Environmental Science and Pollution Research

Recent Advances on Conducting Polymer Based Magnetic Nanosorbents for Dyes and
Heavy Metal removal: Fabrication, Applications, and Perspective
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Manuscript Number: ESPR-D-22-21958

Full Title: Recent Advances on Conducting Polymer Based Magnetic Nanosorbents for Dyes and
Heavy Metal removal: Fabrication, Applications, and Perspective

Article Type: Review Article

Abstract: The massive production of hazardous heavy metal ions (HMIs) and dyes by various
industries and their improper disposal intensify water pollution. Much attention is
required on the development of efficient and cost-effective technologies and
approaches for removing toxic HMIs and dyes from wastewater as they pose a severe
threat to public health and aquatic ecosystems. Due to the proven superiority of
adsorption over other alternative methods various nanosorbents have been developed
for the efficient removal of HMIs and dyes from wastewater and aqueous solutions.
Being a good adsorbent, conducting polymer-based magnetic nanocomposites (CP-
MNCPs) has drawn more attention for HMIs and dye removal. The present review
focuses on the production strategies and applications of CP-MNCPs for HMIs and dye
removal. The review also sheds light on the adsorption mechanism, adsorption
efficiency, kinetic and adsorption models, and regeneration capacity of the various CP-
MNCPs.

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1 Recent Advances on Conducting Polymer Based Magnetic Nanosorbents for

2 Dyes and Heavy Metal removal: Fabrication, Applications, and Perspective

3 Madhav Krishna Goswami1, Abhishek Srivastava1*, Rajeev Kumar Dohare2, Anjani Kumar
4 Tiwari3, Anupam Srivastava4

1
5 Department of Chemistry, GLA University, Mathura, 281006, U.P. (India)
2
6 Department of Chemical Engineering, Malaviya National Institute of Technology, Jaipur, India
7 3Department of Chemistry, Babasaheb Bhimrao Ambedkar University, Lucknow 226025, U.P.
8 India
4
9 Department of Chemistry, Dayalbagh Educational Institute, Dayalbagh Agra, 282005, U.P. India
10 Corresponding author Email: *aabhichem@gla.ac.in
11
12 Abstract
13 The massive production of hazardous heavy metal ions (HMIs) and dyes by various industries and
14 their improper disposal intensify water pollution. Much attention is required on the development
15 of efficient and cost-effective technologies and approaches for removing toxic HMIs and dyes
16 from wastewater as they pose a severe threat to public health and aquatic ecosystems. Due to the
17 proven superiority of adsorption over other alternative methods various nanosorbents have been
18 developed for the efficient removal of HMIs and dyes from wastewater and aqueous solutions.
19 Being a good adsorbent, conducting polymer-based magnetic nanocomposites (CP-MNCPs) has
20 drawn more attention for HMIs and dye removal. The present review focuses on the production
21 strategies and applications of CP-MNCPs for HMIs and dye removal. The review also sheds light
22 on the adsorption mechanism, adsorption efficiency, kinetic and adsorption models, and
23 regeneration capacity of the various CP-MNCPs.

24 Keywords: Magnetic nanocomposites; conducting polymers; Nanosorbents; Organic dyes; Heavy

25 metal ions; Wastewater remediation.

26 Abbreviations

27 HMIs: Heavy metal ions; CP: Conducting polymer; NCPs: Nanocomposites; MNCPs: Magnetic

28 nanocomposites; CP-MNCPs: Conducting polymer-based-magnetic nanocomposites; PPy:

29 Polypyrrole; PANI: Polyaniline; APS: Ammonium persulfate; PTh: Polythiophene; CL: Coral
1
30 like; MO: Methyl orange; CV: Crystal violet; BB3: Basic blue 3, AB40: Acid blue 40; MG:

31 Malachite green; ARS: Alizarin red S; RHB: Rhodamine B; IC: Indigo carmine; CR: Congo red;

32 TCH: Tetracycline hydrochloride; CNTs: Carbon nano tubes; AF: Acid fuchsin; MB: Methyl blue;

33 JG: Janus green; FB: Fuchsin basic; PS: Polystyrene; CS: Chitosan; MWCNTs: Multiwall carbon

34 nano tubes; GS: Graphene; CBZ: Carbamazepine.

35 Introduction

36 Water pollution, undoubtedly among the most severe problems that human civilization has faced

37 throughout history affects the wellness of billions of people worldwide and causes diseases such

38 as cancer, diarrhea, and cholera, as well as issues with the liver, kidneys, brain, lungs, and skin

39 (Dahiya 2022; Prakash et al. 2021). World Health Organization (WHO) statistics indicate that

40 water-borne diseases account for 80% of all diseases. The quality of drinking water in various

41 countries does not adhere to WHO standards (Chan et al. 2021). The production of a massive

42 amount of hazardous chemical waste by different industries, as well as its inappropriate disposal,

43 is continuously intensifying water pollution (Sharma et al. 2022b). Numerous hazardous and

44 infectious contaminants including dyes, heavy metal ions (HMIs), pesticides, and radioactive

45 elements are present in the large amount of wastewater (Yasasve et al. 2022). HMIs are primarily

46 produced by the ceramic, glass, and tannery industries, electroplating, battery, metal processing,

47 and finishing industries, as well as by the mining industries and petroleum refining (Velusamy et

48 al. 2021). Organic dyes from paints, textile, pharmaceuticals, food, leather, pulp, paper, and

49 coating industries are the most significant source of wastewater contamination (Ardila-Leal et al.

50 2021; Dassanayake et al. 2021). We need efficient and cost-effective technologies and approaches

51 to remove toxic HMIs and dyes from wastewater as they pose a serious threat to public health and

52 aquatic ecosystems (Elgarahy et al. 2021).

2
53 For the purpose of removing HMIs from aqueous solutions and wastewater, a variety of approaches

54 including physical and chemical precipitation, solvent extraction, membrane filtration,

55 electrochemical treatment, reverse osmosis, ion exchange, and adsorption processes are frequently

56 used (Yadav et al. 2021). On the other hand, membrane separation, anaerobic and aerobic

57 microbial degradation, electrochemistry, ozonation, chemical oxidation, oxidative degradation,

58 photo-catalysis, nano-filtration, microfiltration, coagulation, and adsorption have frequently been

59 employed to remove dyes from wastewater (Selvaraj et al. 2021). Figure 1 summarizes various

60 dye and HMIs removal techniques reported in the literature to meet environmental standards.

61 Despite being effective, these technologies have some disadvantages, limited removal efficiency,

62 time-consuming, high initial investment, high operational expenses and energy requirements, and

63 the issue of disposing of leftover metal sludge (Shrestha et al. 2021a; Yadav et al. 2020). Although

64 several biological and chemical techniques have been developed, adsorption is thought to be one

65 of the most efficient and practical methodologies for water treatment when it comes to removing

66 dyes and HMIs from aqueous solutions and wastewater (Ikram et al. 2021; Shrestha et al. 2021a).

67 Adsorption has been shown to outperform competing approaches in terms of design versatility,

68 effectiveness, ease of operation, low setup and operating costs, and resistance to toxic pollution

69 (Hamzezadeh et al. 2022). Furthermore, it doesn't lead to the creation of dangerous substances

70 (Taghizadeh et al. 2020). As a result, a wide variety of adsorbent materials have been designed to

71 remove such harmful dyes and HMIs from wastewater (Rathi et al. 2021).

72 The advancement in nanotechnology has demonstrated remarkable promise for resolving

73 environmental issues. Because of their distinctive physicochemical features, particularly their high

74 selectivity, high adsorption capacity, and high specific-surface-area-to-volume ratio,

75 nanomaterials have been employed as effective adsorbents for water remediation (Wadhawan et

3
76 al. 2020). In this context, the use of nano-adsorbent materials has advanced significantly and

77 quickly in comparison to conventional adsorbents (Kutluay 2021).

78 Conducting polymers (CPs) consist of conjugated π bonds and have potential applications in

79 biomedicine (Jadoun et al. 2021b), corrosion prevention (Jiang et al. 2022), gas sensors (Liu et al.

80 2022), biosensors (Ma et al. 2021b), and adsorbents (Lahreche et al. 2022), all of which are

81 frequently mentioned in the literature. Although conducting polymers have many restrictions in

82 their pure state, these issues can be solved by combining them with other materials (Heck et al.

83 2021). Due to the ability of conducting polymers to combine with other nanomaterials, CP-based

84 nanocomposites (NCPs) have garnered a lot of attention as the NCP exhibits the potential

85 characteristics of all the individual components into a single material (Jadoun et al. 2021a). CP-

86 MNCPs have drawn considerable attention to high adsorption due to their special

87 superparamagnetic properties, which can facilitate their convenient separation from wastewater by

88 applying an exterior magnetic field, furthermore the presence of numerous functional groups viz.

89 NH2, C=N, -S-, -NH-, and OH on the surface of polymer nanocomposites facilitate the adsorption

90 of metal ions via different types of interactions (Ahmad et al. 2020; Dutta et al. 2020). These

91 nanocomposites are highly sought-after due to their environmental stability, affordable monomer,

92 high conductivity, simplicity of synthesis, regeneration capacity, and distinctive physicochemical

93 features for dye and HMIs removal from wastewater.

94 There isn't a solitary, exhaustive review that is devoted exclusively to the preparation and

95 applications of CP-MNCPs for wastewater remediation. The review article by Khan et al.

96 highlighted the uses of CP-MNCPs as adsorbents for environmental applications (Khan et al.

97 2021). In addition to this, a review by Zare et al. offers more in-depth information on the use of

98 polyaniline-based nanosorbent for the removal of HMIs and dyes (Zare et al. 2018a). Other

4
 99 reviews do exist, but they tend to focus on a particular conductive polymer and its composites

100 (Hajjaoui et al. 2021). The current review specifically focuses on an in-depth discussion of the

101 production approaches and applications of CP-MNCPs in HMIs and dye removal. The review also

102 provides insights into the batch parameters viz. pH of the solution, adsorbent dose, ionic strength,

103 adsorbent concentration, interaction time, and temperature that significantly affect the adsorption

104 efficiency. The review also sheds light on the adsorption mechanism, adsorption efficiency, kinetic

105 and adsorption models, and regeneration capacity of the developed materials to provide a

106 foundation for future research.

107 Strategies for the fabrication of conducting polymer-based magnetic nanocomposites

108 Numerous approaches are available regarding the fabrication of CPs, including electrochemical

109 polymerization, chemical oxidation, photochemical methods, hydrothermal, vapor phase

110 synthesis, plasma polymerization, solid state method, inclusion method, self-assembly,

111 electrospinning, template-assisted, and solvothermal methods (Abbas et al. 2021; Barros et al.

