Different approaches for preparing a novel thiol-functionalized graphene oxide/Fe-Mn and its application for aqueous methylmercury removal

被引:135
作者
Huang, Yao [1 ]
Tang, Jingchun [1 ]
Gai, Longshuang [1 ]
Gong, Yanyan [2 ]
Guan, Hongwei [3 ]
He, Ruozhu [1 ]
Lyu, Honghong [1 ]
机构
[1] Nankai Univ, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria, Minist Educ,Tianjin Engn Ctr Environm Diag & Cont, Tianjin 300350, Peoples R China
[2] Jinan Univ, Sch Environm, Guangzhou Key Lab Environm Exposure & Hlth, Guangzhou 510632, Guangdong, Peoples R China
[3] Beijing Univ Technol, Water Environm Restorat Res Ctr, Coll Architecture & Civil Engn, Beijing 100124, Peoples R China
基金
中国国家自然科学基金;
关键词
Methylmercury sorption; Thiol-functionalized graphene oxide/Fe-Mn; 3-Mercaptopropyltrimethoxysilane (3-MPTS); X-RAY PHOTOELECTRON; RAMAN-SPECTROSCOPY; INORGANIC MERCURY; METHYL MERCURY; METAL-IONS; ADSORPTION; SURFACE; HG(II); SORPTION; WATER;
D O I
10.1016/j.cej.2017.03.015
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A novel thiol-functionalized graphene oxide/Fe-Mn composite (SGO/Fe-Mn) was synthesized via three different methods, i.e., acetic acid method (SGO/Fe-Mn-ac), neutral method (SGO/Fe-Mn-ne), and ammonium hydroxide method (SGO/Fe-Mn-am). The composites were characterized and tested for aqueous methylmercury removal. SGO/Fe-Mn was prepared using 3-mercaptopropyltrimethoxysilane (3-MPTS) as a silanizing reagent, and hydrolyzed 3-MPTS mainly interacted with GO/Fe-Mn through surface oxygen-containing groups (i.e., OH, C=O, epoxy C-O-C, carboxyl O=C-O, and C-O) and pi-pi interactions, partially through self-polymerization. SGO/Fe-Mn-am showed the largest hydrodynamic diameter, strongest pi-pi bond, fewest S oxidation products, most thiol groups, negative charge, spa defects, and FeOOH. Pseudo-second-order kinetic model and Langmuir and Freundlich isotherm models fitted well with methylmercury sorption kinetic and isotherm data, respectively, resulting in a CH3Hg+ maximum sorption capacity of 43.88 mg/g for SGO/Fe-Mn-am, 36.33 mg/g for SGO/Fe-Mn-ac, and 28.00 mg/g for SGO/Fe-Mn-ne. The removal mechanism was described by electrostatic attraction, ligand exchange, and surface complexation. This study demonstrates potential and viability of SGO/Fe-Mn for enhanced immobilization of CH3Hg+ in surface water, groundwater, and soil/sediments. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:229 / 239
页数:11
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