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

Handle URI:
http://hdl.handle.net/10754/623192
Title:
Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions
Authors:
Zheng, Yao; Jiao, Yan ( 0000-0003-1329-4290 ) ; Zhu, Yihan; Cai, Qiran; Vasileff, Anthony; Li, Lu Hua; Han, Yu ( 0000-0003-1462-1118 ) ; Chen, Ying ( 0000-0002-7322-2224 ) ; Qiao, Shi-Zhang ( 0000-0002-4568-8422 )
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.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division
Citation:
Zheng Y, Jiao Y, Zhu Y, Cai Q, Vasileff A, et al. (2017) Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions. Journal of the American Chemical Society 139: 3336–3339. Available: http://dx.doi.org/10.1021/jacs.6b13100.
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
21-Feb-2017
DOI:
10.1021/jacs.6b13100
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
We acknowledge financial support by the Australian Research Council (DP 170104464, DP160104866, DP140104062, and DE160101163). NEXAFS and EXAFS were performed at Australian Synchrotron. DFT calculations were carried out using the NCI National Facility systems.
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/jacs.6b13100
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorZheng, Yaoen
dc.contributor.authorJiao, Yanen
dc.contributor.authorZhu, Yihanen
dc.contributor.authorCai, Qiranen
dc.contributor.authorVasileff, Anthonyen
dc.contributor.authorLi, Lu Huaen
dc.contributor.authorHan, Yuen
dc.contributor.authorChen, Yingen
dc.contributor.authorQiao, Shi-Zhangen
dc.date.accessioned2017-04-13T11:51:00Z-
dc.date.available2017-04-13T11:51:00Z-
dc.date.issued2017-02-21en
dc.identifier.citationZheng Y, Jiao Y, Zhu Y, Cai Q, Vasileff A, et al. (2017) Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions. Journal of the American Chemical Society 139: 3336–3339. Available: http://dx.doi.org/10.1021/jacs.6b13100.en
dc.identifier.issn0002-7863en
dc.identifier.issn1520-5126en
dc.identifier.doi10.1021/jacs.6b13100en
dc.identifier.urihttp://hdl.handle.net/10754/623192-
dc.description.abstractOrganometallic 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.en
dc.description.sponsorshipWe acknowledge financial support by the Australian Research Council (DP 170104464, DP160104866, DP140104062, and DE160101163). NEXAFS and EXAFS were performed at Australian Synchrotron. DFT calculations were carried out using the NCI National Facility systems.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.6b13100en
dc.titleMolecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactionsen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalJournal of the American Chemical Societyen
dc.contributor.institutionSchool of Chemical Engineering, University of Adelaide , Adelaide, SA 5005, Australia.en
dc.contributor.institutionInstitute for Frontier Materials, Deakin University , Waurn Ponds, VIC 3216, Australia.en
kaust.authorZhu, Yihanen
kaust.authorHan, Yuen
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