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Removal of arsenate with hydrous ferric oxide coprecipitation:Effect of humic acid
作者姓名:Jingjing Du  Chuanyong Jing  Jinming Duan  Yongli Zhang  Shan Hu
作者单位:State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Xi'an 710055, China;College of Architecture and Environment, Sichuan University, Chengdu 610065, China;State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
基金项目:This work was supported by the National Natural Science Foundation of China (No. 41373123, 41023005, 21321004) and Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences (No. YSW2013A01).
摘    要:Insights from the adverse effect of humic acid(HA) on arsenate removal with hydrous ferric oxide(HFO) coprecipitation can further our understanding of the fate of As(V) in water treatment process. The motivation of our study is to explore the competitive adsorption mechanisms of humic acid and As(V) on HFO on the molecular scale. Multiple complementary techniques were used including macroscopic adsorption experiments, surface enhanced Raman scattering(SERS), extended X-ray absorption fine structure(EXAFS) spectroscopy, flow-cell attenuated total reflectance Fourier transform infrared(ATR-FTIR) measurement, and charge distribution multisite complexation(CDMUSIC) modeling. The As(V) removal efficiency was reduced from over 95% to about 10% with the increasing HA concentration to 25 times of As(V) mass concentration. The SERS analysis excluded the HA-As(V) complex formation. The EXAFS results indicate that As(V) formed bidentate binuclear surface complexes in the presence of HA as evidenced by an As-Fe distance of 3.26–3.31 ?. The in situ ATR-FTIR measurements show that As(V) replaces surface hydroxyl groups and forms innersphere complex. High concentrations of HA may physically block the surface sites and inhibit the As(V) access. The adsorption of As(V) and HA decreased the point of zero charge of HFO from 7.8 to 5.8 and 6.3, respectively. The CD-MUSIC model described the zeta potential curves and adsorption edges of As(V) and HA reasonably well.

关 键 词:水合氧化铁  共沉淀法  腐殖酸  傅里叶变换红外光谱  ATR-FTIR  X-射线吸收精细结构  表面增强拉曼散射  表面增强拉曼光谱
收稿时间:1 November 2013
修稿时间:20 December 2013

Removal of arsenate with hydrous ferric oxide coprecipitation: Effect of humic acid
Jingjing Du,Chuanyong Jing,Jinming Duan,Yongli Zhang,Shan Hu.Removal of arsenate with hydrous ferric oxide coprecipitation: Effect of humic acid[J].Journal of Environmental Sciences,2014,26(2):240-247.
Authors:Jingjing Du  Chuanyong Jing  Jinming Duan  Yongli Zhang and Shan Hu
Institution:State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;School of Environmental and Municipal Engineering, Xi'an University of Architecture and Technology, Xi'an 710055, China;College of Architecture and Environment, Sichuan University, Chengdu 610065, China;State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
Abstract:Insights from the adverse effect of humic acid (HA) on arsenate removal with hydrous ferric oxide (HFO) coprecipitation can further our understanding of the fate of As(V) in water treatment process. The motivation of our study is to explore the competitive adsorption mechanisms of humic acid and As(V) on HFO on the molecular scale. Multiple complementary techniques were used including macroscopic adsorption experiments, surface enhanced Raman scattering (SERS), extended X-ray absorption fine structure (EXAFS) spectroscopy, flow-cell attenuated total reflectance Fourier transform infrared (ATR-FTIR) measurement, and charge distribution multisite complexation (CD-MUSIC) modeling. The As(V) removal efficiency was reduced from over 95% to about 10% with the increasing HA concentration to 25 times of As(V) mass concentration. The SERS analysis excluded the HA-As(V) complex formation. The EXAFS results indicate that As(V) formed bidentate binuclear surface complexes in the presence of HA as evidenced by an As-Fe distance of 3.26-3.31 Å. The in situ ATR-FTIR measurements show that As(V) replaces surface hydroxyl groups and forms inner-sphere complex. High concentrations of HA may physically block the surface sites and inhibit the As(V) access. The adsorption of As(V) and HA decreased the point of zero charge of HFO from 7.8 to 5.8 and 6.3, respectively. The CD-MUSIC model described the zeta potential curves and adsorption edges of As(V) and HA reasonably well.
Keywords:arsenate  humic acid  HFO  adsorption  multiple spectroscopic techniques
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