mitigation of MO from aqueous solution; living biomass that is made up of fungi
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[69-71], Algae [72-74], and other microbial cultures [75-77]; Dead biomass [71, 78];
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agricultural wastes such as fibers [79, 80], leaves [81-83], fruit peels [84-86], tree barks [87,

88], and plant straws [89, 90]; and Industrial solid waste [91]. The mechanism of uptake of

dyes by biosorbents include physical sorption such as Van der Waals force or ion exchange

electrostatic interaction, chemical sorption by micro-precipitation and complexation/chelation

[92-94]. The performance of the various sorbents which include both modified and unmodified

biosorbents that have been used in the removal of MO from solutions is given in Table 2.

Table 2. Adsorption performance of MO by Group A adsorbents

Adsorbent Name Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of 𝒒𝒎𝒂𝒙 Ref.


RE% (mg/g) (oC) (m2/g) determination
Polyethyleneimine-modified persimmon tannin 97.6 877.2 4.00 50.0 8.130 Langmuir [95]
Aminated pumpkin seed powder - 200.3 3.00 45.0 - Langmuir [96]

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Coffee waste/cetylpyridinium chloride - 62.50 3.50 25.0 - Langmuir [97]
Coffee waste/cetyltrimethyl ammonium - 58.82 3.50 25.0 - Langmuir [97]
bromide
Sulfactant-modified pineapple leaf - 47.62 3.00 - - Langmuir [98]
Epiphyton biofilm 99.8 - 7.00 30.0 - - [99]

3.2 Group B: Activated carbon (AC)

Activated carbons are carbon-based materials such as charcoal, coal, carbonised plant

matter, peat and lignite that have undergone physical or chemical treatment to increase their

surface area as well as porosity in a bid to boost the sorption capacity of the material [100-

102]. AC is produced from carbon-based materials at very high temperatures, usually above

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700 ℃ with activated gas such as flue gas or steam. Activated carbon is a popular choice for

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the adsorption of MO because they are characterised by high surface area, high adsorption
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capacity, active free valences, porous structure, thermal stability, surface reactivity and
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inertness [103-105]. As a result of these properties and more, AC has become the most versatile
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type of adsorbent for the removal of dyes from solution and also due to its very high affinity
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for different types of dyes [106, 107]. The two major forms of AC are granulated activated

carbon (GAC) and powdered activated carbon (PAC) [108, 109]. Examples of materials that
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have been used in the fabrication of AC for the mitigation of MO dye from aqueous solution
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include; coal [110], egg shells [111, 112], coconut shells [113], wood [114], lignin [115], and

date stones [116]. The adsorption capacity in four significant figures of the various AC which

include both chemically modified and unmodified activated carbon that has been used in the

removal of MO from solutions is given in Table 3.

Table 3. Adsorption performance of MO by Group B adsorbents

Adsorbent Name Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of 𝒒𝒎𝒂𝒙 Ref.


RE% (mg/g) (oC) (m2/g) determination
Rayon-based AC fibers - 7000 6.00 - 2126 Langmuir [117]
AC from coffee waste - 1017 3.00 30.0 - Dubinin- [118]
Radushkevich
AC from popcorn 48.5 969.0 - 25.0 3291 Experiments [119]
Pomelo peel-derived porous carbon - 680.3 3.00 50.0 1892 Langmuir [120]
AC from waste tire rubber 80.0 588.0 3.60 23.0 - Langmuir [121]
AC from aloe vera - 196.1 3.00 25.0 - Langmuir [82]

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AC from sugarcane mills boiler residue - 161.8 5.0 25.0 1073 Langmuir [122]
AC from coconut shell 100 3.000 - 25.0 1640 Experiments [123]

3.3 Group C: Biochar

Biochar is described as the solid carbonaceous product of the carbonisation, pyrolysis

or gasification of biomass in the absence or presence of oxygen [124-126]. It is common as an

adsorbent due to its surface area, porous nature and large amounts of surface functional groups

[127-129]. Biochar is made from biomass at a lower temperature than AC which is usually less

than 700 ℃ under anaerobic conditions. Even though its surface area is not as high as that of

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AC, it has more surface functional groups than AC. Feedstock that has been utilised in the

production of biochars used for the removal of MO from aqueous solution include; forestry

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waste [130, 131], manure [132, 133], and agricultural waste [134-136]. Table 4 shows the
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various biochars that have been used in the mitigation of MO in decreasing order of adsorption
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capacity.
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Table 4. Adsorption performance of MO by Group C adsorbents


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Adsorbent Name Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of Ref.


