文献类型：期刊文献

英文题名：Mechanical insight into direct singlet oxygen generation pathway: The significance of Co-O-X bond formation anchored by cobalt single atoms on mesoporous oxides

作者：Yuan, Cong[1];Zhu, Xiaoxiao[1];Pan, Jiaqi[1];Xu, Minghao[1];Jiang, Yongjun[3,4];Dai, Sheng[3,4];Huang, Yikai[1];Lu, Leixi[1];Zhou, Lei[1,2];Tian, Chengcheng[1,2]

机构：[1]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai 200237, Peoples R China;[2]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[3]East China Univ Sci & Technol, Inst Fine Chem, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2024

卷号：484

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001186922500001)】；

基金：This work was finically supported by the National Natural Science Foundation of China (NSFC, Grant No. 22176059 & 52170109) , the Shanghai Science and Technology Innovation Plan (22DZ1208600) , and the Innovation Program of Shanghai Municipal Education Commission (2023ZKZD41) .

语种：英文

外文关键词：Co single atoms; Mesoporous oxides; PMS; Co-O-X; Singlet oxygen

摘要：The understanding of how single atoms anchoring on oxides contribute to high-activity catalysis in the sulfate radical -advanced oxidation process (SR-AOP) remains obscure. Here we presented a new strategy for regulating singlet oxygen (1O2) generation in peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) by engineering the Co -O -X active sites on oxide supports in this study. The Co single atoms supported on mesoporous oxides (CoSA-XO2) were first successfully developed using a modified sol-gel solvent vaporization self-assembly method. We found that CoSA-XO2 catalysts served as efficient PMS activators for pollutant decomposition over a wide pH range. Notably, CoSA-TiO2 exhibited exceptional performance, achieving nearly 100% removal of sulfasalazine (SSZ) within 10 min. Furthermore, evidenced by experimental results and density functional theory (DFT) calculations,1O2 was confirmed to be predominately active oxidizing species by the unique Co -O -X bonds for activating PMS in CoSA-XO2/PMS system, resulting in an excellent pollution degradation. This study provides valuable insights into the construction of highly loaded single-atom catalysts using oxide substrates in the PMSAOP system, along with the mechanism of regulating reactive oxygen species (ROS) formation through interfacial bonding between active metal and support.