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Comprehensive systematic review and meta-analysis of dyes adsorption by carbon-

based adsorbent materials: Classification and analysis of last decade studies

Ali Azari, Ramin Nabizadeh, Simin Nasseri, Amir Hossein Mahvi, Ali Reza
Mesdaghinia

PII: S0045-6535(20)30431-8
DOI: https://doi.org/10.1016/j.chemosphere.2020.126238
Reference: CHEM 126238

To appear in: ECSN

Received Date: 30 December 2019

Revised Date: 9 February 2020
Accepted Date: 14 February 2020

Please cite this article as: Azari, A., Nabizadeh, R., Nasseri, S., Mahvi, A.H., Mesdaghinia, A.R.,
Comprehensive systematic review and meta-analysis of dyes adsorption by carbon-based adsorbent
materials: Classification and analysis of last decade studies, Chemosphere (2020), doi: https://
doi.org/10.1016/j.chemosphere.2020.126238.

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1 Comprehensive systematic review and meta-analysis of dyes adsorption by

2 carbon-based adsorbent materials: Classification and analysis of last decade

3 studies

4 Ali Azari 1, Ramin Nabizadeh *1,2, Simin Nasseri 1, Amir Hossein Mahvi 1, Ali Reza Mesdaghinia 1
5
1
6 Department of Environmental Health Engineering, School of Public Health, Tehran University of
7 Medical Sciences, Tehran, Iran
2
8 Center for Air Pollution Research (CAPR), Institute for Environmental Research (IER), Tehran
9 University of Medical Sciences, Tehran, Iran
10

11 Correspondence to: Ramin Nabizadeh, Department of Environmental Health Engineering, Floor

12 Number 5, Ghods Avenue, Enghelab Street, Enghelab Square, P.O. Box, 14155-6446, Tehran, Iran.

13 E-mail addresses: rnabizadeh@gmail.com, rnabizadeh@tums.ac.ir

14

1
15 Abstract

16 Carbon-based materials and their modifications have received significant attention over the last decades
17 given the outstanding adsorption behavior toward various dyes from aqueous solutions. In this systematic
18 review and meta-analysis, the adsorption capability of dyes on carbon-based adsorbent materials
19 (CBAMs) has been compiled. Further, the effects of process variables i.e., pH, adsorbent dosage, contact
20 time, and initial concentration), adsorption kinetics, and isotherms were investigated while considering
21 the classification of different groups of dyes and adsorbents.

22 The Metafor package provides functions for conducting meta-analyses in R software. Electronic
23 databases, including PubMed, Web of Science, and Scopus were systematically searched based on
24 Medical Subject Headings (MeSH) from January 1, 2009 to May 1, 2018. The following parameters were
25 evaluated according to predetermined inclusion and exclusion criteria.

26 After detailed screening and analysis, 835 articles were eligible for the review section. Among them, 87
27 studies met all quantitative criteria for the meta-analysis. The meta-analysis was performed using a
28 random-effects model with a high heterogeneity (I2 = 99.99%). According to the evidence, basic dyes
29 with n= 661 (~50%) and powder activated carbon (PAC) sorbent with n= 752 (~57%) have received the
30 most attention among researchers. The results revealed that the mean of removal efficiency-based dyes
31 classification was between 79.9 and 93.7 % and the adsorption capacity was lied within the range of 76.8
32 to 303.6 mg/g. Meanwhile, the maximum adsorption capacity belongs to graphene families with Qm> 320
33 mg/g, while the minimum Qm was related to G and GAC with capacities of 108.5 and 110.7 mg/g,
34 respectively. Pseudo-second-order kinetic model with 88.7% and Langmuir isotherm with 74% had the
35 best fitting with the data studied. Baujat plot revealed that two studies (ID: 75 and 12) had the minimum
36 influence on adsorption capacity with the highest dffits and cook's distance. According to the pooled data,
37 the mean adsorption capacity varied between 140.90 and 208.25, with a mean of 174.57 mg/g across all
38 studies. The results of Egger’s test (t= 0.1332, p=0.0844) and Begg’s test (z=0.8458, p=0.3977) were not
39 statistically significant, suggesting that no potential publication bias existed.

40 Keywords: Systematic review and meta-analysis, Metafor package, Carbon-based adsorbent materials,
41 Dyes, Classification

2
42 1. Introduction
43 In the historical development of human societies, water has been one of the most important resources for
44 humans' living and development. However, water contamination has become a serious environmental
45 issue and has caused international concern in recent years, especially for various pollutants that are
46 entering aquatic systems. Contamination of ground and surface waters even at trace amounts by industrial
47 dyes is a threat to the human health and other living organisms. Synthetic dyes are widely used in
48 industries such as textile, paper manufacturing and processing, leather manufacturing, plastics, cosmetics,
49 rubber industries, printing, and dyeing (Basheer, 2018a; Pavithra and Jaikumar, 2019).

50 Literature has shown that the discharge of dyes into the environment has turned to the one of the main
51 sources of hydrosphere contamination due to their resistance and stability in aquatic environments
52 (Basheer, 2018b; Liu et al., 2019). The presence of dyes in water resources will reduce the permeability
53 of sunlight into deep areas thereby causing disturbances in photochemical and biological activities of
54 aquatic organisms (Bouazizi et al., 2017; Ali et al., 2018b). Inbreed, Liberation of colors on carbon-
55 based-water bodies reduces the photosynthetic activities and dissolved oxygen content. Further, the
56 accumulation of synthetic dyes and derivatives of their destruction in marine organisms and sediments, in
57 addition to possessing a mutagenic property, can also significantly reduce the BOD and COD levels in
58 water resources (Ali et al., 2013; Gürses et al., 2016). Given the disadvantages of the dye’s presence in
59 water resources and since more than 7000000 tons of commercial dyes (over 100,000 types of dyes are
60 known) are produced annually, the removal of dye pollution from wastewater is inevitable and necessary
61 (Ali et al., 2017).

62 Up to now, various methods such as ozonation, flocculation, membrane separation, aerobic or anaerobic
63 treatment, coagulation, and adsorption have been applied to remove dyes from wastewater (Dos Santos et
64 al., 2007; Singh and Arora, 2011; Verma et al., 2012). Among the variety of techniques used, adsorption
65 has been recognized as a promising and effective method for wastewater treatment containing dye
66 pollutants due to its simplicity of operation, low cost, easy regeneration, sludge-free operation, and not
67 producing harmful and dangerous final or intermediate products (Crini, 2006; Liu et al., 2015b; Burakova
68 et al., 2018). Nevertheless, in the adsorption process, development of good adsorbents remains a major
69 challenge for researchers. Activated carbon is usually a good and effective option for dye removal
70 because of high specific surface area, as well as high porosity and adsorption capacity. Nonetheless, the
71 high cost, difficult separation after the purification process, and the low regeneration rate have reduced
72 the applications of this substance (El Qada et al., 2008; Saleem et al., 2019). Thus, to provide a stable, re-
73 generable, cost effective and highly efficient sorbent, some researchers have recently focused on

3
 74 developing carbon-based adsorbents (CBAs) i.e. Carbon Nano Tubes (MWCNT and SWCNT), Graphene
75 (G, GO, rGO), Granular Activated Carbon (GAC), and their modifications.

76 So far, carbon-derived adsorbents have been intensively studied as a potential material to removal of dyes
77 in original papers. Even, over the recent years can see that the review articles published about the
78 application of this family of materials in the dyes containing wastewater treatment (Singh et al., 2003;
79 Hadi et al., 2015). However, very few studies (perhaps no studies) can be found that have
80 comprehensively examined the adsorption of all dyes by CBAs over the last 10 years. Indeed, the
81 available review studies have considered one type of dye and/or absorbent, which will not be
82 comprehensive and complete. For example, Gupta et al. (Gupta et al., 2013) summarized the application
83 of various carbon nanotube adsorbents (such as SWCNTs, MWCNTs, and their modifications) for dye
84 removal from contaminated water. K Zare et al. compared the adsorption capacity between CNTs and
85 activated carbon as adsorbents for removal of noxious synthetic dyes (Zare et al., 2015). Demirbas et al.
86 (Demirbas, 2009) reviewed various agriculture-based activated carbons with chemical and physical
87 modifications for dye pollutant removal. On the other hand, it is very interesting to know that adsorption
88 of dyes by CBA materials (CBAMs) and their modifications have not been studied systematically.

89 Thus, taking into account the above-mentioned points, in this paper, we try to summarize and collect the
90 recent studies which have not already gained enough attention, and to provide an overall and systematic
91 understanding of this area. As detailed earlier, this systematic review aims to give an overview of the
92 main research on the application of CBAMs and their modifications for the adsorption of various dyes
93 from aqueous solutions, and to present some suggestions in the hope of contributing to the development
94 of this area. To achieve this purpose, the following objectives were kept in mind: to examine (a)
95 adsorption capacities and removal efficiency of dyes by CBAMs in recent decades, (b) Optimized value
96 of adsorption process parameters including pH, contact time, initial concentration, and adsorbent dosage,
97 (c) Dyes and sorbents classification based on their property, (d) Descriptive analysis of data in terms of
98 predetermined categories, (e) isotherms and kinetics of process, (f) A meta-analysis of the dye adsorption
99 by the CBAM adsorbents over the last decade. Finally, some valuable information about adsorption
100 process and the corresponding knowledge is also discussed in this paper.

101

102

4
103 2. Materials and Methods
104 2.1. Literature sources and search strategy

105 Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) guidelines was
106 employed for a systematic search of the literature. The literatures were extracted from the main electronic
107 databases i.e. PubMed, Web of Science, and Scopus between January 1, 2009, and May 1, 2018.
108 Electronic databases were systematically searched based on Medical Subject Headings (MeSH) using
109 following terms: (Activated carbon) OR (AC) OR (PAC) OR (GAC) OR (GO) OR (G) OR (CNT) OR
110 (MWCNT*) OR (SWCNTS) OR (carbon*) OR (charcoal*) OR (graphene*) OR (graphite*) OR (
111 nanotube*) OR (Coal) AND (dye remov*) OR (dye adsor*) OR (decolor*) OR (dye sorption) OR ( dye
112 biosor*)). The gray literature was investigated by the Open Grey online database. Further, the references
113 of searched studies were also reviewed to explore more relevant studies.

