Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N-4 Active Site Identification Revealed by X-ray Absorption Spectroscopy

doi:10.1021/acscatal.8b00138

CAS OpenIR > 中科院上海应用物理研究所2011-2020年

	Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N-4 Active Site Identification Revealed by X-ray Absorption Spectroscopy
	Xiao, ML ; Zhu, JB ; Ma, L ; Jin, Z ; Ge, J ; Deng, XJ ; Hou, Y ; He, QG ; Li, JK ; Jia, QY ; Mukerjee, S ; Yang, R ; Jiang, Z ; Su, DS ; Liu, CP ; Xing, W
	2018
Source Publication	ACS CATALYSIS
ISSN	2155-5435
Volume	8 Issue:4 Pages:2824-2832
Subtype	期刊论文
Abstract	Developing highly efficient, low-cost oxygen reduction catalysts, especially in acidic medium, is of significance toward fuel cell commercialization. Although pyrolyzed Fe-N-C catalysts have been regarded as alternatives to platinum based catalytic materials, further improvement requires precise control of the Fe-N-x structure at the molecular level and a comprehensive understanding of catalytic site structure and the ORR mechanism on these materials. In this report, we present a microporous metal-organic-framework-confined strategy toward the preferable formation of single-atom dispersed catalysts. The onset potential for Fe-N-C is 0.92 V, comparable to that of Pt/C and outperforming most noble-metal-free catalysts ever reported. A high-spin Fe3+-N-4 configuration is revealed by the Fe-57 Mossbauer spectrum and X-ray absorption spectroscopy for Fe L-edge, which will convert to Fe2+-N-4 at low potential. The in situ reduced Fe2+-N-4 moiety from high-spin O-x-Fe3+-N-4 contributes to most of the ORR activity due to its high turnover frequency (TOF) of ca. 1.71 e s(-1) sites(-1).
Keyword	Oxygen Reduction Reaction Electrolyte Fuel-cells Nitrogen-doped Graphene Fe/n/c-catalysts Carbon Electrocatalysts Transition-metal Iron Efficient Cobalt Phthalocyanine
DOI	10.1021/acscatal.8b00138
Indexed By	SCI
Language	英语
WOS ID	WOS:000430154100025
Citation statistics
Document Type	期刊论文
Identifier	http://ir.sinap.ac.cn/handle/331007/29072
Collection	中科院上海应用物理研究所2011-2020年
Affiliation	1.Xiao, ML 2.Zhu, JB 3.Ma, L 4.Jin, Z 5.Ge, J 6.Deng, XJ 7.Hou, Y 8.He, QG 9.Li, JK 10.Jia, QY 11.Mukerjee, S 12.Yang, R 13.Jiang, Z 14.Su, DS 15.Liu, CP 16.Xing, W
Recommended Citation GB/T 7714	Xiao, ML,Zhu, JB,Ma, L,et al. Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N-4 Active Site Identification Revealed by X-ray Absorption Spectroscopy[J]. ACS CATALYSIS,2018,8(4):2824-2832.
APA	Xiao, ML.,Zhu, JB.,Ma, L.,Jin, Z.,Ge, J.,...&Xing, W.(2018).Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N-4 Active Site Identification Revealed by X-ray Absorption Spectroscopy.ACS CATALYSIS,8(4),2824-2832.
MLA	Xiao, ML,et al."Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N-4 Active Site Identification Revealed by X-ray Absorption Spectroscopy".ACS CATALYSIS 8.4(2018):2824-2832.

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