Journal
CARBON
Volume 132, Issue -, Pages 623-631Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2018.02.082
Keywords
Metal-free catalyst; Oxygen reduction reaction; Heteroatom-doped graphene; Metal-free graphene
Funding
- Air Force Office of Scientific Research [FA9550-14-1-0111]
- Office of Naval Research [N00014-15-1-2372]
- Ken Kennedy Institute for Information Technology Shell Graduate Fellowship
- National Center for Research Resources [5 G12RR013646-12]
- NSF-PREM [DMR 0934218]
- Welch Foundation [AX-1615]
- National Natural Science Foundation of China [11605225]
- Youth Innovation Promotion Association, Chinese Academy of Science
- Jialin Xie Foundation of Institute of High Energy Physics, Chinese Academy of Sciences
- NATIONAL CENTER FOR RESEARCH RESOURCES [G12RR013646] Funding Source: NIH RePORTER
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [S06GM008194] Funding Source: NIH RePORTER
- National Institute on Minority Health and Health Disparities [G12MD007591] Funding Source: NIH RePORTER
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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. (c) 2018 Elsevier Ltd. All rights reserved.
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