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Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN4 Sites for Oxygen Reduction.
Li, Jiazhan; Zhang, Hanguang; Samarakoon, Widitha; Shan, Weitao; Cullen, David A; Karakalos, Stavros; Chen, Mengjie; Gu, Daming; More, Karren L; Wang, Guofeng; Feng, Zhenxing; Wang, Zhenbo; Wu, Gang.
Afiliación
  • Li J; Department MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.
  • Zhang H; Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
  • Samarakoon W; Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
  • Shan W; School of Chemical Biological, and Environmental Engineering, Oregon State University, Corvallis, OR, 97331, USA.
  • Cullen DA; Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, PA, 15261, USA.
  • Karakalos S; Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
  • Chen M; Department of Chemical Engineering, University of South Carolina, Columbia, SC, 29208, USA.
  • Gu D; Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
  • More KL; Department MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.
  • Wang G; Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
  • Feng Z; Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, PA, 15261, USA.
  • Wang Z; School of Chemical Biological, and Environmental Engineering, Oregon State University, Corvallis, OR, 97331, USA.
  • Wu G; Department MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China.
Angew Chem Int Ed Engl ; 58(52): 18971-18980, 2019 Dec 19.
Article en En | MEDLINE | ID: mdl-31633848
ABSTRACT
FeN4 moieties embedded in partially graphitized carbon are the most efficient platinum group metal free active sites for the oxygen reduction reaction in acidic proton-exchange membrane fuel cells. However, their formation mechanisms have remained elusive for decades because the Fe-N bond formation process always convolutes with uncontrolled carbonization and nitrogen doping during high-temperature treatment. Here, we elucidate the FeN4 site formation mechanisms through hosting Fe ions into a nitrogen-doped carbon followed by a controlled thermal activation. Among the studied hosts, the ZIF-8-derived nitrogen-doped carbon is an ideal model with well-defined nitrogen doping and porosity. This approach is able to deconvolute Fe-N bond formation from complex carbonization and nitrogen doping, which correlates Fe-N bond properties with the activity and stability of FeN4 sites as a function of the thermal activation temperature.
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Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2019 Tipo del documento: Article País de afiliación: China
Texto completo
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2019 Tipo del documento: Article País de afiliación: China