RE% (mg/g) (oC) (m2/g) 𝒒𝒎𝒂𝒙
determination
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Protonated amine-modified hydrochar - 909.1 - - 11.76 Langmuir [137]


Biochar from hazelnut shell - 181.8 - - 23.01 Langmuir [138]
Biochar from cellulose - 166.7 - - 12.87 Langmuir [138]
Activated biochar from pomelo peel 99.9 163.1 3.00 25.0 75.32 Langmuir [85]
waste
Biochar from glucose - 147.1 - - 5.440 Langmuir [138]
Biochar from chicken manure 100 41.49 6.50 45.0 - Langmuir [139]

3.4 Group D: Clays and minerals

Clays can be described as a group of microcrystalline secondary minerals with various

phyllosilicate minerals having sheet-like structures and different amounts of structural water

[140]. Apart from being low-cost, clays are also readily available as adsorbents and can

therefore be a replacement for more expensive adsorbents in the treatment of water [141]. Due

to their ability to adsorb water in their interlayer sites, and their high surface area, clays are

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highly valued as adsorbents [142]. Common types of clay minerals used as adsorbents in the

removal of MO from solutions include; bentonite [143-145], montmorillonite [146-148] and

kaolin [149, 150]. Another mineral that has been utilised as an adsorbent is zeolite. Original

zeolite crystals are made up of aluminate polyatomic ions. Due to the high number of spaces

within the structure of zeolites, it makes it easier for it to remove pollutants in the environment

by ion exchange [151-153]. The adsorption capacity in four significant figures of the various

Clays and minerals that have been used in the removal of MO from solutions is given in Table

5.

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Table 5. Adsorption performance of MO by Group D adsorbents

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Adsorbent Name Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of 𝒒𝒎𝒂𝒙 Ref.

Organosilica
Starch-modified ZnMgAl LDH
RE%
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-p (mg/g)
1708
1555
3.00
(oC)
-
25.0
(m2/g)
10.00
76.80
determination
-
Langmuir
[154]
[155]
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CoFe LDH 80.0 1290 7.50 25.0 108.8 Langmuir [156]
Calcined glycerol-modified nanocrystallined 95.0 1062 4.50 25.0 170.3 Langmuir [157]
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MgAl LDH
CoAl/Cl LDH 98.3 827.5 7.00 20.0 19.70 Langmuir [158]
MnOx-decorated MgAl LDH 90.5 555.6 - 30.0 - Langmuir [159]
Flower-like NiAl LDH - 500.6 3.00 25.0 133.0 Langmuir [160]
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NiCO-LDH 98.0 497.0 - - - Langmuir [161]


Uncalcined glycerol-modified nanocrystallined 93.0 443.5 4.50 25.0 71.40 Langmuir [157]
MgAl LDH
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Trimeric surfactant-modified Na - 368.6 3.00 20.0 7.750 Langmuir [162]


montmorillonite
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Hydrotalcite-like modified bentonite - 333.3 6.50 24.0 83.24 Langmuir [163]


Dimeric surfactant-modified Na - 313.3 3.00 20.0 10.72 Langmuir [162]
montmorillonite
Stone-like NiAl LDH - 292.0 3.00 25.0 90.00 Langmuir [160]
Gemini surfactant-modified Na-montmorillonite - 282.4 300 - 6.700 Langmuir [164]
Cetyltrimethylammonium bromide/H2O2-clay 98.0 268.7 3.00 25.0 21.16 Dubinin- [165]
Radushkevich
HDPy+-clay - 227.3 3.00 - 94.93 Langmuir [166]
NiFe LDH 96.5 205.8 - - 17.85 Langmuir [167]
MgAl LDH - 197.6 - 25.0 - Experiments [168]
Bimorphic Mg-Al mixed metal oxides 99.7 182.8 - 25.0 - Langmuir [169]
Blast furnace slag acid-alkaline precipitate 100 167.0 13.0 25.0 3.450 Langmuir [170]
Organo vermiculite - 157.0 6.90 55.0 - Langmuir [171]
Cd-zeolite imidazolate framework (Cd-ZIF-8) 92.0 145.4 2.00 50.0 1281 Langmuir [172]
CuMgAl LDH 98.0 123.5 7.00 25.0 60.00 Langmuir [173]
Palygorskite - 109.4 7.00 25.0 - Langmuir [174]
Goethite - 55.00 3.00 25.0 4.370 Langmuir [175]
Organic matter-rich clays from Egypt 96.4 41.67 2.00 25.0 59.14 Langmuir [176]
Calcinated organic matter-rich clays from Egypt 92.9 34.48 2.00 25.0 48.32 Langmuir [176]
Biofunctional BiOCl3I solid 100 5.000 - - 29.34 Experiments [177]
CuAl LDH 100 - - 40.0 - - [178]
Tungstosilisic acid/zeolites 85.0 - 2.50 - 362.0 - [179]
Fly ash 66.0 - 8.50 25.0 1.180 - [180]

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3.5 Group E: Polymers and resins

Polymers can be described as any chemical substance having a large number of

molecules that are composed of repeating subunits called monomers [181]. Polymeric-based

adsorbents can be used either in their natural form or in their modified form. The presence of

modifiable functional groups present in the chemical structure of polymers makes polymers a

good adsorbent material [182, 183]. There are two major reactions through which polymers

can be modified to increase their adsorption efficiency and resistance in extreme media

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conditions, and they are; cross-linking reactions (in which macromolecular chains are united

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with each other) and grafting (in which new functional groups are inserted into the original
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material, thereby increasing the number of active sites present on the surface of the polymer)
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[184, 185]. Polymeric adsorbents are preferred to conventional adsorbents due to the simplicity
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in their processing, the possibility to shape them into other forms such as membranes and beads,
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and their relatively easy regeneration. Polymeric adsorbents could either be natural or synthetic

[186, 187]. Natural polymers which have been used for the adsorption of MO include
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polysaccharides such as chitosan [188-190], cellulose, starch [191-193], alginate [194-196],


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and cyclodextrin [197-199]. The adsorption capacity in four significant figures of the various

polymers and resins that have been used in the removal of MO from solutions is given in Table

6.