112 2003; Chu et al. 2019; Heydarnezhad et al. 2018; Karki et al. 2022; Lin et al. 2021; Lu et al. 2020;

113 Meng et al. 2003; Nie et al. 2021; Sha et al. 2019). Oxidation polymerization methods including

114 electrochemical and chemical are typically used for the fabrication of most of the CPs (Fomo et

115 al. 2019; Wang et al. 2018). Chemical oxidation, the most straightforward method, preferred for

116 the fabrication of a large amount of CPs, involves the mixing of monomer precursor and suitable

117 oxidizing agents like ammonium persulfate, potassium dichromate, ferric chloride, ceric sulfate,

118 ceric nitrate, and ammonium peroxydisulfate under ambient condition, preferably in an acidic

119 environment (Abdel‐ Aziz et al. 2021; Melánová et al. 2019; ur Rehman et al. 2020; Yang et al.

120 2019; Yussuf et al. 2018). When the pH of the reaction medium is maintained 1 to 3, the produced

121 polymer exhibits excellent conductivity (Vivekanandan et al. 2011; Yang et al. 2020).

5
122 Electrochemical synthesis is widely used to fabricate highly conductive polymer films, especially

123 for electronic devices (Alqarni et al. 2020; Ashokkumar et al. 2020; Shokry et al. 2022; Zhao et

124 al. 2019). Due to the reduced anode size, the product yield in the electrochemical oxidation process

125 is limited. The controlled morphology and thickness via electrochemical parameters controlling is

126 the main advantage of electrochemical synthesis (Istakova et al. 2019; Ozkazanc et al. 2013; Tang

127 et al. 2020).

128 Various mechanistic schemes have been suggested by authors on the polymerization of CPs (Lyu

129 et al. 2019; Namsheer et al. 2021; Pan et al. 2010). Polypyrrole is one of the most extensively used

130 CPs in the chemical and electrochemical oxidation process. The proposed mechanisms for

131 chemical and electrochemical oxidative polymerization of pyrrole are almost similar. Here in we

132 are discussing the most acceptable chemical oxidative polymerization mechanism of pyrrole

133 [Figure 2]. In the initiation step, a reactive radical cation of a pyrrole monomer is formed via the

134 oxidation of pyrrole. In the propagation step, the formed reactive intermediate reacts with a neutral

135 molecule of pyrrole to produce a dihydro-bipyrrole cation, which undergoes oxidation followed

136 by deprotonation to yield a bipyrrole. The dimeric radical cation formed by the oxidation of

137 bipyrrole reacts with another molecule of neutral pyrrole to yield a trimeric pyrrole. The growth

138 of the polymeric chain takes place through this repeated process which ultimately results in a

139 polymeric chain (Morávková et al. 2021; Nezhad et al. 2018; Pang 2020; Tan et al. 2013).

140 Concerning the magnetic nanoparticles component, various chemical approaches have been

141 developed for size and shape-controlled synthesis of magnetic nanoparticles including pure metal

142 oxides, such as Fe2O3 and Fe3O4; and mixed ferrites such as NiFe2O4, CoFe2O4, and MnFe2O4

143 (Akhlaghi et al. 2021; Ansari et al. 2019; Babu et al. 2020; Pang 2020; Paswan et al. 2021; Varanda

144 et al. 2019). The adopted synthetic strategy will decide the magnetic property of the nanoparticles,

6
145 which can be regulated by surface effect, size effect, phase, and chemical composition. The most

146 popular chemical approaches include sol-gel, thermal decomposition, co-precipitation,

147 emulsification, electrochemical route, and hydrothermal synthesis (Bhagwat et al. 2019; Elsayed

148 et al. 2019; Naik et al. 2022; Stein et al. 2018; Tomar et al. 2020; Tsay et al. 2019). Co-precipitation

149 is the most preferred approach for the size and shape-controlled fabrication of ferrite nanoparticles

150 (Gharibshahian 2020). In principle, for the fabrication of cobalt ferrite (CoFe2O4) nanoparticles,

151 sodium hydroxide solution is added slowly to the mixture of iron nitrate and cobalt nitrate (2:1

152 ratio) solution under stirring. The pH of the reaction mixture is maintained between 11to12. The

153 reaction mixture is then heated at 80 oC for 1 hour with enduring stirring. The black precipitate is

154 magnetically decanted, washed with distilled water and ethanol, and dried overnight at 100 oC.

155 The black substance is ground into a fine powder and then calcined at 600 oC for 6 hours to get

156 CoFe2O4 nanoparticles (Surendra et al. 2011; Vinosha et al. 2017).

157 By combining the two strategies (synthesis of conducting polymer and magnetic nanoparticles) in

158 a specific manner, the CP-coated MNCPs can be synthesized. Many reports have been published

159 on the successful incorporation of magnetic nanoparticles into the CP matrix, and the ultimate

160 properties of the prepared nanocomposites have been strongly influenced by the adopted procedure

161 (Praveena et al. 2014; Scindia et al. 2019; Singh et al. 2020a). The homogeneous dispersion of

162 magnetic nanoparticles is one of the major challenges, because due to magnetostatic interactions

163 the nanoparticle may get aggregated that generally changes the characteristics of the material, and

164 could limit its expected applications (Cardoso et al. 2018; Kudr et al. 2017; Shrestha et al. 2020).

165 In general, four different synthetic approaches have been applied for the fabrication of colloidally

166 stable nanocomposites [Figure 3].To overcome the aggregation problem and to get uniform

167 dispersibility, the nanoparticles have usually been covered with organic ligands or surfactants. A

7
168 homogeneous thin layer of the polymer has successfully been built on previously coated

169 nanoparticles.

170 In the first route, the magnetic nanoparticles and the polymer are synthesized separately and then

171 both components are mixed under vigorous stirring to get nanocomposites. This methodology is

172 not generally adopted as the method typically results in the formation of heterogeneous composites

173 with larger particles, also the non-solubility of CPs in common solvents creates a problem. The

174 second route has been mostly utilized for size and shape-controlled synthesis of homogeneous

175 nanocomposites. This method involves the production of magnetic nanoparticles at first and

176 thereafter polymerization has been performed to obtain CP-MNCPs. The third strategy involves

177 the synthesis of nanocomposite via the preparation of magnetic nanoparticles within the pre-

178 synthesized CPs (Ramírez-Ortega et al. 2021). Although the produced nanocomposites are

179 homogeneous, the polymer solubilization in common solvents and the nanoparticle size

180 management are major concerns (Prunet et al. 2021). The fourth method consists of the in-situ

181 synthesis of both nanoparticles and CPs to produce nanocomposites. Despite its rapidity and

182 simplicity, the method is not very common because of its poor influence on the nanoparticles and

183 polymer.

184 Physical Methods

185 Fabrication of CP-MNCPs typically involves the mixing or blending of polymer and metal

186 nanoparticles in the melt or solution (Chen et al. 2018a). The insolubility of CPs in general solvents

187 and extremely high melting temperature, and heterogeneous blending of metal nanoparticles (at

188 high content) limit the use of these strategies (Chen et al. 2018b; Iqbal et al. 2018; Li et al. 2019).

189 MNCPs based on CPs can be synthesized in the solution phase only when the polymer is either

190 dispersible or soluble in the solvent and also the magnetic nanoparticles are colloidally stable.

8
191 Taccola et al. fabricated PEDOT:PSS (polystyrene sulfonate)/Iron Oxide NP nanofilms by

192 blending the concentrate dispersion of PEDOT:PSS with iron oxide nanoparticles for about 30

193 min. The morphology and magnetic properties of resulting NCPs are strongly influenced by the

194 iron oxide nanoparticles (Taccola et al. 2013). To make PPy water soluble, Temizel et al.

195 functionalized the PPy with phosphonic acid, and the resultant poly(N-pyrrole phosphonic acid)

196 (PPPA) was stirred with Fe3O4 nanoparticles in a sonicator to get PPPA coated MNCP (Temizel

197 et al. 2011). The FTIR analysis of the fabricated nanocomposite suggests the interaction of all

198 three oxygen of phosphate groups with the Fe3O4 nanoparticle surface (Figure 4). The solution

199 method has also been used by adding the water-soluble poly(1-vinyl-1,2,4-triazole) (PVTri) to an

200 aqueous dispersion of Fe3O4 nanoparticles under stirring to produce Fe3O4–PVTri nanocomposite

201 (Kavas et al. 2010).

202 The solubility problem of magnetic nanoparticles and the heterogeneous dispersion of bulk

203 magnetic nanoparticles can be overcome by the solid-state process like ball milling (Yu et al.

204 2018). Ball milling of CPs, carried out in cryogenic conditions, is referred to as cryomilling. In

205 cryomilling, by blending the components under cryogenic conditions, the compatibility between

206 nanoparticles and polymer has been improved by overcoming the viscoelastic nature of the

207 polymer. This technique has been effectively utilized for the fabrication of PANI-iron NCPs using

208 iron in the nanometer and micrometer range, with both magnetic and conducting properties (Zhu

209 et al. 2008).

210 In-situ oxidative polymerization in presence of magnetic nanoparticles

211 Oxidative polymerization, the most exhaustively used approach for the synthesis of CP-based

212 nanocomposites involves the in-situ polymerization of monomer in the presence of

213 heterogeneously or homogeneously (in surfactant) dispersed magnetic nanoparticles. The solvent

9
214 selection plays a vital role in this approach, the magnetic nanoparticles should be colloidally stable

215 in the solvent to prevent their aggregation and the monomer must be soluble in the selected solvent

216 (Diauudin et al. 2020). Due to the limited water solubility of most of the monomers, they are

217 generally dissolved in dilute acids and/or organic solvents, furthermore to avoid agglomeration

218 and to get proper dispersion of magnetic nanoparticles, sonication and/or vigorous stirring of the

219 reaction mixture are normally required during the polymerization process (Scindia et al. 2019).

220 Figure 5 demonstrates the schematic presentation for the in-situ monomer polymerization in the

221 presence of magnetic nanoparticles to get CP-MNCPs.

222 Ammonium persulfate is a typical oxidizing agent used in aniline polymerization in an aqueous

223 acidic media.(Das et al. 2022) Numerous PANI-based NCPs have been reported by incorporating

224 different magnetic nanoparticles into an acidic aniline solution containing APS. The magnetic

225 nanoparticle includes ZnFe2O4, CoFe2O4, NiFe2O4, and Fe3O4 (Donescu et al. 2017; Ghasemi et

226 al. 2022; Henaish et al. 2021; Sadeghpour et al. 2022). APS as an oxidizing agent has also been

227 used by a few researchers for the fabrication of PTh-MNCPs (Figure 6) (Hussain et al. 2020a).

