Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions

Yao Zheng, Yan Jiao, Yihan Zhu, Qiran Cai, Anthony Vasileff, Lu Hua Li, Yu Han, Ying Chen, Shi-Zhang Qiao

Research output: Contribution to journalArticlepeer-review

669 Scopus citations

Abstract

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.
Original languageEnglish (US)
Pages (from-to)3336-3339
Number of pages4
JournalJournal of the American Chemical Society
Volume139
Issue number9
DOIs
StatePublished - Feb 27 2017

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