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Editor: Dr. GL Dotto Methylene blue (MB) is a heterocyclic aromatic compound used as a medication or as a synthetic dye for textiles.
Due to its ecotoxicity, researchers have been investigating its mitigation by the adsorption process. The aim of
Keywords: this review was to analyse the performance of different classes of adsorbent for MB dye uptake based on their
Adsorption maximum adsorption capacity. MB was chosen for this analysis due to the large volume of work that has been
Activated carbon
done on it over the years. Over 500 research papers published on MB adsorption (within the past 5 years were
Biochar
analysed). This was to help guide the research area on the best class adsorbents for MB uptake thereby pointing
Nanoparticle
Methylene blue the areas of biggest potential to investigators. Composites adsorbents (31%) were the most frequently studied for
MB uptake. Other popularly used types were biosorbents (16%) and activated carbon (16%). Polymers and
resins, and organic and inorganic nanoparticles were the more favoured constituents for composite adsorbent
development. For similar data indices, composite adsorbents yielded a higher adsorption capacity. This suggests
that composite adsorbents (especially with constituents of polymers, resins and nanoparticles) perform better for
MB uptake. Though polymers and resins had the highest mean, the highest median was for activated carbon.
Composite adsorbent was the second highest for mean, median and number of adsorbents above the 1000 mg/g
threshold. It was surmised from the analysis that polymers, resins and composites are the best classes of ad
sorbents for MB uptake.
* Corresponding author at: Department of Chemical Engineering, Nnamdi Azikiwe University, P.M.B. 5025, Awka, Nigeria.
** Corresponding author.
E-mail addresses: oshea.ighalo@yahoo.com, jo.ighalo@unizik.edu.ng (J.O. Ighalo), ca.igwegbe@unizik.edu.ng (C.A. Igwegbe).
1
https://orcid.org/0000-0002-1161-2147.
2
https://orcid.org/0000-0002-8709-100X.
3
https://orcid.org/0000-0002-2104-3582.
4
https://orcid.org/0000-0001-6615-5361.
5
https://orcid.org/0000-0002-5766-7047.
https://doi.org/10.1016/j.jece.2021.105658
Received 20 April 2021; Received in revised form 30 April 2021; Accepted 8 May 2021
Available online 16 May 2021
2213-3437/© 2021 Elsevier Ltd. All rights reserved.
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Class C – Biochar
Class D – Clays and minerals
Class E – Polymers and resins
Class F – Nanoparticles
Class G – Composites adsorbent
Based on these classes, the literature was analysed. The performance
of each class of adsorbent was discussed as stand-alone then compari
sons were made across various adsorbent classes to help draw important
observations and trends. The method of adsorption capacity determi
Fig. 1. Chemical structure of methylene blue dye (N – Nitrogen, S – Sulphur).
nation and the adsorbent specific surface area (SSA) is also stated. The
key process parameters (temperature and pH) at which the optimum
values are achieved are also reported for better specificity of the results.
methemoglobinemia or as a synthetic dye for textiles. The latter is the
All analysis tables were sorted in decreasing magnitude of maximum
more widely known application. MB is a cationic because of the nitrogen
adsorption capacity and values are reported to four significant figures. It
and sulphur atoms in its structure which makes it possess a positive
was important to report the core results data within the paper so that it
charge after ionisation [15].
can serve as a reference point for other researchers for comparing their
A number of processes have been utilised for MB uptake and these
adsorbents’ performance and to know if their findings represent prog
include photodegradation [16], electro-coagulation [17,18], ozonation
ress in the status quo.
[19,20], membrane processes [21–23] and biological processes [24,25].
Adsorption is of advantage to these processes because it can handle
3. Defining the adsorbents classes and listing empirical results
pollutants at low concentration, it is low-cost, can be regenerated and
does not leave behind chemical residues [26,27].
3.1. Class A adsorbents (biosorbents)
Within the last decade, several key papers have reviewed MB
adsorption taking various approaches. The first and most important
Biosorbents are a class of adsorbents derived from biomass and other
review on MB adsorption was by Rafatullah et al. [28]. The focus was on
bio-materials that do not undergo any thermochemical breakdown
low-cost adsorbents alone and did not cover the entire spectrum of the
before utilisation. The key feature of biosorbents is that they retain the
different adsorbent types. Though comprehensive, the review was
original composition of the source bio-material. For the case of biomass,
published over a decade ago and much work has been done since then.
the constituents start degrading at > 300 ◦ C [33]. Any biomass material
Mohammed et al. [9] reviewed MB adsorption with a focus also on
processed at a lower temperature can still be considered as a biosorbent.
