Synergies of Fe Single Atoms and Clusters on N-Doped Carbon Electrocatalyst for pH-Universal Oxygen Reduction

Mengjie Liu, Jeongyeon Lee, Tsung Cheng Yang, Fangyuan Zheng, Jiong Zhao, Chia Min Yang, Lawrence Yoon Suk Lee

Research output: Journal article publicationJournal articleAcademic researchpeer-review

133 Citations (Scopus)

Abstract

Single atomic metal–N–C materials have attracted immense interest as promising candidates to replace noble metal-based electrocatalysts for the oxygen reduction reaction (ORR). The coordination environment of metal–N–C active centers plays a critical role in determining their catalytic activity and durability, however, attention is focused only on the coordination of metal atoms. Herein, Fe single atoms and clusters co-embedded in N-doped carbon (Fe/NC) that deliver the synergistic enhancement in pH-universal ORR catalysis via the four-electron pathway are reported. Combining a series of experimental and computational analyses, the geometric and electronic structures of catalytic sites in Fe/NC are revealed and the neighboring Fe clusters are shown to weaken the binding energies of the ORR intermediates on Fe–N sites, hence enhancing both catalytic kinetics and thermodynamics. This strategy provides new insights into the understanding of the mechanism of single atom catalysis.

Original languageEnglish
Article number2001165
JournalSmall Methods
Volume5
Issue number5
DOIs
Publication statusPublished - 12 May 2021

Keywords

  • Fe clusters
  • Fe–N–C
  • oxygen reduction reaction
  • porous carbon
  • single atom catalysis

ASJC Scopus subject areas

  • General Chemistry
  • General Materials Science

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