Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density

Author:

Zhou Xiao12,Ke Ming-Kun3ORCID,Huang Gui-Xiang3,Chen Cai2,Chen Wenxing4,Liang Kuang2,Qu Yunteng2,Yang Jia2,Wang Ying1ORCID,Li Fengting1,Yu Han-Qing3ORCID,Wu Yuen25ORCID

Affiliation:

1. College of Environmental Science and Engineering, Tongji University, State Key Laboratory of Pollution Control and Resources Reuse, Shanghai 200092, China

2. Hefei National Laboratory for Physical Sciences at the Microscale, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei 230026, China

3. Chinese Academy of Sciences Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei 230026, China

4. Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

5. Dalian National Laboratory for Clean Energy, Dalian 116023, China

Abstract

Significance The Fenton-like process based on peroxymonosulfate (PMS) has been widely investigated and recognized as a promising alternative in recent years for the degradation of persistent organic pollutants. However, the sluggish kinetics of PMS activation results in prohibitive costs and substantial chemical inputs, impeding its practical applications in water purification. This work demonstrates that tuning the electronic structure of single-atom sites at the atomic level is a powerful approach to achieve superior PMS activation kinetics. The Cu-based catalyst with the optimized electronic structure exhibits superior performance over most of the state-of-the-art heterogeneous Fenton-like catalysts, while homogeneous Cu(II) shows very poor activity. This work provides insights into the electronic structure regulation of metal centers and structure–activity relationship at the atomic level.

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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