low-cost adsorbents. Recently, Mashkoor and Nasar [1] reviewed MB
The plant part can be the leaves [34–36], bark [37], husk [38,39], peels
adsorption by magnetic adsorbents. Santoso et al. [29] conducted a
[40,41], flower spikes [42], seeds [43], leaves [44,45], stem [46] and
comprehensive review on MB adsorption albeit with carbon-based
living or dead cells of microorganism [47,48]. Biosorbents can also be
adsorbent.
from animal sources such as wool fibres [49], egg shells [50] and baker’s
The reason for the choice of MB in this study is the massive amount of
yeast [51]. Though biosorbents do not possess a very large surface area,
literature being churned out on the subject without any proper synthesis
the abundance of various functional groups on the material affords it the
of the available knowledge. This is unsurprising as MB is the most
capability of MB uptake by a variety of physico-chemical interaction
commonly utilised dye [9]. Trying out new adsorbent materials and new
mechanisms [52,53]. The performance of modified and unmodified
modification techniques are good but there is a need to summarise
biosorbents for the uptake of MB used in this analysis is summarised in
findings so researchers can understand where the best prospects are
Table 1 reported to four significant figures and sorted in decreasing
[30]. Understanding the best adsorbent class and their performance
order of magnitude.
relative to other adsorbent classes will help shape the direction of the
research area. This is an important gap in knowledge that needs to be
3.2. Class B adsorbents (activated carbon)
explored.
In view of this, the aim of this review is to analyse the performance of
Activated carbon (AC) is a highly porous carbonaceous material
different classes of adsorbents for MB dye uptake based on their
produced by the carbonisation and activation of biomass [120]. It can be
maximum adsorption capacity. Over five hundred (500) papers have
activated chemically by acids, alkalis and salts or activated physically by
been published on MB adsorption in the five (5) years. These will form
steam or CO2. Using chemical activation, the reagents are usually
the basis for this literature analysis.
impregnated under wet or dry conditions [121] v. At the devolatilisation
of the biomass material at high temperatures, these reagents help to
2. Methodology for literature analysis
initiate tortuous and highly porous features in the microstructure of the
residual carbon there leading to high surface areas [34,122]. Chemical
The scope of the literature considered in this study was all papers on
activation has an advantage over physical activation because it requires
the adsorption of MB from 2016 to the current time. This was done
lesser processing temperature and time [123]. The developed carbons
irrespective of the type of adsorbent used. The papers were sourced from
can be microporous (pore diameter < 2 nm), mesoporous (pore diam
google scholar. The index for the analysis of adsorbent performance was
eter 2–50 nm) or macroporous (pore diameter > 50 nm) [124,125].
the maximum adsorption capacity. Though the maximum removal ef
The main feature of AC is its high specific surface area (usually above
ficiency was reported, it was not the basis of the analysis. It has been
700 m2/g). Adsorption being a surface phenomenon, the large surface
explained that the removal efficiency is overly dependent on the choice
area of AC makes it suitable for the application. Commercial AC can be
of operational parameters such as the initial concentration of the
in powdered (PAC) or granulated (GAC) form [126] and both forms have
adsorbate and the dosage of the adsorbent [31,32]. This makes it un
been used in adsorption application [127,128]. Commercial AC usually
suitable for making a comparison across different research papers. On
has a high cost hence researchers are now exploring low-cost alternative
the other hand, the maximum adsorption capacity gives a better repre
feedstock for AC production [129]. The nature of these low-cost alter
sentation of the adsorbents’ intrinsic potential for MB. The adsorbents
natives also affects the properties of the AC developed [130,131]. The
were classed as follows:
performance of modified and unmodified activated carbon for the up
Class A – Biosorbents
take of MB used in this analysis is summarised in Table 2 reported to four
Class B – Activated carbon
significant figures and sorted in decreasing order of magnitude.
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K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 1
Adsorption performance of MB by class A adsorbents.
Adsorbent name Highest RE qmax (mg/ pH Temp Method of qmax SSA (m2/ Ref.
% g) (◦ C) determination g)
3
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 1 (continued )
Adsorbent name Highest RE qmax (mg/ pH Temp Method of qmax SSA (m2/ Ref.
% g) (◦ C) determination g)
3.3. Class C adsorbents (biochar) impregnation takes place either by pillaring [263–265] or intercalation
[264,266]. The principle of intercalation and pillaring of clays is shown
Biochar is the residue of biomass thermochemical processing such as in Fig. 2 [267]. The advantage of intercalation and pillaring is that it
pyrolysis [211,212], air gasification [213,214], steam gasification [215, helps the clay to prevent swelling upon hydration thereby instilling a
216] and retort carbonisation [217,218]. Biochar is different from AC. permanent porosity on the material. The performance of clays and
Usually, these thermochemical processes are conducted with more in minerals for the uptake of MB is summarised in Table 4 reported to four
terest being in the fluid products (liquid and gaseous species) hence the significant figures and sorted in decreasing order of magnitude.
