• 文献标题:   Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium
  • 文献类型:   Article
  • 作  者:   ZHANG CH, SHA JW, FEI HL, LIU MJ, YAZDI S, ZHANG JB, ZHONG QF, ZOU XL, ZHAO NQ, YU HS, JIANG Z, RINGE E, YAKOBSON BI, DONG JC, CHEN DL, TOUR JM
  • 作者关键词:   oxygen reduction reaction, nitrogendoped graphene oxide, atomically dispersed ruthenium, electrocatalyst
  • 出版物名称:   ACS NANO
  • ISSN:   1936-0851 EI 1936-086X
  • 通讯作者地址:   Rice Univ
  • 被引频次:   100
  • DOI:   10.1021/acsnano.7b02148
  • 出版年:   2017

▎ 摘  要

The cathodic oxygen reduction reaction (ORR) is essential in the electrochemical energy conversion of fuel cells. Here, through the NH3 atmosphere annealing of a graphene oxide (GO) precursor containing trace amounts of Ru, we have synthesized atomically dispersed Ru on nitrogen-doped graphene that performs as an electrocatalyst for the ORR in acidic medium. The Ru/nitrogendoped GO catalyst exhibits excellent four-electron ORR activity, offering onset and half-wave potentials of 0.89 and 0.75 V, respectively, vs a reversible hydrogen electrode (RHE) in 0.1 M HClO4, together with better durability and tolerance toward methanol and carbon monoxide poisoning than seen in commercial Pt/C catalysts. X-ray adsorption fine structure analysis and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy are performed and indicate that the chemical structure of Ru is predominantly composed of isolated Ru atoms coordinated with nitrogen atoms on the graphene substrate. Furthermore, a density function theory study of the ORR mechanism suggests that a Ru-oxo-N-4 structure appears to be responsible for the ORR catalytic activity in the acidic medium. These findings provide a route for the design of efficient ORR single-atom catalysts.