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Synergies of Fe Single Atoms and Clusters on N‐Doped Carbon Electrocatalyst for pH‐Universal Oxygen Reduction
Author(s) -
Liu Mengjie,
Lee Jeongyeon,
Yang TsungCheng,
Zheng Fangyuan,
Zhao Jiong,
Yang ChiaMin,
Lee Lawrence Yoon Suk
Publication year - 2021
Publication title -
small methods
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 4.66
H-Index - 46
ISSN - 2366-9608
DOI - 10.1002/smtd.202001165
Subject(s) - electrocatalyst , catalysis , carbon fibers , metal , oxygen reduction , chemistry , oxygen , oxygen reduction reaction , atom (system on chip) , doping , oxygen atom , transition metal , kinetics , materials science , inorganic chemistry , nanotechnology , electrochemistry , molecule , physics , electrode , organic chemistry , computer science , optoelectronics , composite material , quantum mechanics , composite number , embedded system
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.