TY - JOUR
T1 - Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions
AU - Zheng, Yao
AU - Jiao, Yan
AU - Zhu, Yihan
AU - Cai, Qiran
AU - Vasileff, Anthony
AU - Li, Lu Hua
AU - Han, Yu
AU - Chen, Ying
AU - Qiao, Shi-Zhang
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.
PY - 2017/2/27
Y1 - 2017/2/27
N2 - 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.
AB - 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.
UR - http://hdl.handle.net/10754/623192
UR - http://pubs.acs.org/doi/abs/10.1021/jacs.6b13100
UR - http://www.scopus.com/inward/record.url?scp=85014645556&partnerID=8YFLogxK
U2 - 10.1021/jacs.6b13100
DO - 10.1021/jacs.6b13100
M3 - Article
C2 - 28221033
SN - 0002-7863
VL - 139
SP - 3336
EP - 3339
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 9
ER -