114

115 2.2. Inclusion and exclusion criteria

116 In the initial research, after removing duplicate papers using EndNote X9 (Bld12062, Thompson Reuter,
117 CA), based on the title assessment, some papers were excluded (Ali, 2018). Then, the abstract of the
118 remaining articles was carefully checked, and some irrelevant papers were excluded. The full texts of the
119 remaining papers were downloaded and checked to examine the final inclusion criteria. Then, the selected
120 papers were assessed carefully to determine predetermined parameters. Briefly, the eligibility assessment
121 of references was carried out based on pre-defined inclusion and exclusion criteria as follows:

122 i. The original articles were included, which were published in English language in peer-reviewed
123 journals about the removal of various dyes through different types of CBAMs, alone or in combination
124 with other compounds.
125 ii. The abstracts, books, presentations, meta-analysis, conference papers, reviews, and letters to the
126 editor about the removal of various dyes were excluded from the study.
127 iii. Further, the articles with unrelated topic, duplicate content, and manuscripts with absence or
128 inconsistency methods, evaluation criteria or results also were excluded.

129
130
131 2.3. Selection of systematic reviews and data extraction

132 After identifying potentially eligible articles, two reviewers extracted and summarized the data of the
133 researched studies independently, assessing the inclusion and exclusion criteria based on the standardized
5
134 collection. Any disagreements were resolved via discussions and consensus with a supervisor. The
135 information extracted from each included literature (using a standard data extraction form) was comprised
136 of the following items: (a) The name of author, journal, title and the year of publication; (b) type of dyes;
137 (c) the adsorbent used; factors affecting the dye adsorption including optimum amounts of (d) pH, (e)
138 contact time, (f) CBAMs dosage, (g) initial concentration, (h) adsorption kinetic; (i) adsorption isotherm
139 and (j) maximum adsorbent capacity (Qm based Langmuir equation) (Ali et al., 2018a; Ali et al., 2019c).

140
141 2.4. Assessment of methodological quality

142 As detailed earlier, we did not find any systematic reviews about adsorption of dyes by CBAMs
143 adsorbent. Thus, in the present study, a checklist consisting of 10 items was developed and used to assess
144 the methodological quality of the published papers which were included in the review. Each item in the
145 checklist was assessed by the criterion of “Yes “or “No”. The article with more than 5 “Yes” was rated as
146 high quality, yes = 5 indicated moderate quality, and studies with < 5 “yes” were considered as low
147 quality. Since the low-quality studies had high bias, then all low-quality studies were excluded from
148 present research. The quality analysis was performed by two investigators independently, for assessing
149 the risk of bias before date extraction step (See Table S1).

150
151 2.5. Meta-analysis of data

152 The articles that investigated adsorption of dyes according to the experimental design modeling (DOE) by
153 different software as well as articles with sample size available in their full-texts were considered for
154 conducting meta-analysis. The meta-analysis was performed based on the coefficient of determination,
155 study sample sizes, and adsorption capacities (mg/g) of dyes in the samples. Statistical heterogeneity was
156 tested via the quantitative tool of I2, Tau2 and Q-statistic. A heterogeneity (I2) between 25 and 50% is
157 regarded as not important, 50 and 75% is moderate, and > 75% is high. According to the Cochrane
158 Handbook (version 5.1.0), the value of I2> 50% was considered to have considerable heterogeneity. A
159 fixed effects model was conducted to pool the data which presented the respective 95% confidence
160 intervals (CI) when the heterogeneity was trivial or moderate, while a random effects model was
161 performed if there was considerable heterogeneity (Tesfamariam et al., 2018). The publication bias was
162 assessed visually by funnel plots and calculated in Egger’s test/Begg’s test through the R software,
163 version 3.6.0 (Missouri, USA). P-value < 0.05 (α = 0.05) was judged as statistically significant for the
164 results, suggesting that the study has publication bias.

6
165

166 3. Results and discussion

167 3.1. Literature search and study characteristics

168 A total of 4881 articles were preliminarily identified through literature searching in the mentioned
169 electronic databases. The flowchart of the article search and selection in the meta-analysis is presented in
170 Fig 1S. Out of them, 1496 studies were omitted for the reason of duplication. Then, 2067 publications
171 were further excluded, based on detailed screening and analysis of titles and abstract, for the following
172 reasons: unrelated to article topics, not full-text papers (only abstract published), non-English language
173 articles (only abstract was in English), systematic reviews and meta-analysis papers, and checking the
174 dyes’ adsorption in the column mode. Two independent reviewers read 1318 full-text papers and finally
175 835 studies met our inclusion criteria. Of them, 483 articles were excluded after full-text reading, because
176 of inappropriate experimental criteria, missed sufficient data, focus on simultaneous removal of dyes and
177 other pollutants, study of the biological elimination or degradation (oxidation or reduction) of the dyeing
178 agent (very little attention was paid to the dye adsorption process and the details were very flawed) and
179 irrelevant observation criteria, which seemed inconsistent with the criteria mentioned earlier. Overall, a
180 total of 835 articles were included for the review (Supplementary Excel File 1). After full-text review of
181 the remaining articles, only 92 studies met all quantitative criteria for the meta-analysis. Among them, 14
182 articles were excluded as they had insufficient quality (low quality with < 5 “yes”) to enter the meta-
183 analysis. Supplementary Excel File 2 presents the characteristics of the included meta-analysis.

184

185 3.2. Systematic review

186 3.2.1. Description of studies
187 3.2.1.1. Classification of dyes (dye types Vs. Re and Qm)

188 According to Fig. 1 (a and c) and Table 1, it can be found that over the last decades (from 2009 to 2018),
189 researchers have been studying the adsorption of 1318 dyes by CBAMs. Among them, the highest rate of
190 dye adsorption studies was related to 2017 (n=226) and the lowest one to 2009 (55 studies). Further
191 exploration indicated that the number of dyes studied has had an ascending trend over time. Furthermore,
192 in the present research, for better and more focused analysis of the results, 1318 dye species that were
193 investigated in previous studies have been classified into 7 different categories including acidic, basic,
194 reactive, disperse, direct, vat, and azo types. The evidence suggests that most researchers have focused on
195 the adsorption of basic dyes by CBAMs, while the order of other dyes was as acidic> reactive> azo>
196 direct> disperse> vat. Indeed, it can be statistically reported that more than 50% of studies have been
7
197 carried out on basic types of dyes with the total of acidic and basic colors comprising about 75% of
198 studies. Meanwhile, by analyzing the results of the 7-category classification, it can be reported that
199 Methyl Orange (MO), Methyl blue (MB), Reactive Black 5 (RB5), Disperse Blue (DB), Direct Red 23
200 (DR23), Indigo Carmine (IC) and Sunset yellow (SY) had the highest use as pollutants in their
201 classification. The mean of removal efficiency-based dyes classification was between 79.9 and 93.7 %
202 and the adsorption capacity lied within the range of 76.8 to 303.6 mg/g. The highest mean efficiency
203 (93.7 %) and adsorption capacity (303.6mg/g) were also calculated for Vat dyes and their lowest
204 associated to disperse dyes with mean efficiency of 79.9 % and adsorption capacity of 76.8 mg/g.

205
206 Fig 1.
207
208 3.2.1.2. Classification of adsorbents (sorbent types Vs. Re and Qm)

209 From 2009 to 2018, 826 types of CBMs as adsorbents have been used by researchers to extract and
210 remove dyes. The application of carbon-based adsorbent materials such as dyes has been on the rise over
211 time. In the following, CBMs adsorbents have been divided into 8 main groups (as shown in Fig. 1 (b
212 and d) and Table 1) including Graphene (Gr), Graphene Oxide (GO), Powder Activated carbon (PAC),
213 Carbon Nano Tube (MWCNT and SWCNT), Graphite (G), Coal (Co), Granular Activated Carbon
214 (GAC), and Reduced Graphene Oxide (RGO) for further studies. Interesting results were obtained.
215 Despite the development of CBMs adsorbents and synthesis of new series (generations) of this sorbent’s
216 family, powdered activated carbon has still the most usage in dye removal with a 57.1% share of total
217 sorbents. It was followed by carbon nanotubes and graphene oxide with 13.4% and 13.2% usage, while
218 GAC is the last one. Another interesting point is that the activated carbon prepared from waste claims the
219 main part of AC categories with a 65.6% share. Meanwhile, the maximum adsorption capacity belongs to
220 graphene families with Qm> 320 mg/g, while minimum of Qm was related to G and GAC with capacities
221 of 108.5 and 110.7 mg/g, respectively. The mean adsorption efficiency for carbon nanotubes, reduced
222 graphene oxide, and graphene has been very close together. On the other hand, adsorption by carbon
223 nanotubes and reduced graphene oxide with a yield of about 93.5% can be reported as the maximum
224 absorption efficiency. The granular activated carbon was the lowest with 80.6%

225

226 Table 1.
227

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228
229 3.2.2. Influence of key factors on dye adsorption

230 There are many factors affecting the dye adsorption process i.e. solution pH, contact time, adsorbent dose,
231 initial dye concentration, and temperature. Thus, the effects of the mentioned parameters and their optimi
232 zation should be examined. Optimization of conditions can help the development of industrial-scale dye tr
233 eatment process. In the next section, some of the factors affecting adsorption of dyes are discussed (Mesd
234 aghinia et al., 2017; Ali et al., 2019b).
235
236
237 3.2.2.1. pH

238 During the adsorption process, solution pH is one of the significant variables that affects the speciation of
239 dye, magnitude of electrostatic charges, degree ionization, and the surface characteristics of CBAMs
240 (Mudunkotuwa and Grassian, 2010; Al-Shaalan et al., 2019). The optimum pH in terms of various dyes
241 and sorbent types has been summarized in Supplementary Excel File 1. It was observed that the best pH
242 depends on the target dyestuff and types of CBAMs. Initial statistical analysis of the data showed that the
243 minimum and maximum pH in studies were 1 and 13, and the mean and median were 5.73 and 6,
244 respectively (1st Qu. =3, 3rd Qu. = 7.00). The pH variations (without any classification) presented in Fig.
245 2 (a and b) indicate that pH within the range of 6 to 8 was the most commonly used
246 (frequency=203+210= 413) in removing dyes during the studied years while PH> 12 had the least
247 application with only three reports.