produced char is considered a residue. Though biochar is a pyrogenic
carbon-rich material like AC, it does not possess a very high specific 3.5. Class E adsorbents (polymers and resins)
surface area and unique pore properties like the latter. The char is
termed ‘biochar’ since the feedstock for the processes is biomass [219]. Polymers are substances with long repeated chains of a specific
Char from hydrothermal carbonisation is however termed ‘hydrochar’ chemical unit (known as a monomer) [297]. They can either be from
[220]. A major advantage of biochar utilisation as adsorbents is its natural sources or synthetic sources. Due to their ease of manipulation
biodegradability [221]. Even if some amount of the adsorbent is unre by chemical modification, a broad spectrum of chemical and physical
covered and leaves with treated effluent, it does not bear any ecotoxi properties can be achieved by polymers [298]. Wide range of properties
cological risk. This is its major advantage over polymeric adsorbents by consequence yields wide application areas. Both natural and syn
which might not be bio-degradable and nano-particle adsorbents which thetic polymers have been used as adsorbents. Resins are solids or highly
have serious ecotoxicity [222,223]. The performance of modified and viscous polymeric liquids of natural or synthetic origins [299]. Different
unmodified biochar for the uptake of MB used in this analysis is sum types of polymeric adsorbents have their advantages and limitations.
marised in Table 3 reported to four significant figures and sorted in Bio-polymers like chitosan and cyclodextrin for example are easily de
decreasing order of magnitude. natured at high process conditions and are unsuitable for use in packed
columns due to their physical nature [300]. Polymeric adsorbents have
3.4. Class D adsorbents (clays and minerals) the major advantage of being easily tuneable to achieve selectivi
ty/affinity for specific pollutant species using various chemical modifi
Clays and their minerals are natural earth materials that have small cation techniques [300]. The major limitation is its cost. It is relatively
particle sizes and a porous layered structure with a large surface area more expensive to synthesise than for other adsorbent classes. Further
[256]. This allows for strong physical, chemical interactions with dis more, inorganic/synthetic polymeric adsorbents are not biodegradable
solved species such as MB in aqueous media [257]. Clays are and if not fully recovered before effluent release can have a deleterious
alumina-silicates with two building blocks: aluminium octahedron effect on the environment. The performance of polymers and resins for
(gibbsite sheet) and silicon–oxygen tetrahedron (Si2O5)2− [258]. The the uptake of MB used in this analysis is summarised in Table 5 reported
tetrahedral sheets have tetrahedrons within them which share three in to four significant figures and sorted in decreasing order of magnitude.
every four oxygen atoms. The main classes of clay are kaolinite, mont
morillonite, Illite, bentonite and chlorite [258]. Most natural clays are a 3.6. Class F adsorbents (nanoparticles)
mixture of different types of these classes of clay [259]. Clays can be
modified in a variety of ways to improve their adsorption capacity for Nanoparticles are a class of materials that have sizes between 1 and
pollutants but the most popular of them is the use of surfactants 100 nm [352]. Due to their very small size, they possess large surface
[260–262]. Metals can also be impregnated into the clay matrix as a areas [353]. Materials with large surface areas will always be favoured
means of modification. Due to the structural nature of clay, this for adsorptive applications because adsorption is a surface phenomenon.
4
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 2
Adsorption performance of MB by class B adsorbents.
Adsorbent name Highest RE% qmax (mg/g) pH Temp (◦ C) Method of qmax determination SSA (m2/g) Ref.
5
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 2 (continued )
Adsorbent name Highest RE% qmax (mg/g) pH Temp (◦ C) Method of qmax determination SSA (m2/g) Ref.
Carbon fibre aerogel from cotton – 102.2 – 25.0 Langmuir 457.7 [196]
AC from corn cobs 99.9 100.0 7.0 27.0 Langmuir – [197]
AC from corncob – 82.71 7.0 30.0 Langmuir – [198]
Commercial AC (Darco S-51) – 80.00 7.0 25.0 Experiments 599.5 [185]
AC from Banana trunk – 64.66 – – Experiments – [199]
AC from rice straw 99.7 62.50 7.0 25.0 Langmuir – [200]
AC from Phragmites australis biomass 96.6 62.50 6.5 25.0 Langmuir – [103]
AC from sawdust 99.2 58.14 7.0 30.0 Langmuir – [201]
AC from Ackee apple pods 99.9 49.99 6.2 25.0 Experiments 812.8 [202]
AC – 48.30 – 25.0 Langmuir – [203]
AC from Fiscus carica 85.0 47.62 7.8 30.0 Langmuir – [204]
AC from steel slag – 41.62 7.0 20.0 Experiments 66.65 [205]
AC from sawdust – 30.00 7.0 30.0 Experiments 468.0 [194]
AC from Coconut fibres – 21.30 3.0 – Experiments 1556 [206]
AC from textile – 17.83 6.2 60.0 Langmuir 221.5 [207]
AC from tannery leather – 15.00 7.0 30.0 Experiments 316.0 [194]
AC from waste tyre 90.0 1.050 3.0 25.0 Langmuir 396.0 [208]
AC from Banana peels 94.0 0.125 4.0 – Langmuir 30.49 [116]
AC from Groundnut shell > 99.0 – 9.0 – Experiments – [209]
AC from hydnocarpus pentandra 98.8 – 7.8 25.0 Experiments – [210]
Table 3
Adsorption performance of MB by class C adsorbents.
