Journal
NATURE CATALYSIS
Volume 2, Issue 8, Pages 688-695Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-019-0297-4
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Funding
- Australia Research Council [ARC DP170103317, ARC DP170102267, ARC DP190103881]
- ARC [ARC DE180101030]
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Owing to the difficulty in controlling the dopant or defect types and their homogeneity in carbon materials, it is still a controversial issue to identify the active sites of carbon-based metal-free catalysts. Here we report a proof-of-concept study on the active-site evaluation for a highly oriented pyrolytic graphite catalyst with specific pentagon carbon defective patterns (D-HOPG). It is demonstrated that specific carbon defect types (an edged pentagon in this work) could be selectively created via controllable nitrogen doping. Work-function analyses coupled with macro and micro-electrochemical performance measurements suggest that the pentagon defects in D-HOPG served as major active sites for the acidic oxygen reduction reaction, even much superior to the pyridinic nitrogen sites in nitrogen-doped highly oriented pyrolytic graphite. This work enables us to elucidate the relative importance of the specific carbon defects versus nitrogen-dopant species and their respective contributions to the observed overall acidic oxygen reduction reaction activity.
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