228 Generally, chloroform is used for the solubilization of thiophene. Several scientists have also

229 worked on the in-situ pyrrole polymerization by APS in the dispersion of distinct magnetic

230 nanoparticles. A few examples regarding the synthesis of magnetic nanoparticles-functionalized

231 poly-conducting nanocomposites using APS are also available in the literature (Shahryari et al.

232 2021).

233 The possible aggregation of magnetic nanoparticles due to magnetostatic interactions during the

234 synthesis of composite core-shell particles can be prevented by its treatment with FeCl3 solution

235 (Chen et al. 2003). The Fe3O4 nanoparticles shell acquires a positive charge via the adsorption of

236 a large amount of Fe3+ ions onto the Fe3O4 surface, common ion effect is the likely reason for this

10
237 adsorption. Fe3+ adsorption on the Fe3O4 surface not only prevents nanoparticle agglomeration but

238 also activates the Fe3O4 surface for the polymerization of monomers (Chen et al. 2003). The

239 formed Fe3+ ion shell acts as an oxidizing agent in monomer polymerization to produce CP–Fe3O4

240 core-shell nanocomposites. FeCl3 has been used by many researchers for the fabrication of PPy,

241 and PANI-based nanocomposites (Ghorbani et al. 2013; Phukan et al. 2021).

242 Instead of an aqueous medium, monomer polymerization has also been performed in the presence

243 of suitable surfactants like cetyltrimethylammonium bromide (CTAB), p-toluene sulfonic (TSA),

244 sodium dodecyl sulfate (SDS), sodium dodecylbenzene sulfonate (NaDS), dodecyl benzene

245 sulphonic acid (DBSA), tetramethyl ammonium chloride, and tetramethyl ammonium hydroxide

246 (Diauudin et al. 2020). The concentration of the surfactant must be greater than its critical micellar

247 concentration (CMC), the added surfactant enhances the dispersibility and stability of the magnetic

248 nanoparticles via micellar aggregation. The polymerization of the monomer will take place at the

249 surface of the magnetic nanoparticles with an enhanced rate to produce core-shell structures. The

250 surfactant also improves the smoothness, conductivity, and adhesion power of the substrate of the

251 final nanocomposite (Bulla et al. 2021; Scindia et al. 2019).

252 Emulsification, one of the most reliable and versatile strategies for the controlled fabrication of

253 nanoparticles has also been utilized to synthesize CP-based core-shell nanocomposites (Li et al.

254 2016). In a typical procedure, a transparent surfactant-water-oil-alkyl alcohol (as co-surfactant)

255 micro-emulsion has been prepared under stirring. After sthe dispersion of the magnetic

256 nanoparticles, the oxidative polymerization of the monomer with an oxidizing agent (APS/FeCl3)

257 in the micro-emulsion leads to the formation of CP-MNCPs with core-shell structure (Jiang et al.

258 2010). Various core-shell structures have been reported using distinct water-in-oil micro-

259 emulsions (Abass et al. 2022).

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260 The mechanistic development of the chemical oxidative method for electro-conducting polymer

261 synthesis gives the idea that electro-polymerization with magnetic nanoparticles can also be done

262 via an electrochemical approach (Song et al. 2017). The electrochemical strategy does not require

263 any oxidant, the monomer oxidation is highly influenced by the electrode material while polymer

264 deposition on the electrode depends on the hydrophilic/hydrophobic nature of the electrode and its

265 surface energy (Choudhary et al. 2021). The relatively high potential required for electro-

266 polymerization on nanoparticles is the major limitation of the process. Three electrode cell

267 arrangement (working electrode, reference electrode, and counter electrode) is normally used to

268 perform the electrochemical synthesis of CPs (Unger et al. 2021). The working and counter

269 electrodes are made from inert materials like ITO glass, glassy carbon, graphite, Au, and Pt, while

270 Ag/AgCl or Hg/HgCl2 electrode works as a reference electrode. Polymerization and polymer

271 deposition happens on the working electrode (anode), while the reference electrode controls the

272 cell potential (Pascariu et al. 2015b).

273 Galvanostatic polymerization of PTAA (poly(3-thiophene-acetic-acid)) in Bu4NBF4-nitrobenzene

274 solution on Au-coated quartz crystal (working electrode) at a 3.0 mA/cm2 current density has been

275 performed by Janaky et al. to deposit PTAA-magnetite composite thin films on working electrode

276 (Janáky et al. 2009). In another report 1.0 mA/cm2 current density has been galvanostaticlly

277 applied for the electrochemical cladding of PPy on Fe3O4 nanoparticles surface (Tang et al. 2017).

278 In-situ electrochemical polymerization of pyrrole on TiO2 nanoparticle in SDS aqueous solution

279 by applying constant voltage produces PPy-TiO2 nanocomposite. In the experimental setup, TiO2

280 nanoparticle-coated Ti wire works as an anode and the Pt rod works as a counter electrode (Ma et

281 al. 2021a). PANI has been galvanostaticlly deposited onto nickel nanoparticles-nickel foams

282 (Ni/NF) by applying 0.5 mA/cm2 current density. The formed PANI/Ni/NF nanocomposite exhibit

12
283 excellent performance toward H2 evolution (Song et al. 2017). Pascariu et al. reported the three-

284 electrode arrangement, Ag/AgCl (reference electrode), Pt wire (counter electrode), and ITO glass

285 (working electrode) for the electrochemical deposition of PTh–Ni nanocomposites on the ITO

286 electrode and polymerization of thiophene in acetonitrile solution at 2.5 V of constant potential

287 (Pascariu et al. 2015a). Moreover, the electrochemical deposition of conducting polymers on

288 magnetic nanoparticles has also been performed by other researchers (Lakard 2020).

289 A polymeric film of aniline on Fe2O3 nanoparticles (PANI-IO) has been obtained by plasma

290 polymerization in the absence of a buffer gas using a DC glow discharge reactor. The

291 polymerization of aniline was initiated via ignition of DC glow discharge by applying a discharge

292 current of 30 mA and 1500 V potential between electrodes (Butoi et al. 2022a).

293 Conducting polymer nanocomposite fabrication has also been reported via photo-polymerization

294 of monomers. Poddar et al. performed photo-polymerization of aniline by applying UV irradiation

295 using AgNO3 as the electron acceptor. Uniform dispersion of pyrrole containing AgNO3 and

296 photoinitiator (to increase polymerization rate) with manganese zinc ferrite nanoparticles (MZFO)

297 was prepared and coated onto the glass substrate, the overnight UV-irradiation leads to the

298 formation of PPy-doped MZFO nanocomposite (Poddar et al. 2004).

299 In Situ Fabrication of Magnetic Nanocomposites via fabrication of magnetic NPs into

300 Conducting Polymers

301 In order to enhance the dispersion of semiconductor nanoparticles into the CP, the in situ

302 fabrication of magnetic nanoparticles into the polymeric aqueous solution has been carried out by

303 a few investigators (Das et al. 2019; Maleki et al. 2019; Veisi et al. 2018; Zhang et al. 2020).

304 Because of the insolubility of polyaniline in water, Wan et al. used water-soluble poly(aniline-co-

305 aminobenzenesulfonic acid) (PAOABSA), a copolymer of polyaniline for the in situ synthesis of

13
306 MNCPs. Wan et al. added an aqueous solution of FeCl2 to the alkaline aqueous solution of

307 PAOABSA under stirring and allowed the synthesis of Fe2O3 nanoparticles in the PAOABSA

308 solution (Wan et al. 1998). Wan et al. also synthesized PANI-Fe3O4 nanocomposite by the in situ

309 preparation of Fe3O4 nanoparticles into the pre-synthesized PANI by adding FeSO4 aqueous

310 solution to a polymeric solution of N-methyl pyrrolidone. FeSO4 concentration and the reaction

311 temperature strongly influence the magnetic behavior of the synthesized nanocomposite (Zhang et

312 al. 2017).

313 The well-established co-precipitation method regarding the fabrication of magnetite nanoparticles

314 has been utilized for the synthesis of poly(3-pyrrol-1-ylpropanoic acid) (PPyAA)–Fe3O4

315 nanocomposite, for that pre-synthesized PPyAA and NaOH solution, was added to the Fe(III) and

316 Fe(II) salts solution under vigorous stirring at 80 oC. FT-IR analysis of nanocomposite suggests

317 the monodentate conjugation of polypyrrole acetic acid to the Fe3O4 nanoparticle (Figure 7)

318 (Karaoğlu et al. 2011).

319 Instead of the aqueous solution of polymer, Barbosa et al. suspended PANI in water and the PANI-

320 Fe3O4 nanocomposite was synthesized by the co-precipitation method (Barbosa et al. 2012). Wang

321 et al. proposed a sequential in-situ route for the fabrication of Fe3O4/PPy/PVA nanohydrogels

322 exhibiting both magnetic and conducting properties. Firstly they prepared PPy/PVA hydrogels by

323 oxidative polymerization of pyrrole in PVA aqueous suspension, thereafter co-precipitation

324 approach was employed to synthesize Fe3O4/PPy/PVA nanohydrogels (Wang et al. 2020).

325

326 In-situ synthesis of both conducting polymer and magnetic nanoparticles

327 This strategy involves the polymerization of monomers and the synthesis of magnetic

328 nanoparticles in a single pot for the production of the homogenous nanocomposite. Aphesteguy et

14
329 al proposed a single-step synthesis of PANI/Fe3O4 nanocomposites by adding aniline to a mixed

330 solution of FeCl2 and FeCl3. The pH of the reaction mixture was controlled by NaOH/NH4OH.

331 Simultaneous oxidative polymerization of aniline with FeCl3 and co-precipitation of FeCl2 and

332 FeCl3 in alkaline medium results in a black precipitate of PANI/Fe3O4 nanocomposites (Jacobo et

333 al. 2007). In another approach chemical oxidative polymerization of p-phenylenediamine (pPD)

334 with Fe(NO3)3 and APS in an acidic medium resulted in PpPD-Fe3O4 nanocomposites. Fe2+ formed

335 via the reduction of Fe3+ facilitates the formation of magnetic nanoparticles (Yang et al. 2012).

