Coordination tunes selectivity

two‐electron oxygen reduction on high‐loading molybdenum single‐atom catalysts

Cheng Tang, Yan Jiao, Bingyang Shi, Jia-Ning Liu, Zhenhua Xie, Xiao Chen, Qiang Zhang, Shizhang Qiao

Research output: Contribution to journalArticle

14 Citations (Scopus)

Abstract

Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and metal loading. However, doing so is still a great challenge because of the limited synthesis approach and insufficient understanding of the structure–property relationships. Herein, we report a new kind of Mo SAC with a unique O,S coordination and a high metal loading over 10 wt %. The isolation and local environment was identified by high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure. The SACs catalyze the oxygen reduction reaction (ORR) via a 2 e pathway with a high H2O2 selectivity of over 95 % in 0.10 m KOH. The critical role of the Mo single atoms and the coordination structure was revealed by both electrochemical tests and theoretical calculations.

Original languageEnglish
Pages (from-to)9171-9176
Number of pages6
JournalAngewandte Chemie - International Edition
Volume59
Issue number23
DOIs
Publication statusPublished - 2 Jun 2020
Externally publishedYes

Keywords

  • electrocatalysis
  • molybdenum
  • oxygen reduction reaction (ORR)
  • selectivity
  • single-atom catalyst

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