Insights into simultaneous adsorption and oxidation of antimonite[Sb(III)]by crawfish shell-derived biochar:spectroscopic investigation and theoretical calculations  

作　　者：Hanbo Chen Yurong Gao Jianhong Li Chenghua Sun Binoy Sarkar Amit Bhatnagar Nanthi Bolan Xing Yang Jun Meng Zhongzhen Liu Hong Hou Jonathan WCWong Deyi Hou Wenfu Chen Hailong Wang 

机构地区：[1]School of Environmental and Chemical Engineering,Foshan University,528000 Foshan,Guangdong,China [2]Agronomy College,Shenyang Agricultural University,110866 Shenyang,China [3]Key Laboratory of Biochar and Soil Improvement,Ministry of Agriculture and Rural Affairs,110866 Shenyang,China [4]Department of Chemistry and Biotechnology,Center for Translational Atomaterials,Swinburne University of Technology,3122 Hawthorn,VIC,Australia [5]Future Industries Institute,University of South Australia,Mawson Lakes,SA 5095,Australia [6]Department of Separation Science,LUT School of Engineering Science,LUT University,Sammonkatu 12,FI-50130 Mikkeli,Finland [7]School of Agriculture and Environment,The University of Western Australia,6001 Perth,WA,Australia [8]The UWA Institute of Agriculture,The University of Western Australia,6001 Perth,WA,Australia [9]Institute of Agricultural Resources and Environment,Guangdong Academy of Agricultural Sciences,510640 Guangzhou,China [10]State Key Laboratory of Environmental Criteria and Risk Assessment,Chinese Research Academy of Environmental Sciences,100012 Beijing,China [11]Department of Biology,Hong Kong Baptist University,Kowloon Tong,Hong Kong SAR,China [12]School of Environment,Tsinghua University,100084 Beijing,China [13]Guangdong Green Technologies Co.,Ltd,528100 Foshan,China

出　　处：《Biochar》2022年第1期561-576,共16页生物炭（英文）

基　　金：the National Key Research and Development Program of China(2020YFC1807704);the National Natural Science Foundation of China(21876027);the Science and Technology Innovation Project of Foshan,China(1920001000083).

摘　　要：Removal of antimonite[Sb(Ⅲ)]from the aquatic environment and reducing its biotoxicity is urgently needed to safeguard environmental and human health.Herein,crawfish shell-derived biochars(CSB),pyrolyzed at 350,500,and 650℃,were used to remediate Sb(Ⅲ)in aqueous solutions.The adsorption data best fitted to the pseudo-second-order kinetic and Langmuir isotherm models.Biochar produced at 350℃(CSB350)showed the highest adsorption capacity(27.7 mg g^(−1)),and the maximum 78%oxidative conversion of Sb(Ⅲ)to Sb(V).The adsorption results complemented with infrared(FTIR),X-ray photoelectron(XPS),and near-edge X-ray absorption fine structure(NEXAFS)spectroscopy analyses indicated that the adsorption of Sb(Ⅲ)on CSB involved electrostatic interaction,surface complexation with oxygen-containing functional groups(C=O,O=C-O),π-πcoordination with aromatic C=C and C-H groups,and H-bonding with-OH group.Density functional theory calculations verified that surface complexation was the most dominant adsorption mechanism,whilstπ-πcoordination and H-bonding played a secondary role.Furthermore,electron spin resonance(ESR)and mediated electrochemical reduction/oxidation(MER/MEO)analyses confirmed that Sb(Ⅲ)oxidation at the biochar surface was governed by persistent free radicals(PFRs)(•O_(2)^(−)and•OH)and the electron donating/accepting capacity(EDC/EAC)of biochar.The abundance of preferable surface functional groups,high concentration of PFRs,and high EDC conferred CSB350 the property of an optimal adsorbent/oxidant for Sb(Ⅲ)removal from water.The encouraging results of this study call for future trials to apply suitable biochar for removing Sb(Ⅲ)from wastewater at pilot scale and optimize the process.

关 键 词：SORPTION Heavy metal SYNCHROTRON Density functional theory Contaminated water 

分 类 号：O64[理学—物理化学]