Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide

The electrocatalytic hydrogen evolution reaction (HER) has been explored using mono- and bimetallic Pt-Ru nanoparticles (NPs) deposited onto nitrogen-doped reduced graphene oxide (NH2-rGO) in acidic media. In this contribution, monometallic and bimetallic nanoparticles with three different Pt/Ru rat...

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Autores: Hou, Heting|||0000-0002-7806-1781, Cerezo Navarrete, Christian|||0000-0001-9537-0642, Fenoll, Didac A.|||0000-0003-1141-8114, Kraft, Matilda|||0009-0008-9528-9797, Marini, Carlo, Rodríguez-Santiago, Luis|||0000-0003-4983-4228, Solans-Monfort, Xavier|||0000-0002-2172-3895, Martínez-Prieto, Luis Miguel|||0000-0002-3401-4967, Romero Fernández, Nuria|||0000-0002-2704-7779, García-Antón, Jordi|||0000-0002-2401-0401, Sala, Xavier|||0000-0002-7779-6313
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:324288
Acceso en línea:https://ddd.uab.cat/record/324288
https://dx.doi.org/urn:doi:10.1039/d5qi00451a
Access Level:acceso abierto
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spelling Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxideHou, Heting|||0000-0002-7806-1781Cerezo Navarrete, Christian|||0000-0001-9537-0642Fenoll, Didac A.|||0000-0003-1141-8114Kraft, Matilda|||0009-0008-9528-9797Marini, CarloRodríguez-Santiago, Luis|||0000-0003-4983-4228Solans-Monfort, Xavier|||0000-0002-2172-3895Martínez-Prieto, Luis Miguel|||0000-0002-3401-4967Romero Fernández, Nuria|||0000-0002-2704-7779García-Antón, Jordi|||0000-0002-2401-0401Sala, Xavier|||0000-0002-7779-6313The electrocatalytic hydrogen evolution reaction (HER) has been explored using mono- and bimetallic Pt-Ru nanoparticles (NPs) deposited onto nitrogen-doped reduced graphene oxide (NH2-rGO) in acidic media. In this contribution, monometallic and bimetallic nanoparticles with three different Pt/Ru ratios (1/5, 1/1, and 5/1) have been used, yielding five different materials denoted as PtxRuy@NH2-rGO (x = 0, y = 1; x = 1, y = 0; x = 1, y = 5; x = 1, y = 1; x = 5, y = 1). The materials were characterized using a variety of state-of-the-art techniques, including high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-Ray spectroscopy (EDX) and X-Ray absorption spectroscopy (XAS), enabling the investigation of differences in morphology, coordination environment and oxidation state as a function of the metal composition of the graphene-supported NPs. The materials exhibited HER activity and demonstrated competitive overpotentials close to the thermodynamic limit. The initial catalytic activity of the as-synthesized materials enhances as the Pt/Ru ratio increases. Chronopotentiometry cathodic experiments showed that under reductive conditions the electrocatalytic performance is drastically impacted. Ru-rich materials were activated, whereas Pt-rich materials showed poor stability. Upon applying a reducing potential for 58 h, Pt1Ru5@NH2-rGO reached the best catalytic activity with outstanding overpotentials of η0 = 0 mV and η10 = 3 mV and no signs of deactivation even after 12 additional hours of electrolysis. According to DFT calculations, all nanoparticles present surface sites whose hydrogen adsorption energy is optimal for HER. In agreement with the experimental data, the Pt1Ru5 model shows the highest number of highly active sites, especially those involving Ru centres close to the Pt-Ru interface. Combining in-depth characterization and computational modelling, this work reveals that the synergy between the two metals, structural features, and their affinity for the support are responsible for the observed differences in catalytic activities and stabilities. 22025-01-0120252025-01-01Articlehttp://purl.org/coar/resource_type/c_6501VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://ddd.uab.cat/record/324288https://dx.doi.org/urn:doi:10.1039/d5qi00451areponame:Dipòsit Digital de Documents de la UABinstname:Universitat Autònoma de BarcelonaInglésengAgencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2019-104171RB-I00Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2023-146787OB-I00Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2021-126080OA-I00Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 TED2021-132087A-I00Ministerio de Ciencia, Innovación y Universidades https://doi.org/10.13039/100014440 CNS2023-145078Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2023-151738NB-I00open accesshttp://purl.org/coar/access_right/c_abf2Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original.https://creativecommons.org/licenses/by-nc/4.0/info:eu-repo/semantics/openAccessoai:ddd.uab.cat:3242882026-06-06T12:50:31Z
dc.title.none.fl_str_mv Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
title Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
spellingShingle Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
Hou, Heting|||0000-0002-7806-1781
title_short Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
title_full Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
title_fullStr Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
title_full_unstemmed Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
