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Sci Rep. 2013;3:1810. doi: 10.1038/srep01810.

Facile, scalable synthesis of edge-halogenated graphene nanoplatelets as efficient metal-free eletrocatalysts for oxygen reduction reaction.

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Interdisciplinary School of Green Energy, Low-Dimensional Carbon Materials Center, Ulsan National Institute of Science and Technology (UNIST), 100 Banyeon, Ulsan, South Korea.


A series of edge-selectively halogenated (X = Cl, Br, I) graphene nanoplatelets (XGnPs = ClGnP, BrGnP, IGnP) were prepared simply by ball-milling graphite in the presence of Cl2, Br2 and I2, respectively. High BET surface areas of 471, 579 and 662 m(2)/g were observed for ClGnP, BrGnP and IGnP, respectively, indicating a significant extent of delamination during the ball-milling and subsequent workup processes. The newly-developed XGnPs can be well dispersed in various solvents, and hence are solution processable. Furthermore, XGnPs showed remarkable electrocatalytic activities toward oxygen reduction reaction (ORR) with a high selectivity, good tolerance to methanol crossover/CO poisoning effects, and excellent long-term cycle stability. First-principle density-functional calculations revealed that halogenated graphene edges could provide decent adsorption sites for oxygen molecules, in a good agreement with the experimental observations.

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