248
249 Fig 2.
250
251
252 Generally, at low pH, the dye removal efficiency will be reduced for cationic type, while anionic dyes
253 show an inverse result (Baziar et al., 2017; Badi et al., 2018). At high pHs, the result is completely
254 different such that the conditions for cationic dye adsorption are far more favorable compared to those for
255 anionic counterparts (Ali et al., 2019a). In the present study, similar results were obtained by examining
256 the changes of pH vs. dye type’s classification. As can be seen in Fig. S2(a) and Table 2, acidic dye types
257 have a better efficiency at mean pH< 4.64, while basic types have a better performance at pH means >7.
258 In other classifications, the highest adsorption efficiency was reported at pH~ 4.62, 3.45, 4.02, 4.33, and
259 5.15 with respect to azo, direct, disperse, reactive, and vat types, respectively. Indeed, the reduction in the

9
260 positive charge in the interface layer and emergence of the negative charge on the adsorbent surface at
261 high solution pHs result in improved efficiency of cationic dye (i.e. basic types) adsorption (Nodeh et al.,
262 2016). In contrast, at a low pH, the positive charge on the solution interface will growth and induced into
263 the absorbent surface, which will lead to an increase in anionic dye (i.e. acidic types) adsorption and a
264 decline in cationic dye adsorption (Nodeh et al., 2016). The interesting point in Table 2 is that in all dye
265 classification, acidic conditions offered better removal efficiency except for the basic type.

266 Some researchers studied the effect of solution pH on the adsorption of cationic dye i.e. Acid red 88,
267 Congo red, Acid brilliant scarlet, Methyl orange and Acid red 183 by magnetic 3D graphene
268 aerogel/CaCO3, starch derived zinc carbon foam-like, chemical preparation of crab shell-based activated
269 carbon (AC-KOH), CNT@NiCo2O4, Organic carbon aerogels (CAs) ((Arsalani et al., 2018) They
270 observed that at alkaline pH, the efficiency and adsorption capacity were maximum. Elsewhere, other
271 studies ((Chang et al., 2010), (Othman et al., 2018), (Chen et al., 2018), (Sahu et al., 2017), and (Xiao et
272 al., 2016)), measured the adsorption capacity of Crystal violet, Methylene blue, Malachite green,
273 Rhodamine B , Neutral red as part of the anionic dyes onto the Starch-derived carbon aerogels, Magnetic
274 graphene oxide, Carbon material based on quinoa husk, ORMOSIL-Fe3O4-RGO, and L-Cysteine reduced
275 graphene oxide (RGO-Cys). They reported that by increasing the pH from acidic to alkali, the adsorption
276 capacity diminished dramatically.

277

278 Table 2.
279
280 Fig. S2(b) presents the variations in pH vs. sorbent types’ classification. The results reveal that all of the
281 8 adsorbents outperformed at pH between 5.1 and 6.7 (acidic range). The isoelectric point (pHIEP) or
282 point of zero charge (pHpzc) terms are frequently used in the dye adsorption process. The pHpzc is one of
283 the important parameters of pH sensitive sorbents, which determines the linear range of pH sensitivity and
284 allows assumptions to be made about types of surface-active centers and adsorption abilities of
285 surfaces. The pHpzc of the sample was measured using the pH drift method. For this purpose, the pH of the
286 solution was adjusted within different ranges by adding HCl or NaOH. Then, a fixed amount of adsorbent
287 should be added to the solutions. Once the pH had stabilized (shaken until equilibrium usually 24 hours),
288 the final pH was recorded. The plot of final pH versus initial pH was used to determine the point, where
289 pHpzc is the point when pH initial=pH final. Indeed, many researchers have focused on the pHpzc of CBAMs
290 adsorbents to better understand the adsorption mechanism between the adsorbent and adsorbate. The
291 general rule about pHpzc; (a) at pH> pHpzc, cationic dye adsorption is more favorable, due to presence of
10
292 functional groups such as OH-, COO- groups; and (b) at pH> pHpzc, anionic dye adsorption is favored
293 where the surface becomes positively charged.

294 Sivarajasekar et al. reviewed the adsorption of cationic dyes onto agriculture waste biomass. They found
295 that their zero point of charge was about 4, while the maximum adsorption capacity observed at pH was
296 more than 6, i.e. pH> pHpzc (Sivarajasekar and Baskar, 2015). As can be seen, the results for the anionic
297 dyes are completely different, where the maximum capacity of Brilliant Yellow and Congo red onto the
298 sepiolite and Indian Jujuba seeds were obtained at pH 6–7 and 2 and the calculated pHpzc was 7.4 and 11,
299 respectively (Bingol et al., 2010; Reddy et al., 2012). In simple terms, the best performance for anionic
300 dyes adsorption occurred at pHpzc greater than the solution pH.

301
302 3.2.2.2. Initial concentration
303 Initial dye concentration is another important parameter in the adsorption process. The initial
304 concentration can play a significant role in the removal of dyes by affecting the active sites and/or
305 available binding sites of the adsorbent surface (Ali and Aboul-Enein, 2002; Nodeh et al., 2016). The
306 distribution and effect of the dye concentration (without any category and the overall look) on the
307 adsorption process is shown in Fig. 3(a-c). The minimum, 1st Qu., median, mean, 3rd Qu. and maximum
308 range of the initial dye concentration were 0.2, 20, 50, 140, 105, and 2100 mg/L, respectively. Almost the
309 majority of investigations have focused on the initial concentration variations within the range of 100 to
310 200 mg/L. By plotting the initial dye concentration distribution against Qm parameter, the mean optimum
311 capacity for dye adsorption can be seen on the CBAMs= 203.48 mg/g within the measured ranges of the
312 dye concentration.

313

314 Fig 3.
315
316 Generally, increase in the initial concentration of dyes is associated with a decline in the removal
317 efficiency (Ali et al., 2005). The lower uptake (adsorption percentage) at higher concentrations arises
318 from an increased ratio of initial adsorption number of dye molecules vs. the available surface area; hence
319 fractional becomes dependent on the initial concentration (Ali et al., 2005). At a low concentration, there
320 are sufficient unoccupied active sites on the adsorbent surface to absorb the dyes, which will saturate with
321 their concentration elevation. This causes lack of the active sites required for adsorption of the dye
322 molecules. On the other hand, the initial dye concentration provides an important driving force to

11
323 overcome the mass transfer resistance of the dye between the aqueous and solid phases. Thus, at higher
324 initial dye concentrations, the number of ions competing for the available sites on the surface of adsorbent
325 is high, thus causing higher dye adsorption capacity (loading capacity of the adsorbent). Here, by
326 analyzing the dataset related to the concentration of the dyes in the Supplementary Excel File 1 and
327 accuracy on the red line in Fig. 3(c) (indicating the change trend), it can be concluded that the adsorption
328 capacity grows with increasing the concentration of pollutants (dyeing agents) about 3 times of the
329 obtained mean. Plotting the initial dye concentration values against different dye classes (see Fig. S3(a)
330 and Table 3) respectively showed that the optimum concentrations for acidic, azo, basic, direct, disperse,
331 reactive, and vat dye types were 155.3, 99.13, 132.41, 75.72, 48.92, 207.21, and 102.75 mg/L
332 respectively. Concerning CBAMs, the ideal dye concentrations were 160.94, 123.70, 131.39, 140, 92.41,
333 109.26, 61.39, and 122.87 mg/L for PAC, CNT, Co, GAC, Gr, GO, G and RGO types respectively (Fig.
334 S3(b) and Table 3).

335 In studies on the adsorption of methylene blue (MB) as a representative of cationic dyes by Graphene
336 oxide reinforced alginate/PVA double network hydrogels (Liu et al., 2018), mesoporous carbon from
337 peach stones (Álvarez-Torrellas et al., 2016), and montmorillonite-pillared graphene oxide (Liu et al.,
338 2015a) at a pre-determined (fixed) adsorbent dose, contact time, temperature, and pH, the adsorption
339 capacity increased from 23.09 mg/g to 313.09 mg/g , 29 to 239 mg/g, and 123 to 345 mg/g when MB
340 concentrations were elevated from 20 to 200 mg/L, 25 to 200 mg/L, and 50 to 350 mg/L. However, in all
341 the mentioned studies, the percentage of dye removal declined dramatically from ≥ 95% to ≤ 45%.
342 Similar results were obtained for anionic dyes. For example, Jin (Jin et al., 2018) and Geyikçi (Geyikçi,
343 2013) et al. examined the adsorption of Congo red and Acid Blue 161 by Ni/PC-CNT and MWCNTs.
344 They reported that an increase in the concentration from 25 to 200 mg/L and 10 to 200 mg/L resulted in
345 enhanced capacity from 72 to 818 mg/g and 456 to 1000 mg/g.

346

347 Table 3.
348
349 3.2.2.3. Adsorbent dosage

350 Enhanced interaction and contact between the dyes and adsorption sites can improve the efficiency and ef
351 fectiveness of the adsorbent. According to the data, over the last 10 years, the adsorbent dosage has been
352 considered within the range of 0.002 to 30 g/L. The values of other parameters i.e. 1st Qu., median, mean,
353 and 3rd Qu. were also 0.3, 0.6, 1.69, and 1.5, respectively.

12
354
355
356
357 Fig 4.
358
359
360 The histogram and box plot of adsorbent dose vs. adsorption capacity are illustrated in Fig. 4(a and b). A
361 ccordingly, it can be reported that the dose of 0.002 to 2 g/L with the frequency of 998 times has been stu
362 died by the researchers more than other values. The dye removal efficiency (%) has increased once the do
363 sage of the adsorbent grows due to the greater accessibility of surface binding sites upon the elevated dosa
364 ge of the adsorbent. This can be explained by increasing available sites with the adsorbent dosage elevatio
365 n for the interaction with the target molecule in the solution. This culminates in enhanced removal efficie
366 ncy of the target dyes. For example, under a neutral medium, adsorption of malachite green onto multi-wa
367 lled carbon nanotubes was studied at dosages from 0.02 to 0.1 g/L under the initial concentration of 20 m
368 g/L. The results showed that the removal of MG increased from 38 to 92 % with the rise of the adsorbent
369 dose (Eksperimen, 2016). In other research, adsorption of MB (contact time = 90 min) and MV (conta
370 ct time = 120 min) onto GO was studied at the initial dye concentration = 30 mg/L. The study sugges
371 ted that with elevation of the sorbent dosage from 50 to 400 mg/L, the removal of MB and MV increased
372 from 63 to 92% and 89 to 99.5% respectively, which was attributed to the increase in the active site/dye r
373 atio (Ramesha et al., 2011). However, when nearly all the dyes in the aqueous solutions were adsorbed on
374 to the adsorbent, the number of remaining unsaturated adsorption sites increased, causing reduction of ads
375 orption capacities. The descending trend (red line) of the Qm parameter with elevation of the adsorbent d
376 ose is clearly visible in Fig. 4 (c). This decline can also be attributed to a decrease in the total adsorption s
377 urface area and increase in the diffusion path length resulting from overlapping or aggregation of adsorpti
378 on sites. In a recent study, adsorption of MB, NR, and BCB on magnetic multi-wall carbon nanotubes (MMWC
379 NTs) was explored with dosage increment from 0.3 to 0.9 g/L at pH of 7 and a contact time of 24 h. The aut
380 hors observed that the percentage of dye removal increased sharply from 30.1 to 99.16%, from 17.11 to 98.3
381 3%, and from 17.6 to 98.8% in MB, NR, and BCB, respectively upon the dosage augmentation from 0.3 to 0.9 g/
382 L and then reached a plateau. In this study, the Q (mg/g) values were 15.74 mg/g, 20.33 mg/g, and 23.55 mg/
383 g, respectively (Gong et al., 2009).
384 Evaluation of dosage changes with respect to colorants’ classification (Fig. S4(a) and Table 4) revealed t
385 hat the mean of optimum sorbent dose lied within the range of 1.28-3.91 g/L. The same analysis on the ad
386 sorbents’ classification showed that the best CBAMs dosages for PAC, CNT, Co, GAC, Gr, GO, G, and
387 RGO types were 2.176, 0.778, 2.98, 1.116, 1.441, 1.014, 1.441, 0.56, and 0.587 g/L, respectively (Fig. S4
13
388 (a)). Note that the removal of high concentrations of dyes (pollutants) by lower adsorbent content will be
389 more economical on a large and real scale, which is a great and undeniable advantage.
390
391 Table 4.
392
393 3.2.2.4. Contact time