Table 6. Adsorption performance of MO by Group E adsorbents

Adsorbent Name Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of 𝒒𝒎𝒂𝒙 Ref.


RE% (mg/g) (oC) (m2/g) determination
UiO-66 MOF - 4545 12.0 25.0 1276 Langmuir [200]
Polyethyleneimine-functionalised graphene - 3059 3.00 - - Langmuir [201]
aerogel
MOF-derived nanoporous carbon - 872.0 6.00 - 1731 Langmuir [202]
N-acyl thiolated chitosan 88.0 588.2 7.00 26.0 10.00 Langmuir [203]
Viologen-based β-cyclodextrin polymer 77.0 370.0 - - 22.00 Langmuir [204]
Epibromohydrin-modified polyamine resin 99.0 358.3 - - - Langmuir [205]
Amine-modified PIM-1 fibrous membrane - 312.5 - - 15.00 Langmuir [206]

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3D scaffolds from thiol group-modified 90.0 305.0 7.00 - - Langmuir [207]
chitosan
Chitosan microspheres - 207.0 3.10 - - Langmuir [208]
Protonated cross-linked chitosan - 180.2 4.50 45.0 - Langmuir [209]
Cd-based MOF - 166.7 7.00 25.0 384.0 Langmuir [210]
Amino groups functionalised UiO-66 MOF 87.4 148.4 5.0 25.0 9.527 Experiments [211]
Polyaniline powder - 147.0 7.00 29.0 11.80 Langmuir [212]
Polyvinylene fluoride/PEDOT mats 75.0 146.2 3.00 20.0 5.691 Langmuir [213]
Acid promoted UiO-66 - 84.80 - - 1090 Experiments [214]
Poly-melamine formaldehyde - 81.20 - - 979.9 Experiments [215]
Immobilised polyaniline 97.6 77.50 6.50 30.0 8.500 Langmuir [216]
Chitosan beads - 73.00 3.00 25.0 10.81 Langmuir [175]
Poly(N-isopropylacrylamide)-based ionic - 64.80 - 25.0 - Langmuir [217]
hydrogels
Salecan polyssacharides 93.0 56.20 - - - Experiments [218]
Ionic-liquid-crafted zeolite - 38.00 - - - Langmuir [219]
Mesoporous ZSM-5 zeolite 94.3 25.00 1.00 30.0 - Langmuir [220]
Chitosan schiff bases - 20.00 8.00 80.0 - Experiments [221]

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Zeolite imidazolate framework-8 - 18.00 - - 1007 Langmuir [222]

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Cellulose from Stipa tenacissina L - 16.94 3.70 25.0 - Langmuir [223]
ZIF-67 - 16.30 - - 989.0 Experiments [224]
Surfactant-added ZIF-8 - 10.10 - - 891.0 Experiments [225]

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Banana pseudo steam-based hydrogel - 9.470 7.00 - - Experiments [226]
Zeolitic imidazolate framework-8 (ZIF-8)
Multifunctional Cd(ll) MOFs
-
100
-p
9.200
-
-
-
-
-
1007
517.0
Experiments
-
[224]
[227]
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Methylsilsesquioxane aerogels 95.0 - - - - [228]
Cadmium MOFs 39.0 - - - - - [229]
Zirconium MOF (UiO-66) 31.0 - 2.00 25.0 - - [230]
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3.6 Group F: Nanoparticles


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Nanoparticles are materials with a size less than 100 nm [231, 232]. Due to their very
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small size, they have gained popularity not just in the adsorption of dyes from solutions but
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also in the removal of different varieties of pollutants from the environment [233, 234].

Nanoparticles both from organic or inorganic sources exhibit intrinsic surface activity, high

surface areas and reactive atoms or functional groups that enable them to bind strongly with

the dye molecules [235]. Its small size, surface structure and inter-particle interaction make

nanoparticles to be efficient adsorbents [236, 237]. The adsorption capacity in four significant

figures of the various nanoparticles that have been used in the removal of MO from solutions

is given in Table 7.

Table 7. Adsorption performance of MO by Group F adsorbents

Adsorbent Name Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of 𝒒𝒎𝒂𝒙 Ref.


