文献类型：期刊文献

英文题名：Selectively photoelectrocatalytic reduction of oxygen to hydroxyl radical and singlet oxygen: Mechanism and validation in coal wastewater

作者：Feng, Zhiyuan[1];Tian, Qingling[1];Yang, Qianqian[1];Zhou, Yanbo[2];Zhao, Hongying[1];Zhao, Guohua[1]

机构：[1]Tongji Univ, Shanghai Key Lab Chem Assessment & Sustainabil, Key Lab Yangtze River Water Environm, Sch Chem Sci & Engn, Siping Rd 1239, Shanghai 200092, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Coal Gasificat & Energy Chem Engn, Minist Educ, Meilong Rd 130, Shanghai 200092, Peoples R China

年份：2021

卷号：286

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20210509836300);WOS:【SCI-EXPANDED(收录号:WOS:000621615000007)】；

基金：The authors acknowledge funding from the National Natural Science Foundation P.R. China (Project No. 22076142, 21677106, 22076140), National Key Basic Research Program of China (2017YFA0403402), National Natural Science Foundation of China (U1932119), the Science & Technology Commission of Shanghai Municipality (14DZ2261100), the Fundamental Research Funds for the Central Universities. The authors thank the staff of the 11B beamline at the Shanghai Synchrotron Radiation Facility (SSRF) for data collection. This work was also supported by shanghai large Scientific facilities center.

语种：英文

外文关键词：Photoelectrocatalytic process; Oxygen reduction reaction; Hydroxyl radical; Singlet oxygen; Coal wastewater

摘要：The fine-tuning of generating hydroxyl radical ((OH)-O-center dot) and singlet oxygen (O-1(2)) was firstly proposed via the selectively photoelectrochemical (PE) reduction of oxygen with Cu-coordinated carbon-nitride-electrode (CuCN). Complete removal efficiency and trace Cu leaching (<0.01 ppm) were achieved during treatment of dimethyl phthalate and atrazine, which were mainly oxidized by (OH)-O-center dot and O-1(2), respectively. Besides, no toxic intermediates was detected in the whole degradation process. The overall oxygen reduction pathway in PE system was demonstrated by electron paramagnetic resonance measurements and quenching tests. The valence band position of CuCN was designed to be more negative (-1.5 V-SHE) for favoring the photocatalytic oxygen reduction. Specifically, Cu-N-2-C as active sites optimized the Gibbs free energy of intermediate *OOH (AG(*OOH) = 3.99 eV) to improve the reactivity of two-electron oxygen reduction. The CuCN/photoelectrochemical system is applied for treatment of coal water slurry gasification (CWS) wastewater with high concentration of salt. The TOC of CWS was successfully decreased from 127 to 1.9 mg.L-1 in 3 h with a low specific energy consumption of 0.024-0.05 kW.h.g(-1).TOC-1. The treated CWS wastewater can be used for recovery and utilization of salt as chemical raw materials. This work highlights the important role of synergistic photo-electro-catalytic effect in regulating the generation of active oxygen species via oxygen reduction pathway, which can be a promising way especially for salinity coal wastewater remediation.