Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium
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
2017
发表期刊ACS NANO
ISSN1936-0851
卷号11期号:7页码:6930-6941
文章类型期刊论文
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.
关键词X-ray-absorption Total-energy Calculations Membrane Fuel-cells Wave Basis-set Carbon Electrocatalysts Oxidation Iron Oxide Performance Cobalt
DOI10.1021/acsnano.7b02148
关键词[WOS]X-RAY-ABSORPTION ; TOTAL-ENERGY CALCULATIONS ; MEMBRANE FUEL-CELLS ; WAVE BASIS-SET ; CARBON ELECTROCATALYSTS ; OXIDATION ; IRON ; OXIDE ; PERFORMANCE ; COBALT
收录类别SCI
语种英语
WOS记录号WOS:000406649700041
引用统计
文献类型期刊论文
条目标识符http://ir.sinap.ac.cn/handle/331007/28819
专题中科院上海应用物理研究所2011-2018年
推荐引用方式
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Zhang, CH,Sha, JW,Fei, HL,et al. Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium[J]. ACS NANO,2017,11(7):6930-6941.
APA Zhang, CH.,Sha, JW.,Fei, HL.,Liu, MJ.,Yazdi, S.,...&Tour, JM.(2017).Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium.ACS NANO,11(7),6930-6941.
MLA Zhang, CH,et al."Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium".ACS NANO 11.7(2017):6930-6941.
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