RE% (mg/g) (oC) (m2/g) determination

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Mesoporous carbon - 9091 3.00 - 2944 Langmuir [238]
Magnetic nanoporous Fe/MCM-41 96.7 5000 2.00 20.0 1216 Langmuir [239]
Magnetic hierarchical porous carbon 99.9 1523 - 30.0 603.0 Langmuir [240]
sphere
Mesoporous MCM-41 92.0 1000 2.00 20.0 1451 Langmuir [239]
Bismuth nitrate NP 97.0 730.0 - - 5.290 Langmuir [241]
Cu2O/Ag - 709.2 - - 55.36 Langmuir [242]
Copper hydroxide nitrate nanosheets - 428.8 - - - Experiments [243]
MnO2 deposited diatomic nanosheets 95.0 420.2 3.00 25.0 - Langmuir [244]
Carbon nanostructure from Bengal gram - 418.4 - - 1710 Langmuir [245]
bean husk
NiO NPs - 370.4 8.00 60.0 78.37 Langmuir [246]
Amino-functionalised magnetic multi- 99.6 355.8 6.00 50.0 598.0 Langmuir [247]
MOF
Nitrogen-doped porous carbon - 337.8 7.10 20.0 1259 Langmuir [248]
pTSA-PANI/PLLA nanofiber mat 70.0 333.0 6.00 25.0 1276 Langmuir [249]
MnO2 deposited diatomic nanowires 99.0 324.7 3.00 25.0 - Langmuir [244]
p-CNTs/chlorine chloride - 310.2 2.00 - 197.8 Langmuir [250]

f
Sulfamic acid/Cr-MIL-101 70.0 291.5 2.00 25.0 944.0 Langmuir [62]

oo
p-CNTs/N,N-diethylethanol ammonium - 263.1 2.00 - 169.7 Langmuir [250]
chloride
Reduced graphene oxide - 243.9 7.00 - - Langmuir [251]

r
Cobalt hydroxide NPs 87.0 234.0 5.00 - - Langmuir [252]
MgAL-LDHs nanosheets
Nitrogen-doped nanoporous carbon
-
95.2
-p
229.8
222.2
-
6.00
-
25.0
65.94
1152
Experiments
Langmuir
[253]
[254]
re
CuO NPs - 217.4 6.50 60.0 6.188 Langmuir [246]
Nitrogen-doped mesoporous carbon - 202.4 - 25.0 968.0 Langmuir [255]
NiO nanoflakes 84.6 165.8 2.00 - 9.720 Langmuir [256]
lP

CuO nanoflakes 93.2 158.7 2.00 - 69.27 Langmuir [256]


Mesoporous MCM-41/microfiltration 99.0 151.5 4.00 25.00 1451 Langmuir [257]
membrane
na

Mesoporous carbon nanofibers - 126.6 7.00 45.0 392.3 Langmuir [258]


Magnetic lignin-based CNPs 90.7 113.0 5.00 20.0 82.80 Langmuir [259]
Non-functionalised CNTs (p-CNTs) - 110.4 2.00 - 123.5 Langmuir [250]
ur

Cu2O particles - 96.42 - - 1.130 Langmuir [260]


Polyaniline nano-adsorbent 98.2 75.90 10.0 65.0 10.44 Langmuir [261]
Polyanilined-based nanoadsorbent 97.0 75.90 6.00 45.0 10.34 Langmuir [262]
Jo

ZIF-67 nanostructure 70.2 75.59 - - 593.6 Langmuir [263]


Porous Al-doped ZnO nanosheets 99.3 74.57 7.00 25.0 34.30 Langmuir [264]
Al-doped CNTs 99.4 69.70 4.50 - 118.8 Langmuir [265]
β-Ni(OH)2 nanostructures 20.6 48.14 - - - Experiments [266]
Co3O4 NPs - 46.08 6.00 - - Langmuir [267]
nanodiamond - 41.74 - - 282.0 Experiments [268]
Flower-like MoSe2 microspheres - 36.91 - - 25.00 Langmuir [269]
α-Fe2O3 NPs 90.0 28.90 2.00 25.0 - Langmuir [270]
Amorphous CNTs 99.9 21.51 3.00 25.0 Langmuir [271]
Amorphous CNTs 95.0 21.39 - - - Langmuir [272]
Nanoporous carbon 100 18.80 - 25.0 814.0 Langmuir [273]
Graphene oxide - 16.83 3.00 25.0 1330 Langmuir [274]
Nitrogen-doped TiO2 - 14.10 - 20.2 232.4 Langmuir [275]
CuO nanostructures 100 - - 65.0 24.10 - [276]
Cu2O NPs 100 - - - 6.150 - [277]
Palladium nanocubes/MWCNTs 99.3 - - - - - [278]
Porous ZnO spheres 96.3 - - - 114.6 - [279]
Scoria-Ni/TiO2 NPs 95.9 - 7.00 - - - [280]
Ag3PO4 91.8 - 9.00 - - [281]
Mesoporous silica NPs 91.1 - 3.00 70.0 - - [282]
Nickel hydroxide nanocatalyst 80.0 - - 30.0 87.00 - [283]

14
3.7 Group G: Composites

The search for more efficient and cost-effective adsorbents have led scientists to

develop an array of composite adsorbents for the removal of various pollutants from the

environment. Composite adsorbents are a distinct category of adsorbents that comprise two or

more materials or categories of other adsorbents [284, 285]. The characteristics of the

individual adsorbent are usually distinct from the properties of the composite material formed

by them. Such materials usually have better adsorption properties than the individual

compound used to make up the composite [286, 287]. The adsorption capacity in four

f
oo
significant figures of the various composites that have been used in the removal of MO from

r
solutions is given in Table 8.
-p
Table 8. Adsorption performance of MO by Group G adsorbents
re
Adsorbent Name Adsorbent Highest 𝒒𝒎𝒂𝒙 pH Temp SSA Method of 𝒒𝒎𝒂𝒙 Ref.
lP