Adsorbent name Highest RE% qmax (mg/g) pH Temp (◦ C) Method of qmax determination SSA (m2/g) Ref.
Nanoparticles can be synthesised from organic and inorganic sources [358–360], and others [361–364]. For chemical vapour deposition, the
using a variety of techniques which include chemical vapour deposition nanoparticles are synthesised by chemical reactions in the gaseous phase
[354], precipitation [355], sol-gel [356,357], hydrothermal synthesis in the vicinity of a heated surface [365]. Precipitation is the most
6
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
7
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 4
Adsorption performance of MB by class D adsorbents.
Adsorbent name Highest RE% qmax (mg/g) pH Temp (◦ C) Method of qmax determination SSA (m2/g) Ref.
interactions that could facilitate MB uptake. If the adsorbent has ben surface charge of the adsorbent (to determine if it will be attractive or
zene rings, then uptake can be facilitated by π-π interactions (8–10 kJ/ repulsive) depends on its isoelectric point [581]. The isoelectric point
mol). The presence of electronegative heteroatoms like Nitrogen and (or the point of zero charge) is the pH value at which the adsorbent will
sulphur on the MB structure (see Fig. 1) could facilitate hydrogen bonds have a net zero surface charge. At pH values greater than this, the
(4–40 kJ/mol) with the hydrogen on the polymers or resins. Other adsorbent has a net negative surface charge thereby facilitating uptake
physical interactions like ion – dipole (5–60 kJ/mol), dipole – dipole by electrostatic attraction. This is why optimum pH for MB uptake can
(0.5–15 kJ/mol), ion – induced dipole (0.4–4 kJ/mol), dipole – induced sometimes go as high as 10–11. However, the isoelectric point is
dipole (0.4–4 kJ/mol) and dispersion (4–40 kJ/mol) interactions are dependent on the nature of the adsorbent material hence pH effects is
also possible. Based on the nature of the polymer, it could possess an usually not similar for all adsorbents.
energetically homogenous or heterogeneous surface. These will affect π-π interactions are induced by the stacking effect of electron-rich
the nature of bond energy and the energetically heterogeneous surface regions of the benzene ring on the adsorbent with those on the adsor
might allow stronger chemical interactions first followed by weaker bate. This is possible for MB because it has three benzene rings, albeit
interactions on the successive layers of the multilayer. Hence covalent with two carbons substituted at the ‘para’ positions of the middle ring
(200–800 kJ/mol) and ionic (40–400 kJ/mol) interactions or complexes (see Fig. 6). Adsorbents from clays, minerals and some types of poly
could form the first layer of uptake before successive layers by physical meric materials might not be able to interact with MB by this mecha
mechanisms. nism. Biochar and activated carbons with high aromaticity will favour
uptake by the mechanism. The aromaticity of the biochar is usually
5. Discussions on the mechanism of MB adsorption elucidated by lower values of the H/C atomic ratio [582]. The H/C
values very close to 1 indicate high aromaticity as benzene has a H/C
In this section, the mechanism of MB adsorption is elaborated. The ratio of 1. The presence of electronegative heteroatoms like nitrogen and
discussion will proceed with a focus on the MB molecule and how the sulphur on the MB structure could also facilitate hydrogen bonds. This is
nature of the adsorbent will influence the mechanism of uptake. Elec possible when the adsorbent surface possesses functional groups with
trostatic interaction between the adsorbent and MB depends on the so hydrogen atoms (Fig. 6). Hence, it can be surmised that electrostatic
lution pH. The acid dissociation constant of MB is 3.14 [580]. This is the attraction, π-π interactions and hydrogen bonds are the most important
pH value above which the dye will exist in its cationic (positively chemical mechanisms of MB adsorption [583].
charged) form in solution. In the pH regime > 3.14, the possibility of It is very difficult to notice the hydrophobic effect during MB uptake
electrostatic attraction with a negatively charged adsorbent surface or due to its very high solubility. MB as a solubility of 43,600 mg/L at 25 ◦ C
repulsion against a positively charged surface is significant. The net [580]. Only compounds with lower solubility get this advantage during
8
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 5
Adsorption performance of MB by class E adsorbents.
Adsorbent name Highest RE qmax (mg/ pH Temp Method of qmax SSA (m2/ Ref.
% g) (◦ C) determination g)
9
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 6
Adsorption performance of MB by class F adsorbents.
