期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 42, 页码 15089-15097出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201907915
关键词
electrocatalysis; metal-air batteries; metal-free electrocatalysts; oxygen reduction reaction; porous carbon
资金
- National Natural Science Foundation of China [21872104, 21932002, 21821004, 21776219, 21725301, 91645115, 21673273, 21872163]
- National Key R&D Program of China [2017YFB0602200]
- Australian Commonwealth Government
- Australian government
- Government of Western Australia
- China Postdoctoral Science Foundation [2018M631746]
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 sp(3)/sp(2) carbon interface derived from ionic liquids via a simple pyrolysis process. The tunable hybrid sp(3) and sp(2) 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 sp(3)/sp(2) 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 sp(3)/sp(2) carbon interface, which can lower the theoretical overpotential of the ORR.
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