Class RE% (mg/g) (oC) (m2/g) determination


Waste straws/citric acid group/acrylamide G(B-E) 80.0 3053 3.00 - - Langmuir [288]
Ni-Co-S/hexadecyltrimethyl ammonium bromide G(E-F) 99.0 2355 - 25.0 12.73 Langmuir [289]
na

CoFe2O3/MgAl-hydrotalcite G(D-F) - 1220 6.00 25.0 - Langmuir [290]


Mesoporous ZIF-67/LDH G(D-E) 98.0 1030 6.00 30.0 172.3 Langmuir [291]
Chitosan/chitosan-sodium zeolites G(E-E) 95.5 909.0 8.00 30.0 - Langmuir [292]
Chitosan/Fe3O4 G(E-F) 95.0 758.0 7.00 25.0 - Langmuir [293]
ur

Fe3O4/poly(stylenesulfonate)/ZIF-67 G(E-F) 92.0 738.0 8.00 25.0 1042 Experiments [294]


Graphene oxide/ZnO G(F-F) 75.0 714.3 7.00 - - Langmuir [295]
Fe3O4/graphene oxide nanocomposite G(F-F) - 714.3 6.00 - - Langmuir [296]
Jo

Cellulose nanofiber/chitosan G(E-F) 96.3 655.2 5.00 25.0 - Langmuir [297]


Graphene oxide/NiFe LDH G(D-F) - 438.0 - - 145.0 - [298]
Chitosan/PVA/TiO2 G(E-E-F) - 425.0 - - - Langmuir [299]
Chitosan/Al2O3/Fe3O4 G(E-F-F) 96.0 419.0 6.00 25.0 21.87 Experiments [300]
Amine/Fe3O4-resin G(E-F) - 416.7 5.50 45.0 - Langmuir [301]
Ni-Al LDH/AC G(B-D) - 412.8 4.50 30.0 1158 Sips [302]
Al-doped MOF/grapheme oxide G(E-F) - 400.0 8.00 - 1309 Langmuir [303]
NDA88 MOF/Cu G(E-F) - 398.8 - - 370.4 Langmuir [304]
Chitosan/β-cyclodextrin polymer G(E-E) 90.7 392.0 5.00 25.0 - Langmuir [305]
Starch/NiFe LDH G(A-D) 99.0 387.6 3.00 25.00 - Langmuir [306]
Calcium ferrite/zirconia G(F-F) 98.9 370.4 2.00 30.0 95.32 Langmuir [307]
Fe2O3/AC G(B-F) 80.0 362.0 3.00 20.0 1110 Langmuir [308]
ZnO/CuO G(F-F) 93.0 341.0 - 25.0 - Experiments [309]
Graphene/β-cyclodextrin G(E-F) - 328.2 - - - Experiments [310]
Fe2O3/Mn3O4 magnetic nanocomposites G(F-F) 97.7 322.6 2.00 25.0 178.3 Langmuir [311]
Chitosan/Fe(OH)3 beads G(D-E) 91.1 314.5 3.00 - 10.20 Langmuir [312]
Chitosan/PVA/TiO2 nanofiber G(E-E-F) 94.0 314.0 - - - Langmuir [313]
Reduced graphene oxide/NiCr-CO3 LDH G(D-F) - 312.5 - - - Langmuir [314]
Manganese ferrite/hausmannite NP G(F-F) 97.4 303.0 2.00 25.0 100.6 Langmuir [315]
Chitosan/H2O2 activated anthracite G(D-E) 98.8 297.3 3.00 25.0 - Langmuir [316]
Polyaniline/AC G(B-E) 70.0 285.0 6.50 - 36.00 Langmuir [317]
Zn-Al LDH/ZnO G(D-F) 96.9 276.6 - - - Langmuir [318]
Ni NPs/porous carbon-carbon nanotubes G(F-F) - 274.0 - - 999.0 Langmuir [319]
Zn-Al LDH/SiO2 G(D-F) 88.9 266.5 - - - Langmuir [318]

