Multifunctional carbon armor: synchronously improving oxygen reaction kinetics, mass transfer dynamics, and robustness of transition metal alloy based hybrid catalyst
Multifunctional carbon armor: synchronously improving oxygen reaction kinetics, mass transfer dynamics, and robustness of transition metal alloy based hybrid catalyst
Construction of robust protective cover on delicate active sites is a frequently-used scheme to enhance the durability of air-cathode catalyst working in harsh environment, thus the lifespan of rechargeable Zinc-air batteries (ZABs). Paradoxically, this would degrade the activity due to the constricted accessibility of active sites to reactants. Herein, carbon nanotubes with abundant mesoporous defects and Fe-N4 species were elaborately designed to be multifunctional protective armor to encapsulate Ni3Fe nano-alloys (Ni3Fe@CNTs/Fe-N4) for bifunctional oxygen electrocatalyst. In/ex-situ spectroscopy analysis and theoretical calculations reveal that the constructed mesoporous carbon defects effectively facilitate the multiphase mass transfer and the oxygen evolution reaction kinetics via strong electrons coupling with packaged Ni3Fe nano-alloys. Meanwhile, the synchronously introduced Fe-N4 moieties could serve as oxygen reduction active sites. Thus, the obtained Ni3Fe@CNTs/Fe-N4 hybrid electrocatalyst simultaneously exhibits remarkable bifunctional catalytic activity (E1/2=0.86/Ej=10=1.59 V vs RHE) and durability over 450 h in the chronoamperometric test at 1.59 V, endowing the assembled Zn-air batteries (ZABs) with a high power density (150 mW cm−2) and lifespan (307 h), much better than that employing benchmark Pt/C+RuO2 mixed catalyst. This work demonstrates an innovative design route for the multifunctional armor to concurrently enhance the durability, activity and robustness of air-cathode-catalyst for ZABs.
Bifunctional oxygen catalyst, Multifunctional carbon armor, Single-atom catalysis, Transition metal alloy, Zinc-air battery
Zhang, Lei
e9a272bb-6497-4a84-baf9-425361f20830
Jiang, He
0a342e00-3c27-446e-b2a0-84ef5824aa67
Tang, Min
974c2fd4-30b3-4a33-b4ee-e5a8a6935996
Jiang, Ying
e6e39ee2-e0a6-4e60-9604-ce363c7ce5f9
Tang, Bing
7641b253-ad60-4b5f-80cf-4f115348ce16
Tan, Hao
77aec41f-64e8-4467-a2ba-9d462b38b210
Kong, Yuan
412d4b09-72d4-4b4f-aa05-e64e2dfb503a
Hu, Haibo
5b48ed5d-af08-4c9a-9fa0-b571ecf78a41
6 May 2024
Zhang, Lei
e9a272bb-6497-4a84-baf9-425361f20830
Jiang, He
0a342e00-3c27-446e-b2a0-84ef5824aa67
Tang, Min
974c2fd4-30b3-4a33-b4ee-e5a8a6935996
Jiang, Ying
e6e39ee2-e0a6-4e60-9604-ce363c7ce5f9
Tang, Bing
7641b253-ad60-4b5f-80cf-4f115348ce16
Tan, Hao
77aec41f-64e8-4467-a2ba-9d462b38b210
Kong, Yuan
412d4b09-72d4-4b4f-aa05-e64e2dfb503a
Hu, Haibo
5b48ed5d-af08-4c9a-9fa0-b571ecf78a41
Zhang, Lei, Jiang, He, Tang, Min, Jiang, Ying, Tang, Bing, Tan, Hao, Kong, Yuan and Hu, Haibo
(2024)
Multifunctional carbon armor: synchronously improving oxygen reaction kinetics, mass transfer dynamics, and robustness of transition metal alloy based hybrid catalyst.
Applied Catalysis B: Environmental, 354, [124151].
(doi:10.1016/j.apcatb.2024.124151).
Abstract
Construction of robust protective cover on delicate active sites is a frequently-used scheme to enhance the durability of air-cathode catalyst working in harsh environment, thus the lifespan of rechargeable Zinc-air batteries (ZABs). Paradoxically, this would degrade the activity due to the constricted accessibility of active sites to reactants. Herein, carbon nanotubes with abundant mesoporous defects and Fe-N4 species were elaborately designed to be multifunctional protective armor to encapsulate Ni3Fe nano-alloys (Ni3Fe@CNTs/Fe-N4) for bifunctional oxygen electrocatalyst. In/ex-situ spectroscopy analysis and theoretical calculations reveal that the constructed mesoporous carbon defects effectively facilitate the multiphase mass transfer and the oxygen evolution reaction kinetics via strong electrons coupling with packaged Ni3Fe nano-alloys. Meanwhile, the synchronously introduced Fe-N4 moieties could serve as oxygen reduction active sites. Thus, the obtained Ni3Fe@CNTs/Fe-N4 hybrid electrocatalyst simultaneously exhibits remarkable bifunctional catalytic activity (E1/2=0.86/Ej=10=1.59 V vs RHE) and durability over 450 h in the chronoamperometric test at 1.59 V, endowing the assembled Zn-air batteries (ZABs) with a high power density (150 mW cm−2) and lifespan (307 h), much better than that employing benchmark Pt/C+RuO2 mixed catalyst. This work demonstrates an innovative design route for the multifunctional armor to concurrently enhance the durability, activity and robustness of air-cathode-catalyst for ZABs.
Text
accepted version
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More information
Accepted/In Press date: 1 May 2024
e-pub ahead of print date: 3 May 2024
Published date: 6 May 2024
Keywords:
Bifunctional oxygen catalyst, Multifunctional carbon armor, Single-atom catalysis, Transition metal alloy, Zinc-air battery
Identifiers
Local EPrints ID: 491555
URI: http://eprints.soton.ac.uk/id/eprint/491555
ISSN: 0926-3373
PURE UUID: e1829f64-ba5e-4484-b70c-17c535de76f0
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Date deposited: 26 Jun 2024 16:30
Last modified: 26 Jun 2024 16:30
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Contributors
Author:
Lei Zhang
Author:
He Jiang
Author:
Min Tang
Author:
Ying Jiang
Author:
Bing Tang
Author:
Hao Tan
Author:
Yuan Kong
Author:
Haibo Hu
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