Adsorbent name Highest RE% qmax (mg/g) pH Temp (◦ C) Method of qmax determination SSA (m2/g) Ref.
10
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 7
Adsorption performance of MB by class G adsorbents.
Adsorbent name Adsorbent Highest RE qmax (mg/ pH Temp Method of qmax SSA (m2/ Ref.
class % g) (◦ C) determination g)
Chitosan/biosorbent from rice husk G(E-A) 98.0 4955 6.0 33.0 Langmuir – [425]
Modified sodium alginate/TiO2 G(E-F) 100 2257 – 25.0 Langmuir – [426]
Starch/Rice husk ash G(A-B) 96.9 2225 6.0 33.0 Langmuir – [427]
β-cyclodextrin/chitosan/graphene oxide G(D-E) – 2180 12 55.0 Langmuir 17.60 [428]
Chitosan-g-poly(acrylic acid)/nanocellulose G(E-F) 98.0 2037 6.0 25.0 Langmuir – [429]
Bentonite/alginate G(D-E) – 2024 7.0 25.0 Langmuir 31.80 [430]
Gelatin/alginate G(E-E) – 1937 6.0 25.0 Langmuir 14.90 [431]
Chitosan/congo red G(E-E) 99.7 1457 6.5 25.0 Experiments – [432]
Gum ghatti/Ti2O G(E-F) 98.0 1451 7.0 45.0 Langmuir 1.120 [433]
Graphene oxide/Fe3O4 G(F-F) 99.6 1429 9.0 – Langmuir 84.60 [434]
Zeolite/AC G(E-B) 83.0 1398 – 25.0 Langmuir 378.0 [435]
Alginate/Bentonite G(E-D) 96.3 1309 6.5 25.0 Langmuir 11.00 [436]
Chitin/ZSM-5 zeolite G(E-E) 86.6 1217 – 55 Langmuir – [437]
Biochar from bamboo/calcium alginate G(C-E) 91.0 1211 5.0 25.0 Langmuir 298.0 [238]
Graphene oxide/lignin G(F-E) 99.3 1210 7.0 40.0 Langmuir 41.50 [438]
MWCNTs/alginate G(F-E) 91.0 1189 – 22.0 Langmuir 86.60 [312]
Chitosan/graphene oxide/lignosulfonate G(E-F-E) 99.0 1080 7.0 50.0 Langmuir – [439]
Amino-iron/Graphene oxide G(E-F) – 1047 12 25.0 Langmuir – [440]
Cellulose/lignin from Nerium oleander G(E-E) 96.0 1000 6.0 55.0 Langmuir – [441]
Cellulose/lignin from Populus tremula G(E-E) – 1000 6.0 55.0 Langmuir – [441]
Graphene oxide/ Nickel G(E-F) 94.6 946.1 8.3 45 Experiments – [442]
Magnetic alginate/ MWCNTs G(E-F) 99.5 905.5 – 25.0 Langmuir – [443]
Maghemite/Alginate/MWCNTs G(E-F) – 905.5 – 25.0 Langmuir – [383]
Biochar from banana peel/ FeSO4 G(C-D) – 862.0 6.0 40.0 Langmuir – [444]
Reduced graphene oxide/TiO2 G(F-F) – 847.5 10.8 55.0 Langmuir – [445]
Graphene oxide/MgO G(E-F) 92.0 833.0 11 – Langmuir – [411]
Xanthan grafted acrylic/graphene oxide G(E-F) 99.5 793.7 5.0 25.0 Langmuir – [446]
Hectorite/alginate G(D-E) 99.0 785.5 12 25.0 Langmuir 205.0 [447]
Polyvinyl alcohol/sodium alginate/graphene oxide G(E-E-F) – 759.3 – 25.0 Experiments 19.70 [448]
Polyamine/graphene oxide G(E-F) 99.0 740.7 5.9 45.0 Langmuir – [449]
Graphene Oxide/Hydrogel G(F-E) – 714.3 7.0 – Langmuir 33.00 [450]
Halloysite/Fe3O4 G(D-F) – 714.3 10 45.0 Langmuir – [451]
Tannic acid/graphene G(E-F) – 714.0 – 25.0 Langmuir 196.0 [452]
SDS/ZnFe2O4 G(E-F) – 699.3 12 15.0 Experiments 55.20 [453]
SiO2 – Polydopamine-cysteamine hydrochloride G(E-E) – 688.9 7.0 25.0 Langmuir – [454]
Commercial AC/AgCl G(B-F) 96.0 666.7 7.0 25.0 Langmuir 99.40 [455]
Graphene oxide/ĸ-carrageenan G(E-A) – 658.4 5.2 25.0 Langmuir – [456]