15
Polydopamine/cellulose nanofibril/polyethylene- G(E-F) - 265.9 4.00 25.0 - Langmuir [320]
imine
Date palm ash/MgAl-LDH G(C-D) 93.0 243.0 3.00 25.0 140.7 Langmuir [321]
ZnO/polyaniline G(E-F) 99.1 240.8 4.00 - 63.17 Langmuir [322]
Polydopamine/polyethyleneimine/graphene oxide G(E-E-F) - 237.5 - 40.00 - Langmuir [323]
Chitosan/graphene nanoplates G(E-F) 96.0 230.9 3.00 25.0 - Langmuir [324]
Immobilised Fe/chitosan G(E-F) - 205.0 4.00 50.0 - Langmuir [58]
Polyethyleneimine/β-cyclodextrin/Fe3O4 G(D-E) - 192.2 1.00 30.0 17.51 Langmuir [325]
Catechol/amine resin G(E-E) 94.5 189.4 - 30.0 13.13 Langmuir [326]
Chitosan/PVA electrospun nanofiber G(E-F) - 183.0 - - - Langmuir [327]
Carbon dots/ZnFe2O4 G(F-F) - 181.2 5.00 20.0 161.8 Langmuir [328]
ZIF-67/CoAl-LDH G(D-E) 72.3 180.5 - - 274.3 Langmuir [263]
Silica daisogel/vinylbenzyl N,N-diethyl 2- G(D-E) 100 180.3 5.50 25.0 - Langmuir [329]
hydroxyethyl ammonium moieties
AC/polytetrafluoroethylene G(B-E) - 176.0 - 25.0 700.0 Experiments [330]
Mg NP/modified nanosized Si2-Al2O3 G(D-F) 89.3 167.2 6.50 25.0 101.0 Sips [331]
Immobilised chitosan/montmorillonite G(D-E) 94.6 154.4 6.30 30.0 4.380 Langmuir [332]
Chitosan/PVA/zeolite electrospun s membrane G(E-E-F) - 153.0 - - - Langmuir [333]
Fe3O4/AC G(B-F) - 150.4 7.00 25.0 1200 Liu [334]
Fe3O4/polypyrrole G(E-F) - 149.5 - 25.0 - Langmuir [335]

f
Activated organic-bentonite/sodium alginate G(D-E) - 141.2 11.0 23.0 80.00 Langmuir [336]

oo
Chitosan/bentonite G(D-E) 99.7 136.8 3.00 25.0 - Langmuir [337]
Nitrilotriacetic acid/β-cyclodextrin/chitosan G(E-E) 94.0 132.5 - - - Sips [338]
Chitosan/ethylene glycol diglycidyl ether biofilm G(E-E) - 131.2 3.00 30.0 0.820 Langmuir [339]

r
Copper sulphide NPs/AC G(B-F) 99.0 122.0 5.00 25.0 1286 Langmuir [340]
Chitosan/ethylene glycol diglycidyl ether beads
Magnetic pectin/chlorella vulagaris
NiFe LDH nanoflakes/montmorillonite
G(E-E)
G(A-F)
G(D-E)
-p -
-
91.8
112.4
109.1
108.8
-
-
30.0
30.0
25.0
-
-
103.9
Langmuir
Langmuir
Langmuir
[341]
[342]
[343]
re
Co3O4 nanocube/polyaniline G(E-F) 94.0 107.0 7.00 25.0 43.00 Experiments [344]
Amino-functionalised magnetic bacterial G(B-F) 82.8 103.3 3.00 45.0 - Langmuir [345]
cellulose/AC
lP

MgO/carbon nanocomposites G(F-F) - 101.8 - - 59.34 Langmuir [346]


Polyaniline/glass plates G(E-E) 100 93.00 7.00 29.0 3.700 Langmuir [212]
Ag-N-ZnO/coconut husk AC G(B-F) 98.8 90.42 - - 472.0 Experiments [347]
Magnetic pressler/chitosan/Fe3O4 G(E-F-F) 97.0 88.50 6.00 45.0 - Langmuir [348]
na

Goethite/chitosan beads G(D-E) - 84.00 3.00 25.0 17.81 Langmuir [175]


Graphene oxide/isophorone diisocyanate/β- G(E-E-F) 92.4 83.40 6.00 25.0 32.13 Langmuir [349]
cyclodextrin
ur

γ-Fe2O3/2C nanocomposites G(F-F) 99.9 72.68 4.80 25.0 394.1 Langmuir [350]
UiO-66/nanocellulose aerogels G(F-F) - 71.70 - - 826.0 Experiments [351]
Spent tea leaves/polyethyleneimine G(A-E) 91.1 62.11 3.00 25.0 2.330 Langmuir [352]
Jo

NaX/MgO-TiO2 zeolite G(E-F) 95.0 53.76 6.50 45.0 - Langmuir [353]


