文献类型：期刊文献

英文题名：Degradation of bisphenol a using peroxymonosulfate activated by single-atomic cobalt catalysts: Different reactive species at acidic and alkaline pH

作者：Wang, Qi[1];Liu, Cun[2];Zhou, Dongmei[3];Chen, Xiurong[1];Zhang, Meng[1];Lin, Kuangfei[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]Chinese Acad Sci, Key Lab Soil Environm & Pollut Remediat, Inst Soil Sci, 71 East Beijing Rd, Nanjing 210008, Peoples R China;[3]Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Peoples R China

年份：2022

卷号：439

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20221311837732);WOS:【SCI-EXPANDED(收录号:WOS:000795542300002)】；

基金：Acknowledgment This work was supported by The National Key Research and Devel-opment Program of China (2018YFC1803304, 2018YFC1800705 and 2019YFC1806103) . The authors thank Research Center of Analysis and Test of for the help on EPR analysis.

语种：英文

外文关键词：Single-atom cobalt catalyst; Peroxymonosulfate; High-valent Co; Singlet oxygen; Density function theory

摘要：Peroxymonosulfate-assisted advanced oxidation processes (PMS-AOPs) catalyzed by single-atom catalysts have become state-of-the-art technologies for environmental remediation. In this study, Cobalt single-atom catalysts supported by graphitic carbon nitride (SA-CoCN) containing Co-N-4 active sites were developed as PMS activators for bisphenol A (BPA) degradation. BPA (10 mg L-1) was completely removed with 0.1 g L-1 SA-CoCN and 0.5 mM PMS, and this process was pH-dependent. Instead of the widely recognized generation of free radicals (SO4 center dot- and center dot OH), high-valent cobalt [Co(IV)] and singlet oxygen (O-1(2)) were the predominant reactive species for pollutant degradation under acidic and alkaline conditions, respectively. The conversion of methyl phenyl sulfoxide (PMSO) to methyl phenyl sulfone (PMSO2), electron paramagnetic resonance tests and radical scavenger experiments were used to probe these reactive species. According to density functional theory calculations, the formation of Co(IV) and O-1(2) was thermodynamically favorable, and the generation pathways of Co(IV) and O-1(2) were further discussed. This study provides an insight into the single-atom cobalt catalyst/PMS process.