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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; Xing, W (reprint author), Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Jilin, Peoples R China.; Ge, J (reprint author), Chinese Acad Sci, Changchun Inst Appl Chem, Lab Adv Power Sources, Changchun 130022, Jilin, Peoples R China.; He, QG (reprint author), Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China.
2018-04-01
Source PublicationACS CATALYSIS
ISSN2155-5435
Volume8Issue:4Pages:2824-2832
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).; 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).
description.department[xiao, meiling ; zhu, jianbing ; xing, wei] chinese acad sci, changchun inst appl chem, state key lab electroanalyt chem, changchun 130022, jilin, peoples r china ; [ma, liang] china univ geosci, fac mat sci & chem, wuhan 430074, hubei, peoples r china ; [jin, zhao ; ge, junjie ; liu, changpeng] chinese acad sci, changchun inst appl chem, lab adv power sources, changchun 130022, jilin, peoples r china ; [deng, xin ; hou, yang ; he, qinggang] zhejiang univ, coll chem & biol engn, hangzhou 310027, zhejiang, peoples r china ; [li, jingkun ; jia, qingying ; mukerjee, sanjeev] northeastern univ, dept chem & chem biol, 360 huntington ave, boston, ma 02115 usa ; [yang, ruoou ; jiang, zheng] chinese acad sci, shanghai inst appl phys, shanghai synchrotron radiat facil, shanghai 201204, peoples r china ; [su, dangsheng] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang, liaoning, peoples r china
KeywordOxygen Reduction Reaction Electrolyte Fuel-cells Nitrogen-doped Graphene Fe/n/c-catalysts Carbon Electrocatalysts Transition-metal Iron Efficient Cobalt Phthalocyanine
Subject AreaChemistry, Physical
Funding OrganizationNational Natural Science Foundation of China [21633008, 21433003, U1601211, 21733004]; National Science and Technology Major Project [2016YFB0101202]; Jilin Province Science and Technology Development Program [20150101066JC, 20160622037JC, 20170203003SF, 20170520150JH]; Chinese Academy of Sciences; Recruitment Program of Foreign Experts [WQ20122200077]; National Synchrotron Light Source (NSLS) II, Brookhaven National Laboratory under U.S. DOE [DE-SC0012704]; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
Indexed BySCI
Language英语
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/79376
Collection中国科学院金属研究所
Corresponding AuthorXing, W (reprint author), Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Jilin, Peoples R China.; Ge, J (reprint author), Chinese Acad Sci, Changchun Inst Appl Chem, Lab Adv Power Sources, Changchun 130022, Jilin, Peoples R China.; He, QG (reprint author), Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China.
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.,...&He, QG .(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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