Journal
CHEMISTRY OF MATERIALS
Volume 27, Issue 4, Pages 1181-1186Publisher
AMER CHEMICAL SOC
DOI: 10.1021/cm5037502
Keywords
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Funding
- Welch Foundation [C-1716]
- NSF [DMR-0928297, CNS-0821727, OCI-0959097]
- U.S. Army Research Office MURI [W911NF-11-1-0362]
- Air Force Office of Scientific Research [FA9550-09-1-0581]
- Air Force Office of Scientific Research MURI [FA9550-12-1-0035]
- Office of Naval Research MURI [N000014-09-1-1066]
- Wigner Fellowship through Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL)
- ORNL's Center for Nanophase Materials Sciences (CNMS) - Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. DOE
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We show that nanoribbons of boron- and nitrogen-substituted graphene can be used as efficient electrocatalysts for the oxygen reduction reaction (ORR). Optimally doped graphene nanoribbons made into three-dimensional porous constructs exhibit the highest onset and half-wave potentials among the reported metal-free catalysts for this reaction and show superior performance compared to commercial Pt/C catalyst. Furthermore, this catalyst possesses high kinetic current density and four-electron transfer pathway with low hydrogen peroxide yield during the reaction. First-principles calculations suggest that such excellent electrotatalytic properties originate from the abundant edges of boron- and nitrogen-codoped graphene nanoribbons, which significantly reduce the energy barriers of the rate-determining steps of the ORR reaction.
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