336 Chemical Vapor Deposition (CVD)

337 Few reports are also available on oxidative polymerization to synthesize CP nanocomposites using

338 Chemical Vapor Deposition (CVD) technique (Dianatdar et al. 2022). The technique involves the

339 deposition of the polymer formed through a chemical reaction on the preselected substrate. The

340 typical polymerization will occur at a high temperature after injecting monomer and oxidant in the

341 gas/vapor phase to the vacuum chamber using an inert gas (N2) as diluent (Rane et al. 2018).

342 Alizadeh et al. synthesized PPy layered copper interdigital electrodes by CVD technique using

343 FeCl3 as oxidant and N2 as carrier gas at room temperature for chemiresistor sensing (Alizadeh et

344 al. 2015). In another work, PANI-coated titania nanotubes (TNT) were prepared via plasma

345 deposition using a rotating-bed plasma-enhanced chemical vapor deposition (RB-PECVD) system.

346 PECVD technique does not require any carrier gas and oxidant, the aniline monomer in the gaseous

347 phase reacts under reduced pressure in the reaction chamber to produce PANI-coated TNT (Butoi

348 et al. 2022b).

349 Spin Coating

350 The spin coating includes the formation of thin films on a solid substrate via the application of

351 centrifugal force. In this technique casting solution was firstly prepared by mixing conducting

15
352 polymer and magnetic nanoparticles in a suitable solvent, thereafter the casting solution was added

353 to the substrate and allowed to spin until the thickness of the casting layer comes to the nano-range

354 (Figure 8). The evaporation of solvent leads to nanocomposite film. Navale et al used the spin

355 coating technique to fabricate PPy-Fe2O3 nanocomposite films on a glass substrate (Navale et al.

356 2014). In a similar way, Sasikumar and Subiramaniyam prepared TiO2/PANI nanocomposites

357 sensor for humidity sensing (Sasikumar et al. 2018). In another research, Sharif et al. reported a

358 spin coating method for the Mg/Zn ferrites nanoparticles incorporation into a polyvinyl alcohol

359 (PVA) network matrix (Sharif et al. 2022). Additionally, using this approach, Chou et al. create a

360 unique polymer ferromagnetic semiconductor film via dispersing Fe3O4 nanoparticles in poly(3-

361 hexylthiophene-2,5-diyl) (P3HT) (Chou et al. 2022).

362

363 Effect of batch parameters on the adsorption of HMIs and dyes

364 The adsorption of HMI and dyes on CP-MNCPs is influenced by a variety of factors. The pH of

365 the solution, the amount of adsorbent used, the interaction time between adsorbate and adsorbent,

366 the concentration of initial HMI or dyes, ionic strength, and the temperature are among these

367 factors (Chávez-Guajardo et al. 2015; Muhammad et al. 2019a; Zare et al. 2018b) . The removal

368 of HMI and dyes may be significantly aided by the optimization of these conditions.

369 The pH is the most critical factor in affecting the adsorption efficiency because the

370 protonation/deprotonation of the adsorbents' surface functional groups, surface charge, and the

371 behavior of the adsorbate ions in solution all affect the interface characteristics of the adsorbent

372 and adsorbate (Mahto et al. 2014; Muhammad et al. 2019a). The solution pH and the CP-MNCPs

373 isoelectric point should be coordinated to maximize the advantages of the adsorption reaction using

374 the CP-MNCPs to remove pollutants. The pH of the solution is referred to as the isoelectric point

16
375 (pI) when there is no net charge on the surface of the CP-MNCPs. When pH > pI, the surface

376 charge of CP-MNCPs is negative, making it suitable for the efficient removal of cationic

377 pollutants. When pH < pI, the CP-MNCPs has a positive charge and can be effectively used for

378 anionic pollutants removal (Dai et al. 2021). The impact of pH on the adsorptive removal of methyl

379 orange (MO) and crystal violet (CV) dyes by magnetic chitosan (MChs)/Ppy nanocomposites has

380 been represented in Figure 9a.

381 A substance that can adsorb molecules of solids, liquids, and gases without undergoing any

382 noticeable alteration of its own physical or chemical properties is referred to as an adsorbent(Zare

383 et al. 2018b). One of the most important factors that influence the accomplishment of the

384 adsorption process is the quantity of the adsorbent used. In general, an increase in adsorbent dose

385 leads to an increase in removal efficiency. However, no significant change in removal efficiency

386 was observed at much higher adsorbent doses (Mohammadi Nodeh et al. 2018b; Sun et al. 2017)

387 . Mashkoor et al. investigated the quantitative impact of chitosan-based magnetic sorbent

388 (MChs/Ppy) on the adsorptive removal of MO and CV dyes (Figure 9b). When the adsorbent

389 amount is increased from 0.4 g to 6.0 g/L, MChs/Ppy exhibits a considerable improvement in the

390 MO removal efficiency from 59.98 to 98.76 % and CV removal efficiency from 48.76 to 95.39 %.

391 Continuously increasing adsorption efficiency is attributed to the more active adsorbing sites and

392 larger adsorbent surface area at higher dosages. However, at higher adsorbent dosages, the

393 adsorbent's active sites overlap and get aggregated causing a decrease in the active adsorbing sites

394 and surface area, resulting in reduced MChs/Ppy adsorption capacity (Mashkoor et al. 2020). This

395 study assisted in determining the optimal adsorbent amount for efficient dye/HMI removal.

396 Electrostatic interactions, including ionic strength, have a significant impact on adsorbent surface

397 properties and, ultimately, adsorption capacity. Changes in ionic strength affect the chemical

17
398 properties of water as well as the electrical properties around the adsorbent's surface. As a result,

399 it is critical to investigate the impact of coexisting ions, particularly when foreign ions and target

400 pollutants compete for adsorption (Dai et al. 2021) . The effect of ionic strength is determined by

401 the charge present on the adsorbent and adsorbate; if both are oppositely charged, adsorption

402 capacity decreases with an increase in ionic strength, exhibiting a negative salt effect (Muhammad

403 et al. 2019c). Muhammad et al. reported that the increase in ionic strength (by Na2SO4) reduces

404 the adsorptive removal of anionic basic blue 3 (BB3) dye on the PANI/Fe3O4 composites (Figure

405 9c). The decrease in adsorption capacity is due to the competition of BB3 dye with Na + or SO42-

406 ions for the PANI/Fe3O4 surface active sites, which ultimately reduces the electrostatic attraction

407 between the positively charged PANI/Fe3O4 composites and anion form of BB3 (Muhammad et

408 al. 2019a). However, when the charge on the adsorbent and dye is identical, an increasing the ionic

409 strength promotes adsorption. Muhammad et al. synthesized PANI/Fe3O4 composite and used it to

410 remove acid blue 40 (AB40) dye from an aqueous solution in the 5-6 pH range. The ionic strength

411 variation shows that the adsorption capacity decreases with added Na2SO4. This is due to a large

412 number of lone-pair electron sites on the PANI/Fe3O4 surface composite, which act as negatively

413 charged groups (Muhammad et al. 2019a) .For efficient adsorption, the initial dye/HMI

414 concentration is a significant parameter in determining the adsorption rate. The initial

415 concentration of the HMI or dye directly influences the amount of dye/HMI that adsorbs (Zare et

416 al. 2018b). The effect of initial dye/HMI concentrations depends on interactions with accessible

417 adsorbent surface sites. Generally, the percentage removal of dye/HMI reduced with increasing

418 starting concentration because the dosage of adsorbent was fixed, limiting the total available active

419 sites and decreasing removal efficiency (Ebrahim et al. 2016; Liang et al. 2018). However, the

420 initial dye/HMI concentration increased adsorption capacity. Higher initial dye/HMI

18
421 concentrations give more driving force needed to overcome the mass transfer barrier of dye/HMI

422 molecules between solid and aqueous phases, resulting in higher adsorption capabilities (Tang et

423 al. 2020).

424 Adsorption is a time-dependent process that is crucial for designing new adsorption systems

425 (Nezhad et al. 2018). The interaction time between dye/HMI with adsorbents allows researchers

426 to determine the potential speed of binding and removal of dye/HMI as well as the ideal window

427 of time for maximum removal (Ebrahim et al. 2016). The adsorption efficiency typically rises with

428 interaction time until it reaches the optimal time, after which it almost remains constant. The initial

429 rapid adsorption is caused by the strong interaction between the dye/HMI molecules and

430 adsorbent’s active sites. The gradual occupation of these surface sites decreased the adsorption

431 rate as the process progressed. The constancy in the adsorption rate is due to the saturation of

432 adsorbent’s surface active sites. This time period is referred to as the “dynamic equilibrium time”.

433 Adsorption and desorption take place simultaneously and at the same rate during the equilibrium

434 time (Muhammad et al. 2019b). The contact time necessary to achieve adsorption equilibrium is a

435 critical economic measure for assessing adsorbent ability, it is dependent on the affinity between

436 the adsorbate and the adsorbent; high affinity required less time.

437 The adsorbent's capacity for dye/HMIs removal is strongly related to the interaction temperature

438 (Mahto et al. 2014). The decreased adsorption capacities of the dye/HMIs with temperature

439 indicate the exothermic nature of adsorption. The decline in adsorption capacities at elevated

440 temperatures is due to the reduction in adsorptive forces between the adsorbent and molecules of

441 dye/HMI. The influence of temperature on the removal of malachite green (MG) dye by the

442 Fe3O4@PANI nanocomposite was studied by Mahto et al. Because the removal efficiency of MG

443 dye decreases with rising temperature, the adsorption is exothermic in nature (Mahto et al. 2014).

19
444 The adsorption, however, reflects the endothermic interactions between the dye/HMI and the

445 adsorbent's active sites if higher solution temperatures enhanced dye/HMI adsorption capacities

446 (Liang et al. 2018). The enhanced diffusion rate of dye/HMI and more availability of active sites

447 at higher temperatures resulted in increased adsorption capacities. Furthermore, as the temperature

448 rises, the viscosity of the solution decreases, accelerating the dye/ HMI diffusion process (Mahto

449 et al. 2014). Taleb et al. investigated the removal of Fe(II), Cu(II), and Mn(II) onto a

450 SiO2/CuFe2O4/PANI nanocomposite at various temperatures. The results show that higher

451 temperatures improve the adsorption capabilities of Fe(II), Cu(II), and Mn(II) ions, demonstrating

452 endothermic interactions between adsorbate and adsorbent. High temperatures are typically not

453 used in the adsorption process because they raise operating costs.

