Solar-Driven Arsenic(V) Transformation, Speciation, and Adsorption on the Chalcopyrite Surface

Ge, Qiuyue1,2; Zheng, Renji1; Liu, Yangyang2; Shangguan, Yangzi1,3; Feng, Xuezhen1; Yang, Dazhong1; Wei, Wenfei1; Wang, Ranhao1; Ji, Yongfei4; Duan, Lele5; Lin, Jia3; Zhang, Liwu2; Chen, Hong1

2024-06-01

10.1021/acsestwater.4c00059

ACS ES&T WATER   影响因子和分区

2690-0637

Understanding the dynamics of arsenic species (As(V) and As(III)) in water is crucial for mitigating their significant health risks. Here, we demonstrate the exceptional ability of chalcopyrite minerals to convert As(V) into As(III), and achieve 100% removal over a broad range of concentrations (0.005-50 mg/L). This unique process combines adsorption with photocatalytic redox reactions, where As(V) is first adsorbed on the mineral surface and then reduced to As(III) by photogenerated electrons. Density functional theory calculations reveal the "Cu(I)-Fe(III) redox-couple" within chalcopyrite as the key driver of this efficient photocatalysis. This redox-couple exhibits excellent light absorption and excitation dynamics, facilitating the rapid transfer of photogenerated electrons to the Fe site for As(V) reduction. This research unveils a previously unknown pathway for arsenic adsorbed and reduction in the natural environment, potentially impacting our comprehension of the global geochemical cycle of the toxic As element.

chalcopyrite minerals arsenic adsorbed and reduction Cu(I)-Fe(III) redox-couple global geochemicalcycle of the toxic As element

ESCI

英语

第一 ; 通讯

Stable Support Plan Program of Shenzhen Natural Science Foundation[20231122110855002] ; High level of special funds[G03050K001] ; National Natural Science Foundation of China["21777045","61875119"] ; Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control[2023B1212060002] ; Shanghai Rising-Star Program[19QA1405000] ; U.S. Department of Energy, Office of Science, Basic Energy Sciences[DE-AC02-76SF00515]

Environmental Sciences & Ecology ; Water Resources

Environmental Sciences ; Water Resources

WOS:001247426400001

AMER CHEMICAL SOC

Web of Science

1.Southern Univ Sci & Technol, Sch Environm Sci & Engn, State Environm Protect Key Lab Integrated Surface, Guangdong Prov Key Lab Soil & Groundwater Pollut C, Shenzhen 518055, Peoples R China
2.Fudan Univ, Dept Environm Sci & Engn, Shanghai 200433, Peoples R China
3.Shanghai Univ Elect Power, Dept Phys, Shanghai 200090, Peoples R China
4.Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou 510006, Peoples R China
5.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Ge, Qiuyue,Zheng, Renji,Liu, Yangyang,et al. Solar-Driven Arsenic(V) Transformation, Speciation, and Adsorption on the Chalcopyrite Surface[J]. ACS ES&T WATER,2024.

Ge, Qiuyue.,Zheng, Renji.,Liu, Yangyang.,Shangguan, Yangzi.,Feng, Xuezhen.,...&Chen, Hong.(2024).Solar-Driven Arsenic(V) Transformation, Speciation, and Adsorption on the Chalcopyrite Surface.ACS ES&T WATER.

Ge, Qiuyue,et al."Solar-Driven Arsenic(V) Transformation, Speciation, and Adsorption on the Chalcopyrite Surface".ACS ES&T WATER (2024).