394 In most studies, the rate of removal efficiency and dye adsorption capacity were initially fast and then dec
395 lined gradually until the sorption system reached equilibrium. The fast adsorption rate at the primary stage
396 s is attributed to the presence of vacant and abundant active sites and/or reaction sites on the adsorbents w
397 hich are occupied over time and become saturated, thereby yielding equilibrium. Based on Fig. 5 (a-b), th
398 e adsorption studies have been conducted in the period between 0.5 and 4320 minutes (1st Qu. = 30, medi
399 an= 65, mean= 264, 3rd Qu. = 240). As shown, most surveys have focused on contact time between 0 and
400 500 min with the highest frequency (n=1163). Adsorption of Malachite green (MG) by activated carbon d
401 erived from durian seed (DSAC) was investigated by Ahmad et al. (Ahmad et al., 2014). The authors foun
402 d that within the first 6 h, about 50 % of MG dye adsorption occurred. In the second part (6 h < t < 22 h), t
403 he slopes became milder resulting in an additional 20 % adsorption. In the third part (t > 22 h), the dye ads
404 orption uptake was steady and the adsorption reached equilibrium. Ahmad reported there was an initial sh
405 arp increase in the MG dye adsorption uptake due to the large number of available active sites. The gradu
406 al slower adsorption at the end is probably due to the saturation of active sites and a decline in the dye con
407 centration. Kerkez et al. studied the effects of contact time (in range 0-100 min) on the adsorption of MG
408 and RB onto the Fe3O4/MWCNT at 298 K. They observed that > 90% of total adsorption of dyes occurre
409 d within the first 80 min and then reached adsorption equilibrium. They believed that the initial part of the
410 curve signaled the rapid attachment of the dye molecules to the external surface of the adsorbent (Kerkez
411 and Bayazit, 2014). In physical adsorption, most of the adsorbate species are adsorbed within a short inter
412 val of contact time; thus, the physical adsorption of the MG and RB on Fe3O4/MWCNT was confirmed b
413 y the short time to equilibrium.
414 Fig. S5(a-b) and Table 5 present the distribution of equilibrium times in the dye and adsorbent categories
415 . Assessment of equilibrium times by considering dye classification revealed that the means of equilibriu
416 m times for basic, reactive, acidic, azo, vat, disperse, and direct types were 248.97, 314.75, 294.27, 206.0
417 5, 227.25, 319.15, and 249.88 min, respectively. Interestingly, the results are remarkably close together, w
418 ith the minimum and maximum equilibrium times being related to azo and disperse types. Contrary to the
419 results obtained from equilibrium time variations in a different dye classification, the sorbents organizatio
420 ns have very wide ranges (Gholami et al., 2014). The equilibrium times for Gr, RGO, PAC, GO, Co, CNT
14
421 , G, and GAC types were 199.81, 156.03, 327.37, 188.56, 79.57, 137.92, 111.45, and 755 min, respectivel
422 y. The higher efficiency at shorter times demonstrates a higher ability of adsorbent and justifies the econo
423 my of the used process.
424
425
426 Fig 5.
427
428
429 Table 5.
430
431 3.2.3. Adsorption kinetics and equilibrium
432 3.2.3.1. Adsorption kinetics

433 Studying the kinetics of the process by determining the mechanism of adsorption and its potential rate-lim
434 iting steps plays an important role in the design and practical application of adsorption processes. Meanw
435 hile, information on the dye’s kinetics uptake is required to select the ideal condition for full-scale batch d
436 ye removal processes (Khosravi et al., 2015; Gholami et al., 2016).
437
438
439 Fig 6.
440
441
442 The best-fitting kinetic model in batch experiments is established by linear and/or non-linear regression m
443 odels (Khosravi et al., 2018). According to studies, it can be found that pseudo-second-order (PSO), pseu
444 do-first-order (PFO), intraparticle diffusion (ID), Elovich (E), general order (GO), fractionary-order (FO),
445 Avrami fractional order (AFO), fractal (F), Paterson’s and Nernst Plank’s (PNP), and Weber-Morris (WM
446 ) models have been widely used for sorption kinetic studies. The best fit of kinetic models for adsorption
447 of various type of dyes onto CBAMs has been summarized in Fig. 6 (a). As shown in the table, more than
448 89% of studies (the bulk of studies) followed pseudo-second-order kinetic model (PSO with n=907) regar
449 dless of the type of adsorbent and adsorbate. The pseudo-second-order model assumes that chemisorption
450 may be the rate-controlling step in the adsorption processes. PSO was followed by PFO, GO, E, and ID m
451 odels.
452 Lunhong et al. (Ai and Li, 2013) applied PFO, PSO, and ID diffusion models to fit the experimental kinet
453 ic data for MB removal by carbon supported on montmorillonite clay (MMT@C). They found that the ps
454 eudo-second-order model with R2 >0.99 is suitable for characterizing the kinetic data. Halbus et al. (Halb
15
455 us et al., 2013) reported that the pseudo-second order model was more appropriate to describe the adsorpti
456 on kinetic behaviors for disperse blue dye ions onto Iraqi date palm seeds activated carbon where the che
457 misorption was the rate-controlling mechanism. In another study, the adsorption of azo reactive dye onto
458 charcoal ash was examined by Özbay et al. (Özbay et al., 2013). Pseudo-second-order kinetic model was f
459 ound to best represent the kinetic data considering closer values of experimental and calculated dye amou
460 nts adsorbed by the unit sorbent mass. For Malachite green and Safranine O adsorption onto Marine algae
461 Ulva lactuca (ULV-AC) and Systoceira stricta (SYS-AC) based activated carbons (Salima et al., 2013), th
462 e authors reported that the kinetic data followed the pseudo-second-order model with a better correlation c
463 oefficient R2> 0.99 and a higher rate constant. Ribeiro et al. (2012) used both pseudo-first-order and pseu
464 do-second-order kinetic models to fit the experimental kinetic data for Orange II (OII) and Chromotrope 2
465 R (C2R) adsorption by activated carbon xerogels at T = 303 K, sorbent dosage of 0.1 g/L, and pH = 3. Th
466 e results suggested that the experimental data were fitted better by the pseudo-second order model with R2
467 >0.998. A similar conclusion was observed in another study, where Ojedokun et al. found that the adsorpt
468 ion of Congo red by guava leaf-based activated carbon followed the pseudo-second-order kinetic equation
469 and the rate constant diminished with increasing initial dye concentrations. A diffusion kinetics study sho
470 wed that the adsorption process was controlled by more than one mechanism with the film diffusion proce
471 ss being the rate-limiting one (Ojedokun and Bello, 2017).
472
473 3.2.3.2. Adsorption equilibrium

