Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium

Zhang, Chenhao; Sha, Junwei; Fei, Huilong; Liu, Mingjie; Yazdi, Sadegh; Zhang, Jibo; Zhong, Qifeng; Zou, Xiaolong; Zhao, Naiqin; Yu, Haisheng; Jiang, Zheng; Ringe, Emilie; Yakobson, Boris I.; Dong, Juncai; Chen, Dongliang; Tour, James M.

doi:10.1021/acsnano.7b02148

Title: Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium

Journal Article · Wed Jun 28 00:00:00 EDT 2017 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.7b02148· OSTI ID:1414051

Zhang, Chenhao;

^[1]; Fei, Huilong; Liu, Mingjie; Yazdi, Sadegh; Zhang, Jibo; Zhong, Qifeng; Zou, Xiaolong; Zhao, Naiqin ^[1]; Yu, Haisheng ^[2];

^[2]; Ringe, Emilie; Yakobson, Boris I.; Dong, Juncai ^[3]; Chen, Dongliang ^[3];

School of Materials Science and Engineering, Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin 300350, China, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300350, China
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

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/nitrogen-doped 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-N4 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.

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Research Organization:: Rice Univ., Houston, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012547

OSTI ID:: 1414051

Alternate ID(s):: OSTI ID: 1473883; OSTI ID: 1508003

Journal Information:: ACS Nano, Journal Name: ACS Nano Vol. 11 Journal Issue: 7; ISSN 1936-0851

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
oxygen reduction reaction
nitrogen-doped graphene oxide
atomically dispersed ruthenium
electrocatalysts

Title: Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium

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