Agar/Graphene oxide aerogel G(E-E) – 578.0 6.0 40.0 Langmuir – [457]
Cellulose/polyurethane G(A-E) 97.0 554.8 – – Langmuir – [458]
WOx/Carbon nanowires G(E-F) 550.7 7.0 25.0 Langmuir 82.50 [310]
Montmorillonite Nanosheets/Chitosan G(E-F) – 538.0 – 45.0 Langmuir – [459]
Fe3O4/SiO2/chitosan/graphene oxide G(F-F-E-F) – 529.1 10 – Langmuir – [460]
CMC/ Dextran sulphate G(E-E) 98.0 526.3 7.0 25.0 Langmuir – [461]
Cellulose/SiO2 G(E-F) – 526.0 7.0 – Langmuir – [462]
Xanthan grafted acrylic acid/MWCNT G(E-F) 99.6 521.0 6.0 30.0 Langmuir – [463]
Magnetic biosorbent/SiO2 G(A-D) 99.0 516.9 7.0 25.0 Langmuir 276.0 [464]
Biochar/SDS G(C-F) – 503.0 7.0 25.0 Langmuir 85.60 [465]
Ball-milling biochar/Fe3O4 G(C-F) – 500.5 – – Langmuir 90.60 [195]
Cyanobacteria/Polypropylene G(A-E) – 490.0 – – Experiments 2811 [466]
MoS2 nanosheets/graphene G(E-F) – 485.4 7.0 25.0 Langmuir 4.300 [467]
Cellulose/Graphene oxide fibres G(E-E) – 480.8 6.0 45.0 Langmuir – [468]
Reduced graphene oxide/TiO2 G(F-F) – 467.6 10.8 55.0 Langmuir – [445]
Fe3O4 NPs/Sodium alginate/AC G(C-D-F) 89.5 465.1 7.0 25.0 Langmuir 183.6 [469]
AC from coconut/CuO G(B-F) 99.3 464.2 9.0 45.0 Sips 262.3 [470]
Fe3O4/polyglycerol G(F-E) – 458.7 7.0 25.0 Langmuir – [471]
Polyaniline/TiO2 G(E-F) 99.0 458.1 – 25.0 Experiments 11.89 [472]
Modified carbon quantum dots/silica G(F-F) 97.0 454.5 7.0 40.0 Langmuir – [473]
Cellulose/soy protein G(E-E) – 454.0 8.0 – Langmuir – [474]
Sodium alginate/γ- Fe2O3 G(E-F) – 438.6 – 25.0 Langmuir – [383]
Polyacrylamide/graphene oxide G(E-F) – 429.2 8.0 40.0 Langmuir – [475]
Magnesium silicate/AC G(F-B) – 418.4 5.3 45.0 Langmuir 55.86 [476]
Corn straw core/graphene oxide G(A-D) – 414.0 12 25.0 Experiments – [477]
Layered double hydroxide (MgAl)/Biochar G(D-C) 95.0 406.5 12 40.0 Langmuir 46.43 [478]
Tannin from persimmon/graphene oxide G(E-F) 98.0 404.9 8.0 50.0 Langmuir 8.110 [479]
AC/Cu G(B-F) – 373.0 7.0 50.0 Langmuir 1534 [480]
Montmorillonite/MnO2 nanosheets G(D-F) 97.7 363.6 2.0 – Langmuir 63.64 [481]
Graphene oxide/chitosan/Cu-MOF G(F-E-F) 96.0 357.2 7.0 – Langmuir 947.3 [482]
Magnetic alginate/Rice husk G(A-E) 89.0 344.0 – – Langmuir – [483]
Graphene oxide/MgO G(D-F) – 333.0 11 – Langmuir – [411]
Fe2O3/MOF G(G-E) 94.6 325.6 8.9 45.0 Langmuir 197.8 [484]
Fe2O3/graphene oxide coated corn straw/citric acid G(A-E-F) – 315.5 12 25.0 Experiments 50.74 [485]
Fe2O3/graphene oxide G(E-F) – 306.5 9.0 25.0 Langmuir – [385]
Ball-milling biochar/Fe3O4/AC G(B-C-F) 100 304.2 – – Langmuir 75.40 [195]
(continued on next page)
11
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 7 (continued )
Adsorbent name Adsorbent Highest RE qmax (mg/ pH Temp Method of qmax SSA (m2/ Ref.
class % g) (◦ C) determination g)
12
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Table 7 (continued )
Adsorbent name Adsorbent Highest RE qmax (mg/ pH Temp Method of qmax SSA (m2/ Ref.