474 The adsorption isotherm models provide valuable information about (a) distribution of available sites acro
475 ss the adsorbent surface, (b) maximum adsorption capacity of the sorbent, (c) interaction of adsorbate wit
476 h the adsorbent, and (d) the adsorbing characteristics of the system (Dargahi et al., 2015; Rezaei Kalantry
477 et al., 2016). A wide range of models have been applied to investigate experimental data and describe the
478 equilibrium of adsorption, which consist of two-parameter isotherm models i.e. Langmuir, Freundlich, Du
479 binin–Radushkevich (D–R), and Temkin; three-parameter isotherm models i.e. Redlich–Peterson, Sips, T
480 oth, and Koble–Corrigan, Khan; and multilayer physisorption isotherms i.e. Brunauer–Emmett–Teller, Fr
481 enkel–Halsey–Hill and MacMillan–Teller isotherms (Babaei et al., 2016; Jonidi Jafari et al., 2016). The s
482 ummaries of the best fit of isotherm models for adsorption of dyes using various CBAMs and their maxim
483 um adsorption capacity (Qm) are shown in Supplementary Excel File 1. Also, according to Fig. 6 (b), the L
484 angmuir followed by Freundlich isotherms have been the most popular and widely used models to describ
485 e the equilibrium of dyes by CBAMs.
486 The number of isotherms selected as the most appropriate in the last decade studies is as follows: the Lan
487 gmuir (L) = 855, Freundlich (F) = 170, Sips (S) = 26, Fritz–Schlunder (FS) = 3, Dubinin-Radushkevitch (
16
488 DR) = 1, Toth (To) = 6, Liu (Li) = 14, Langmuir-Freundlich (L-F) = 11, Vieth–Sladek (VS) = 3, Redlich-
489 Peterson (RP) = 38, Koble-Corrigan (KC) = 3 , BET (B) = 6, Guggenheim–Anderson–de Boer (G) =2 and
490 Harkins-Jura (HJ) =1. According to Langmuir isotherm assumption, surface phase is considered as a mon
491 olayer. Indeed, the Langmuir isotherm is used to describe the adsorption process where the occupancy occ
492 urs at one adsorption site within an energetically homogeneous range of adsorption sites (Jonidi Jafari et a
493 l., 2016; Rezaei Kalantary et al., 2016).
494 Zhu et al. (Zhu et al., 2014) reported that adsorption of MB and MG onto zeolite–reduced graphene oxide
495 (zeolite–rGO) followed the Langmuir model, which indicated that the adsorption mechanism followed mo
496 nolayer adsorption. They found that adsorption of dyes was favorable and the maximum adsorption capac
497 ity of methylene blue and malachite green reached 53.3 mg/g and 48.6 mg/g, respectively. Asfaram et al. (
498 2017) applied four isotherms (including Langmuir, Freundlich, Temkin and D–R models) to describe the
499 adsorption equilibrium data of brilliant green (BG) and malachite green (MG) on Mn-doped Fe3O4-nanop
500 article-loaded activated carbon. They found that at different concentrations the experimental data fitted be
501 tter (R2 > 0.996) the Langmuir models than by other models. The values of 1/n were found to be less than
502 1, while the values of RL for MG and BG were obtained to be within the ranges 0.0076–0.0574 and 0.008
503 0–0.0606, respectively, strongly supporting the favorable adsorption. Further, in the case of Disulphine Bl
504 ue (DB), adsorption of Eosin Yellow (EY) and Safranin O (SO) dyes onto a copper sulfide nanoparticle-l
505 oaded activated carbon absorbent, a higher value of correlation coefficients (R2), and the Qmax value, clo
506 ser to the Qmax (exp.), calculated by the Langmuir model, demonstrated that the monolayer Langmuir ad
507 sorption isotherm described the experiment data more precisely (Momtazan et al., 2018). Lijuan et al. (Lv
508 et al., 2018) studied the isotherm of methylene blue (MB) adsorption onto nitrogen-doped porous carbon (
509 PCM-K) composite beads. According to them, higher values of R2 and lower values of χ2 showed that the
510 adsorption process was better explained by Langmuir isotherm. The Langmuir model can also predict that
511 the maximum MB adsorption capacity of PCM-K is 769.2 mg/g, which is in excellent agreement with the
512 experimental result (766.9 mg/g). A similar trend was found in the adsorption of methyl orange (MO) and
513 methylene blue (MB) dyes onto nitrogen-doped nanoporous carbon nanospheroids (N@CNSs). The autho
514 rs reported that the isotherm data were well represented by the Langmuir model for all studied dyes (Kun
515 du et al., 2018).
516
517 3.3. Meta-analysis
518 3.3.1. Quality assessment

519 The quality and specific assessments of the studies included in the meta-analysis ranged within low, mode
520 rate, and high. All studies included in the meta-analysis were considered as having a low risk of bias (Yes
17
521 => 5). The dataset includes the basic characteristics of the studies e.g. number of studies, sample size, F-v
522 alue, P-value, R2, SS, MS, questionnaires filled with scoring (quality studies) ,and the type of method use
523 d for data modeling as provided in Supplementary Excel File 1 and Table 6. Finally, by excluding low
524 quality studies (Yes< 5), a total of 78 studies were included in the meta-analysis.
525
526
527 Table 6.
528

529 3.3.2. Heterogeneity

530 Calculating the Q-statistic, which is the ratio of observed variation to within-study variance, reveals how
531 much of the overall heterogeneity can be attributed to actual between-studies variation. The statistically si
532 gnificant Q-statistic indicates that the included studies do not share a common effect size. The related I2 st
533 atistic is a percentage that represents the proportion of observed variation that can be attributed to the actu
534 al difference between studies, rather than within-study variance. I2 thresholds with 25, 50, and 75% repres
535 ent low, moderate, and high variance, respectively. Tau2 can also be used to estimate the total degree of st
536 udy heterogeneity in models. When Tau2 is zero this is indicative of no heterogeneity. A pool of published
537 results (k=78) revealed that the effect size of Qm obtained was 174.57 (95% CI = 135.09 to 214.05, p < 0.
538 001). According to Table 7, I2 in terms of pooled adsorption capacity data was 99.99 % (95% CI: 99.999-
539 100.00) representing high variance between studies. This indicates that ~ 100% of variation reflected actu
540 al differences in the population mean. Meanwhile, Q-statistic and Tau2 were obtained as 98069.55 (p =< 0
541 .0001) and 31646.40 (95% CI: 23621.72- 44610.49) for the adsorption capacity. The available evidence cl
542 early shows very high heterogeneity found across studies.
543
544
545 Table 7.
546
547
548 The Q-statistic and I2 can provide evidence for heterogeneity, though they do not provide information on
549 which studies may be influencing the overall heterogeneity. Thus, construction of a Bajaut plot can illustr
550 ate studies that contribute to overall heterogeneity and the overall result. The Bajaut plot for Qm (sorption
551 capacity, mg/g) based study IDs are as follows:
552
553
554
18
555 Fig 7.
556
557 Studies falling into the top right quadrant of the Baujat plot contribute to the overall heterogeneity and the
558 overall result. A closer look to the plots reveals that two studies (ID: 75 and 12) contribute to both factors
559 in terms of Qm. The Influence of overall heterogeneity in model studies considering their weight is
560 visualized in Fig. 7. Studies marked with red circles have heterogeneity and very minor impact on the
561 observed outcome (Overall mean). Indeed, studies 75 and 12 had the minimum influence on the
562 adsorption capacity with highest dffits and cook's distance. Note that among all studies, red circle studies
563 have the highest rstudent, dffits, and cook.d compared to others. Accordingly, it can be reported that study
564 # 75 will have less impact than study # 12 on Qm parameter (the statistical parameters are presented in
565 Table S2).

566 3.3.3. Forest plots

567 The forest plots (Fig. 8) visualize the adsorption capacity and 95% CIs of the included studies along
568 with the computed their Summery (reporting the mean adsorption capacity of dyes onto the adsorbents).
569 Each study is represented by a point estimate, which is bounded by a CI for the effect. The Summery (and
570 95% CI) of removal efficiency and adsorption capacity are represented by the polygon at the bottom of
571 the plot where edges of the polygon represent the 95% confidence limit. Note the different sizes of each
572 square, where the studies with larger squares have contributed more to the summary. Based on the results
573 in Table 7 and forest plots, the mean adsorption capacity varied between 134.91 and 214.23 with a mean
574 of 174.57 mg/g over all studies. In terms of adsorption capacity, the maximum (890.10 mg/g, 95% CI=
575 888.24-891.96) and minimum (0.5 mg/g, 95% CI= -1.37-2.37) reductions of dyes belonged to methyl-
576 orange by activated carbon from waste Chinese hickory husk biomass (Study No. 777) and Naphthol blue
577 black by carbonaceous material from avocado peel (Study No. 349), respectively. Furthermore,
578 considering the 78 (k=78) studies and average adsorption capacity of 174.57 mg/g, it can be stated that
579 ~36% of the studies revealed a better capacity than overall (summary) value, while in other cases, the
580 capacities were less than the average.

581

582 Fig 8.

583

584 3.3.4. Publication bias

19
585 Fig. 9 depicts the visual inspection of the pooled adsorption capacity as the midpoint to draw the funnel
586 plot. The funnel plot was semi asymmetry visually. Nevertheless, results of Egger’s test (t= 0.1332,
587 P=0.0844) and Begg’s test (z=0.8458, P=0.3977) for Qm were statistically not significant, suggesting that
588 no potential publication bias existed.

589

590 Fig 9.

591

592 4. Conclusion

593 In this systematic review, the adsorption potential of carbon-based adsorbent materials including Gr, GO,
594 PAC, MWCNT and SWCNT, G, Co, GAC, and RGO were studied in the removal of dye molecules from
595 aqueous solutions by R software (Metafor package) over the last decade. This paper presented dye and
596 adsorbent classifications according to their chemical nature and structure. The evidence suggests that
597 most researchers have focused on adsorption of basic dyes by CBAMs, while the order of other dyes was
598 as acidic> reactive> azo> direct> disperse> vat. Also, powdered activated carbon is still the most widely
599 used material in dye removal with a 57.1% share of total sorbents. Another interesting point was that the
600 activated carbon prepared from waste claims the major portion of AC categories with a 65.6% share. The
601 Langmuir isotherm and pseudo-second-order kinetic model have been the most popular and widely used
602 models to describe the equilibrium of dyes by CBAMs. In the meta-analysis, the maximum adsorption
603 capacity of CBAMs pooled based random effect model was obtained as 174.57 mg/g (CI 95% =134.91
604 and 214.23). Q-statistic, I2 statistic, and Tau2 confirmed the high heterogeneity of studies in the model.
605 Finally, Egger’s and Begg’s indicated that no potential publication bias existed.

606

607 Limitations

608 Some limitations in this systematic review and meta-analysis should be acknowledged:

609 1. In reviews such as the present study, typically the sample size is not reported or not considered at
610 all. This make meta-analysis impossible; thus, to perform a meta-analysis, only the studies that modeled
611 the effects of factors were considered including DOE, ANN, Taguchi, etc.

20
612 2. In the present study, removal efficiency (%) was not considered as a response factor because in
613 modeling studies, the goal is to maximize the efficiency, and the results would be unrealistic. Thus, we
614 focused on Maximum adsorption capacity (Qm) as a response.
615 3. No checklists have been considered in adsorption, degradation, or oxidation and same studies for
616 quality assessment of articles until now. In the present study, this problem was resolved by providing a
617 checklist simulated by other studies.
618 4. Among all statistical parameters, only correlation coefficients (R2) were reported in all studies,
619 while the other statistical parameters were not reported. It is tasteful (Personalized) and each article
620 calculated a type of statistical parameter; this makes meta-analysis of data difficult.

621 Conflicts of interest

622 The authors declare that they have no known competing financial interests or personal relationships that
623 could have appeared to influence the work reported in this paper.
624

625 Acknowledgements

626 The present study was adapted from the PhD thesis of Ali Azari at Tehran University of Medical
627 Sciences. The authors gratefully acknowledge the financial support given by the Tehran University of
628 Medical Sciences [grant No. 97-03-27-39476].

629

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25
Table captions:

Table 1. Descriptive analysis on classification of dyes and adsorbents in term of removal

efficiency (Re, %) and adsorption capacity (Qm, mg/g)
Table 2. Descriptive analysis on effect of pH on adsorption process with considering the
classification of dyes and adsorbents

Table 3. Descriptive analysis on effect of initial dye concentration on adsorption process with
considering the classification of dyes and adsorbents

Table 3. Descriptive analysis on effect of initial dye concentration on adsorption process with
considering the classification of dyes and adsorbents
Table 5. Descriptive analysis on effect of times on adsorption process with considering the
classification of dyes and adsorbents
Table 6. Characteristics of the included studies to meta-analysis and their questionnaire.

