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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 PublicationACS CATALYSIS
ISSN2155-5435
Volume8Issue:4Pages:2824-2832
Subtype期刊论文
AbstractDeveloping 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).
KeywordOxygen Reduction Reaction Electrolyte Fuel-cells Nitrogen-doped Graphene Fe/n/c-catalysts Carbon Electrocatalysts Transition-metal Iron Efficient Cobalt Phthalocyanine
DOI10.1021/acscatal.8b00138
Indexed BySCI
Language英语
WOS IDWOS:000430154100025
Citation statistics
Cited Times:57[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/29072
Collection中科院上海应用物理研究所2011-2019年
Affiliation1.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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