KMS Chongqing Institute of Green and Intelligent Technology, CAS
Selective electrophilic attack towards organic micropollutants with superior Fenton-like activity by biochar-supported cobalt single-atom catalyst | |
Liu, Chen1,2; He, Xinxia1,2; Li, Jinglu1,2; Ma, Jun1,2; Yue, Junpeng3; Wang, Ziwei4; Chen, Ming1,2 | |
2024-03-01 | |
摘要 | The global shortage of freshwater and inadequate supply of clean water have necessitated the implementation of robust technologies for wastewater purification, and Fenton-like chemistry is a highly-promising approach. However, realizing the rapid Fenton-like chemistry for high-efficiency degradation of organic micropollutants (OMs) remains challenging. Herein, one novel system was constructed by a Co single-atom catalyst activating peroxymonosulfate (PMS), and the optimal system (SA-Co-NBC-0.2/PMS) achieved unprecedented catalytic performance towards a model OM [Iohexol (IOH)], i.e., almost 100% decay ratio in only 10 min (the observed rate constant: 0.444 min(-1)) with high electrophilic species O-1(2) (singlet oxygen) generation. Theoretical calculations unveiled that Co-N-4 sites preferred to adsorb the terminal-O of PMS (more negative adsorption energy than other O sites: -32.67 kcal/mol), promoting the oxidation of PMS to generate O-1(2). Iodine (I)23 (0.1097), I24 (0.1154) and I25 (0.0898) on IOH with higher f(-) electrophilic values were thus identified as the main attack sites. Furthermore, 16S ribosomal RNA high-throughput sequencing and quantitative structure-activity rela-tionship analysis illustrated the environmentally-benign property of the SA-Co-NBC-0.2 and the tapering ecological risk during IOH degradation process. Significantly, this work comprehensively checked the compe-tence of the SA-Co-NBC-0.2/PMS system for organics abatement in practical wastewater. |
关键词 | Biochar-supported single-atom catalysts Organic micropollutants Fenton-like chemistry Theoretical calculations Wastewater purification |
DOI | 10.1016/j.jcis.2023.11.131 |
发表期刊 | JOURNAL OF COLLOID AND INTERFACE SCIENCE |
ISSN | 0021-9797 |
卷号 | 657页码:155-168 |
通讯作者 | Chen, Ming(chenming@cigit.ac.cn) |
收录类别 | SCI |
WOS记录号 | WOS:001127853800001 |
语种 | 英语 |