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题名

Photo-assisted reductive cleavage and catalytic hydrolysis-mediated persulfate activation by mixed redox-couple-involved CuFeS2 for efficient trichloroethylene oxidation in groundwater

作者
通讯作者Hu,Xijun; Hu,Xijun
发表日期
2022-08-15
DOI
发表期刊
ISSN
0043-1354
EISSN
1879-2448
卷号222
摘要

Persulfate (PS, SO) activation through transition metal sulfides (TMS) has gained increasing attention since it can decompose a wide variety of refractory halogenated organic compounds in groundwater and wastewater. However, the processes of PS activation by TMS and particularly the formation of •OH radical under anoxic and acidic conditions (pH ∼2.8) remain elusive. Herein, by employing mixed redox-couple-involved chalcopyrite (CuFeS) (150 mg/L) nanoparticles for PS (3.0 mM) activation, 96% of trichloroethylene was degraded within 120 min at pH 6.8 under visible light irradiation. The combination of experimental studies and theoretical calculations suggested that the Cu(I)/Fe(III) mixed redox-couple in CuFeS plays a crucial role to activate PS. Cu(I) acted as an electron donor to transfer electron to Fe(III), then Fe(III) served as an electron transfer bridge as well as a catalytic center to further donate this received electron to the O–O bond of PS, thus yielding SO for trichloroethylene oxidation. Moreover, for the first time, •OH radicals were found to form from the catalytic hydrolysis of PS onto CuFeS surface, where SO anion was hydrolyzed to yield HO and these ensuing HO were further transformed into •OH radicals via photoelectron-assisted O–O bond cleavage step. Our findings offer valuable insights for understanding the mechanisms of PS activation by redox-couple- involved TMS, which could promote the design of effective activators toward PS decomposition for environmental remediation.

关键词
相关链接[Scopus记录]
收录类别
SCI ; EI
语种
英语
重要成果
NI论文
学校署名
其他
资助项目
Basic and Applied Basic Research Foundation of Guangdong Province[2020A1515110723] ; National Natural Science Foundation of China[21777045]
EI入藏号
20223212544492
EI主题词
Anesthetics ; Catalytic Oxidation ; Chemical Activation ; Copper Compounds ; Electrons ; Free Radical Reactions ; Free Radicals ; Groundwater ; Groundwater Pollution ; Hydrolysis ; Iron Compounds ; Transition Metals ; Trichloroethylene
EI分类号
Groundwater:444.2 ; Air Pollution Control:451.2 ; Water Pollution Sources:453.1 ; Metallurgy And Metallography:531 ; Chemical Reactions:802.2 ; Chemical Agents And Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1
ESI学科分类
ENVIRONMENT/ECOLOGY
Scopus记录号
2-s2.0-85135411825
来源库
Scopus
引用统计
被引频次[WOS]:14
成果类型期刊论文
条目标识符http://sustech.caswiz.com/handle/2SGJ60CL/375627
专题工学院_环境科学与工程学院
作者单位
1.Department of Civil and Environmental Engineering,The Hong Kong University of Science and Technology,Hong Kong,China
2.Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials,State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control,Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control,School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
3.School of Chemistry and Chemical Engineering,Guangzhou University,Guangzhou,510006,China
4.School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou,510641,China
5.State Key Laboratory of Urban Water Resource and Environment,Shenzhen Key Laboratory of Organic Pollution Prevention and Control,Harbin Institute of Technology,Shenzhen,518055,China
6.Department of Chemical and Biological Engineering,The Hong Kong University of Science and Technology,Hong Kong,China
7.Department of Civil and Environmental Engineering,The Hong Kong University of Science and Technology,Hong Kong,China
8.Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials,State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control,Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control,School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
9.School of Chemistry and Chemical Engineering,Guangzhou University,Guangzhou,510006,China
10.School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou,510641,China
11.State Key Laboratory of Urban Water Resource and Environment,Shenzhen Key Laboratory of Organic Pollution Prevention and Control,Harbin Institute of Technology,Shenzhen,518055,China
12.Department of Chemical and Biological Engineering,The Hong Kong University of Science and Technology,Hong Kong,China
第一作者单位环境科学与工程学院
推荐引用方式
GB/T 7714
Huang,Junyi,Zhou,Yuanhao,Deng,Shimao,et al. Photo-assisted reductive cleavage and catalytic hydrolysis-mediated persulfate activation by mixed redox-couple-involved CuFeS2 for efficient trichloroethylene oxidation in groundwater[J]. WATER RESEARCH,2022,222.
APA
Huang,Junyi.,Zhou,Yuanhao.,Deng,Shimao.,Shangguan,Yangzi.,Wang,Ranhao.,...&Chen,Hong.(2022).Photo-assisted reductive cleavage and catalytic hydrolysis-mediated persulfate activation by mixed redox-couple-involved CuFeS2 for efficient trichloroethylene oxidation in groundwater.WATER RESEARCH,222.
MLA
Huang,Junyi,et al."Photo-assisted reductive cleavage and catalytic hydrolysis-mediated persulfate activation by mixed redox-couple-involved CuFeS2 for efficient trichloroethylene oxidation in groundwater".WATER RESEARCH 222(2022).
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