Study of the evolution of FeNxCy and Fe3C species in Fe/N/C catalysts during the oxygen reduction reaction in acid and alkaline electrolyte

被引：37
作者：
Garcia, Alvaro [1 ]
Pascual, Laura [2 ]
Ferrer, Pilar [3 ]
Gianolio, Diego [3 ]
Held, Georg [3 ]
Grinter, David C. [3 ]
Pena, Miguel A. [1 ]
Retuerto, Maria [1 ]
Rojas, Sergio [1 ]
机构：
[1] CSIC, Inst Catalisis & Petr Quim, Grp Energia & Quim Sostenibles, Marie Curie 2, Madrid 28049, Spain
[2] CSIC, Inst Catalisis & Petr Quim, Marie Curie 2, Madrid 28049, Spain
[3] Diamond Light Source, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England
来源：
JOURNAL OF POWER SOURCES | 2021年 / 490卷
关键词：
Fe/N/C; ORR; Fe-N-pyridinic; Fe-N-pyrrolic; NEXAFS; Surface sites;
D O I：
10.1016/j.jpowsour.2021.229487
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
The nature and evolution of FeNxCy moieties in Fe/C/N catalysts has been studied by analysing Fe and N environments. TEM and Fe-XAS reveal the presence of FeNx moieties and Fe3C particles in the fresh catalyst. NEXAFS reveals the presence of two groups of (Fe)NxCy ensembles, namely (Fe)N-x-pyridinic and (Fe)N-x-pyrrolic. The architecture of the FeNxCy ensembles and their evolution during the ORR has been analysed by XAS, NEXAFS, and identical locations TEM. NxCy, FeNxCy and Fe3C species are partially removed during the ORR, resulting in the formation of Fe2O3 and Fe3O4 particles with different morphologies. The process is more severe in acid electrolyte than in alkaline one. (Fe)N-x-pyrrolic moieties are the main ones in the fresh catalysts, but (Fe) N-x-pyridinic groups are more stable after the ORR. The correlation between the evolution of the ORR activity and that of the FeNxCy ensembles indicates that FeNx-pyridinic ensembles are responsible for the ORR activity.
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页数：10
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