Chitosan/rectorite/CNTs G(D-E-F) 80.5 50.75 5.00 8.303 Langmuir [354]
Functionalised CNTs/TiO2 G(F-F) 100 42.68 6.50 25.0 - Langmuir [355]
Chitosan/diatomic G(D-E) 88.4 35.12 5.00 20.0 - Langmuir [356]
Fe2O3/mesoporous carbon G(F-F) 26.50 3.00 20.0 69.00 Langmuir [308]
LDH/Fe3O4/polyvinyl alcohol G(A-F) 97.0 19.59 6.00 25.0 87.00 Langmuir [357]
Nanofibrillated cellulose-based cryogel/N-doped G(A-D-F) 99.0 17.60 - 20.0 - Langmuir [358]
TiO2
Bi2O3/TiO2/powdered AC G(B-F) - 16.33 - - 83.30 Experiments [359]
Fe2O3/biochar G(C-F) 100 16.05 2.86 25.0 15.30 Langmuir [360]
Fe2O3/polypeptidylated hemoglobin G(E-F) - 15.20 25.0 - Langmuir [361]
AgGaO2 nanocomposites G(F-F) - 11.39 7.50 25.0 23.35 Experiments [362]
Starch/ascorbic acid-modified MWCNTs G(A-F) 70.0 11.11 2.00 - - Langmuir [363]
Chitosan/PVA/Na-titanate/TiO2 G(E-E-E-F) 99.9 6.860 - - - Experiments [364]
Fe NPs/SiO2-NH2/glycerol G(A-D-F) 100 3.020 3.00 25.0 171.0 Experiments [365]
Fe NPs/SiO2-NH2/black tea extract G(A-D-F) 100 2.970 3.00 25.0 89.10 Experiments [365]
Fe NPs/SiO2-NH2/yerba mate extract G(A-D-F) 100 2.840 3.00 25.0 113.1 Experiments [365]
Fe3O4/CNTs G(F-F) - 2.760 - - - Experiments [366]
Fe3O4/polydopamine G(E-F) - 2.070 - - - Experiments [366]
Cellulose acetate/polyurethane G(E-E) 25.5 0.185 - - - Langmuir [367]
Silver NP/zeolite X G(E-F) 100 - 5.00 - 552.6 - [368]
TiO2/aluminosilicate zeolite (ZSM-5) G(E-F) 99.6 - 7.50 1151 - [369]
Graphene/Fe3O4 G(F-F) 99.2 - - - - - [370]
Chitosan/polyaniline/copper(ll) oxide G(E-E-F) 98.9 - 4.00 - - - [371]
Au/Cu2O G(F-F) 98.8 - - - 16.00 - [372]
Fe-based MOF/graphene oxide G(E-F) 98.0 - 3.00 30.0 1602 - [373]

16
Biochar from waste walnut shells/TiO2 G(C-F) 96.9 - - - 66.06 - [374]
Pisum sativum peels/Fe3O4 NPs G(A-F) 96.2 - 6.00 - 17.60 - [375]
NiFe2O4/LDH composite G(D-F) 94.3 - - 25.0 - - [376]
Chitosan/polyvinyl alcohol (PVA)/zeolite G(E-E-E) 94.0 - - - - - [377]
Chitosan/Co-MCM-15 G(E-F) 76.0 - 8.00 - - - [378]
TiO2/pure calcium silicate G(D-F) 60.0 - - - 126.0 - [379]
TiO2/slag-made calcium silicate G(D-F) 43.7 - - - 149.0 - [379]

4. Discussion on the performance of the various adsorbent groups

The frequency of the various adsorbents that have been employed by researchers in the

past five years for the mitigation of MO from aqueous solutions as shown in Figure 3 in

decreasing order is given by; composites > nanoparticles > polymers and resins > clay and

f
oo
minerals > activated carbon > biosorbents > biochars. The most frequently used adsorbent

group are the composite adsorbents (>40%). This may be due to its perceived high adsorption

r
-p
ability which is contributed by the individual adsorbents that make up the composite. Other
re
adsorbent groups also used are nanoparticles, which may be due to their increasing popularity
lP

as a result of their very small size. This contributes to their high surface area which invariably

increases their adsorption capacity.


na

From Figure 4, it was observed that nanoparticles were the most frequently used in the
ur

manufacture of composite adsorbents for MO uptake in the past five years. The choice of
Jo

nanoparticles in composite adsorbents could be due to their flexibility in going into the matrices

of other material types due to their small sizes. Even though the composite material formed

have distinct properties from its parent material, the parent materials also contribute to the

excellent properties of the composite material. Another group of adsorbents frequently used

for this same purpose in the past five years are clays and minerals. This could be due to their

ability to adsorb water in their interlayer sites, and their high surface area which are properties

of a good adsorbent.

For Table 9, we will have to ignore the results for groups 1-3 because their data (based

on published papers in the last 5 years) is not large enough to be statistically significant. Hence

it would be erroneous to draw generic or specific inferences from such results. Considering the

17
other four classes of adsorbents, nanoparticles have the second highest mean performance for

MO uptake. However, clays and minerals have the greatest proportion of adsorbents with MO

uptake capacity greater than the 1000 mg/g threshold.

f
r oo
-p
re
lP

Figure 3. Frequency of the various groups of adsorbents used for the mitigation of MO in the

last five years.


na
ur
Jo

Figure 4. Frequency of the individual groups of adsorbents used for the synthesis of composite

adsorbents used for the mitigation of MO in the last five years.

18
Table 9. Mean adsorption capacity for various adsorbent types (The ranking is shown in the

parenthesis and was done in decreasing order of magnitude)

Class Name Mean (mg/g) % with 𝒒𝒎𝒂𝒙 > 1000 mg/g


A Biosorbents 249.3 (7th) 0%
B Activated carbon 1327 (1st) 25%
C Biochar 268.2 (6th) 0%
D Clays and mineral 426.8 (4th) 14%
E Polymers and resins 514.0 (3rd) 6.9%
F Nanoparticles 552.1 (2nd) 8.8%
G Composites 291.8 (5th) 4.5%

