Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis

Air-breathing gas-diffusion electrodes (GDEs) eliminating energy-intensive aeration hold great promise for industrial-scale hydrogen peroxide electrosynthesis. However, this configuration suffers from limited O2 mass transport and easy flooding. Herein, the active region of GDEs was extended beyond...

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Autores: Xia, Pan, He, Tianwei, Xu, Tong, Zhu, Zhong-Shuai, Sun, Yu, Duan, Xiaoguang, Wang, Chao, He, Qiang, Sirés Sadornil, Ignacio, Ye, Zhihong
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2025
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/224195
Acceso en línea:https://hdl.handle.net/2445/224195
Access Level:acceso embargado
Palabra clave:Càtodes
Electroquímica
Reacció d'oxidació-reducció
Cathodes
Electrochemistry
Oxidation-reduction reaction
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spelling Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesisXia, PanHe, TianweiXu, TongZhu, Zhong-ShuaiSun, YuDuan, XiaoguangWang, ChaoHe, QiangSirés Sadornil, IgnacioYe, ZhihongCàtodesElectroquímicaReacció d'oxidació-reduccióCathodesElectrochemistryOxidation-reduction reactionAir-breathing gas-diffusion electrodes (GDEs) eliminating energy-intensive aeration hold great promise for industrial-scale hydrogen peroxide electrosynthesis. However, this configuration suffers from limited O2 mass transport and easy flooding. Herein, the active region of GDEs was extended beyond the three-phase boundary into the flooded domain by designing an alveolate carbon-supported Co single-atom electrocatalyst featuring abundant edge-located asymmetric CoN2O2 sites (eCoN2O2) to modulate the catalytic layer. The porous framework facilitates O2 mass transport, while the eCoN2O2 sites enable efficient O2 activation, sustaining fast ORR thanks to rational electrode design across the scales. Moreover, the superior O2 enrichment capability of eCoN2O2 allows efficient utilization of dissolved O2. Notably, the eCoN2O2-based GDE delivers a high H2O2 yield of 738.5 mg L−1 after 6 h at 25 mA cm−2, showing a 3.8-fold increase over basal-plane CoN4 moiety and even outperforming many aeration-driven systems. This work paves the way for integrated design of electrocatalysts and GDE architectures.Elsevier B.V.2025info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttps://hdl.handle.net/2445/224195Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésVersió postprint del document publicat a: https://doi.org/10.1016/j.apcatb.2025.126099Applied Catalysis B-Environmental, 2025, vol. 383, p. 1-13https://doi.org/10.1016/j.apcatb.2025.126099cc-by-nc-nd (c) Elsevier B.V., 2025http://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/embargoedAccessoai:diposit.ub.edu:2445/2241952026-05-27T06:46:51Z
dc.title.none.fl_str_mv Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
title Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
spellingShingle Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
Xia, Pan
Càtodes
Electroquímica
Reacció d'oxidació-reducció
Cathodes
Electrochemistry
Oxidation-reduction reaction
title_short Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
title_full Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
title_fullStr Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
title_full_unstemmed Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
title_sort Unlocking flooded domains in air-breathing cathodes with edge-located asymmetric CoN2O2 sites for robust H2O2 electrosynthesis
dc.creator.none.fl_str_mv Xia, Pan
He, Tianwei
Xu, Tong
Zhu, Zhong-Shuai
Sun, Yu
Duan, Xiaoguang
Wang, Chao
He, Qiang
Sirés Sadornil, Ignacio
Ye, Zhihong
author Xia, Pan
author_facet Xia, Pan
He, Tianwei
Xu, Tong
Zhu, Zhong-Shuai
Sun, Yu
Duan, Xiaoguang
Wang, Chao
He, Qiang
Sirés Sadornil, Ignacio
Ye, Zhihong
author_role author
author2 He, Tianwei
Xu, Tong
Zhu, Zhong-Shuai
Sun, Yu
Duan, Xiaoguang
Wang, Chao
He, Qiang
Sirés Sadornil, Ignacio
Ye, Zhihong
author2_role author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Càtodes
Electroquímica
Reacció d'oxidació-reducció
Cathodes
Electrochemistry
Oxidation-reduction reaction
topic Càtodes
Electroquímica
Reacció d'oxidació-reducció
Cathodes
Electrochemistry
Oxidation-reduction reaction
description Air-breathing gas-diffusion electrodes (GDEs) eliminating energy-intensive aeration hold great promise for industrial-scale hydrogen peroxide electrosynthesis. However, this configuration suffers from limited O2 mass transport and easy flooding. Herein, the active region of GDEs was extended beyond the three-phase boundary into the flooded domain by designing an alveolate carbon-supported Co single-atom electrocatalyst featuring abundant edge-located asymmetric CoN2O2 sites (eCoN2O2) to modulate the catalytic layer. The porous framework facilitates O2 mass transport, while the eCoN2O2 sites enable efficient O2 activation, sustaining fast ORR thanks to rational electrode design across the scales. Moreover, the superior O2 enrichment capability of eCoN2O2 allows efficient utilization of dissolved O2. Notably, the eCoN2O2-based GDE delivers a high H2O2 yield of 738.5 mg L−1 after 6 h at 25 mA cm−2, showing a 3.8-fold increase over basal-plane CoN4 moiety and even outperforming many aeration-driven systems. This work paves the way for integrated design of electrocatalysts and GDE architectures.
publishDate 2025
dc.date.none.fl_str_mv 2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/224195
url https://hdl.handle.net/2445/224195
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Versió postprint del document publicat a: https://doi.org/10.1016/j.apcatb.2025.126099
Applied Catalysis B-Environmental, 2025, vol. 383, p. 1-13
https://doi.org/10.1016/j.apcatb.2025.126099
dc.rights.none.fl_str_mv cc-by-nc-nd (c) Elsevier B.V., 2025
http://creativecommons.org/licenses/by-nc-nd/4.0/
info:eu-repo/semantics/embargoedAccess
rights_invalid_str_mv cc-by-nc-nd (c) Elsevier B.V., 2025
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv embargoedAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Elsevier B.V.
publisher.none.fl_str_mv Elsevier B.V.
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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