Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media

Polynary transition-metal atom catalysts are promising to supersede platinum (Pt)-based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the key to catalyst performance enhancement. Different from the previously reported single-atom or dual-ato...

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Main Authors: Wang, Zhe, Jin, Xiaoyan, Zhu, Chao, Liu, Yipu, Tan, Hua, Ku, Ruiqi, Zhang, Yongqi, Zhou, Liujiang, Liu, Zheng, Hwang, Seong-Ju, Fan, Hong Jin
Other Authors: School of Physical and Mathematical Sciences
Format: Journal Article
Language:English
Published: 2022
Subjects:
Online Access:https://hdl.handle.net/10356/154780
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author Wang, Zhe
Jin, Xiaoyan
Zhu, Chao
Liu, Yipu
Tan, Hua
Ku, Ruiqi
Zhang, Yongqi
Zhou, Liujiang
Liu, Zheng
Hwang, Seong-Ju
Fan, Hong Jin
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Wang, Zhe
Jin, Xiaoyan
Zhu, Chao
Liu, Yipu
Tan, Hua
Ku, Ruiqi
Zhang, Yongqi
Zhou, Liujiang
Liu, Zheng
Hwang, Seong-Ju
Fan, Hong Jin
author_sort Wang, Zhe
collection NTU
description Polynary transition-metal atom catalysts are promising to supersede platinum (Pt)-based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the key to catalyst performance enhancement. Different from the previously reported single-atom or dual-atom configurations, a new type of ternary-atom catalyst, which consists of atomically dispersed, nitrogen-coordinated Co-Co dimers, and Fe single sites (i.e., Co2 -N6 and Fe-N4 structures) that are coanchored on highly graphitized carbon supports is developed. This unique atomic ORR catalyst outperforms the catalysts with only Co2 -N6 or Fe-N4 sites in both alkaline and acid conditions. Density functional theory calculations clearly unravels the synergistic effect of the Co2 -N6 and Fe-N4 sites, which can induce higher filling degree of Fe-d orbitals and favors the binding capability to *OH intermediates (the rate determining step). This ternary-atom catalyst may be a promising alternative to Pt to drive the cathodic ORR in zinc-air batteries.
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spelling ntu-10356/1547802023-02-28T19:43:05Z Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media Wang, Zhe Jin, Xiaoyan Zhu, Chao Liu, Yipu Tan, Hua Ku, Ruiqi Zhang, Yongqi Zhou, Liujiang Liu, Zheng Hwang, Seong-Ju Fan, Hong Jin School of Physical and Mathematical Sciences School of Materials Science and Engineering Engineering::Materials Metal–Air Batteries Oxygen Reduction Reaction Polynary transition-metal atom catalysts are promising to supersede platinum (Pt)-based catalysts for oxygen reduction reaction (ORR). Regulating the local configuration of atomic catalysts is the key to catalyst performance enhancement. Different from the previously reported single-atom or dual-atom configurations, a new type of ternary-atom catalyst, which consists of atomically dispersed, nitrogen-coordinated Co-Co dimers, and Fe single sites (i.e., Co2 -N6 and Fe-N4 structures) that are coanchored on highly graphitized carbon supports is developed. This unique atomic ORR catalyst outperforms the catalysts with only Co2 -N6 or Fe-N4 sites in both alkaline and acid conditions. Density functional theory calculations clearly unravels the synergistic effect of the Co2 -N6 and Fe-N4 sites, which can induce higher filling degree of Fe-d orbitals and favors the binding capability to *OH intermediates (the rate determining step). This ternary-atom catalyst may be a promising alternative to Pt to drive the cathodic ORR in zinc-air batteries. Agency for Science, Technology and Research (A*STAR) Accepted version H.J. F. thanks the financial support from Agency for Science, Technology, and Research (A*STAR), Singapore by AME Individual Research Grants (A1983c0026). 2022-01-10T05:46:58Z 2022-01-10T05:46:58Z 2021 Journal Article Wang, Z., Jin, X., Zhu, C., Liu, Y., Tan, H., Ku, R., Zhang, Y., Zhou, L., Liu, Z., Hwang, S. & Fan, H. J. (2021). Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media. Advanced Materials, 33(49), 2104718-. https://dx.doi.org/10.1002/adma.202104718 0935-9648 https://hdl.handle.net/10356/154780 10.1002/adma.202104718 34626018 2-s2.0-85116568471 49 33 2104718 en A1983c0026 Advanced Materials This is the peer reviewed version of the following article: Wang, Z., Jin, X., Zhu, C., Liu, Y., Tan, H., Ku, R., Zhang, Y., Zhou, L., Liu, Z., Hwang, S. & Fan, H. J. (2021). Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media. Advanced Materials, 33(49), 2104718-, which has been published in final form at https://doi.org/10.1002/adma.202104718. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. application/pdf
spellingShingle Engineering::Materials
Metal–Air Batteries
Oxygen Reduction Reaction
Wang, Zhe
Jin, Xiaoyan
Zhu, Chao
Liu, Yipu
Tan, Hua
Ku, Ruiqi
Zhang, Yongqi
Zhou, Liujiang
Liu, Zheng
Hwang, Seong-Ju
Fan, Hong Jin
Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
title Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
title_full Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
title_fullStr Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
title_full_unstemmed Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
title_short Atomically dispersed Co₂ -N₆ and Fe-N₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
title_sort atomically dispersed co₂ n₆ and fe n₄ costructures boost oxygen reduction reaction in both alkaline and acidic media
topic Engineering::Materials
Metal–Air Batteries
Oxygen Reduction Reaction
url https://hdl.handle.net/10356/154780
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