The role of metal-oxo intermediate to oxygen reduction reaction catalysis: A theoretical investigation using nitrogen-substituted carbon nanotube models

Yu Te Chan, Ming Kang Tsai

研究成果: 雜誌貢獻期刊論文同行評審

摘要

The electrochemical oxygen reduction mechanism (ORR) using the transition metal embedded and nitrogen substituted carbon-material models – TM–N4L (TM = Fe, Ru, Os, Co, Rh, Ir, Ni, Pt, and Cu; L = CNT(5,5) and graphene) are investigated. The models of group 9 elements (Co, Rh, Ir) appear to give the most uniform stepwise free energy along the 4e reduction pathway in comparison with the ideal electrochemical steps, and that could provide the most stable electric potential generation in fuels cell applications. The free energy of formation for the oxo intermediates is the determinant factor to cause the deviation from the ideal steps. The models of group 8 elements (Fe, Ru, Os) preferentially form multiple coordination bonds with the oxo intermediate via the empty d-orbitals of metal centers. In the 2e vs. 4e reduction comparison, the Fe–N4L models are found to favor 4e pathway because of the accessible O–O bond breaking barrier of Fe(OOH) intermediate around 0.5 eV while the Co models could favor the 2e pathway to form HOOH(aq). This theoretical analysis of metal-based chemistry for ORR catalysis could be helpful to the future ORR catalyst development.

原文英語
頁(從 - 到)301-305
頁數5
期刊Surface Science
677
DOIs
出版狀態已發佈 - 2018 十一月

ASJC Scopus subject areas

  • 凝聚態物理學
  • 表面和介面
  • 表面、塗料和薄膜
  • 材料化學

指紋

深入研究「The role of metal-oxo intermediate to oxygen reduction reaction catalysis: A theoretical investigation using nitrogen-substituted carbon nanotube models」主題。共同形成了獨特的指紋。

引用此