title_sort Enhanced electrocatalytic hydrogen evolution with bimetallic Ru/Pt nanoparticles supported on nitrogen-doped reduced graphene oxide
dc.creator.none.fl_str_mv Hou, Heting|||0000-0002-7806-1781
Cerezo Navarrete, Christian|||0000-0001-9537-0642
Fenoll, Didac A.|||0000-0003-1141-8114
Kraft, Matilda|||0009-0008-9528-9797
Marini, Carlo
Rodríguez-Santiago, Luis|||0000-0003-4983-4228
Solans-Monfort, Xavier|||0000-0002-2172-3895
Martínez-Prieto, Luis Miguel|||0000-0002-3401-4967
Romero Fernández, Nuria|||0000-0002-2704-7779
García-Antón, Jordi|||0000-0002-2401-0401
Sala, Xavier|||0000-0002-7779-6313
author Hou, Heting|||0000-0002-7806-1781
author_facet Hou, Heting|||0000-0002-7806-1781
Cerezo Navarrete, Christian|||0000-0001-9537-0642
Fenoll, Didac A.|||0000-0003-1141-8114
Kraft, Matilda|||0009-0008-9528-9797
Marini, Carlo
Rodríguez-Santiago, Luis|||0000-0003-4983-4228
Solans-Monfort, Xavier|||0000-0002-2172-3895
Martínez-Prieto, Luis Miguel|||0000-0002-3401-4967
Romero Fernández, Nuria|||0000-0002-2704-7779
García-Antón, Jordi|||0000-0002-2401-0401
Sala, Xavier|||0000-0002-7779-6313
author_role author
author2 Cerezo Navarrete, Christian|||0000-0001-9537-0642
Fenoll, Didac A.|||0000-0003-1141-8114
Kraft, Matilda|||0009-0008-9528-9797
Marini, Carlo
Rodríguez-Santiago, Luis|||0000-0003-4983-4228
Solans-Monfort, Xavier|||0000-0002-2172-3895
Martínez-Prieto, Luis Miguel|||0000-0002-3401-4967
Romero Fernández, Nuria|||0000-0002-2704-7779
García-Antón, Jordi|||0000-0002-2401-0401
Sala, Xavier|||0000-0002-7779-6313
author2_role author
author
author
author
author
author
author
author
author
author
description The electrocatalytic hydrogen evolution reaction (HER) has been explored using mono- and bimetallic Pt-Ru nanoparticles (NPs) deposited onto nitrogen-doped reduced graphene oxide (NH2-rGO) in acidic media. In this contribution, monometallic and bimetallic nanoparticles with three different Pt/Ru ratios (1/5, 1/1, and 5/1) have been used, yielding five different materials denoted as PtxRuy@NH2-rGO (x = 0, y = 1; x = 1, y = 0; x = 1, y = 5; x = 1, y = 1; x = 5, y = 1). The materials were characterized using a variety of state-of-the-art techniques, including high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), energy dispersive X-Ray spectroscopy (EDX) and X-Ray absorption spectroscopy (XAS), enabling the investigation of differences in morphology, coordination environment and oxidation state as a function of the metal composition of the graphene-supported NPs. The materials exhibited HER activity and demonstrated competitive overpotentials close to the thermodynamic limit. The initial catalytic activity of the as-synthesized materials enhances as the Pt/Ru ratio increases. Chronopotentiometry cathodic experiments showed that under reductive conditions the electrocatalytic performance is drastically impacted. Ru-rich materials were activated, whereas Pt-rich materials showed poor stability. Upon applying a reducing potential for 58 h, Pt1Ru5@NH2-rGO reached the best catalytic activity with outstanding overpotentials of η0 = 0 mV and η10 = 3 mV and no signs of deactivation even after 12 additional hours of electrolysis. According to DFT calculations, all nanoparticles present surface sites whose hydrogen adsorption energy is optimal for HER. In agreement with the experimental data, the Pt1Ru5 model shows the highest number of highly active sites, especially those involving Ru centres close to the Pt-Ru interface. Combining in-depth characterization and computational modelling, this work reveals that the synergy between the two metals, structural features, and their affinity for the support are responsible for the observed differences in catalytic activities and stabilities.
publishDate 2025
dc.date.none.fl_str_mv 2
2025-01-01
2025
2025-01-01
dc.type.none.fl_str_mv Article
http://purl.org/coar/resource_type/c_6501
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://ddd.uab.cat/record/324288
https://dx.doi.org/urn:doi:10.1039/d5qi00451a
url https://ddd.uab.cat/record/324288
https://dx.doi.org/urn:doi:10.1039/d5qi00451a
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2019-104171RB-I00
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2023-146787OB-I00
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2021-126080OA-I00
Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 TED2021-132087A-I00
Ministerio de Ciencia, Innovación y Universidades https://doi.org/10.13039/100014440 CNS2023-145078
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2023-151738NB-I00
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://creativecommons.org/licenses/by-nc/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
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https://creativecommons.org/licenses/by-nc/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Dipòsit Digital de Documents de la UAB
instname:Universitat Autònoma de Barcelona
instname_str Universitat Autònoma de Barcelona
reponame_str Dipòsit Digital de Documents de la UAB
collection Dipòsit Digital de Documents de la UAB
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