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Carbon v.132, 2018년, pp.623 - 631   SCI SCIE
본 등재정보는 저널의 등재정보를 참고하여 보여주는 베타서비스로 정확한 논문의 등재여부는 등재기관에 확인하시기 바랍니다.

Manganese deception on graphene and implications in catalysis

Ye, Ruquan (Department of Chemistry, Rice University, 6100 Main Street, Houston, TX 77005, USA ) ; Dong, Juncai (Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China ) ; Wang, Luqing (Department of Materials Science and NanoEngineering, Rice University, 6100 Main Street, Houston, TX 77005, USA ) ; Mendoza-Cruz, Rubén (Department of Physics and Astronomy, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, USA ) ; Li, Yilun (Department of Chemistry, Rice University, 6100 Main Street, Houston, TX 77005, USA ) ; An, Peng-Fei (Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China ) ; Yacamán, Miguel José (Department of Physics and Astronomy, University of Texas at San Antonio, One UTSA Circle, San Antonio, TX 78249, USA ) ; Yakobson, Boris I. (Department of Chemistry, Rice University, 6100 Main Street, Houston, TX 77005, USA ) ; Chen, Dongliang (Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China ) ; Tour, James M. (Department of ) ;
  • 초록  

    Abstract Heteroatom-doped metal-free graphene has been widely studied as the catalyst for the oxygen reduction reaction (ORR). Depending on the preparation method and the dopants, the ORR activity varies ranging from a two-electron to a four-electron pathway. The different literature reports are difficult to correlate due to the large variances. However, due to the potential metal contamination, the origin of the ORR activity from “metal-free” graphene remains confusing and inconclusive. Here we decipher the ORR catalytic activities of diverse architectures on graphene derived from reduced graphene oxide. High angle annular dark field scanning transmission electron microscopy, X-ray absorption near edge structure, extended X-ray absorption fine structure, and trace elemental analysis methods are employed. The mechanistic origin of ORR activity is associated with the trace manganese content and reaches its highest performance at an onset potential of 0.94 V when manganese exists as a mononuclear-centered structure within defective graphene. This study exposes the deceptive role of trace metal in formerly thought to be metal-free graphene materials. It also provides insight into the design of better-performing catalyst for ORR by underscoring the coordination chemistry possible for future single-atom catalyst materials. Graphical abstract [DISPLAY OMISSION]


  • 주제어

    Metal-free catalyst .   Oxygen reduction reaction .   Heteroatom-doped graphene .   Metal-free graphene.  

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