Table 7. Random-Effects Model (k = 78), Heterogeneity statistics, and Model fit statistics and
information criteria-based adsorption capacity
 Table 1. Descriptive analysis on classification of dyes and adsorbents in term of removal
efficiency (Re, %) and adsorption capacity (Qm, mg/g)

Data Dye types N total N missing Mean SD SE Min Q1 Med Q3 Max P90 P95 P99
Basic 415 246 92.6 12.5 0.6 1.2 92.4 97 99 100 100 100 100
Reactive 98 52 90.3 11 1.1 43 87 93.5 98.3 100 99.4 99.9 100
Acidic 189 129 90.1 13.1 1 14 89 94 98 100 99.5 99.9 100
Re (%)

Azo 78 45 87.6 18.6 2.1 6 86.5 94.8 98 100 99.8 100 100
Vat 5 3 93.7 6.4 2.9 86 87.5 97.2 98.2 99.5 99.5 99.5 99.5
Disperse 10 3 79.9 10.4 3.3 66.5 75 75.8 90.2 100 95.5 100 100
Direct 31 14 90.3 9.6 1.7 64 86 93.5 97 100 98.6 99.9 100
Basic 658 3 287.2 360.5 14.1 0.5 51 176.4 386.9 3372 730 909 1714.2
Reactive 150 0 207 274.8 22.4 0.7 35.6 120.8 280 2022.9 529.2 639.8 1694.3
Qm (mg/g)

Acidic 316 2 261.2 348.6 19.6 0.5 40.1 137.5 346.7 2650 643 970 1667
Azo 123 0 190.3 254.8 23 0.5 39 107.1 246.9 1679.9 468.6 606.1 1488
Vat 8 0 303.6 318.5 112.6 45.9 104.3 191.9 392.4 1005.7 1005.7 1005.7 1005.7
Disperse 13 0 76.8 133.6 37.1 1.6 5.4 36.5 83.3 500 133.3 500 500
Direct 45 0 232 286.5 42.7 2.6 61.4 111 312.5 1428.5 607.8 769.2 1428.5
Sorbent
Data N total N missing Mean SD SE Min Q1 Med Q3 Max P90 P95 P99
types
Gr 48 30 92.5 11.5 1.7 22.1 90 93 98.5 100 99.9 100 100
RGO 37 30 93.6 8.5 1.4 59.7 93.1 97 99 100 100 100 100
PAC 513 239 90.8 13 0.6 14 89 95 98.6 100 99.9 100 100
Re (%)

GO 98 76 90.7 16.2 1.6 1.2 90 95 98.5 100 99.9 100 100

Co 23 5 88.5 10.6 2.2 67 84.4 93 96 100 98.4 99 100
CNT 87 90 93.5 8.3 0.9 63 93 96 98.7 100 99.9 100 100
G 13 11 84.6 28 7.8 18.4 85 99.5 100 100 100 100 100
GAC 7 11 80.6 16.6 6.3 63 63 90.5 95.6 97.2 97.2 97.2 97.2
Gr 78 0 320.5 327.6 37.1 2.3 103.6 206.2 453 1910 791 909 1910
RGO 67 0 303.4 340.3 41.6 13.2 93.4 199.4 357.7 1714.2 730 1200 1714.2
PAC 749 3 249.7 314.2 11.5 0.5 36 138.6 352.3 2650 628.9 840 1515
Qm (mg/g)

GO 172 2 298 475.9 36.3 1.4 41.5 131.9 348 3372 714.3 1231 2687.6
Co 28 0 197.2 221.6 41.9 1.6 11.3 160.3 281.3 881 581 647.5 881
CNT 177 0 260.8 312.8 23.5 0.7 63.3 152 312 2039 714.2 970.9 1428.5
G 24 0 108.5 112.9 23.1 20.7 40.3 52.4 167 440 222.3 384.6 440
GAC 18 0 110.7 114.4 27 2.6 25.2 91.4 167.1 433.7 298.4 433.7 433.7
 Table 2. Descriptive analysis on effect of pH on adsorption process with considering the
classification of dyes and adsorbents

N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99

Basic 550.0 7.0 2.4 0.1 7.0 1.0 6.0 7.0 8.0 13.0 10.5 11.0 12.0
Reactive 133.0 4.3 2.9 0.3 2.0 1.0 2.0 3.0 6.4 12.3 9.0 10.7 12.0
Acidic 263.0 4.6 2.2 0.1 2.0 1.0 3.0 4.9 6.4 11.0 7.0 8.0 11.0
Azo 108.0 4.6 2.6 0.2 2.0 1.0 2.3 4.0 7.0 12.0 7.1 9.0 11.0
Vat 8.0 5.2 2.7 1.0 2.0 2.0 2.0 6.4 7.0 8.5 8.5 8.5 8.5
Disperse 13.0 4.0 2.4 0.7 6.0 1.0 1.5 5.8 6.0 7.0 6.0 7.0 7.0
Direct 40.0 3.5 2.0 0.3 2.0 1.0 2.0 2.8 4.0 7.5 7.1 7.5 7.5
N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99
Gr 62.0 6.7 2.5 0.3 6.0 2.0 5.0 6.3 9.0 12.0 10.0 10.0 12.0
RGO 52.0 5.9 2.2 0.3 7.0 2.0 4.0 7.0 7.0 11.0 7.4 9.0 11.0
PAC 651.0 5.5 2.7 0.1 7.0 1.0 3.0 6.0 7.0 13.0 9.0 11.0 12.0
GO 145.0 6.5 2.9 0.2 7.0 1.0 4.0 7.0 8.5 12.0 10.5 11.0 12.0
Co 26.0 6.6 3.6 0.7 2.0 1.5 3.0 7.0 10.0 12.0 11.0 12.0 12.0
CNT 145.0 5.5 2.6 0.2 7.0 2.0 3.0 6.0 7.0 13.0 9.0 10.0 11.0
G 19.0 5.1 3.6 0.8 1.0 1.0 2.0 4.0 8.0 11.0 11.0 11.0 11.0
GAC 15.0 6.6 2.1 0.5 7.4 1.0 6.5 7.0 7.4 10.0 8.5 10.0 10.0
N Miss Mean SD SE Lower 95% Upper 95% Mode Min Q1 Med Q3 Max Range
1115.0 196.0 5.73 2.75 0.08 5.57 5.89 7 1 3 6 7 13 12
Disturb Fit tests Statistics P-value Decision
Normal K-S test 0.111 0.000 Reject
 Table 3. Descriptive analysis on effect of initial dye concentration on adsorption process
with considering the classification of dyes and adsorbents

N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99

Basic 661.0 132.4 208.6 8.1 100.0 0.2 20.0 50.0 120.0 1500.0 400.0 500.0 1000.0
Reactive 150.0 207.2 337.0 27.5 100.0 3.2 40.0 100.0 200.0 2100.0 550.0 1000.0 1500.0
Acidic 318.0 155.3 264.2 14.8 50.0 0.2 20.0 50.0 125.0 1700.0 400.0 800.0 1500.0
Azo 123.0 99.1 164.9 14.9 100.0 2.0 20.0 40.0 100.0 1000.0 200.0 300.0 1000.0
Vat 8.0 102.8 114.4 40.4 100.0 12.0 25.0 75.0 125.0 360.0 360.0 360.0 360.0
Disperse 13.0 48.9 31.7 8.8 50.0 15.0 31.0 40.0 50.0 125.0 100.0 125.0 125.0
Direct 45.0 75.7 89.2 13.3 50.0 8.0 20.0 50.0 100.0 500.0 150.0 250.0 500.0
N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99
Gr 78.0 92.4 141.4 16.0 20.0 2.0 20.0 40.0 100.0 800.0 250.0 450.0 800.0
RGO 67.0 122.9 169.9 20.8 500.0 0.2 20.0 40.0 125.0 700.0 500.0 500.0 700.0
PAC 752.0 160.9 259.0 9.4 100.0 2.0 20.0 70.0 200.0 2100.0 400.0 700.0 1500.0
GO 174.0 109.3 218.0 16.5 50.0 0.2 20.0 50.0 100.0 1500.0 250.0 600.0 1500.0
Co 28.0 131.4 180.0 34.0 100.0 5.0 28.0 45.0 150.0 730.0 500.0 500.0 730.0
CNT 177.0 123.7 223.7 16.8 100.0 2.9 20.0 50.0 100.0 1500.0 300.0 600.0 1200.0
G 24.0 61.4 54.7 11.2 10.0 6.4 20.0 30.0 112.5 200.0 125.0 127.0 200.0
GAC 18.0 140.0 87.0 20.5 250.0 20.0 80.0 100.0 250.0 250.0 250.0 250.0 250.0
N Miss Mean SD SE Lower 95% Upper 95% Mode Min Q1 Med Q3 Max Range
1318.0 0.0 140.4 235.2 6.5 127.7 153.1 100.0 0.2 20.0 50.0 105.0 2100.0 2099.8
Disturb Fit tests Statistics P-value Decision
Normal K-S test 0.3 0.0 Reject
 Table 4. Descriptive analysis on effect of dosage changes on adsorption process with
considering the classification of dyes and adsorbents

N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99

Basic 652 1.40 2.87 0.11 1 0.002 0.25 0.5 1 30 2.5 5 16
Reactive 149 2.93 4.73 0.38 1 0.005 0.6 1.5 3 29.2 6 10 25
Acidic 315 1.65 3.87 0.21 1 0.005 0.3 0.6 1 30 2.8 7 20
Azo 121 1.64 2.97 0.27 2 0.01 0.25 0.5 2 20 3 10 10
Vat 8 2.09 3.61 1.27 0.33 0.03 0.266 0.33 2.76 10 10 10 10
Disperse 13 3.91 3.82 1.06 1 0.1 1 3 5 12 10 12 12
Direct 44 1.28 2.10 0.31 0.2 0.025 0.2 0.5 1 10 3 6 10
N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99
Gr 77 1.44 2.95 0.33 0.5 0.01 0.1 0.5 16 0.9 2.7 5 16
RGO 65 0.58 0.91 0.11 1 0.002 0.17 0.3 5 0.53 1 2 5
PAC 747 2.17 4.12 0.15 1 0.005 0.4 1 30 1.6 5 10 25
GO 166 1.01 1.99 0.15 1 0.005 0.25 0.5 20 0.75 2 2.5 13.25
Co 28 2.98 4.34 0.82 1 0.1 0.9 1 20 1.1 10 10 20
CNT 177 0.77 0.82 0.06 0.4 0.005 0.2 0.4 4 0.8 2 2.5 3
G 24 0.56 0.52 0.10 0.2 0.13 0.2 0.35 2 0.6 1 2 2
GAC 18 1.11 0.93 0.22 1 0.1 0.8 1 4 0.2 2 4 4
N Miss Mean SD SE Lower 95% Upper 95% Mode Min Q1 Med Q3 Max Range
1302 16 1.68 3.43 0.09 1.50 1.87 1 0.002 0.3 0.6 1.5 30 29.99
Disturb Fit tests Statistics P-value Decision
Normal K-S test 0.31 6.74E-115 Reject
 Table 5. Descriptive analysis on effect of times on adsorption process with considering
the classification of dyes and adsorbents