454 Figure 10a, 10b, and 10c demonstrate the influence of starting concentration of HMI, interaction

455 time, and temperature respectively on the adsorption capacity of SiO2/CuFe2O4/PANI for Mn(II),

456 Fe(II), and Cu(II) removal (Taleb et al. 2020).

457 Removal of heavy metal pollutants in wastewater

458 The majority of water contamination is triggered by industrial waste products. Heavy metal ions

459 spresent in this tainted water include chromium, lead, cadmium, nickel, copper, and arsenic.

460 Because of their non-biological degradation, accumulation in living things, and toxicity, the heavy

461 metal ions in surface water are a major environmental concern (Manisalidis et al. 2020; Shrestha

462 et al. 2021b). It is therefore very important to remove the pollutants from wastewater before they

463 are transported and cycled into the environment.

464 Mechanism of removal

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465 The steps to remove Cr(VI) over PANI-nanocomposite (PANI-NCPs) are outlined in Figure 11

466 (Yang et al. 2014). Protonation of the -NH- and =N- groups takes place first in an acidic

467 environment (pH = 2.0), followed by adsorption of HCrO4- (Cr(VI)) onto the adsorbent surface as

468 a result of possible chemical interaction and electrostatic attraction between Cr(VI) and nitrogen

469 species. This was accompanied by the simultaneous oxidation of -NH- to =N- and the reduction

470 of Cr(VI) to Cr(III) (Ebrahim et al. 2016; Krishnani et al. 2013). The redox behavior of =N-/-NH

471 couples, as well as their larger reduction potential as compared to the Cr(VI)/Cr(III) redox couple,

472 were thought to be responsible for the in-situ Cr(VI) reduction (Ebrahim et al. 2016). It is

473 important to note that a small number of Cr(III) may dissolve in water and it could also be removed

474 via chelation with nitrogen-bearing entities in the PANI-NCPs (Jiang et al. 2022). Overall, the

475 Cr(VI) removal takes place simultaneously via in-situ Cr(VI) reduction to Cr(III), and adsorption.

476 This is attributed to the existence of specific functional groups and their redox activity on the

477 PANI-NCPs.

478 Figure 12 is provided to show the mechanism by which PTH-MNCPs removes Hg2+. For the

479 adsorption of Hg2+ on the surface of the PTH-MNCPs, two alternative hypothesized processes are

480 put forward (H. Kamel et al. 2020). The first is physical adsorption on the polythiophene layer's

481 surface or in the adsorbent's porosity. The last process involves chemical adsorption caused by

482 interactions between Hg2+ ions and the PTh layer (H. Kamel et al. 2020).

483 Chromium is a typical heavy metal that not only has detrimental effects on human health but also

484 severely pollutes the environment and is challenging to remove (Sharma et al. 2022a). Chromium

485 has hexavalent Cr(VI), and trivalent Cr(III) oxidation states. In the ecological system, Cr(III) is

486 less mobile and less hazardous to organisms (Uddin et al. 2021). In contrast, the US Environmental

487 Protection Agency has designated Cr(VI) as one of the top-priority hazardous contaminants

21
488 because it is a very dangerous pollutant that can cause cancer and mutation in both humans and

489 animals (Fan et al. 2019). Because of this, its concentration must be lowered to an acceptable level

490 before being released into the environment. For the purpose of adsorptive removal of Cr(VI), Singh

491 and Rachna fabricated CuFe2O4-PANI (CF-PANI) nanocomposite using the in-situ polymerization

492 process. They noted that the adsorption of Cr(VI) reached a maximum value (92%) at pH 2 with

493 an interaction time of 35 min. The results demonstrated that pH increase resulted in a decline in

494 the % elimination of the Cr(VI) ion. Because of protonation, the solution's lower pH causes the

495 surface of the CF-PANI to be positive. This could result in a powerful attraction between the Cr

496 oxyanions and the PANI nanocomposite. Langmuir adsorption isotherm and pseudo-second-order

497 kinetics model were used to describe the adsorption process. Thermodynamic parameters showed

498 that although adsorption occurs spontaneously in nature, it gets decreased as the temperature

499 rises.(Singh et al. 2020b) In another study, Lyu et al. reported the elimination of Cr(VI) by

500 Fe3O4@CL-PANI and CL-PANI@Fe3O4 nanocomposites. The developed absorbents

501 demonstrated highly efficient adsorption capabilities for Cr(VI) ions, mostly by redox reaction and

502 electrostatic interaction, with a maximum adsorption ability observed at pH 2.0, and 318 K.

503 Fe3O4@CL-PANI displayed additional complexing sites for the decreased Cr(III), better

504 adsorption and reduction capacity, and a shorter adsorption equilibrium time as compared to CL-

505 PANI@Fe3O4. PPy/Fe3O4/SiO2 nanocomposite, prepared by the co-precipitation-polymerization

506 method was used for the efficient elimination of Cr(VI) from an aqueous medium (Alzahrani et al.

507 2021; Lyu et al. 2019). The highest adsorption, at pH=4, with an equilibrium contact time of 480

508 min, was observed to be more consistent with the Langmuir model. The regeneration study

509 revealed that the nanocomposite may be utilized to remove Cr(VI) repeatedly. Lei et al. developed

510 a polyaniline@Fe3O4-chitosan (PANI-MCTS) nanocomposite material exhibiting a high

22
511 adsorption capacity of 186.6 mg/g and a good magnetic separation. The Cr(VI) monolayer

512 adsorption on PANI@MCTS was demonstrated to follow pseudo-second-order kinetics (80%

513 elimination within 15 min), and this could be adequately explained by the Langmuir isotherm

514 model. The removal of Cr(VI) proceeds simultaneously via electrostatic interaction between the

515 positively charged nitrogen of PANI@MCTS and Cr(VI) and the redox activity of the prepared

516 material which promotes the chemical reduction of Cr(VI) to Cr(III) (Lei et al. 2020;

517 Pourmortazavi et al. 2019) .

518 Mercury, one of the most toxic metals accumulates up to high concentrations in living beings.

519 Along with extreme toxicity, its possible adsorption through the skin, lungs, and gastrointestinal

520 tract makes mercury one of the most dangerous elements for humans and animals (Cáceres-Saez

521 et al. 2022). The European Union (EU) has established 5 g/L as the upper limit for Hg(II) in

522 wastewater disposal (Danmaliki et al. 2017a; Danmaliki et al. 2017b). Adsorptive removal of

523 Hg(II) from an aqueous solution has been reported by Kamel et al. using CuFe2O4@PTh

524 nanocomposite (H. Kamel et al. 2020). The reported nanocomposite exhibits promising Hg(II)

525 adsorption ability due to strong interactions between the Hg(II) ions and sulfur of thiophene. With

526 an adsorption capacity of 208.77 mg/g, the adsorbent exhibits second-order kinetics and follows

527 the Langmuir model. No significant decrease in the removal efficacy of the nanocomposite was

528 noticed even after five cycles of Hg(II) removal (Falahian et al. 2018). In situ polymerization

529 method was used to fabricate PPy/Fe3O4 nanocomposite for the fast and homogeneous adsorption

530 of Hg(II) (Falahian et al. 2018). The high stability of adsorbent in an acidic medium is extremely

531 helpful for separating mercury from waste streams, which are primarily acidic. The adsorbent had

532 a high adsorption capacity of 173.16 mg g-1 under ideal circumstances. The pseudo-second-order

533 rate model adequately describes the kinetic experimental data (Falahian et al. 2018). Zhao et al.

23
534 prepared a cost-effective novel magnetic nano-adsorbent (CoFe2O4@SiO2-Ppy) to remove of

535 Hg(II) from wastewater. The nano-adsorbent exhibit a remarkable 680.2 mg/g Hg(II) adsorption

536 capability. The spontaneous and endothermic adsorption of Hg(II) on CoFe2O4@SiO2-Ppy

537 followed Langmuir models and pseudo-second-order kinetics (Zhao et al. 2019).

538 Lead is a hazardous element found in industrial waste and water. Even at a 15 μg/L concentration,

539 lead ions in drinking water are dangerous. Sadeghi et al. prepared PANI/Fe3O4 nanocomposite and

540 optimized the process condition as pH = 9.3 and interaction time of 60 min for the removal of lead

541 with the maximum adsorption capability of 111.11 mg/g (Pieper et al. 2017). The pseudo-second-

542 order kinetic model was followed during the lead (II) adsorption. Results showed that the

543 Langmuir isotherm had a high correlation coefficient and described experimental findings better

544 than the Freundlich isotherm (Sadeghi et al. 2018). In another approach Polyaniline

545 tungstomolybdate nanocomposite (PSTM) was synthesized by the sol-gel approach for the

546 successful removal of Pb(II) in an aqueous solution. Pseudo-first-order kinetics was proposed for

547 Pb(II) removal under the optimal conditions of pH = 6-8, Temperature = 40-50 oC, with a contact

548 time of 60 min (Bushra et al. 2015).

549 Arsenic (III), a non-degradable toxic metal can accumulate in living tissues, the food chain, and

550 groundwater and causes serious health issues or even death if consumed in a little amount over an

551 extended period of time. The lowest residual limit for arsenic ions in drinking water was set at 10

552 g/L by the WHO. Nodeh et al. prepared PANI–SrTiO3 magnetic nanocomposite exhibiting high

553 removal efficiency of 95.24 % for As(III). At pH 6, nanocomposites exhibit a high ability (67.11

554 mg/g) to adsorb As(III). Adsorption is governed by pseudo-first-order kinetics and the Langmuir

555 model. Results showed that As(III) will adhere to the adsorbent in a monolayer pattern, followed

556 by an exothermic and physisorption mechanism. Reductive deposition of nano-Fe0 onto the PANI

24
557 nanofibers matrix was used to fabricate PANI/Fe0 nano-sorbent to remove both As(V), and As(III)

558 from aqueous solutions (Mohammadi Nodeh et al. 2018a). The prepared nano-sorbent shows a

559 very high adsorption capacity (232.5 mg/g) at pH 7.0. The mechanisms for the elimination process

560 include surface complexation and electrostatic interactions between arsenic species and PANI/Fe0

561 surface sites.

562 Cadmium, a hazardous heavy metal, found in agricultural, industrial, and natural environments

563 can destroy organs (lungs, liver, and kidneys), and the immune system, and cause heart disease.

564 Tanzif et al. used an oxidative polymerization process to prepare PPy/TiO2 nanocomposite. The

565 nanosorbent exhibit 24.52 mg/g of adsorption capacity at pH 2.5 and follows the Freundlich model

566 (Tanzifi et al. 2017) .

567 Cu(II) is a necessary trace element for life and plays a crucial role in the proper operation of

568 numerous enzymes (Khanvilkar et al. 2021). Accumulation of too much copper is dangerous. It

569 can cause brain damage, liver failure, or death if not treated (Yuan et al. 2021).

