Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery

ABSTRACT The key to obtaining high intrinsic catalytic activity of Me‐Nx‐C electrocatalysts for Zn‐air batteries is to form high‐density bifunctional Me‐Nx active sites during the pyrolysis of the precursor while maintaining structural stability. In this study, a host–guest spatial confinement strat...

Full description

Saved in:
Bibliographic Details
Main Authors: Yisi Liu, Zongxu Li, Yonghang Zeng, Meifeng Liu, Dongbin Xiong, Lina Zhou, Yue Du, Yao Xiao
Format: Article
Language:English
Published: Wiley 2025-04-01
Series:Carbon Energy
Subjects:
Online Access:https://doi.org/10.1002/cey2.682
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1850139980799672320
author Yisi Liu
Zongxu Li
Yonghang Zeng
Meifeng Liu
Dongbin Xiong
Lina Zhou
Yue Du
Yao Xiao
author_facet Yisi Liu
Zongxu Li
Yonghang Zeng
Meifeng Liu
Dongbin Xiong
Lina Zhou
Yue Du
Yao Xiao
author_sort Yisi Liu
collection DOAJ
description ABSTRACT The key to obtaining high intrinsic catalytic activity of Me‐Nx‐C electrocatalysts for Zn‐air batteries is to form high‐density bifunctional Me‐Nx active sites during the pyrolysis of the precursor while maintaining structural stability. In this study, a host–guest spatial confinement strategy was utilized to synthesize a composite catalyst consisting of Co3Fe7 nanoparticles confined in an N‐doped carbon network. The coupling between the host (MIL‐88B) and guest (cobalt porphyrin, CoPP) produces high‐density bimetallic atomic active sites. By controlling the mass of guest molecules, it is possible to construct precursors with the highest activity potential. The Co3Fe7/NC material with a certain amount of the guest displays a better electrocatalytic performance for both oxygen reduction reaction and oxygen evolution reaction with a half‐wave potential (E1/2) of 0.85 V and an overpotential of 1.59 V at 10 mA cm−2, respectively. The specific structure of bimetallic active centers is verified to be FeN2‐CoN4 using experimental characterizations, and the oxygen reaction mechanism is explored by in‐situ characterization techniques and first‐principles calculations. The Zn‐air battery assembled with Co3Fe7/NC cathode exhibits a remarkable open‐circuit voltage of 1.52 V, an exceptional peak power density of 248.1 mW cm−2, and stable cycling stability over 1000 h. Particularly, the corresponding flexible Zn‐air battery affords prominent cycling performance under different bending angles. This study supplies the idea and method of designing catalysts with specific structures at the atomic and electronic scales for breaking through the large‐scale application of electrocatalysts based on oxygen reactions in fuel cells/metal‐air batteries.
format Article
id doaj-art-e948606a0f9e4e79a17faef8de49c3ad
institution OA Journals
issn 2637-9368
language English
publishDate 2025-04-01
publisher Wiley
record_format Article
series Carbon Energy
spelling doaj-art-e948606a0f9e4e79a17faef8de49c3ad2025-08-20T02:30:00ZengWileyCarbon Energy2637-93682025-04-0174n/an/a10.1002/cey2.682Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air BatteryYisi Liu0Zongxu Li1Yonghang Zeng2Meifeng Liu3Dongbin Xiong4Lina Zhou5Yue Du6Yao Xiao7Hubei Key Laboratory of Photoelectric Materials and Devices, School of Material Science and Engineering Hubei Normal University Huangshi ChinaHubei Key Laboratory of Photoelectric Materials and Devices, School of Material Science and Engineering Hubei Normal University Huangshi ChinaHubei Key Laboratory of Photoelectric Materials and Devices, School of Material Science and Engineering Hubei Normal University Huangshi ChinaHubei Key Laboratory of Photoelectric Materials and Devices, School of Physical and Electronic Science Hubei Normal University Huangshi ChinaHubei Key Laboratory of Photoelectric Materials and Devices, School of Material Science and Engineering Hubei Normal University Huangshi ChinaHubei Key Laboratory of Photoelectric Materials and Devices, School of Material Science and Engineering Hubei Normal University Huangshi ChinaHubei Key Laboratory of Photoelectric Materials and Devices, School of Material Science and Engineering Hubei Normal University Huangshi ChinaCollege of Chemistry and Materials Engineering Wenzhou University Wenzhou ChinaABSTRACT The key to obtaining high intrinsic catalytic activity of Me‐Nx‐C electrocatalysts for Zn‐air batteries is to form high‐density bifunctional Me‐Nx active sites during the pyrolysis of the precursor while maintaining structural stability. In this study, a host–guest spatial confinement strategy was utilized to synthesize a composite catalyst consisting of Co3Fe7 nanoparticles confined in an N‐doped carbon network. The coupling between the host (MIL‐88B) and guest (cobalt porphyrin, CoPP) produces high‐density bimetallic atomic active sites. By controlling the mass of guest molecules, it is possible to construct precursors with the highest activity potential. The Co3Fe7/NC material with a certain amount of the guest displays a better electrocatalytic performance for both oxygen reduction reaction and oxygen evolution reaction with a half‐wave potential (E1/2) of 0.85 V and an overpotential of 1.59 V at 10 mA cm−2, respectively. The specific structure of bimetallic active centers is verified to be FeN2‐CoN4 using experimental characterizations, and the oxygen reaction mechanism is explored by in‐situ characterization techniques and first‐principles calculations. The Zn‐air battery assembled with Co3Fe7/NC cathode exhibits a remarkable open‐circuit voltage of 1.52 V, an exceptional peak power density of 248.1 mW cm−2, and stable cycling stability over 1000 h. Particularly, the corresponding flexible Zn‐air battery affords prominent cycling performance under different bending angles. This study supplies the idea and method of designing catalysts with specific structures at the atomic and electronic scales for breaking through the large‐scale application of electrocatalysts based on oxygen reactions in fuel cells/metal‐air batteries.https://doi.org/10.1002/cey2.682bifunctional electrocatalytic performancebimetal active siteshost−guest engineeringMIL‐88BZn‐air battery
spellingShingle Yisi Liu
Zongxu Li
Yonghang Zeng
Meifeng Liu
Dongbin Xiong
Lina Zhou
Yue Du
Yao Xiao
Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery
Carbon Energy
bifunctional electrocatalytic performance
bimetal active sites
host−guest engineering
MIL‐88B
Zn‐air battery
title Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery
title_full Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery
title_fullStr Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery
title_full_unstemmed Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery
title_short Host–Guest Engineering of Dual‐Metal Nitrogen Carbides as Bifunctional Oxygen Electrocatalysts for Long‐Cycle Rechargeable Zn‐Air Battery
title_sort host guest engineering of dual metal nitrogen carbides as bifunctional oxygen electrocatalysts for long cycle rechargeable zn air battery
topic bifunctional electrocatalytic performance
bimetal active sites
host−guest engineering
MIL‐88B
Zn‐air battery
url https://doi.org/10.1002/cey2.682
work_keys_str_mv AT yisiliu hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT zongxuli hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT yonghangzeng hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT meifengliu hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT dongbinxiong hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT linazhou hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT yuedu hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery
AT yaoxiao hostguestengineeringofdualmetalnitrogencarbidesasbifunctionaloxygenelectrocatalystsforlongcyclerechargeableznairbattery