class % g) (◦ C) determination g)
Biochar from reed/Tannic acid G(C-E) – 77.35 8.0 25.0 Sips 37.50 [248]
Red mud/sucrose based carbon G(A-D) – 76.92 11 – Langmuir 105.1 [536]
Polyamide/vermiculite G(D-E) 99.0 76.42 10 – Langmuir 12.30 [537]
Dextrin-g-poly m-phenylenediamine/ Graphene G(E-E) > 98.0 76.33 8.0 25.0 Langmuir – [538]
oxide
Fe/bentonite G(F-D) – 74.07 6.0 50.0 Langmuir 305.4 [539]
Polyacrylonitrile based AC nanofibers G(B-E) 85.0 72.46 – – Langmuir – [540]
AC from coconut leaves/FeCl3 G(B-F) 74.9 66.00 5.6 30.0 Langmuir – [541]
Poly(trimesoyl chloride-melamine)/Palygorskite G(D-E) 100 64.50 – 25.0 Langmuir 45.00 [542]
Modified Fe3O4/SiO2 G(F-F) – 63.99 11 25.0 Langmuir – [543]
AC/ Fe3O4 G(B-F) – 62.80 10.8 – Experiments – [544]
Lignin/silica G(A-E) 99.0 59.88 – 25 Langmuir 74.00 [545]
Nigella sativa/Fe2O3/SnO2 G(A-F-F) 98.0 58.82 7.0 27.0 Langmuir – [546]
Zn-MOF/Fe3O4/SiO2 G(F-F-F) 99.0 58.67 – – Langmuir – [547]
BiOBr/Bi2MoO6 G(F-F) 99.5 58.01 2.0 30.0 Experiments 55.57 [548]
Tannin/Cellulose G(E-E) 95.0 57.54 8.0 30.0 Langmuir – [549]
Sodium alginate/Almond peanut oil G(A-E) 90.0 57.14 6.0 45.0 Langmuir – [550]
Zeolite/ Nickel ferrite/Sodium Alginate G(A-E) – 54.05 5.0 25.0 Experiments 219.1 [551]
Fe3O4 modified Clinoptilolite G(F-E) 99.9 52.00 9.0 25.0 Langmuir – [350]
Fe2O3 NPs/Biochar from paper sludge G(C-F) 99.0 50.00 12 – Langmuir 15.30 [250,
248]
Cornstalk-based hydrogel G(A-D) 99.7 49.01 – 30.0 Experiments – [552]
Fe3O4/poly(cyclotriphosphazene-co-4,4′ - G(F-E) – 47.89 7.0 35.0 Langmuir 80.55 [553]
sulfonyldiphenol)
Biosorbent from cotton/MnOx G(A-F) 96.0 46.30 6.9 25.0 Langmuir – [554]
Biochar from mango peel/Fe2O3 G(C-F) 95.0 46.30 7.0 – Langmuir 831.5 [555]
Magadiite/chitosan G(E-E) – 45.25 4.5 30.0 Langmuir – [556]
Magnetic clinoptilolite/chitosan/EDTA G(E-F) 99.4 44.44 5.5 31.0 Langmuir – [557]
Graphene oxide/MnFe2O4 G(E-F) 60.1 42.20 10 – Langmuir – [533]
Chitosan/sepiolite G(E-D) – 40.99 9.0 30.0 Langmuir 45.46 [558]
Polydopamine/graphene oxide/kaolin G(D-E) 97.3 39.66 – – Langmuir 35.35 [559]
Activated lignin-chitosan pellets G(E-E) 87.7 36.25 7.0 20.0 Langmuir 80.77 [560]
Bentonite/zeolite G(D-E) 94.0 36.23 5.0 – Langmuir 512.0 [561]
Polyurethane foam/Polydopamine/CNT G(E-E-F) – 32.00 – 25.00 Langmuir – [156]
Lignin/chitosan G(E-E) – 30.25 – – Experiments – [562]
Graphene oxide/chitosan/Fe3O4 G(F-E-F) 100 30.10 10.5 – Langmuir – [563]
Polydopamine/kaolin G(D-E) 84.3 28.41 – – Langmuir 8.620 [559]
Graphene oxide/Kaolin G(D-E) 92.0 28.01 7.0 – Langmuir 24.92 [564]
Graphene oxide/TiO2 G(F-F) 100 26.30 6.8 25.0 Langmuir 239.2 [565]
TiO2/Carbon G(F-F) – 25.73 6.0 55.0 Langmuir 67.22 [566]
Shrimp waste chitosan/Zeolite G(A-E) 84.9 24.51 9.0 – Langmuir – [567]
NZVI/ZSM-5 zeolite G(E-F) – 20.68 7.0 – Langmuir 116.0 [532]
Polyaniline/ZnO/Seaweed G(E-F-A) 92.0 20.55 7.0 25.0 Langmuir 30.68 [568]
Fe3O4/Chitosan G(F-E) – 20.41 12 – Langmuir – [569]
Cellulose/ZnO/biochar from bamboo G(E-F-C) 80.7 17.01 – – Langmuir – [570]
CMC/k-carrageenan/activated montmorillonite G(D-A) 92.0 12.25 6.0 30.0 Experiments – [571]
Membrane from Electrospun nanofibers/ZnO NPs G(E-E-F) – 11.64 – 45 Langmuir – [572]
Membrane from Electrospun nanofibers G(E-E) – 10.22 – 45 Langmuir – [572]
Polyurethane foam/Polydopamine G(E-E) – 10.00 – 25.00 Langmuir – [156]
Modified MWCNTs/polyacrylonitrile G(F-E) 80.0 9.580 10 25.0 Scatchard – [573]
Porous PVA/Zn-Fe-Mn oxide G(E-F) – 7.750 – – Langmuir – [574]
Co-Zn/ Fe2O3 G(F-F) – 3.400 – – Langmuir – [575]
Graphene/alginate beads G(E-F) – 2.300 8.0 25.0 Langmuir 37.60 [576]
Graphene/alginate beads G(E-F) – 1.800 8.0 25.0 Langmuir 3.400 [576]
Modified Zn-MOF/graphene oxide G(F-F) 97.0 – – 30.0 – – [577]
Alginate/pandan G(E-A) 61.0 – 5.0 27.0 – – [578]
Clay/polyethylene G(D-E) – – 9.0 55.0 – 154.7 [579]
their removal. The lessened solubility makes the molecules more hy 6. Future perspectives
drophobic and gives them more affinity for the solid phase (the adsor
bent material). This makes it easier for the adsorbate to overcome the The analysis presented in this study has led to some important
