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Highly active sites of low spin FeN4species:The identification and the ORR performance
引用本文:Huizhu Cai,Bingbing Chen,Xiao Zhang,Yuchen Deng,Dequan Xiao,Ding Ma,Chuan Shi. Highly active sites of low spin FeN4species:The identification and the ORR performance[J]. Nano Research, 2021, 14(1): 122-130. DOI: 10.1007/s12274-020-3054-8
作者姓名:Huizhu Cai  Bingbing Chen  Xiao Zhang  Yuchen Deng  Dequan Xiao  Ding Ma  Chuan Shi
作者单位:State Key Laboratory of Fine Chemicals;College of Chemistry and Molecular Engineering and College of Engineering;Center for Integrative Materials Discovery
基金项目:the National Key R&D Program of China(No.2017YFA0700103);the National Natural Science Foundation of China(Nos.21932002,21872014,21707015,21902018,21577013);the Postdoctoral Science Foundation of China(Nos.2019 T 120210,2018M 641687);the Natural Science Foundation of Liaoning Province(No.2019-MS-053).
摘    要:Over recent years,catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction(ORR).However,the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being obtained.Herein Fe3C/C and Fe2N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15%CH4/H2and pure NH3,respectively.By acid leaching of Fe2N/C sample,only single sites of FeN4species were presented,providing an ideal model for identification of catalytic functions of the single sites of FeN4in ORR.A correlation was conducted between the concentration of FeN4in low spin state by Mossbauer spectra and the kinetic current density at 0.8 V in alkaline media,and such a structure-performance correlation assures the catalytic roles of low spin FeN4 species as highly active sites for the ORR.

关 键 词:single  sites  of  FeN4  oxygen  reduction  reaction  structure-performance  correlation  ELECTROCATALYSIS

Highly active sites of low spin FeIIN4 species: The identification and the ORR performance
Cai,Huizhu,Chen,Bingbing,Zhang,Xiao,Deng,Yuchen,Xiao,Dequan,Ma,Ding,Shi,Chuan. Highly active sites of low spin FeIIN4 species: The identification and the ORR performance[J]. Nano Research, 2021, 14(1): 122-130. DOI: 10.1007/s12274-020-3054-8
Authors:Cai  Huizhu  Chen  Bingbing  Zhang  Xiao  Deng  Yuchen  Xiao  Dequan  Ma  Ding  Shi  Chuan
Affiliation:1.State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China
;2.College of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing, 100871, China
;3.Center for Integrative Materials Discovery, Department of Chemistry and Chemical Engineering, University of New Haven, New Haven, CT, 06516, USA
;
Abstract:

Over recent years, catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction (ORR). However, the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being obtained. Herein Fe3C/C and Fe2N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15% CH4/H2 and pure NH3, respectively. By acid leaching of Fe2N/C sample, only single sites of FeN4 species were presented, providing an ideal model for identification of catalytic functions of the single sites of FeN4 in ORR. A correlation was conducted between the concentration of FeIIN4 in low spin state by Mössbauer spectra and the kinetic current density at 0.8 V in alkaline media, and such a structure-performance correlation assures the catalytic roles of low spin FeIIN4 species as highly active sites for the ORR.

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