催化作用
碳纤维
热解
材料科学
金属有机骨架
金属
氧气
连接器
无机化学
结晶学
化学
物理化学
有机化学
冶金
吸附
复合数
计算机科学
复合材料
操作系统
作者
Xinrui Li,Guanying Ye,Weiwei Zhu,Min Tian,R.-C. Wang,Suqin Liu,Zhen He
出处
期刊:ACS Nano
[American Chemical Society]
日期:2024-08-21
标识
DOI:10.1021/acsnano.4c08695
摘要
Regulating the coordination environment of Fe–Nx sites is an efficient but challenging approach for promoting the intrinsic catalytic activity of single-atom Fe/N-codoped carbon (Fe–N–C) toward the oxygen reduction reaction (ORR). Herein, low-coordination Fe–N3 sites coupled with carbon vacancies (Fe–N3/CV) are directionally constructed in Fe–N–C via pyrolysis of a metal–organic framework (MOF) precursor with N3–Zn–O–Fe moieties, which are delicately prefabricated by chemically anchoring Fe3+ onto a H2O-etching induced linker-missing Zn–N3 site in the MOF precursor. The optimized Fe–N–C with the Fe–N3/CV sites displays a high ORR half-wave potential of 0.92 V (vs RHE), which is attributed to the optimized electronic structure and binding strengths of the active Fe center toward the ORR intermediates stemming from the synergy of the asymmetric configuration of Fe–N3 as well as the adjacent carbon vacancies. This work could be enlightening for the design and construction of high-activity coupling sites in metal and nitrogen-codoped carbon catalysts.
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