mass transfer limitation at the solid-liquid interphase. Depending on the findings. In this section, we discuss the wider implications of these
nature and functionality of the adsorbent, complexes can be formed with findings for researchers on MB adsorption and the positive consequences
MB to facilitate its uptake. These discussions reveal that the nature of the on sustainable water resource management and environmental protec
adsorbent material is one of the most important criteria that determine tion. Having observed that polymers, resins and composites adsorbents
MB adsorptive interactions and its eventual uptake capacity. This there (majorly with polymeric constituents) have especially high capacities
justifies the need for an empirical investigation such as this to help for MB uptake, the onus is now on the environmental engineering
analyse the literature and identify the best adsorbent class. research community to focus their effort on these adsorbents classes and
develop even better adsorbent materials for the current application.
Adsorbents can be improved in a variety of ways besides their
adsorption capacity. It is important to improve its affinity (sometimes
13
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
Fig. 3. The volume of research output for each adsorbent class (in the past 5 years).
Fig. 4. Frequency of constituent classes utilised in composite adsorbents (in the past 5 years).
Table 8
Analysis of research data (The ranking of each descriptor is stated in the
parenthesis next to the numerical value. Ranking was done in decreasing order).
Class Name Mean Median % with qmax
(mg/g) (mg/g) > 1000 mg/g
14
K.O. Iwuozor et al. Journal of Environmental Chemical Engineering 9 (2021) 105658
termed selectivity) so that MB can compete favourably with other spe physico-chemical interactions based on the nature of the parent
cies in aqueous media. Real adsorbent applications usually encounter a polymer.
multi-component aqueous phase [584,585]. These intricacies are usu
ally not captured by batch adsorption experiments (and by consequence Compliance with ethical standards
the adsorption capacity values) where standard MB solutions are syn
thesised. There might be some adsorbate species that could hamper MB This article does not contain any studies involving human or animal
uptake and drastically reduce its uptake capacity [586]. This is why subjects.
investigations on more selective and higher affinity adsorbent for MB is
required. Funding
For industrial applications, packed columns can be used for
adsorption purposes [587,588]. They are also used as a final treatment There was no external funding for the study.
phase for polluted water before environmental release [589,590]. The
MB desorption from these high-performance adsorbents (polymers, CRediT authorship contribution statement
resins and composites) should be an important consideration aside from
the adsorption capacity. Good regeneration ability suggests that it can Kingsley O. Iwuozor: Conceptualization, Data curation, Methodol
be used efficiently in these columns. ogy, Writing - review & editing, Validation. Joshua O. Ighalo:
Conceptualization, Methodology, Investigation, Writing - original draft,
7. Conclusion Writing - review & editing, Supervision, Validation, Project adminis
tration. Lawal Adewale Ogunfowora: Data curation. Writing - review
In this study, the performance of various classes of adsorbent for the & editing, Validation. Adewale George Adeniyi: Writing - review &
removal of MB from aqueous media was analysed. Several important editing, Validation. Chinenye Adaobi Igwegbe: Writing - review &
conclusions were drawn from the study. Composites adsorbents (31%), editing, Validation.
are the most frequently studied for MB uptake. Other popularly used
types are biosorbents (16%) and activated carbon (16%). Though Declaration of Competing Interest
composites are the most utilised, polymers and resins (E), and organic
and inorganic nanoparticles (F) are the more favoured constituents for The authors declare that there are no conflicts of interest.
composite adsorbent development. For similar data indices, composite
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