Atomically dispersed quintuple nitrogen and oxygen co-coordinated zirconium on graphene-type substrate for highly efficient oxygen reduction reaction.

Zhao, Xue; Wang, Jing; Wang, Jinming; Yang, Meng; Yan, Chenglin; Zou, Guodong; Tse, John S.; Fernandez, Carlos; Peng, Qiuming

Abstract

A cost-effective and long stability catalyst with decent electrochemical activity would play a crucial role in accelerating applications of metal-air batteries. Here, we report quintuple nitrogen and oxygen co-coordinated Zr sites on graphene (Zr-N/O-C) by using a ball-milling, solid-solution-assisted pyrolysis method. The as-prepared Zr-N/O-C catalyst with 2.93 wt % Zr shows a half-wave potential of 0.910 V, an onset potential of 1.000 V in 0.1 M KOH, impressive durability (95.1% remains after 16,000 s), and long-term stability (5 mV loss over 10,000 cycles). Zn-air batteries with the Zr-N/O-C electrode exhibit a maximum power density of 217.9 mW cm−2 and a high cycling life of over 1,000 h, exceeding the counterpart equipped with a Pt/C benchmark. Theoretical simulations demonstrate that nitrogen and oxygen dual-ligand confinement effectively tunes the d-band center and balances key intermediates binding energy of intrinsic quintuple coordination Zr sites.

Citation

ZHAO, X., WANG, J., WANG, J., YANG, M., YAN, C., ZOU, G., TSE, J.S., FERNANDEZ, C. and PENG, Q. 2022. Atomically dispersed quintuple nitrogen and oxygen co-coordinated zirconium on graphene-type substrate for highly efficient oxygen reduction reaction. Cell reports physical science [online], 3(3), article 100773. Available from: https://doi.org/10.1016/j.xcrp.2022.100773

• Journal Article Type: Article
• Acceptance Date: Jan 25, 2022
• Online Publication Date: Mar 16, 2022
• Publication Date: Mar 16, 2022
• Deposit Date: Mar 18, 2022
• Publicly Available Date: Mar 18, 2022
• Journal: Cell Reports Physical Science
• Print ISSN: 2666-3864
• Electronic ISSN: 2666-3864
• Publisher: Elsevier
• Peer Reviewed: Peer Reviewed
• Volume: 3
• Issue: 3
• Article Number: 100773
• DOI: https://doi.org/10.1016/j.xcrp.2022.100773
• Keywords: Single atomic Zr; Quintuple coordination; Electrochemical catalyst; DFT calculations; Oxygen reduction reaction; Zn-air battery
• Public URL: https://rgu-repository.worktribe.com/output/1625209
• Additional Information: The accompanying file also contains supplementary material which can be found at pages 17-40, at the end of the main text.