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Molecule-level g-C3N4 coordinated transition metals as a new class of electrocatalysts for oxygen electrode reactions

journal contribution
posted on 08.03.2017, 00:00 authored by Y Zheng, Y Jiao, Y Zhu, Qiran CaiQiran Cai, A Vasileff, Luhua LiLuhua Li, Y Han, Ying (Ian) ChenYing (Ian) Chen, S-Z Qiao
Organometallic complexes with metal-nitrogen/carbon (M-N/C) coordination are the most important alternatives to precious metal catalysts for oxygen reduction and evolution reactions (ORR and OER) in energy conversion devices. Here, we designed and developed a range of molecule-level graphitic carbon nitride (g-C3N4) coordinated transition metals (M-C3N4) as a new generation of M-N/C catalysts for these oxygen electrode reactions. As a proof-of-concept example, we conducted theoretical evaluation and experimental validation on a cobalt-C3N4 catalyst with a desired molecular configuration, which possesses comparable electrocatalytic activity to that of precious metal benchmarks for the ORR and OER in alkaline media. The correlation of experimental and computational results confirms that this high activity originates from the precise M-N2 coordination in the g-C3N4 matrix. Moreover, the reversible ORR/OER activity trend for a wide variety of M-C3N4 complexes has been constructed to provide guidance for the molecular design of this promising class of catalysts.

History

Journal

Journal of the American Chemical Society

Volume

139

Issue

9

Pagination

3336 - 3339

Publisher

American Chemical Society

Location

Washington D.C.

eISSN

1520-5126

Language

eng

Publication classification

C1 Refereed article in a scholarly journal

Copyright notice

2017, American Chemical Society