过硫酸盐
电子转移
碳纳米管
环境修复
化学
选择性
空位缺陷
催化作用
机制(生物学)
纳米技术
化学工程
光化学
材料科学
有机化学
污染
生态学
哲学
工程类
结晶学
认识论
生物
作者
Penghui Shao,Shuiping Yu,Xiaoguang Duan,Liming Yang,Hui Shi,Lin Ding,Jiayu Tian,Lixia Yang,Shaobin Wang
标识
DOI:10.1021/acs.est.0c02645
摘要
Nanocarbon-based persulfate oxidation emerges as a promising technology for the elimination of organic micropollutants (OMPs). However, the nature of the active site and its working mechanism remain elusive, impeding developments of high-performance oxidative technology for water treatment practice. Here, we report that defect-rich carbon nanotubes (CNTs) exhibit a superior activity in the activation of peroxymonosulfate (PMS) for OMP oxidation. Quantitative structure-activity relationship studies combined with theoretical calculations unveil that the double-vacancy defect on CNTs may be the intrinsic active site, which works as a conductive bridge to facilitate the potential difference-dominated electron transfer from the highest occupied molecular orbital of OMPs to the lowest unoccupied molecular orbital of PMS. Based on this unique mechanism, the established CNTs@PMS oxidative system achieves outstanding selectivity and realizes the target-oriented elimination of specific OMPs in a complicated aquatic environment. This work sheds new light on the mechanism of carbocatalysis for selective oxidation and develops an innovative technology toward remediation of practical wastewater.
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