文献类型：期刊文献

英文题名：Carbon nitride-based cuprous catalysts induced nonradical-led oxidation by peroxydisulfate: Role of cuprous and dissolved oxygen

作者：Wang, Qi[1];Zhou, Dongmei[2];Lin, Kuangfei[1];Chen, Xiurong[1]

机构：[1]East China Univ Sci & Technol, Sch Resource & Environm Engn, State Environm Protect Key Lab Environm Risk Asse, Shanghai 200237, Peoples R China;[2]Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Peoples R China

年份：2021

卷号：419

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20211510212766);WOS:【SCI-EXPANDED(收录号:WOS:000663664200004)】；

基金：This work was supported by The National Key Research and Development Program of China (2019YFC1803701, 2018YFC1800705 and 2019YFC1806103). The authors thank Research Center of Analysis and Test of East China University of Science and Technology for the help on EPR analysis. Thanks are due to Prof. Cun Liu for assistance with the DFT calculation.

语种：英文

外文关键词：Cuprous; Carbon nitride; Peroxydisulfate; Singlet oxygen

摘要：Nonradical-based advanced oxidation processes are a promising method for pollutant removal due to their inherent superior characteristics. In this study, carbon nitride-based cuprous catalysts (CuCN) synthesized through a one-pot method were discovered as effective peroxydisulfate (PDS) activators for the degradation of Tetrabromobisphenol A (TBBPA). Specifically, TBBPA (2 mg L-1) was completely removed in 20 min under optimized conditions (2 mM PDS, 0.2 g L -1 1-CuCN, and initial pH = 7). The degradation efficiency of TBBPA was hardly inhibited by free radical scavengers and typical background water constituents. The results of XPS, FTIR, and DFT confirmed that Cu(I) atoms in CuCN not only act as active sites, but also form the specific Cu(I) N bonds that increases the charge density of positively charged carbon atoms of the tri-s-triazine structure, which enhances the ability of CuCN to activate PDS. A comprehensive study was conducted by using radical scavengers, electron paramagnetic resonance and different dissolved oxygen conditions to identify the reactive oxygen species (ROS). Singlet oxygen (1O2) was unveiled to be the primary ROS in the 1-CuCN/PDS system, which was generated from superoxide anions (36.2%) and dissolved oxygen (63.8%). This study first elucidated the mechanism that carbon nitride-based cuprous catalysts activated PDS and provided an innovative PDS-based catalytic system for in situ chemical oxidation (ISCO).