570 Polystyrene/Fe3O4@PANI nanocomposite, fabricated by Li et al. shows excellent adsorption

571 properties for Cu(II) in water. The maximal adsorption capacity of nanosorbent is 181.5 mg/g,

572 which is highly dependent on solution pH and contact time. The adsorption of Cu(II) is governed

573 by the Langmuir isotherm model and pseudo-second-order kinetics (Li et al. 2017b). Taleb et al.

574 reported a highly efficient multifunctional SiO2/CuFe2O4/PANI composite for the simultaneous

575 removal of Fe(II), Mn(II), and Cu(II) from environmental water waste. The removal of metal ions

576 proceeds via electrostatic attractions and chelation of metal ions onto the nanocomposite surfaces

577 (Taleb et al. 2020). Makhwedzha et al. used Fe2O3-SiO2-PANI nanocomposite for the adsorptive

578 removal of Cu(II), Cr(III), Al(III), Ba(II), Zn(II), Ni(II), Mn(II), Co(II), and Ti(III) from seawater

579 and synthetic brine samples (Ramutshatsha-Makhwedzha et al. 2019). Nanocomposite exhibit

25
580 98% to 99.9% removal of these metal ions from seawater samples(ABD EL-RAHMAN et al.).

581 Table 1 lists CP-MNCPs for heavy metal removal under different experimental conditions.

582 Removal of dye in wastewater

583 Organic pollutants, such as organic dyes that are typically ecotoxic and non-biodegradable, are

584 more prevalent in wastewater than inorganic contaminants (Kishor et al. 2021; Liu et al. 2020).

585 Among these pollutants, dye-containing wastewater produced by a variety of industries, including

586 those in the cosmetics, textile, leather, plastics, and pharmaceutical sectors (Vashisht et al. 2022),

587 will not only intensify the color of water and affect its perception but will also block sunlight from

588 penetrating the water and consume the dissolved oxygen, which will hinder aquatic organism

589 growth and even lead to the extinction of aquatic flora and fauna, thereby causing long-term

590 adverse effects on the human health and aquatic ecosystem (El-Gaayda et al. 2021). Thus, it is

591 crucial to eliminate or reduce pollutants in dyeing effluents prior to being released into waterways.

592 Polyaniline-based magnetic nanosorbents for dye removal

593 A thorough understanding of the adsorption mechanism is necessary to comprehend the process

594 by which dye is adsorbed onto PANI and PANI-based adsorbents. Adsorbate and adsorbent

595 functional groups, surface and textural characteristics, adsorbate diffusion behavior toward

596 adsorbent, and the manner of their interaction are just a few of the variables that may control the

597 adsorption process. Physisorption, chemisorption, or a combination of the two processes can be

598 used to adsorb dye , depending on how the adsorbent and adsorbate interact with one another

599 (Haque et al. 2020). In many instances, hydrogen bonding, electrostatic attraction, and π–π

600 stacking are involved to carry out the dye adsorption on PANI-based materials.(Samadi et al. 2021)

601 ARS, a commonly used anionic dye, has been used as an adsorbate in Figure 13 to illustrate the

26
602 participation of these interactions on PANI-based adsorbent. The pH of the medium is critical in

603 determining the overall adsorption process.

604 Matho et al. synthesized PANI-modified Fe3O4 nanoparticles for the adsorptive removal of MG, a

605 cationic dye. Electrostatic interaction between the positive portion of the cationic dye and PANI

606 basic sites (imine and amine nitrogens) drove MG dye adsorption into Fe3O4@PANI. Above 7.0,

607 MG dye removal reduced quickly. In acidic mediums, PANI exists as emeraldine salt (protonated

608 quinonoid diimine structures). This PANI salt form had many bipolaron/positively charged

609 polaron sites, which repelled the cationic dye, and resulted in decreased adsorption at lower pH.

610 The higher pH reduced the positive charge on Fe3O4@PANI. Thus, the electrostatic interaction

611 between nanocomposites and cationic dye facilitates dye removal. For initial dye concentration,

612 adsorption increased with contact time and reached equilibrium in 4 h. The decrease in removal

613 efficacy with temperature suggests the exothermic nature of adsorption. Due to the increase in

614 mobility of the dye molecule with temperature, higher temperatures result in less adsorption.

615 Langmuir equation best characterizes MG adsorption on Fe3O4@PANI, according to isotherm

616 modeling. Pseudo-second-order adsorption rates suit kinetic data(Mahto et al. 2014) .

617 In another study, PANI/Fe3O4 composites were used to remove the cationic dye BB3 from an

618 aqueous solution. Due to the synergy between PANI and Fe3O4, PANI/Fe3O4 composites adsorbed

619 a significant quantity of dye (78.13 mg/g) compared to PANI (47.977), and Fe3O4 (7.474 mg/g).

620 Because of the increased surface area and pore volume of hybrid material it exhibits improved

621 adsorption performance. Basic media adsorbed more dye than acidic medium. H+ ions and dye

622 compete for surface active sites (–C–N, and Fe-O) at low pH levels and protonate them. Dye

623 nitrogen and oxygen are also protonated. Adsorption is reduced by electrostatic repulsion between

624 the adsorbent and dye molecule. The dye's oxygen and nitrogen are subsequently protonated,

27
625 which lowers dye adsorption via electrostatic repulsion. At high pH, –C–N–H and Fe–OH

626 deprotonate, creating negatively charged sites like –C–N and Fe–O that interact more strongly with

627 dye and promote adsorption. For PANI/Fe3O4 composites, the equilibrium period of adsorption is

628 attained in 50–60 min. BB3 adsorption on PANI/Fe3O4 composites is maximum at 30 oC and

629 declines afterward, indicating exothermic behavior. Langmuir adsorption isotherm better fits the

630 data while adsorption proceeds via pseudo-second-order kinetics (Muhammad et al. 2019a).

631 PANI, Fe3O4, and PANI/Fe3O4 composite have been employed by Muhammad et al. to remove the

632 anionic dye AB40 from an aqueous solution. SEM images (Figure 14a-f) of Fe3O4, PANI, and

633 PANI/Fe3O4 composites show that the particle size of Fe3O4 and PANI/Fe3O4 are 0.25 µm and

634 0.28 µm respectively. Results demonstrate that the affinity of AB40 dye for PANI is substantially

635 higher than that of Fe3O4 nanoparticles and synthesized composite. The enhanced electrostatic

636 interactions between PANI and dye are liable for the increased dye adsorption. Lone pair electrons

637 on the oxygen in PANI/Fe3O4 composites oppose negatively charged dye and limit adsorption.

638 Adsorption data were better suited by the Freundlich adsorption isotherm model. In acidic

639 environments, the adsorption was significant and exhibited pseudo-second-order kinetics.

640 Adsorption is quick in the first 10–15 min. Strong interactions between adsorbent active sites and

641 dye molecules cause quick initial adsorption. The constancy in the adsorption rate after 40-50

642 minutes is attributed to the saturation of active sites (Muhammad et al. 2019b).

643 Using in situ chemical oxidative polymerization process, NiFe2O4/PANI magnetic composite was

644 synthesized for the removal of alizarine red S (ARS) dye from an aqueous environment (Liang et

645 al. 2018). Maximum ARS adsorption on NiFe2O4/PANI was 186 mg/g at 303 K. Its extraordinary

646 adsorption capability is explained by stronger π-π interaction and weak electrostatic attraction

647 between NiFe2O4/PANI and ARS. Maximum ARS adsorption on NiFe2O4/PANI was 186 mg g-1

28
648 at 303 K. pH impacts the adsorption of ARS, the nanocomposite exhibits maximum adsorption in

649 the 4.0 to 8.6 pH range. When ARS solution pH is below 8.6, it exists in monoanionic or dianionic

650 form, whereas NiFe2O4/PANI is positively charged. The electrostatic interaction between

651 positively charged NiFe2O4/PANI and negative ARS facilitates ARS adsorption. Above pH 8.6,

652 the possible competition between ARS anions and OH- ions for adsorption on NiFe2O4/PANI

653 active sites results in a decrease ARS adsorption. Adsorption is governed by a pseudo-second-

654 order kinetic model. Positive ΔH0 and negative ΔG0 suggest the endothermic and spontaneous

655 behavior of ARS adsorption on NiFe2O4/PANI (Liang et al. 2018) .

656 Rachna et al. prepared and used ZnFe2O4/PANI nanocomposite to remove rhodamine B (RHB)

657 dye from its water solution. pH is the most crucial factor in regulating the adsorption efficacy as it

658 significantly influences the behavior of adsorbate ions and the surface charge of adsorbent in

659 solution. RHB removal by reported nanocomposite dropped from 76% to 6% when pH rose from

660 2 to 10. At low pH levels, the adsorbent surface acquired a positive charge that attracted the anionic

661 RHB dye and facilitate adsorption. At elevated pH, the repulsive forces limit the spontaneous and

662 exothermic removal of dye (Rachna et al. 2018) .

663 Tran et al fabricated Fe3O4-hydrotalcite-PANI (Pan/MHT) composite for MO removal from

664 wastewater. Kinetic results, in agreement with the pseudo-second-order kinetic model, show a

665 maximum adsorption capability of 156:25 mg/g. Surface adsorption or other forms of interactions,

666 like hydrogen bonding, ion exchange, electrostatic interaction, and van der Waals forces, are

667 responsible for MO adsorption onto Pan/MHT composite. The nanocomposite exhibits maximum

668 adsorption capacity in the 3-4 pH range (Tran et al. 2021) .

669 Photocatalytic degradation of carcinogenic indigo carmine (IC) dye by PANI/MgFe2O4, and silica-

670 coated PANI/MgFe2O4 nanocomposite, prepared by self-polymerization of aniline was reported

29
671 by Bashir et al. In comparison to silica-coated PANI/MgFe2O4, PANI/MgFe2O4 composite

672 exhibits higher percentage of IC photo-degradation. Results indicate that photo-degradation is at

673 its highest at pH 2 and that it dramatically decreases in an alkaline medium (Bashira et al. 2019).

674 Mu et al. fabricated superparamagnetic Graphite/PANI/Fe3O4 (GS/PANI/Fe3O4) nanocomposites

675 for the efficient (248.76 mg/g) removal of Congo red (CR) dye. The isoelectric point of the

676 GS/PANI/Fe3O4 nanocomposites was 9.6, showing zero surface charge at this pH. Below 9.6 pH,

677 the nanocomposite exhibits a positive charge. Because of this, the GS/PANI/Fe3O4 composite

678 showed a poor adsorption ratio to cationic brilliant green, but a strong adsorption ratio to anionic

679 CR dye (Mu et al. 2017).

680 Polypyrole-based magnetic adsorbents for dye removal

681 Several researchers have developed polypyrrole-based magnetic nanocomposites to remove

682 different dyes from aqueous solutions. Dye adsorption on polypyrole-based materials generally

683 involves electrostatic interaction and π–π stacking. In Figure 15, ARS, a common anionic dye, was

684 used as an adsorbate to demonstrate the participation of these interactions on Ppy-based adsorbent.

685 In a batch system, PPy-coated iron-doped titania polymerized with itaconic acid [poly(IA)-(Fe-

686 TiO2-PPy)] nanocomposite was utilized by Anirudhan et al. to eliminate tetracycline hydrochloride

687 (TCH) from aqueous solutions. The Langmuir isotherm model best matches the isotherm data,

688 implying that photocatalyst adsorption sites are covered by a monolayer. Pseudo-second-order

689 kinetic model suggested ion exchange followed by complexation. Results showed that pH 5.0 is

690 optimal for adsorption, exploiting H-bonding and electrostatic interactions between the

691 photocatalyst and TCH molecules. Ionic strength reduces adsorption. Swelling experiments show

692 that the maximum swelling occurs at pH 6.5 and that the proportion of swelling increases with

30
693 time. Maximum photo-degradation of TCH was also noticed at 6.5 pH in accordance with the first-

694 order kinetics (Jayachandran 2015) .

695 In another study, Alzahrani et al. synthesized PPy/Fe3O4/SiO2 nanocomposite to remove CR dye

696 from water. Optimal adsorption of 361.43 mg/g for the CR removal was found to be best fitting to

697 the Langmuir model, demonstrating that CR adsorption on the uniform active sites of

698 PPy/Fe3O4/SiO2 nanocomposite followed a monolayer pattern. With increasing contact time, CR

699 removal increases linearly and reaches equilibrium after 480 minutes. At lower pH, the

700 nanocomposite exhibits greater CR removal. Enhanced electrostatic interaction between

701 protonated adsorbent functional groups and negatively charged CR increases CR removal at low

702 pH. Higher pH values result in less effective removal because negatively charged hydroxyl groups

703 compete for adsorption active sites with adsorbate molecules. The regeneration study showed that

704 the nanocomposite can be used multiple times to remove CR, reducing treatment costs (Alzahrani

705 et al. 2021).

706 Magnetic nanocomposite, CNTs-CoFe2O4@PPy, prepared by oxidative polymerization of pyrrole

707 with CNTs-CoFe2O4 (Figure 16(a), and 16 (b)) was utilized by Li et al. for the efficient removal

708 of various anionic dyes (Li et al. 2017a). Methyl Orange (MO), Acid Fuchsin (AF), and Methyl

709 Blue (MB) adsorption data were well fitted to the Langmuir isotherm model, exhibiting adsorption

710 capacities of 132, 116, and 137 mg/g, respectively. Adsorption kinetics are well represented by the

711 pseudo-second-order model. Results show a rapid increase in AR, MO, and MB adsorption

712 capacities on, CNTs-CoFe2O4@PPy at first and then slowly with contact time. MO adsorption on

713 CNTs-CoFe2O4@PPy increased from pH 2.0 to 3.0 and changed slightly above 3.0. More than

714 97% of AR, MO, and MB were removed by CNTs-CoFe2O4@PPy in a pH range of 3.0-9.0 via the

31
715 electrostatic attraction between negatively charged dye and positive nanocomposite surface, and

716 π-π stacking interaction between CNTs' hexagonal skeleton and the dye's aromatic backbone.

717 Alsaiari et al. prepared a novel PPy@Fe3O4-chitosan nanocomposite with several N-containing

718 functional groups for the detoxification of MO from water. Because of its good fit with Langmuir

719 isotherm, MO was adsorbed as a monolayer over PPy@Fe3O4-chitosan nanocomposite. The results

720 show that adsorption increases rapidly with time, reaching saturation after 40 minutes. Low pH

721 increased MO removal capacity due to strong electrostatic interaction between the negative charge

722 of the pollutant and the adsorbent's positive charge. With only a slight decrease in removal

723 efficiency, the reusability study employing 0.1 M NaOH as the eluent demonstrated good

724 reusability up to 5 cycles (Alsaiari et al. 2021) .

725 Nezhad et al. reported a one-step chemical method to fabricate PPy/GO@Fe3O4 magnetic
726 nanocomposite. The nanocomposite exhibits a large adsorption capability of 323.3 mg/g for MB
727 in an aqueous solution and can be magnetically separated from the dye solution. A pH of 8 was
728 shown to be the optimum for MB dye adsorption. Most MB dye adsorption was achieved within
729 10 min, indicating a strong interaction between the adsorbent and dye molecules. The dye
730 adsorption procedure was well fit by Langmuir isotherm and pseudo-second-order kinetic models
731 (Nezhad et al. 2018) .

732 Polythiophene-based magnetic adsorbents for dye removal

733 By in situ chemical oxidative polymerization of thiophene in the presence of NiFe 2O4
734 nanoparticles, Hussain et al. prepared NiFe2O4/PTh nanocomposite to remove Janus green B (JG)
735 and Fuchsin basic (FB) from industrial water waste. Adsorption findings best fit the Langmuir
736 isotherm, indicating homogeneous binding of FB and JG to NiFe2O4/PTh surface. The adsorption
737 kinetics best suit the pseudo-second-order rate process, demonstrating the adsorption of one dye
738 molecule onto two active NiFe2O4/PTh sites. The pH of the dye solution affects adsorption
739 capability. Results show that NiFe2O4/PTh adsorptive capacity rises with solution pH, reaches a
740 maximum at pH 8 and 9 for JG (97.33%) and FB (99.72%) respectively, and thereafter decreases

32
741 with further increase in pH. NiFe2O4 exhibits zero surface charge (pHzpc) at 8.2 pH and is
742 negatively charged above this pH. The greatest removal effectiveness of the composite for FB and
743 JG is approximately at pHzpc, confirming that weak van der Waals forces are prominent for the
744 adsorption process along with π-π, and electrostatic interactions. The thermodynamic parameters
745 support the exothermic, feasible, and overall spontaneity of adsorption (Hussain et al. 2020b) .

746 Kharazi et al. produced ZnFe@PTh nanocomposite by in situ polymerizing thiophene monomers

747 with zinc ferrite nanoparticles. The nanocomposite's surface was subsequently sensitized with

748 porphyrin to create TCPP/ZnFe@PTh. The synthetic nanocomposite exhibits good MB and MO

749 elimination during photocatalytic-adsorption under sunlight and visible LED lamp light, and it can

750 be separated by an external magnet and utilized twice. After 180 minutes of exposure to a visible

751 LED light, UV-Vis spectra of photocatalytic degradation of MO solution at a concentration of 10

752 mgL-1 over TCPP/ZnFe@PTh nanocomposite show that the composite may destroy MO structure

753 by 94% (Kharazi et al. 2018) . Table 2 lists CP-MNCPs for dye removal under different

754 experimental conditions.

755 Conclusion and future perspective

756 This review provides a detailed introduction to the typical synthesis approaches of CPs-magnetic
757 nanocomposites, followed by a discussion of the utilization of composites for removing HMIs and
758 dyes from wastewater. The review also explains how the pH of the solution and the chemical
759 nature of the HMIs/dyes affect the process of adsorption on different nanosorbent. The adsorption
760 efficiency of HMIs/dyes on nanosorbents varies significantly with the pH of the solution,
761 adsorbent dose, ionic strength, adsorbent concentration, interaction time, and temperature of the
762 system, pH of the solution is the most important factor that strongly influences the adsorption
763 efficiency. This study attempts to establish the theoretical underpinnings for the use of CPs-
764 MNCPs in real-world wastewater treatment and offers fresh concepts for developing highly
765 effective conducting polymer-based nanosorbents.

766 A variety of nanosorbents based on CPs and their derivatives have been investigated for their
767 potential to remove HMIs (Cu(II), Cr(VI), Fe(II), Hg(II), As(III), Mn(II), Pb(II), and Cd(II)) and

33
768 dyes (MO, CR, BR, MB, MG, BB3, AB40, IC, ARS, RB, AG, AF, CV, TCH) from wastewater.
769 The most extensively researched HMI using CPs nanocomposite as an adsorbent is Cr(VI). Among
770 CPs-MNCPs, PANI/Fe3O4/SiO2, and CL/PANI/Fe3O4 were the most effective at removing Cr(VI).
771 Other SiO2-based nanocomposites, PANI/SiO2/CuFe2O4 and Ppy/SiO2/CoFe2O4 demonstrated the
772 highest adsorption capacity for Mn(II)/Fe(II), and Hg(II) removal. Hybrid CPs-MNCPs like
773 PANI/MWCNTs/Fe3O4, Ppy/GO/Fe3O4, Ppy/SiO2/Fe3O4 show much higher adsorption capacity
774 for dye removal compared to other metal oxides/CPs nanocomposites.

775 Numerous research articles on CPs-magnetic nanosorbents for the removal of HMIs and dyes have
776 been published. According to the current state of CPs nanocomposites for wastewater remediation,
777 the following are the future prospects for achieving optimal adsorbent performance:

778  Each research finding needs to be expanded from in-lab studies to industrial applications
779 and must also be environmentally and socially responsible. Therefore, in addition to the adsorption
780 capacity, selectivity of pollutant adsorption, and recyclability, large-scale studies with the
781 developed nanocomposites should be performed to determine its operational cost for the treatment
782 of real wastewater.
783  Results show that the combination of SiO2, GO, and MWCNTs with CPs-MNCPs enhances
784 the adsorption capacity of nanocomposites to a large extent, so future research should lean toward
785 the development of cost-effective hybrid CPs-nanocomposites.
786  As we know that the presence of numerous functional groups viz. NH2, C=N, -S-, -NH-,
787 and OH on the surface of CPs nanocomposites facilitate the adsorption of metal ions. The
788 selectivity and adsorption efficiency of the CPs-nanocomposites can be improved by the
789 incorporation of selected functional groups.
790  In contrast to polythiophenes, nanocomposites of polyaniline and polypyrrole have
791 received much more attention as potential adsorption enhancers. Therefore, polythiophenes
792 nanocomposites may offer new avenues to decontaminate wastewater from HMIs and dyes.
793  Several batch parameters viz. pH, adsorbent dose, ionic strength, adsorbent concentration,
794 interaction time, and temperature are investigated to evaluate the impact on removal efficiency of
795 HMIs and dyes. The current laboratory research is primarily directed toward eliminating one or
796 more specific pollutants. To remove competing pollutants simultaneously, a more in-depth study
797 of CPs-magnetic nanocomposites is also required.

34
798 Funding
799 The authors declare that no funds, grants, or other support were received during the preparation of

800 this manuscript.

801 Competing interests

802 The authors have no relevant financial or non-financial interests to disclose.

803 Author Contributions

804 All authors contributed to the study conception and design. Data collection and analysis were

805 performed by [Abhishek Srivastava], [Madhav Krishna Goswami], [Rajeev Kumar Dohare],

806 [Anjani Kumar Tiwari], and [Anupam Srivastava]. The first draft of the manuscript was written

807 by [Abhishek Srivastava], [Madhav Krishna Goswami], [Rajeev Kumar Dohare], [Anjani Kumar

808 Tiwari], and [Anupam Srivastava], and all authors commented on previous versions of the

809 manuscript. All authors read and approved the final manuscript.”

810 Ethical Approval: No ethical approval is required regarding this manuscript.

811
812 Consent to Participate: No consent is required regarding this manuscript
813
814 Consent to Publish: Corresponding author have taken prior consent from the corresponding
815 author and publisher whose data and figures are used in the manuscript.
816
817 Availability of data and materials: We have not generated any data as it is a review article.
818
819
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Figure 1: Techniques to remove HMIs and dyes from wastewater Click here to access/download;Figure;Figure 1.tiff
Figure 2: Proposed mechanistic scheme for polymerization of pyrrole Click here to access/download;Figure;Figure 2.tiff
Figure 3: Important approaches for the fabrication of conducting polymer-based MNCs Click here to access/download;Figure;Figure 3.tiff
Figure 4: Illustration for preparation of CP-MNCPs by pre-synthesized CPs and Click here to access/download;Figure;Figure 4.tiff
magnetic nanoparticles
Figure 5: Schematic presentation for the in-situ monomer polymerization in the Click here to access/download;Figure;Figure 5.tiff
presence of magnetic nanoparticles
Figure 6: Illustrative representation for fabrication of PTh-MNCPs nanocomposites Click here to access/download;Figure;Figure 6.tiff
Figure 7: Illustrative representation of the preparation of magnetic nanoparticles with Click here to access/download;Figure;Figure 7.tiff
pre-synthesized conducting polymer to get conducting polymer nanocomposite
Figure 8: Spin coating of CP-MNCPs on glass Click here to access/download;Figure;Figure 8.tiff
Figure 9: (a) pH dependence on adsorption capacity of MChs/PPy for MO and CV dyes Click here to access/download;Figure;Figure 9.tiff
(b) Ionic strength dependence on adsorption capacity of PANI-Fe3O4 for BB3 dye (c)
Figure 10: Influence of (a) HMIs Initial concentration (b) Interaction time (c) Click here to access/download;Figure;Figure 10.tiff
Temperature, on adsorption capacity of SiO2/CuFe2O4/PANI for Mn(II), Fe(II), and
Figure 11: Possible pathways of Cr(VI) adsorption onto a PANI-NCPs Click here to access/download;Figure;Figure 11.tiff
Figure 12: Possible pathways of Hg(II) adsorption onto a PTh- Click here to access/download;Figure;Figure 12.tiff
MNCPs
Figure 13: Possible pathways of ARS dye adsorption onto a PANI Click here to access/download;Figure;Figure 13.tiff
Figure 14: SEM images of Fe3O4, PANI, and PANI/Fe3O4 Click here to access/download;Figure;Figure 14.tiff
composites before (a, c, e) and after (b, d, f) adsorption of BB3
Figure 15: Possible pathways of ARS dye adsorption onto a Click here to access/download;Figure;Figure 15.tiff
polypyrrole
Figure 16: (a) SEM image of CNTs-CoFe2O4@PPy, (b) TEM image of CNTs- Click here to access/download;Figure;Figure 16.tiff
CoFe2O4@PPy. Reproduced with permission from Ref. [Li et al. 2017]. Copyright
Graphical Abstract Click here to access/download;Figure;Graphical Abstract.tiff
Tables

Table 1. Conducting polymer based nanosorbents for the removal of heavy metal pollutants
Magnetic Nanosorbent Adsorbate Equilibrium Tempe pH Ionic Remov Adsorption Reusability Ref.
Time rature, strength al, % Capacity
o
C (mg/g)
---- >90 Decreased by
PPY-SiO2/CoFe2O4 Hg(II) 8h 25 8 680.2 12.7% after five [54]
adsorption cycles
---- 92.0 60% adsorption
PANI-CuFe2O4 Cr(VI) 35 25 2 ---- capacity retained [162]
after 4 cycles
---- - 90% adsorption
PANI-Fe3O4 Cr(VI) 12 h 25 2 200 capacity retained [194]
after 5 cycles
PANI-β-FeOOH Cr(VI) 5 min 25 2 ---- 99.2% 17.36 - [150]
PANI-NiFe2O4 Cr(VI) - 35 2 ---- - ---- - [195]
---- 95% adsorption
CL-PANI -Fe3O4 Cr(VI) Cr(III) 150 min 45 2 358.8 capacity retained [58]
after 10 cycles
---- 100 Can be reused for 4
Cr(VI) 208.8
PPy/γ-Fe2O3 15min 25 2 adsorption cycle [142]
Cr(II) 170.7
---- 98 90% adsorption
480 min capacity retained
PPy-Fe3O4/SiO2 Cr(VI) 25 3 361.43 after 6 cycles [196]

---- 99.74 89.8% adsorption

PPy-Fe3O4/AgCl Cr(VI) 30-180 25 2 111 capacity retains [147]
after 3 cycles
---- ---- 83% adsorption
PANI-PS/Fe3O4 Cu (II) 120 min 25 5 181.5 capacity retained [177]
after 7 cycles
Cu(II) ---- 5.0 ---- ---- 285.71 Can be reused after
PANI-SiO2/CuFe2O4 Fe(II) 50 5.18 416.67 4 cycle with 2-3 % [153]
Mn(II) 5.3 454.55 decrease
PANI-SiO2/Fe2O3 Cu(II) ---- 25 6 ---- 99.6 113.99 - [197]
 ---- 79.5% adsorption
PANI-SrTiO3 As(III) 150 min 25 6 95.24 67.11 capacity retained [173]
after 10 cycles
---- ---- 98.41 Can be reused for 3
adsorption cycle
PANI-Fe(0) As(III) 25 7 235.5 [198]

---- 99.08 Can be reused for 5

60 min adsorption cycle
PANI-Fe3O4 As(III) 25 8 10.66 [199]

---- ---- 90% adsorption

PPy- Fe3O4 Hg(II) 150 min 55 2.4 173.16 capacity retained [169]
after 1 cycles
---- ---- -
PTh-CS/Fe3O4 Hg(II) 60 min 25 7 53.763 [200]
---- 99.97 97.4% adsorption
capacity retained
PTh-CuFe2O4 Hg(II) 30 min 25 7 208.77 after 5 cycles [158]

---- 96 ----
PANI-Fe3O4 Pb(II) 60 min 25 9 111.11 [171]

PANI-Sn(IV)- ---- ---- ----

Pb(II) 20 6 44.64 [172]
tungstomolybdate 58 min
PPy-TiO2 Cd(II) - 25 2.5 ---- 82.2 24.52 ---- [127]
PANI-MnO2/Fe3O4 Cd(II) 30 min 25 6.3 ---- 99.1 428 ---- [201]
Table 2. Conducting polymer based nanosorbents for the removal of dyes

Magnetic Adsorbate Equilibrium Temperature, pH Ionic Removal, Adsorption Reusability Ref.

o
Nanosorbent Time C strength % Capacity
(mg/g)
MWCNTs/Fe3O4/PANI MO ---- 25 4 ---- ---- 544.99 Adsorption [202]
CR 417.38 capacity
decreased
slightly after 4
cycles
Clay/PANI/Fe3O4 BR 6.3 ---- 96.2 - No decrease in [203]
adsorption
MB 30 min 25 6.3 ---- 99.6 184.48 capacity after 5
cycles
CR 6.3 ---- 98.12

Fe3O4@PANI MG 240 min 25 7 ---- 95 240 95% adsorption [144]

capacity retained
after 1 cycles
PANI/Fe3O4 BB3 - 30 10 0.25 ---- 78.13 - [143]
PANI/Fe3O4 AB40 40-50 min 30 2-12 ---- ---- 216.9 - [152]

GS-PANI-Fe3O4 Congo red 120 min ---- <4 ---- 92.4 248.76 No decrease in [189]
adsorption
capacity after 5
cycles
PANI/Fe3O4 MO 120 min 25 3-4 ---- 65.97 156.25 Can be reused [187]
after 4 cycle

PANI/MgFe2O4 Indigo- car- 60 min ---- 2 ---- 97.52 ---- Can be reused [188]
after 5 cycle
PANI/NiFe2O4 ARS 60-90 min 30 8.6 0-4 93.8 to 186 82% adsorption [151]
81.9 capacity retained
after 6 cycles
 PANI–NiFe2O4 MG 210 25 7 ---- 95.2 4.09 ---- [204]

PANI-ZnFe2O4 RHB ---- 25 2 ---- 85 - 70% adsorption [186]

capacity retained
after 4 cycles
CS–PPy–Fe3O4 AG 60 25 5.4 ---- 96 26.2 - [205]
PPy-CNTs-CoFe2O4 MB ---- 25 ---- ---- 137 116 132 Good reusability [191]
MO
AF
PPy-CS-Fe3O4 CV ---- 29 7 ---- 88.11 62.89 89.29 ---- [148]
MO 92.89

PPy-CS-Fe3O4 MO ---- 25 4.5 ---- ---- 95 62 % adsorption [192]

capacity retained
after 3 cycles
PPy–CS–Fe3O4 CBZ 25 25 6.5- ---- 94.5 121.95 Can be reused [206]
10 after 5 cycle
PPy/GO@Fe3O4 MB 10 25 8 ---- 90 323.2 58 % adsorption [62]
capacity retained
after 5 cycles
poly(IA)-(Fe-TiO2- TCH 180 30 2-10 ---- ---- 149.25 ---- [207]
PPy)
PPy/Fe3O4/SiO2 CR ---- 25 3-4 ---- 99 361 72 % adsorption [163]
capacity retained
after 3 cycles
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