5. Mechanism of MO adsorption

f
In this section, we discuss the mechanism of MO adsorption firstly based on the nature

oo
of the molecule itself, then on the nature of the adsorbent material. Studying the chemical

r
-p
nature of the adsorbent and adsorbate can help to elucidate the specific physico-chemical
re
mechanisms that are involved in the adsorptive uptake [380]. MO is a polycyclic aromatic

compound hence can have electron donor-acceptor (EDA) interactions with adsorbents with
lP

some amount of aromaticity. These physical interactions can be in the form of π - π (8 – 12


na

kJ/mol), cation – π (8 – 25 kJ/mol) and anion – π (20 – 50 kJ/mol) [381]. These are some of
ur

the strongest physical interaction forces for MO uptake. Adsorbents like biochar, activated
Jo

carbons and carbon-based nanoparticles (e.g. SWCNTs and MWCNTs) are strongly aromatic

hence can interact in this way with MO. MO is also able to interact with adsorbents by hydrogen

bonds (4 – 40 kJ/mol) due to the presence of hetero-atoms on its structure. The dimethyl

substituted nitrogen atom on one end and the sodium substituted sulphur atom on the other end

are good points for weak interactions with hydrogen species on adsorbents (See MO structure

in Figure 1). Since MO is an ionisable molecule with a pKa of 3.4, it follows that it can form

strong electrostatic interactions with adsorbents that are not at their isoelectric point.

Electrostatic interactions are strong chemical interactions that can account for a significant

amount of MO uptake in adsorptive systems. The major caveat is the pH which must not be at

the adsorbents’ isoelectric point thereby preventing its electrical neutrality in aqueous media.

19
The type of adsorbent materials also influences the nature of MO uptake interactions.

Biosorbent possesses lower surface areas and porosity but is capable of adsorptive performance

because they possess numerous functional groups that can facilitate different physico-chemical

interactions [382, 383]. The rise of biosorbent utility in adsorption has strengthened the

argument that adsorption is more of a chemical process than a physical one. Activated carbons

and biochar have higher surface areas and are more porous. The surface area ensures the greater

availability of active surface/sites for MO uptake. Based on the dimensions of the pores, the

intra-particle diffusion could be slow hence making it the rate-limiting step [384]. Clays and

f
oo
minerals and well-ordered crystalline inorganic minerals. The sheet-like nature of clays means

r
it can be pillared and intercalated to preserve its adsorptive potential and prevent swelling in
-p
contact with water [385, 386]. It also follows that these clays can adsorb MO by ion exchange.
re
Polymers, resins and nanoparticles usually also interact with MO following the usual physico
lP

chemical interactions explained above. The greatest advantage of nanoparticles is their reduced
na

sizes leading to very large specific surface areas. Their greatest disadvantage is their

ecotoxicology [387]. Nanoparticles, polymers and resins have similar issues of low
ur

environmental friendliness and high cost and are hence only developed for targeted
Jo

environmental applications.

6. Conclusion

Based on this investigation, several conclusions regarding MO adsorption were derived.

In terms of frequency of utilisation of adsorbent group, composites were the most frequently

used group (>40%). It was observed that nanoparticles and polymers were the most frequently

used constituents in the manufacture of composite adsorbents for MO uptake in the past five

years. The choice of nanoparticles in composite adsorbents could be due to their flexibility in

going into the matrices of other material types due to their small sizes. Polymers also act as

20
good matrices for immobilising other composite constituents. Nanoparticles was the best

adsorbent group for MO uptake. However, clays and minerals have the greatest proportion of

adsorbents with uptake capacity greater than the 1000 mg/g threshold. This study is important

as regards future work on MO adsorption. It will be able to guide researchers on the reasonable

choice of adsorbent type that would be suitable for the uptake of MO. Furthermore, researchers

interested in developing composite adsorbents can have a good base for making informed

decisions on constituent types based on our findings. This will also help reduce the arbitrary

choice of adsorbent types for MO adsorption leading to a reduction in the amount of published

f
oo
literature with little/incremental contributions to the field.

r
Disclosure statements
-p
re
Conflict of Interest: The authors declare that there are no conflicts of interest.
lP

Funding: There was no external funding for the study.


na

Compliance with Ethical Standards: This article does not contain any studies involving human

or animal subjects.
ur
Jo

Author contributions

Kingsley O. Iwuozor, Conceptualisation; Methodology; Data curation; Writing - original draft;

Writing - review & editing; Validation; Supervision

Joshua O. Ighalo, Conceptualisation; Methodology; Writing - original draft; Writing - review

& editing; Validation; Supervision

Ebuka Chizitere Emenike, Data curation; Writing - original draft; Writing - review & editing;

Validation

Lawal Adewale Ogunfowora, Writing - original draft; Writing - review & editing; Validation

Chinenye Adaobi Igwegbe, Writing - original draft; Writing - review & editing; Validation

21
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Highlights
 The performance of various adsorbent groups for MO adsorption was reviewed.

 Composites were the most frequently used (>40%) adsorbent group for MO adsorption

 Nanoparticles and polymers were the most frequently used constituents in the composite

 Nanoparticles were the best adsorbents for MO uptake

 Clays and minerals had the greatest proportion of adsorbents with >1000 mg/g capacity

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Declaration of interests

☒ The authors declare that they have no known competing financial interests or personal relationships
that could have appeared to influence the work reported in this paper.

☐The authors declare the following financial interests/personal relationships which may be considered
as potential competing interests:

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