Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment

On-site H2O2 electrosynthesis via two-electron oxygen reduction reaction (ORR) is attracting great interest forwater treatment. The use of carbon black-based gas-diffusion electrodes (GDEs) is especially appealing, but theiractivity, selectivity and long-term stability must be improved. Here, a faci...

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Detalles Bibliográficos
Autores: Xia, Pan, Zhao, Lele, Chen, Xi, Ye, Zhihong, Zheng, Zhihong., He, Qiang, Sirés Sadornil, Ignacio
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/206789
Acceso en línea:https://hdl.handle.net/2445/206789
Access Level:acceso abierto
Palabra clave:Depuració de l'aigua
Reacció d'oxidació-reducció
Electroquímica
Water purification
Oxidation-reduction reaction
Electrochemistry
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spelling Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatmentXia, PanZhao, LeleChen, XiYe, ZhihongZheng, Zhihong.He, QiangSirés Sadornil, IgnacioDepuració de l'aiguaReacció d'oxidació-reduccióElectroquímicaWater purificationOxidation-reduction reactionElectrochemistryOn-site H2O2 electrosynthesis via two-electron oxygen reduction reaction (ORR) is attracting great interest forwater treatment. The use of carbon black-based gas-diffusion electrodes (GDEs) is especially appealing, but theiractivity, selectivity and long-term stability must be improved. Here, a facile GDEs modification strategy usingtrace polymethylhydrosiloxane (PMHS) allowed reaching a outstanding H2O2 production, outperforming theconventional polytetrafluoroethylene (PTFE)-GDE (1874.8 vs 1087.4 mg L-1 at 360 min). The superhydrophobicityconferred by PMHS endowed the catalytic layer with high faradaic efficiencies (76.2%-89.7%)during long-term operation for 60 h. The electrochemical tests confirmed the high activity and selectivity of thePMHS-modified GDE. Moreover, the efficient degradation of several micropollutants by the electro-Fentonprocess demonstrated the great potential of the new GDE. An in-depth understanding of the roles of PMHSfunctional groups is provided from DFT calculations: the -CH3 groups contribute to form a superhydrophobicinterface, whereas Si-H and as-formed Si-O-C sites modulate the coordination environment of active carboncenters.Elsevier B.V.2024202420232024info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion11 p.application/pdfhttps://hdl.handle.net/2445/206789Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésReproducció del document publicat a: https://doi.org/10.1016/j.apcatb.2023.123467Applied Catalysis B-Environmental, 2023, vol. 343, p. 1-11https://doi.org/10.1016/j.apcatb.2023.123467cc-by-nc-nd (c) Xia, P. et al., 2023http://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:recercat.cat:2445/2067892026-05-29T05:05:01Z
dc.title.none.fl_str_mv Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
title Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
spellingShingle Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
Xia, Pan
Depuració de l'aigua
Reacció d'oxidació-reducció
Electroquímica
Water purification
Oxidation-reduction reaction
Electrochemistry
title_short Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
title_full Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
title_fullStr Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
title_full_unstemmed Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
title_sort Polymethylhydrosiloxane-modified gas-diffusion cathode for more efficient and durable H2O2 electrosynthesis in the context of water treatment
dc.creator.none.fl_str_mv Xia, Pan
Zhao, Lele
Chen, Xi
Ye, Zhihong
Zheng, Zhihong.
He, Qiang
Sirés Sadornil, Ignacio
author Xia, Pan
author_facet Xia, Pan
Zhao, Lele
Chen, Xi
Ye, Zhihong
Zheng, Zhihong.
He, Qiang
Sirés Sadornil, Ignacio
author_role author
author2 Zhao, Lele
Chen, Xi
Ye, Zhihong
Zheng, Zhihong.
He, Qiang
Sirés Sadornil, Ignacio
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Depuració de l'aigua
Reacció d'oxidació-reducció
Electroquímica
Water purification
Oxidation-reduction reaction
Electrochemistry
topic Depuració de l'aigua
Reacció d'oxidació-reducció
Electroquímica
Water purification
Oxidation-reduction reaction
Electrochemistry
description On-site H2O2 electrosynthesis via two-electron oxygen reduction reaction (ORR) is attracting great interest forwater treatment. The use of carbon black-based gas-diffusion electrodes (GDEs) is especially appealing, but theiractivity, selectivity and long-term stability must be improved. Here, a facile GDEs modification strategy usingtrace polymethylhydrosiloxane (PMHS) allowed reaching a outstanding H2O2 production, outperforming theconventional polytetrafluoroethylene (PTFE)-GDE (1874.8 vs 1087.4 mg L-1 at 360 min). The superhydrophobicityconferred by PMHS endowed the catalytic layer with high faradaic efficiencies (76.2%-89.7%)during long-term operation for 60 h. The electrochemical tests confirmed the high activity and selectivity of thePMHS-modified GDE. Moreover, the efficient degradation of several micropollutants by the electro-Fentonprocess demonstrated the great potential of the new GDE. An in-depth understanding of the roles of PMHSfunctional groups is provided from DFT calculations: the -CH3 groups contribute to form a superhydrophobicinterface, whereas Si-H and as-formed Si-O-C sites modulate the coordination environment of active carboncenters.
publishDate 2023
dc.date.none.fl_str_mv 2023
2024
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/206789
url https://hdl.handle.net/2445/206789
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1016/j.apcatb.2023.123467
Applied Catalysis B-Environmental, 2023, vol. 343, p. 1-11
https://doi.org/10.1016/j.apcatb.2023.123467
dc.rights.none.fl_str_mv cc-by-nc-nd (c) Xia, P. et al., 2023
http://creativecommons.org/licenses/by-nc-nd/4.0/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by-nc-nd (c) Xia, P. et al., 2023
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 11 p.
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:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.811543

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