N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99

Basic 657.0 249.0 542.4 21.2 60 0.5 25 60 240 4320 600 1440 3000
Reactive 150.0 314.8 603.1 49.2 120 3 50 120 300 3200 550 1440 3000
Acidic 316.0 294.3 614.0 34.5 60 2 30 77.5 180 4320 960 1440 2880
Azo 122.0 206.1 492.7 44.6 30 2 30 60 150 2880 360 720 2880
Vat 8.0 227.3 205.6 72.7 100 3 100 122.5 385 600 600 600 600
Disperse 13.0 319.2 487.1 135.1 120 15 60 100 120 1560 924 1560 1560
Direct 45.0 249.9 464.7 69.3 60 10 60 120 200 2400 360 1440 2400
N total Mean SD SE Mode Min Q1 Med Q3 Max P90 P95 P99
Gr 78.0 199.8 320.6 36.3 180 0.5 20 90 180 1440 720 1120 1440
RGO 65.0 156.0 234.3 29.1 15 5 15 60 120 960 600 720 960
PAC 748.0 327.4 686.6 25.1 60 1 30 90 240 4320 960 1440 3200
GO 173.0 188.6 305.5 23.2 60 0.5 25 60 240 1800 480 720 1800
Co 28.0 79.6 68.9 13.0 60 2 30 60 120 300 180 180 300
CNT 177.0 137.9 222.3 16.7 60 5 40 60 150 1440 300 360 1440
G 24.0 111.5 140.8 28.7 60 20 40 60 120 600 180 480 600
GAC 18.0 755.0 620.2 146.2 240 30 240 480 1500 1500 1500 1500 1500
N Miss Mean SD SE Lower 95% Upper 95% Mode Min Q1 Med Q3 Max Range
1311 7 264.02 558.90 15.43 233.73 294.30 60 0.5 30 80 240 4320 4319.5
Disturb Fit tests Statistics P-value Decision
Normal K-S test 0.318 3.20E-116 Reject
 Table 6. Characteristics of the included studies to meta-analysis and their questionnaire.
Sample F P #
N. R2 SS MS A B C D E F G H I J Q
Size Value Value Y
1 29 26.16 0.0001 0.926 6466.19 461.87 Y Y Y Y N Y Y Y Y N 8 H
16 29 26.28 0.0001 0.9796 5160.88 368.63 Y Y Y Y N Y Y Y Y Y 9 H
16 29 51.49 0.0001 0.9608 2956.86 211.2 Y Y Y Y N Y Y Y Y Y 9 H
21 300 ND ND 0.9702 ND ND Y Y Y Y N Y Y N Y Y 8 H
22 312 ND ND 0.99 ND 0.0003 Y Y Y N N Y Y N Y N 6 H
63 264 ND ND 0.9964 ND ND Y Y Y Y N Y N N Y N 6 H
66 50 110.11 0.0001 0.987 1575.18 78.76 Y Y Y Y N Y Y Y Y Y 9 H
66 50 469.73 0.0001 0.9969 8096.65 404.83 Y Y Y Y N Y Y Y Y Y 9 H
70 81 112.927 0.0001 0.9829 8465.77 313.547 Y Y Y Y N Y Y Y Y Y 9 H
70 81 329.922 0.0001 0.9829 13741.8 508.956 Y Y Y Y N Y Y Y Y Y 9 H
70 82 169.246 0.0001 0.9886 9906.2 366.893 Y Y Y Y N Y Y Y Y Y 9 H
71 31 22.97 0.0001 0.9526 14509.4 2712.8 Y Y Y Y N Y Y Y Y Y 9 H
92 44 42.5 ND 0.9 ND ND Y Y Y N N Y Y N Y Y 7 H
213 16 554.21 0.0001 0.9922 6298.4 6298.4 N Y Y Y N Y Y N Y N 6 H
215 32 1.718 0.1786 0.7575 2451 122.5 Y Y Y Y N Y Y Y Y Y 9 H
215 32 2.646 0.05 0.8279 5792 289.6 Y Y Y Y N Y Y Y Y Y 9 H
216 32 1.91 0.035 0.7765 1971 98.54 Y Y Y Y Y Y Y Y Y Y 10 H
216 32 1.469 0.0491 0.7276 2895 144.8 Y Y Y Y Y Y Y Y Y Y 10 H
226 20 52.16 0.0001 0.965 1753 194.8 Y Y Y Y N N Y Y N Y 7 H
226 20 25.78 0.0001 0.934 102.1 11.34 Y Y Y Y N N Y Y N Y 7 H
227 30 38.067 0.0001 0.9726 1939.71 138.55 N Y N Y N Y Y Y Y Y 7 H
229 46 5.03 0.0025 0.8276 8791.02 1758.2 Y Y Y Y Y N Y Y Y Y 9 H
266 26 223.425 0.00082 0.991 734.14 36.707 Y Y Y Y N Y Y Y Y N 8 H
266 26 283.34 0.0001 0.9987 868.64 43.432 Y Y Y Y N Y Y Y Y N 8 H
266 26 203.97 0.0001 0.9976 3280.8 164.04 Y Y Y Y N Y Y Y Y N 8 H
267 30 347.298 0.0001 0.9969 1290.808 92.2 Y Y Y Y Y Y Y Y Y Y 10 H
272 32 188.4 0.0001 0.9971 1465.1 73.254 Y Y Y Y Y Y Y Y Y Y 10 H
272 32 149.86 0.0001 0.9963 1591.9 79.595 Y Y Y Y Y Y Y Y Y Y 10 H
273 33 113.747 0.0001 0.9984 5144.4 190.54 Y Y Y Y N Y Y Y Y Y 9 H
273 33 81.987 0.0001 0.9977 9309.5 344.77 Y Y Y Y N Y Y Y Y Y 9 H
273 33 1050.31 0.0001 0.9998 10630 393.69 Y Y Y Y N Y Y Y Y Y 9 H
274 25 523.77 0.0001 0.9996 10445.93 522.3 N Y Y Y N Y Y Y Y N 7 H
274 25 9328.68 0.0001 1 11041.64 552.08 N Y Y Y N Y Y Y Y N 7 H
274 25 45.52 0.0001 0.9956 2976.78 148.84 N Y Y Y N Y Y Y Y N 7 H
288 53 6.46 0.034627 0.9864 1.5098 1.5098 Y Y Y Y N Y Y Y Y Y 9 H
288 53 55.672 0.000072 0.9967 6.8283 6.8283 Y Y Y Y N Y Y Y Y Y 9 H
288 53 147.114 0.000002 0.9787 20.9638 20.9638 Y Y Y Y N Y Y Y Y Y 9 H
288 53 348.79 0.0001 0.9929 42.1609 42.16 Y Y Y Y N Y Y Y Y Y 9 H
290 31 159.63 0.0001 0.9929 45789.7 3270.7 Y Y N Y N Y N Y Y N 6 H
316 29 296.27 0.0001 0.9966 4083.23 291.66 Y Y Y Y Y Y Y Y Y Y 10 H
316 29 51.27 0.0001 0.9809 3700.29 264.31 Y Y Y Y Y Y Y Y Y Y 10 H
336 20 29.38 0.0001 0.932 371.06 41.23 Y Y Y Y N Y Y Y Y Y 9 H
342 31 87.51 0.0001 0.987 8266.69 590.478 Y Y Y Y Y Y Y Y Y Y 10 H
342 31 185.121 0.0001 0.994 5472.622 390.902 Y Y Y Y Y Y Y Y Y Y 10 H
343 27 386.133 0.0001 0.9947 272.959 272.959 Y Y Y Y N Y Y Y Y Y 9 H
347 30 105.79 0.0001 0.99 1892.21 135.16 Y Y Y Y N Y Y Y Y Y 9 H
349 12 ND ND 0.953 ND ND N Y Y N N Y N Y Y N 5 M
349 12 ND ND 0.944 ND ND N Y Y N N Y N Y Y N 5 M
349 12 ND ND 0.913 ND ND N Y Y N N Y N Y Y N 5 M
380 50 40.15 0.001 0.922 19912 1659.34 Y Y Y N Y Y Y Y Y Y 9 H
389 31 48.91 0.0001 0.97717 19.151 91 Y Y Y Y N Y Y Y N Y 8 H
390 32 52.78445 0.000749 0.997 3484.166 129.0432 N Y Y Y N Y Y Y Y Y 8 H
390 32 12.91716 0.00145 0.989 123.7145 4.582019 N Y Y Y N Y Y Y Y Y 8 H
391 32 1299 0.0001 0.99394 634.4 634.4 N Y Y Y Y Y Y Y Y Y 9 H
391 32 110.01 0.0002 0.95713 126.6 126.6 N Y Y Y Y Y Y Y Y Y 9 H
391 32 4584 0.0001 0.99844 777.8 777.8 N Y Y Y Y Y Y Y Y Y 9 H
399 30 223.749 0.0001 0.9952 561.0813 40.07723 Y Y Y Y Y Y Y Y Y Y 10 H
409 46 ND ND 0.9506 ND ND Y Y N N N N Y Y Y N 5 M
410 360 ND ND 0.99 ND ND Y Y Y N N Y Y N Y Y 7 H
430 20 9.41 0.0008 0.894 10533.12 1170.35 N Y Y Y N N Y Y Y N 6 H
444 270 ND ND 0.998 ND ND N Y Y N Y Y Y N Y N 6 H
457 27 273.99 0.0001 0.9903 9976.73 4988.36 Y Y Y Y N N Y N Y Y 7 H
491 15 6.61 0.009 0.998 315.095 1.26 N Y Y Y N N N Y Y N 5 M
494 360 ND ND 0.9991 ND ND N Y Y Y N Y N N Y N 5 M
504 9 4.156 0.0034 0.902 458.108 229.054 N Y Y Y Y N N Y N Y 6 H
505 20 48.6 0.0001 0.966 9940 1420 N Y Y Y N Y Y Y Y N 7 H
518 41 ND ND 0.97 ND ND Y Y Y N N Y Y N Y N 6 H
574 23 238.43 0.0001 0.9954 605.37 67.26 Y Y Y Y N Y N Y Y N 7 H
607 17 22.89 0.0002 0.9671 11112.69 1234.74 Y Y N Y N Y N N Y Y 6 M
635 8 790.4 0.026 0.9996 2050.16 683.387 Y Y Y N N Y Y Y Y N 7 H
641 85 ND ND 0.9997 ND ND Y Y Y Y N Y Y N Y N 7 H
654 30 30.47 0.0001 0.966 7951.03 567.93 Y Y Y Y Y Y Y Y Y N 9 H
659 31 14.47 0.0001 0.926 3398.75 364.54 Y Y Y Y N N Y Y Y N 7 H
670 20 11.93 0.0003 0.9148 38285.37 4525.93 Y Y Y Y N N Y Y Y N 7 H
777 9 16.98 0.03309 0.95 0.75 0.38 N Y Y Y N Y N N Y N 5 M
777 9 13.64 0.02741 0.9 0.92 0.46 N Y Y Y N Y N N Y N 5 M
800 15 12.43 0.006 0.957 16465.9 1829.55 Y Y Y Y N N Y N Y N 6 H
809 20 18.28576 0.0001 0.942 5055.22 561.6913 N Y Y Y N Y N Y Y N 6 H
Table 7. Random-Effects Model (k = 78), Heterogeneity statistics, and Model fit statistics
and information criteria-based adsorption capacity

