Construction of a sp3 /sp2 Carbon Interface in 3D N-Doped Nanocarbons for the Oxygen Reduction Reaction

Gao, Wang, Wu, Liu, Wang, Yu, Li, Wang, Song, Gao, Peng, Zhang, Ma, Wang, Zhou, Wang, Yin, Ma (2019) Construction of a sp3 /sp2 Carbon Interface in 3D N-Doped Nanocarbons for the Oxygen Reduction Reaction Angew Chem Int Ed Engl (IF: -1) 58(42) 15089-15097

Abstract

The development of highly efficient metal-free carbon electrocatalysts for the oxygen reduction reaction (ORR) is one very promising strategy for the exploitation and commercialization of renewable and clean energy, but this still remains a significant challenge. Herein, we demonstrate a facile approach to prepare three-dimensional (3D) N-doped carbon with a sp3 /sp2 carbon interface derived from ionic liquids via a simple pyrolysis process. The tunable hybrid sp3 and sp2 carbon composition and pore structures stem from the transformation of ionic liquids to polymerized organics and introduction of a Co metal salt. Through tuning both composition and pores, the 3D N-doped nanocarbon with a high sp3 /sp2 carbon ratio on the surface exhibits a superior electrocatalytic performance for the ORR compared to that of the commercial Pt/C in Zn-air batteries. Density functional theory calculations suggest that the improved ORR performance can be ascribed to the existence of N dopants at the sp3 /sp2 carbon interface, which can lower the theoretical overpotential of the ORR.© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Links

http://www.ncbi.nlm.nih.gov/pubmed/31444841
http://dx.doi.org/10.1002/anie.201907915

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