Litcius/Paper detail

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

Xiao Zhou, Ming‐Kun Ke, Gui‐Xiang Huang, Cai Chen, Wenxing Chen, Kuang Liang, Yunteng Qu, Jia Yang, Ying Wang, Fengting Li, Han‐Qing Yu, Yuen Wu

2022Proceedings of the National Academy of Sciences439 citationsDOIOpen Access PDF

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.

Topics & Concepts

HeteroatomCatalysisActive siteSubstrate (aquarium)ChemistryElectronic structureDensity functional theoryActivation energyActive centerAtom (system on chip)AdsorptionPhotochemistryMaterials sciencePhysical chemistryComputational chemistryOrganic chemistryGeologyEmbedded systemComputer scienceRing (chemistry)OceanographyAdvanced Photocatalysis TechniquesAdvanced oxidation water treatmentElectrocatalysts for Energy Conversion