Z- P- CI CI
Scenario Estimate Se Signif.
value value Lower Bound Upper Bound
174.57 20.14 8.66 <0.0001 134.91 214.23 ***
Tau Tau² I² (%) H² df Q p
Adsorption 177.8944 31646.40 99.99 1750407.72 77 98069.55 < .0001
capacity log-
Models Deviance AIC BIC AICc
likelihood
Maximum-Likelihood -508.20 1016.41 1020.41 1025.10 1020.58
Figures captions:
Fig 1. Classification of dyes (a) adsorbents (b), count and percentage of used dyes (c) and
sorbents (d) over different years.
Fig 2. Investigation of pH distribution over decades (a) and pH box plot (b)

Fig 3. Investigation of initial concentration distribution over decades (a) initial concentration box
plot (b) and its scatter plot and trend line

Fig 4. Investigation of adsorbent dosage distribution over decades (a) adsorbent dosage box plot
(b) and its scatter plot and trend line (c)
Fig 5. Investigation of contact time distribution over decades (a) adsorbent dosage box plot (b)

Fig 6. The count and percentage of best fitted kinetic (a) and isotherm (b) models and their
distribution
Fig 7. The plot of Baujat (a) and Influence of overall heterogeneity in model studies (b)

Fig 8. Forest plot displaying Qm (mg/g) based on the random effects model with 95%
confidence intervals of the average effect size

Fig 9. Funnel plot displaying Qm (mg/g) by standard errors as estimated by the trim-and-fill
method
2020 2020
(a) (b)

2015 2015

2010 2010

Range
Range

2005 2005
Basic Reactive Acidic Azo Vat Disperse Direct Gr RGO PAC GO Co CNT G GAC

661 Dye.Type 752 Sorbent.Type

700 (c) 800 (d)
(50.2%) (57.1%)
Count

Count
600 700

600
500
500
400
318
(24.1%) 400
300
300
200 150 174 177
(11.4%) 123 200 (13.2%) (13.4%)
(9.33%) 78
100 45 67
13 100 (5.92%) (5.08%) 28 24 18
8 (3.41%)
(0.607%) (0.986%) (2.12%) (1.82%) (1.37%)
0 0
Basic Reactive Acidic Azo Vat Disperse Direct Gr RGO PAC GO Co CNT G GAC

Fig 1. Classification of dyes (a) adsorbents (b), count and percentage of used dyes (c)
and sorbents (d) over different years.
250 14
pH

(18.8%)
(18.2%)
(a) 13 (b)

210
13

Range
203
Count

12
(15.7%)

200
175

11
10
9
150
(10.4%)

8
116

7 7
(7.35%)
(7.17%)

100 6 6
82
80

5.73
(5.11%)

5
(5.2%)
57

58
(3.86%)

4
(3.5%)
43
(2.51%)

39

50
(1.88%)
3
28

3
21

(0.269%)
2
3

1 1
0 pH
1 2 3 4 5 6 7 8 9 10 11 12 13 14 0

Fig 2. Investigation of pH distribution over decades (a) and pH box plot (b)
 2200
Count

1200 Dye Con. (mg/L)

1.04E3
(79%)

Dye Con. (mg/L)

2000
1100
(a) 1800
(b)
1000
1600
900
1400
800
700 1200

600 1000

500 800

400 600
(10.5%)

300 400 200

138

(5.39%)

(0.0759%)

(0.0759%)
(0.683%)

140
(0.228%)

200 200
(1.67%)
(1.52%)

(0.91%)
71

105
22
20

1
12

9
3

100 0
(0%)

(0%)

50
0

20
0 -200 0.2
-200 0 200 400 600 800 1000 1200 1400 1600 1800 2000 2200

95% Confidence Band of K"Qm" Dye.Concentration

3000

95% Prediction Band of K"Qm"

Qm
(c)
2500
2000
1500
1000
500
0

0 200 400 600 800 1000 1200 1400 1600 1800 2000

Fig 3. Investigation of initial concentration distribution over decades (a) initial

concentration box plot (b) and its scatter plot and trend line
 32
Count

1200 Adsorbent Dose (g/L) 30

Adsorbent Dose (g/L)

(76.7% )

1100 28 (b)
998

(a)
26
1000
24
900 22
800 20
18
700 16
600 14
12
500
10
400 8
6
(13.3% )

300 3.3
173

4 1.69
200
(0.0768% )

2
(3.84% )

(0.845% )
(2.46% )
(0.461% )

(0.384% )

(0.307% )
(0.154% )

1.5
(1.08% )

(0.23% )

(0.23% )
50

0
32

11

100 0.6
14

1
6

4
2
(0% )

(0% )

(0% )

(0% )
3

-2
0

0.3
0 -4 0.002
-2 0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32

95% Confidence Band of K"Qm" Adsorbent.Dose

1000 1500 2000 2500 3000

95% Prediction Band of K"Qm"

Qm
(c)
500
0

0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30

Fig 4. Investigation of adsorbent dosage distribution over decades (a) adsorbent dosage
box plot (b) and its scatter plot and trend line (c)
 4500
C ount

Time (min)

Time (min)
1400
(a) (b)
4000
(88.6% )
1.16E3

1200
3500

1000 3000

2500
800
2000
600
1500

400 1000
540

500 264
(4.42% )

(0.0763% )
(3.89% )

200
(0.839% )

(0.458% )

(0.458% )

240
58

51

(1.3% )
11

6
17

0
(0% )

(0% )

80
0

0 30

-500 0 500 1000 1500 2000 2500 3000 3500 4000 4500 -500 0.5

Fig 5. Investigation of contact time distribution over decades (a) adsorbent dosage box
plot (b)
 0
200
400
600
800
1000
1 C o u n ts

W
(0.0 97 8% )

90 7
(8 8.7 % )

PSO
10

ID
(0 .9 78% )

74
(7.2 3% )

PFO
11

E
(1.0 8% )

WM
(0.1 96 % )
(a)

12

GO
(1.17% )

4
(0 .39 1% )

AFO
1

F
(0.0 97 8% )

FO
(0.0 97 8% )
Kinetic

0
200
400
600
800
1000

85 5

L
(7 4% )

their distribution
17 0
F (14 .7% )
16
T
(1.3 9% )
38
(3.2 9% )
1
(0 .08 66% )
3
(0.2 6% )
26
(2.25% )
1
(0 .08 66% )
11
(b)

(0 .95 2% )
14
(1 .21 % )
3
Fig 6. The count and percentage of best fitted kinetic (a) and isotherm (b) models and

(0.2 6% )
6
(0 .51 9% )
6
(0 .51 9% )
3
(0.2 6% )
2
RP DR FS S HJ L-F Li KC To B VS G
Isotherm

(0 .17 3% ) C o u n ts
 Influence on Overall Result
75
(a)

0.00 0.10 0.20 12

46
39
673
35
6314
18
49
48
47
60
13
37
361
58
67
70
62
77
65
72
15
38
4 74
76
21
29
53
25
24
43
50
71
27
30
41
40
52
51
57
59
66
69
11
23
22
28
32
31
34
44
61
68
78
56
55
9 16
19
54
17
3
20
64
26
45
5
10 8
42
2
73

0 5 10 15

Squared Pearson Residual

(b)
rstudent dffits
-0.1 0.2 0.5
-2 0 2 4

1 6 12 19 26 33 40 47 54 61 68 75 1 6 12 19 26 33 40 47 54 61 68 75

cook.d cov.r
1.00
0.15

0.85
0.00

1 6 12 19 26 33 40 47 54 61 68 75 1 6 12 19 26 33 40 47 54 61 68 75

tau2.del QE.del
25000 30000

7.5e+07

1 6 12 19 26 33 40 47 54 61 68 75 1 6 12 19 26 33 40 47 54 61 68 75

hat weight
0.0 0.6 1.2
0.010
0.000

1 6 12 19 26 33 40 47 54 61 68 75 1 6 12 19 26 33 40 47 54 61 68 75

Fig 7. The plot of Baujat (a) and Influence of overall heterogeneity in model studies (b)
Fig 8. Forest plot displaying Qm (mg/g) based on the random effects model with 95%
confidence intervals of the average effect size

0.0

0.1
Standard Error

0.2

0.3

0 250 500 750

adsorption capacity mg/g

Fig 9. Funnel plot displaying Qm (mg/g) by standard errors as estimated by the trim-
and-fill method
Highlights

First systematic review and meta-analysis of dyes adsorption by carbon materials

The Metafor package provides functions for conducting meta-analyses in R software

835 articles and 78 studies were eligible for review and meta-analysis respectively

From the pooled of data, adsorption capacity varied between 134.91 and 214.23 mg/g

Potential publication bias did exist base Egger’s (p=0.08) and Begg’s test (p=0.39)
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: