Abstract
A sulfur-coated magnetic multi-walled carbon nanotube (S-M-MWCNT) composite was synthesized via coating a thin S layer on M-MWCNTs via a facile heating process. The prepared superparamagnetic adsorbent was employed for the uptake of mercury(II) (Hg(II)) from aqueous solutions and then magnetically separated without filtration or centrifugation steps. The adsorption of Hg(II) increased with increasing pH and reached a plateau value in the pH range 4.5–8.0. The adsorption kinetics followed the pseudo-second-order (PSO) model and equilibrium was reached within 3 h. The isotherm data obeyed the Langmuir isotherm model, and the maximum adsorption capacity of S-M-MWCNT adsorbent was acquired as 62.11 mg g−1. The adsorption of Hg(II) by the prepared composite is possibly controlled by the interaction between Hg(II) as a soft acid and elemental coated sulfur as a soft base. In addition, the coexist metal ions including copper(II) (Cu(II)), cadmium(II) (Cd(II)), cobalt(II) (Co(II)), lead(II) (Pb(II)), manganese(II) (Mn(II)), zinc(II) (Zn(II)), and chromium(III) (Cr(III)) had no significant effects on Hg(II) removal performance. It was found that the S-M-MWCNT composite could be reused after successive Hg(II) removal without any loss of adsorption capacity. Furthermore, the magnetic adsorbent holds high potential in the treatment of Hg-contaminated wastewater samples.
Similar content being viewed by others
References
Ahmad M, Manzoor K, Chaudhuri RR, Ikram S (2017) Thiocarbohydrazide cross-linked oxidized chitosan and poly (vinyl alcohol): a green framework as efficient Cu (II), Pb (II), and Hg (II) adsorbent. J Chem Eng Data 62:2044–2055
Arvand M, Hassannezhad M (2014) Magnetic core–shell Fe3O4@SiO2/MWCNT nanocomposite modified carbon paste electrode for amplified electrochemical sensing of uric acid. Mater Sci Eng C 36:160–167
Bai H, Zheng Y, Wang T, Peng N (2016) Magnetic solvent-free nanofluid based on Fe3O4/polyaniline nanoparticles and its adjustable electric conductivity. J Mater Chem A 4:14392–14399
Bandaru NM, Reta N, Dalal H, Ellis AV, Shapter J, Voelcker NH (2013) Enhanced adsorption of mercury ions on thiol derivatized single wall carbon nanotubes. J Hazard Mater 261:534–541
Blue LY, Jana P, Atwood DA (2010) Aqueous mercury precipitation with the synthetic dithiolate, BDTH2. Fuel 89:1326–1330
Bower J, Savage KS, Weinman B, Barnett MO, Hamilton WP, Harper WF (2008) Immobilization of mercury by pyrite (FeS2). Environ Pollut 156:504–514
Chen K, Zhang Z, Xia K, Zhou X, Guo Y, Huang T (2019) Facile synthesis of thiol-functionalized magnetic activated carbon and application for the removal of mercury (II) from aqueous solution. ACS Omega 4:8568–8579
Chen PH, Hsu C-F, Tsai DD-W, Lu Y-M, Huang W-J (2014) Adsorption of mercury from water by modified multi-walled carbon nanotubes: adsorption behaviour and interference resistance by coexisting anions. Environ Technol 35:1935–1944
Chen S-R, Zhai Y-P, Xu G-L, Jiang Y-X, Zhao D-Y, Li J-T, Huang L, Sun S-G (2011) Ordered mesoporous carbon/sulfur nanocomposite of high performances as cathode for lithium–sulfur battery. Electrochim Acta 56:9549–9555
Chiarle S, Ratto M, Rovatti M (2000) Mercury removal from water by ion exchange resins adsorption. Water Res 34:2971–2978
Das SK, Das AR, Guha AK (2007) A study on the adsorption mechanism of mercury on Aspergillus versicolor biomass. Environ Sci Technol 41:8281–8287
Deng S, Zhang G, Wang X, Zheng T, Wang P (2015) Preparation and performance of polyacrylonitrile fiber functionalized with iminodiacetic acid under microwave irradiation for adsorption of Cu (II) and Hg (II). Chem Eng J 276:349–357
Deshpande AS, Khomane RB, Vaidya BK, Joshi RM, Harle AS, Kulkarni BD (2008) Sulfur nanoparticles synthesis and characterization from H2S gas, using novel biodegradable iron chelates in W/O microemulsion. Nanoscale Res Lett 3:221
Fayazi M, Afzali D, Taher M, Mostafavi A, Gupta V (2015a) Removal of Safranin dye from aqueous solution using magnetic mesoporous clay: optimization study. J Mol Liq 212:675–685
Fayazi M, Ghanei-Motlagh M, Taher MA (2015b) The adsorption of basic dye (Alizarin red S) from aqueous solution onto activated carbon/γ-Fe2O3 nano-composite: kinetic and equilibrium studies. Mater Sci Semicond Process 40:35–43
Fayazi M, Taher MA, Afzali D, Mostafavi A (2015c) Preparation of molecularly imprinted polymer coated magnetic multi-walled carbon nanotubes for selective removal of dibenzothiophene. Mater Sci Semicond Process 40:501–507
Fayazi M, Taher MA, Afzali D, Mostafavi A (2015d) Removal of dibenzothiophene using activated carbon/γ-Fe2O3 nano-composite: kinetic and thermodynamic investigation of the removal process. Anal Bioanal Chem Res 2:73–84
Fayazi M, Taher MA, Afzali D, Mostafavi A (2016a) Fe3O4 and MnO2 assembled on halloysite nanotubes: a highly efficient solid-phase extractant for electrochemical detection of mercury (II) ions. Sensors Actuators B Chem 228:1–9
Fayazi M, Taher MA, Afzali D, Mostafavi A, Ghanei-Motlagh M (2016b) Synthesis and application of novel ion-imprinted polymer coated magnetic multi-walled carbon nanotubes for selective solid phase extraction of lead (II) ions. Mater Sci Eng C 60:365–373
Fayazi M, Ghanei-Motlagh M (2017) Synthesis and application of novel modified magnetic nanocomposite for solid phase extraction of thallium(I) ions. Anal Bioanal Chem Res 4:189–200
Fayazi M, Afzali D, Ghanei-Motlagh R, Iraji A (2019) Synthesis of novel sepiolite–iron oxide–manganese dioxide nanocomposite and application for lead (II) removal from aqueous solutions. Environ Sci Pollut Res 26:18893–18903
Fiyadh SS, AlSaadi MA, Jaafar WZ, AlOmar MK, Fayaed SS, Mohd NS, Hin LS, El-Shafie A (2019) Review on heavy metal adsorption processes by carbon nanotubes. J Clean Prod 230:783–793
Gao X, Li J, Guan D, Yuan C (2014) A scalable graphene sulfur composite synthesis for rechargeable lithium batteries with good capacity and excellent columbic efficiency. ACS Appl Mater Interfaces 6:4154–4159
Ghanei-Motlagh M, Fayazi M, Taher MA (2014) On the potentiometric response of mercury (II) membrane sensors based on symmetrical thiourea derivatives-experimental and theoretical approaches. Sensors Actuators B Chem 199:133–141
Gupta A, Vidyarthi S, Sankararamakrishnan N (2014) Enhanced sorption of mercury from compact fluorescent bulbs and contaminated water streams using functionalized multiwalled carbon nanotubes. J Hazard Mater 274:132–144
He F, Wang W, Moon J-W, Howe J, Pierce EM, Liang L (2012) Rapid removal of Hg (II) from aqueous solutions using thiol-functionalized Zn-doped biomagnetite particles. ACS Appl Mater Interfaces 4:4373–4379
Henneberry YK, Kraus TE, Fleck JA, Krabbenhoft DP, Bachand PM, Horwath WR (2011) Removal of inorganic mercury and methylmercury from surface waters following coagulation of dissolved organic matter with metal-based salts. Sci Total Environ 409:631–637
Huang L, Shuai Q (2019) Facile approach to prepare sulfur-functionalized magnetic amide-linked organic polymers for enhanced Hg (II) removal from water. ACS Sustain Chem Eng 7:9957–9965
Huttenloch P, Roehl KE, Czurda K (2003) Use of copper shavings to remove mercury from contaminated groundwater or wastewater by amalgamation. Environ Sci Technol 37:4269–4273
Jainae K, Sukpirom N, Fuangswasdi S, Unob F (2015) Adsorption of Hg (II) from aqueous solutions by thiol-functionalized polymer-coated magnetic particles. J Ind Eng Chem 23:273–278
Ji L, Rao M, Zheng H, Zhang L, Li Y, Duan W, Guo J, Cairns EJ, Zhang Y (2011) Graphene oxide as a sulfur immobilizer in high performance lithium/sulfur cells. J Am Chem Soc 133:18522–18525
Jung C, Heo J, Han J, Her N, Lee S-J, Oh J, Ryu J, Yoon Y (2013) Hexavalent chromium removal by various adsorbents: powdered activated carbon, chitosan, and single/multi-walled carbon nanotubes. Sep Purif Technol 106:63–71
Kończyk J, Żarska S, Ciesielski W (2019) Adsorptive removal of Pb (II) ions from aqueous solutions by multi-walled carbon nanotubes functionalised by selenophosphoryl groups: kinetic, mechanism, and thermodynamic studies. Colloids Surf A Physicochem Eng Asp 575:271–282
Langmuir I (1916) The constitution and fundamental properties of solids and liquids. Part I Solids J Am Chem Soc 38:2221–2295
Li R, Liu L, Yang F (2014) Removal of aqueous Hg (II) and Cr (VI) using phytic acid doped polyaniline/cellulose acetate composite membrane. J Hazard Mater 280:20–30
Liu L, Ding L, Wu X, Deng F, Kang R, Luo X (2016) Enhancing the Hg (II) removal efficiency from real wastewater by novel thymine-grafted reduced graphene oxide complexes. Ind Eng Chem Res 55:6845–6853
Luo F, Chen JL, Dang LL, Zhou WN, Lin HL, Li JQ, Liu SJ, Luo MB (2015) High-performance Hg2+ removal from ultra-low-concentration aqueous solution using both acylamide-and hydroxyl-functionalized metal-organic framework. J Mater Chem A 3:9616–9620
Mallakpour S, Abdolmaleki A, Borandeh S (2014) l-Phenylalanine amino acid functionalized multi walled carbon nanotube (MWCNT) as a reinforced filler for improving mechanical and morphological properties of poly (vinyl alcohol)/MWCNT composite. Prog Org Coat 77:1966–1971
Mallakpour S, Behranvand V (2017a) Water sanitization by the elimination of Cd2+ using recycled PET/MWNT/LDH composite: morphology, thermal, kinetic, and isotherm studies. ACS Sustain Chem Eng 5:5746–5757
Mallakpour S, Behranvand V (2017b) Sono-assisted preparation of bio-nanocomposite for removal of Pb2+ ions: study of morphology, thermal and wettability properties. Ultrason Sonochem 39:872–882
Manohar D, Krishnan KA, Anirudhan T (2002) Removal of mercury (II) from aqueous solutions and chlor-alkali industry wastewater using 2-mercaptobenzimidazole-clay. Water Res 36:1609–1619
Mehta D, Mazumdar S, Singh SK (2015) Magnetic adsorbents for the treatment of water/wastewater-a review. J Water Process Eng 7:244–265
Moghaddam HK, Pakizeh M (2015) Experimental study on mercury ions removal from aqueous solution by MnO2/CNTs nanocomposite adsorbent. J Ind Eng Chem 21:221–229
Mustafa S, Dilara B, Nargis K, Naeem A, Shahida P (2002) Surface properties of the mixed oxides of iron and silica. Colloids Surf A Physicochem Eng Asp 205:273–282
Nie Z-y, Liu H-c, Xia J-l, Zhu H-r, Ma C-y, Zheng L, Zhao Y-d, Qiu G-z (2014) Differential utilization and transformation of sulfur allotropes, μ-S and α-S8, by moderate thermoacidophile Sulfobacillus thermosulfidooxidans. Res Microbiol 165:639–646
Pang L-j, Hu J-t, Zhang M-j, Yang C-g, Wu G-z (2018) An efficient and reusable quaternary ammonium fabric adsorbent prepared by radiation grafting for removal of Cr (VI) from wastewater. Environ Sci Pollut Res 25:11045–11053
Parr RG, Pearson RG (1983) Absolute hardness: companion parameter to absolute electronegativity. J Am Chem Soc 105:7512–7516
Rao MM, Reddy DK, Venkateswarlu P, Seshaiah K (2009) Removal of mercury from aqueous solutions using activated carbon prepared from agricultural by-product/waste. J Environ Manag 90:634–643
Reddy MLP, Francis T (2001) Recent advances in the solvent extraction of mercury (II) with calixarenes and crown ethers. Solvent Extr Ion Exch 19:839–863
Salam MA, Mohamed RM (2013) Removal of antimony (III) by multi-walled carbon nanotubes from model solution and environmental samples. Chem Eng Res Des 91:1352–1360
Saleh TA (2015) Isotherm, kinetic, and thermodynamic studies on Hg (II) adsorption from aqueous solution by silica-multiwall carbon nanotubes. Environ Sci Pollut Res 22:16721–16731
Saman N, Johari K, Mat H (2013) Adsorption characteristics of sulfur-functionalized silica microspheres with respect to the removal of Hg (II) from aqueous solutions. Ind Eng Chem Res 53:1225–1233
Shetty D, Boutros S, Eskhan A, De Lena AM, Skorjanc T, Asfari Z, Traboulsi H, Mazher J, Raya J, Banat F, Trabolsi A (2019) Thioether-crown-rich calix[4] arene porous polymer for highly efficient removal of mercury from water. ACS Appl Mater Interfaces 11:12898–12903
Sun Y, Yang S, Sheng G, Guo Z, Wang X (2012) The removal of U (VI) from aqueous solution by oxidized multiwalled carbon nanotubes. J Environ Radioact 105:40–47
Tang SCN, Lo IMC (2013) Magnetic nanoparticles: essential factors for sustainable environmental applications. Water Res 47:2613–2632
Tang W-W, Zeng G-M, Gong J-L, Liu Y, Wang X-Y, Liu Y-Y, Liu Z-F, Chen L, Zhang X-R, Tu D-Z (2012) Simultaneous adsorption of atrazine and Cu (II) from wastewater by magnetic multi-walled carbon nanotube. Chem Eng J 211:470–478
Thakur S, Das G, Raul PK, Karak N (2013) Green one-step approach to prepare sulfur/reduced graphene oxide nanohybrid for effective mercury ions removal. J Phys Chem C 117:7636–7642
Tian S, Yin Y, Cao Z, Yue H, Yang S (2018) Sulfur grown around carbon nanotubes as a cathode material for Li/S battery. Ionics 24:33–41
Trofimov BA, Sinegovskaya LM, Gusarova NK (2009) Vibrations of the S–S bond in elemental sulfur and organic polysulfides: a structural guide. J Sulfur Chem 30:518–554
Vikrant K, Kim K-H (2018) Nanomaterials for the adsorptive treatment of Hg (II) ions from water. Chem Eng J 358:264–282
Vuković GD, Marinković AD, Čolić M, Ristić MĐ, Aleksić R, Perić-Grujić AA, Uskoković PS (2010) Removal of cadmium from aqueous solutions by oxidized and ethylenediamine-functionalized multi-walled carbon nanotubes. Chem Eng J 157:238–248
Wang J, Deng B, Wang X, Zheng J (2009) Adsorption of aqueous Hg (II) by sulfur-impregnated activated carbon. Environ Eng Sci 26:1693–1699
Xu P, Zeng GM, Huang DL, Feng CL, Hu S, Zhao MH, Lai C, Wei Z, Huang C, Xie GX, Liu ZF (2012) Use of iron oxide nanomaterials in wastewater treatment: a review. Sci Total Environ 424:1–10
Yang J, Wu J-X, Lü Q-F, Lin T-T (2014) Facile preparation of lignosulfonate–graphene oxide–polyaniline ternary nanocomposite as an effective adsorbent for Pb (II) ions. ACS Sustain Chem Eng 2:1203–1211
Yang S, Li J, Shao D, Hu J, Wang X (2009) Adsorption of Ni (II) on oxidized multi-walled carbon nanotubes: effect of contact time, pH, foreign ions and PAA. J Hazard Mater 166:109–116
Zeng H, Wang L, Zhang D, Yan P, Nie J, Sharma VK, Wang C (2019) Highly efficient and selective removal of mercury ions using hyperbranched polyethylenimine functionalized carboxymethyl chitosan composite adsorbent. Chem Eng J 358:253–263
Zhang C, Sui J, Li J, Tang Y, Cai W (2012) Efficient removal of heavy metal ions by thiol-functionalized superparamagnetic carbon nanotubes. Chem Eng J 210:45–52
Zhang F-S, Nriagu JO, Itoh H (2005) Mercury removal from water using activated carbons derived from organic sewage sludge. Water Res 39:389–395
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Tito Roberto Cadaval Jr
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
ESM 1
(DOCX 285 kb)
Rights and permissions
About this article
Cite this article
Fayazi, M. Removal of mercury(II) from wastewater using a new and effective composite: sulfur-coated magnetic carbon nanotubes. Environ Sci Pollut Res 27, 12270–12279 (2020). https://doi.org/10.1007/s11356-020-07843-z
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-020-07843-z