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Improving the Stability of Non-Noble-Metal M-N-C Catalysts for Proton-Exchange-Membrane Fuel Cells through M-N Bond Length and Coordination Regulation.
Miao, Zhengpei; Wang, Xiaoming; Zhao, Zhonglong; Zuo, Wenbin; Chen, Shaoqing; Li, Zhiqiang; He, Yanghua; Liang, Jiashun; Ma, Feng; Wang, Hsing-Lin; Lu, Gang; Huang, Yunhui; Wu, Gang; Li, Qing.
Afiliação
  • Miao Z; State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
  • Wang X; Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Shantou, 515063, China.
  • Zhao Z; Department of Physics and Astronomy, California State University Northridge, Northridge, CA, 91330, USA.
  • Zuo W; Key Laboratory of Artificial Micro, and Nano-Materials of Ministry of Education and Hubei Key Laboratory of Nuclear Solid Physics, School of Physics and Technology, Wuhan University, Wuhan, 430072, China.
  • Chen S; Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong, 518055, China.
  • Li Z; State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
  • He Y; Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
  • Liang J; State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
  • Ma F; State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
  • Wang HL; Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong, 518055, China.
  • Lu G; Department of Physics and Astronomy, California State University Northridge, Northridge, CA, 91330, USA.
  • Huang Y; State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
  • Wu G; Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, NY, 14260, USA.
  • Li Q; State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
Adv Mater ; 33(39): e2006613, 2021 Oct.
Article em En | MEDLINE | ID: mdl-34396608
ABSTRACT
An effective and universal strategy is developed to enhance the stability of the non-noble-metal M-Nx /C catalyst in proton exchange membrane fuel cells (PEMFCs) by improving the bonding strength between metal ions and chelating polymers, i.e., poly(acrylic acid) (PAA) homopolymer and poly(acrylic acid-maleic acid) (P(AA-MA)) copolymer with different AA/MA ratios. Mössbauer spectroscopy and X-ray absorption spectroscopy (XAS) reveal that the optimal P(AA-MA)-Fe-N catalyst with a higher Fe3+ -polymer binding constant possesses longer FeN bonds and exclusive Fe-N4 /C moiety compared to PAA-Fe-N, which consists of ≈15% low-coordinated Fe-N2 /N3 structures. The optimized P(AA-MA)-Fe-N catalyst exhibits outstanding ORR activity and stability in both half-cell and PEMFC cathodes, with the retention rate of current density approaching 100% for the first 37 h at 0.55 V in an H2 -air fuel cell. Density functional theory (DFT) calculations suggest that the Fe-N4 /C site could optimize the difference between the adsorption energy of the Fe atoms on the support (Ead ) and the bulk cohesive energy (Ecoh ) relative to Fe-N2 /N3 moieties, thereby strongly stabilizing Fe centers against demetalation.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Ano de publicação: 2021 Tipo de documento: Article
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Ano de publicação: 2021 Tipo de documento: Article