In situ electrogenerated Cu(III) triggers hydroxyl radical production on the Cu- Sb- SnO2 electrode for highly efficient water decontamination

被引:55
作者
Lu, Sen [1 ,2 ]
Li, Xuechuan [1 ,2 ]
Cheng, Yumeng [1 ,3 ]
Zhou, Jia [1 ,3 ]
Zhang, Guan [1 ,2 ]
机构
[1] Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Shenzhen 518055, Peoples R China
[2] Harbin Inst Technol, Shenzhen Key Lab Organ Pollut Prevent & Control, Sch Civil & Environm Engn, Shenzhen 518055, Peoples R China
[3] Harbin Inst Technol, Sch Sci, Shenzhen 518055, Peoples R China
基金
中国国家自然科学基金;
关键词
electrochemical oxidation; water decontamination; Cu(III); hydroxyl radicals; MMO anodes; ELECTROCHEMICAL OXIDATION; EVOLUTION REACTION; OXYGEN; DEGRADATION; PERFORMANCE; MECHANISMS; POLLUTANTS; OXIDES; COPPER; ANODE;
D O I
10.1073/pnas.2306835120
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The electrochemical oxidation process has the unique advantage of in -situ center dot OH generation for deep mineralization of organic pollutants, which is expected to provide a solution for the globally decentralized wastewater treatment and reuse. However, it is still a great challenge to develop low -cost anodes with ultrahigh center dot OH yield and low energy consumption. Here, a low -cost and stable mixed metal oxide (MMO) anode (Cu-Sb-SnO2) developed by a simple and scalable preparation process presents extremely high organic pollutants degradation efficiency and low energy consumption. The tetracycline degradation kinetics constant of the Cu-Sb- SnO2 system (0.362 min(-1)) was 9 to 45 times higher than that of other prepared anodes, which is superior to the existing anodes reported so far. The experimental results and theoretical calculations indicate that the Cu-Sb-SnO2 has moderate oxygen evolution potential, larger water adsorption energy, and lower reaction energy barrier, which is conducive to selective water oxidation to generate center dot OH. Notably, it is systematically and comprehensively confirmed that the generation of center dot OH triggered by in situ electrogenerated Cu(III) increased center dot OH steady -state concentration by over four times. Furthermore, the doped Cu species can play a key role in promoting charge transfer as an "electronic porter" between Sn and Sb in the electrocatalytic process by adjusting the electronic structure of the Sb- SnO2 electrode. This work paves the way for the development of MMO anodes utilizing the advantage of the Cu redox shuttle.
引用
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页数:11
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