Single-Atom Zinc Sites with Synergetic Multiple Coordination Shells for Electrochemical H2O2 Production

Gangya Wei, Yunxiang Li, Xupo Liu, Jinrui Huang, Mengran Liu, Deyan Luan, Shuyan Gao*, Xiong Wen David Lou*

*Corresponding author for this work

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

72 Citations (Scopus)

Abstract

Precise manipulation of the coordination environment of single-atom catalysts (SACs), particularly the simultaneous engineering of multiple coordination shells, is crucial to maximize their catalytic performance but remains challenging. Herein, we present a general two-step strategy to fabricate a series of hollow carbon-based SACs featuring asymmetric Zn−N2O2 moieties simultaneously modulated with S atoms in higher coordination shells of Zn centers (n≥2; designated as Zn−N2O2−S). Systematic analyses demonstrate that the synergetic effects between the N2O2 species in the first coordination shell and the S atoms in higher coordination shells lead to robust discrete Zn sites with the optimal electronic structure for selective O2 reduction to H2O2. Remarkably, the Zn−N2O2 moiety with S atoms in the second coordination shell possesses a nearly ideal Gibbs free energy for the key OOH* intermediate, which favors the formation and desorption of OOH* on Zn sites for H2O2 generation. Consequently, the Zn−N2O2−S SAC exhibits impressive electrochemical H2O2 production performance with high selectivity of 96 %. Even at a high current density of 80 mA cm−2 in the flow cell, it shows a high H2O2 production rate of 6.924 mol gcat−1 h−1 with an average Faradaic efficiency of 93.1 %, and excellent durability over 65 h. © 2023 Wiley-VCH GmbH.
Original languageEnglish
Article numbere202313914
JournalAngewandte Chemie - International Edition
Volume62
Issue number47
Online published3 Oct 2023
DOIs
Publication statusPublished - 20 Nov 2023

Research Keywords

  • Coordination Environment
  • H2O2 Production
  • Hollow Structure
  • Single-Atom Catalysts
  • Synergetic Effects

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