title: Molecule-Level g-C3N4Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions.
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-C3N4catalyst 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-N2coordination in the g-C3N4matrix. Moreover, the reversible ORR/OER activity trend for a wide variety of M-C3N4complexes has been constructed to provide guidance for the molecular design of this promising class of catalysts.
authors.affiliation: School of Chemical Engineering, University of Adelaide , Adelaide, SA 5005, Australia.
authors.forename: Yao
authors.initials: Y
authors.lastname: Zheng
authors.affiliation: School of Chemical Engineering, University of Adelaide , Adelaide, SA 5005, Australia.
authors.forename: Yan
authors.identifier: 0000-0003-1329-4290
authors.initials: Y
authors.lastname: Jiao
authors.affiliation: Advanced Membrane and Porous Materials Center, Physical Science and Engineering Division, King Abdullah University of Science and Technology , Thuwal 23955-6900, Saudi Arabia.
authors.forename: Yihan
authors.initials: Y
authors.lastname: Zhu
authors.affiliation: Institute for Frontier Materials, Deakin University , Waurn Ponds, VIC 3216, Australia.
authors.forename: Qiran
authors.initials: Q
authors.lastname: Cai
authors.affiliation: School of Chemical Engineering, University of Adelaide , Adelaide, SA 5005, Australia.
authors.forename: Anthony
authors.initials: A
authors.lastname: Vasileff
authors.affiliation: Institute for Frontier Materials, Deakin University , Waurn Ponds, VIC 3216, Australia.
authors.forename: Lu Hua
authors.initials: LH
authors.lastname: Li
authors.affiliation: Advanced Membrane and Porous Materials Center, Physical Science and Engineering Division, King Abdullah University of Science and Technology , Thuwal 23955-6900, Saudi Arabia.
authors.forename: Yu
authors.initials: Y
authors.lastname: Han
authors.affiliation: Institute for Frontier Materials, Deakin University , Waurn Ponds, VIC 3216, Australia.
authors.forename: Ying
authors.identifier: 0000-0002-7322-2224
authors.initials: Y
authors.lastname: Chen
authors.affiliation: School of Chemical Engineering, University of Adelaide , Adelaide, SA 5005, Australia.
authors.forename: Shi-Zhang
authors.identifier: 0000-0002-4568-8422
authors.initials: SZ
authors.lastname: Qiao