Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density
Abstract
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.
- Publication:
-
Proceedings of the National Academy of Science
- Pub Date:
- February 2022
- DOI:
- 10.1073/pnas.2119492119
- Bibcode:
- 2022PNAS..11919492Z