Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 53, Issue 40, Pages 10804-10808Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201406695
Keywords
droplets; electrochemistry; fuel cell; graphite; oxygen reduction reaction
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Funding
- AFOSR MURI [FA9550-12-1-0037]
- National Science Foundation [IIP-1343270, CMMI-133123]
- Youth 1000 Talent Program of China
- Inter-discipline Research Program of Hunan University
- Div Of Industrial Innovation & Partnersh
- Directorate For Engineering [1343270] Funding Source: National Science Foundation
- EPSRC [EP/I005145/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/I005145/1] Funding Source: researchfish
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Carbon-based metal-free electrocatalysts for the oxygen reduction reaction (ORR) in alkaline medium have been extensively investigated with the aim of replacing the commercially available, but precious platinum-based catalysts. For the proper design of carbon-based metal-free electrocatalysts for the ORR, it would be interesting to identify the active sites of the electrocatalyst. The ORR was now studied with an air-saturated electrolyte solution droplet (diameter ca. 15 mm), which was deposited at a specified position either on the edge or on the basal plane of highly oriented pyrolytic graphite. Electrochemical measurements suggest that the edge carbon atoms are more active than the basal-plane ones for the ORR. This provides a direct way to identify the active sites of carbon materials for the ORR. Ball-milled graphite and carbon nanotubes with more exposed edges were also prepared and showed significantly enhanced ORR activity. DFT calculations elucidated the mechanism by which the charged edge carbon atoms result in the higher ORR activity.
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