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论文类型：期刊论文

第一作者：Mingjie Huang, Yi Han, Wei Xiang, Delai Zhong, Chen Wang, Tao Zhou,* Xiaohui Wu, and Juan Mao

发表刊物：Environmental Science & Technology

收录刊物：SCI

学科门类：工学

一级学科：环境科学与工程

文献类型：J

卷号：55

页面范围：15361-15370

ISSN号：0013-936X

关键字：persulfate activation, CuO, phenol degradation, phenoxyl radical, selectively, organic wastewater treatment, persulfate utilization efficiency

DOI码：10.1021/acs.est.1c03758

发表时间：2021-10-26

影响因子：11.357

摘要：Transition-metal oxide (MxOy)-based persulfate (PDS) activation processes have demonstrated enormous potential for pollutant degradation in water purification. However, the mechanistic insight of PDS activation by a MxOy catalyst concerning the mediate role of the organic substrate remains obscure. Here, we demonstrated that the in situ-formed phenoxyl radical on the CuO surface can trigger efficient persulfate activation for phenol degradation. The formation of the phenoxyl radical was an innersphere process, which involved the successive steps of chemisorption through surface hydroxyl group substitution and the subsequent spontaneous electron transfer reaction from adsorbed phenol to CuO. The organic substrate phenol can be oxidized by the PDS molecule and surface-bound SO4·- through the nonradical and free-radical pathways, respectively. Such a unique “half-radical” mechanism resulted in an extraordinarily high PDS utilization efficiency of 188.9%. More importantly, a general rule for phenoxyl radical formation was concluded; it can be formed in the cases of organic substrates with a Hammett constant σ+ lower than -0.02 and metal ion of a 3d subshell between half-filled and fully filled. This study clarifies the mediate role of the organic substrate for interfacial PDS activation on MxOy and also gives new insights into the rational design of a highly efficient MxOy catalyst for selective phenolic/aniline pollutant degradation in wastewater.

发布期刊链接：https://pubs.acs.org/doi/10.1021/acs.est.1c03758?cookieSet=1