Affordable Access

Publisher Website

Electron Delocalization Realizes Speedy Fenton-Like Catalysis over a High-Loading and Low-Valence Zinc Single-Atom Catalyst.

Authors
  • Xin, Shaosong1
  • Ni, Luning1
  • Zhang, Peng1
  • Tan, Haobin1
  • Song, Mingyang1
  • Li, Tong1
  • Gao, Yaowen1
  • Hu, Chun1
  • 1 Institute of Environmental Research at Greater Bay, Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou, 510006, China. , (China)
Type
Published Article
Journal
Advanced science (Weinheim, Baden-Wurttemberg, Germany)
Publication Date
Dec 01, 2023
Volume
10
Issue
34
Identifiers
DOI: 10.1002/advs.202304088
PMID: 37840391
Source
Medline
Keywords
Language
English
License
Unknown

Abstract

A zinc (Zn)-based single-atom catalyst (SAC) is recently reported as an active Fenton-like catalyst; however, the low Zn loading greatly restricts its catalytic activity. Herein, a molecule-confined pyrolysis method is demonstrated to evidently increase the Zn loading to 11.54 wt.% for a Zn SAC (ZnSA -N-C) containing a mixture of Zn-N4 and Zn-N3 coordination structures. The latter unsaturated Zn-N3 sites promote electron delocalization to lower the average valence state of Zn in the mix-coordinated Zn-Nx moiety conducive to interaction of ZnSA -N-C with peroxydisulfate (PDS). A speedy Fenton-like catalysis is thus realized by the high-loading and low-valence ZnSA -N-C for PDS activation with a specific activity up to 0.11 min L-1 m-2 , outstripping most Fenton-like SACs. Experimental results reveal that the formation of ZnSA -N-C-PDS* complex owing to the strong affinity of ZnSA -N-C to PDS empowers intense direct electron transfer from the electron-rich pollutant toward this complex, dominating the rapid bisphenol A (BPA) elimination. The electron transfer pathway benefits the desirable environmental robustness of the ZnSA -N-C/PDS system for actual water decontamination. This work represents a new class of efficient and durable Fenton-like SACs for potential practical environmental applications. © 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.

Report this publication

Statistics

Seen <100 times