Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles

The energy efficiency of water electrolysis is limited by the sluggish kinetics of the anodic oxygen evolution reaction (OER), which simultaneously produces a low-value product, oxygen. A promising strategy to address this challenge is to replace OER with a more favorable oxidation reaction that yie...

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Detalles Bibliográficos
Autores: Yang, Longcheng, Ma, Yi, Yu, Jing, Arbiol, Jordi, Li, Junshan, Cabot, Andreu
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/397783
Acceso en línea:http://hdl.handle.net/10261/397783
https://api.elsevier.com/content/abstract/scopus_id/105011680941
Access Level:acceso abierto
Palabra clave:Electrocatalysis
Formate, glycerol oxidation
Glycerol reforming
Hydrogen production
Nickel diselenide
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repository_id_str
dc.title.none.fl_str_mv Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
title Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
spellingShingle Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
Yang, Longcheng
Electrocatalysis
Formate, glycerol oxidation
Glycerol reforming
Hydrogen production
Nickel diselenide
title_short Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
title_full Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
title_fullStr Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
title_full_unstemmed Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
title_sort Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticles
dc.creator.none.fl_str_mv Yang, Longcheng
Ma, Yi
Yu, Jing
Arbiol, Jordi
Li, Junshan
Cabot, Andreu
author Yang, Longcheng
author_facet Yang, Longcheng
Ma, Yi
Yu, Jing
Arbiol, Jordi
Li, Junshan
Cabot, Andreu
author_role author
author2 Ma, Yi
Yu, Jing
Arbiol, Jordi
Li, Junshan
Cabot, Andreu
author2_role author
author
author
author
author
dc.contributor.none.fl_str_mv National Natural Science Foundation of China
Natural Science Foundation of Sichuan Province
Chengdu University
Sichuan University
China Postdoctoral Science Foundation
Generalitat de Catalunya
Ministerio de Ciencia e Innovación (España)
Agencia Estatal de Investigación (España)
European Commission
Universidad Autónoma de Barcelona
Chinese Academy of Sciences
Arbiol, Jordi [0000-0002-0695-1726]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Electrocatalysis
Formate, glycerol oxidation
Glycerol reforming
Hydrogen production
Nickel diselenide
topic Electrocatalysis
Formate, glycerol oxidation
Glycerol reforming
Hydrogen production
Nickel diselenide
description The energy efficiency of water electrolysis is limited by the sluggish kinetics of the anodic oxygen evolution reaction (OER), which simultaneously produces a low-value product, oxygen. A promising strategy to address this challenge is to replace OER with a more favorable oxidation reaction that yields a valuable co-product. In this study, we investigate the electrochemical reforming of glycerol in alkaline media to simultaneously produce hydrogen at a Pt cathode and formate at a NiSe₂ anode. The NiSe₂ electrode achieves a glycerol oxidation reaction (GOR) current density of up to 100 mA cm-2 in a 1 M KOH solution containing 1 M glycerol, significantly outperforming a reference elemental Ni electrode. Both electrodes exhibit high Faradaic efficiencies (FE), achieving around 93 % for formate production at an applied potential of 1.6 V vs. RHE. To rationalize this exceptional performance, density functional theory (DFT) calculations were conducted, revealing that the incorporation of Se into NiSe₂ enhances the glycerol adsorption and modulates the electron density, thereby lowering the energy barrier for the initial dehydrogenation step in the formate formation pathway. These findings provide valuable insights for the design of cost-effective, high-performance electrocatalysts for organic oxidation-assisted hydrogen production, advancing a more sustainable and economically attractive route for hydrogen generation and chemical valorization.
publishDate 2025
dc.date.none.fl_str_mv 2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/397783
https://api.elsevier.com/content/abstract/scopus_id/105011680941
url http://hdl.handle.net/10261/397783
https://api.elsevier.com/content/abstract/scopus_id/105011680941
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
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info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2023-149158OB-C43
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/CEX2021-001214-S
The underlying dataset has been published as supplementary material of the article in the publisher platform at DOI 10.1016/j.jcis.2025.138535
https://doi.org/10.1016/j.jcis.2025.138535
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dc.publisher.none.fl_str_mv Elsevier
publisher.none.fl_str_mv Elsevier
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instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
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spelling Organic oxidation-assisted hydrogen production: glycerol electroreforming to formate on nickel diselenide nanoparticlesYang, LongchengMa, YiYu, JingArbiol, JordiLi, JunshanCabot, AndreuElectrocatalysisFormate, glycerol oxidationGlycerol reformingHydrogen productionNickel diselenideThe energy efficiency of water electrolysis is limited by the sluggish kinetics of the anodic oxygen evolution reaction (OER), which simultaneously produces a low-value product, oxygen. A promising strategy to address this challenge is to replace OER with a more favorable oxidation reaction that yields a valuable co-product. In this study, we investigate the electrochemical reforming of glycerol in alkaline media to simultaneously produce hydrogen at a Pt cathode and formate at a NiSe₂ anode. The NiSe₂ electrode achieves a glycerol oxidation reaction (GOR) current density of up to 100 mA cm-2 in a 1 M KOH solution containing 1 M glycerol, significantly outperforming a reference elemental Ni electrode. Both electrodes exhibit high Faradaic efficiencies (FE), achieving around 93 % for formate production at an applied potential of 1.6 V vs. RHE. To rationalize this exceptional performance, density functional theory (DFT) calculations were conducted, revealing that the incorporation of Se into NiSe₂ enhances the glycerol adsorption and modulates the electron density, thereby lowering the energy barrier for the initial dehydrogenation step in the formate formation pathway. These findings provide valuable insights for the design of cost-effective, high-performance electrocatalysts for organic oxidation-assisted hydrogen production, advancing a more sustainable and economically attractive route for hydrogen generation and chemical valorization.This research was supported by the National Natural Science Foundation of China Grant No. 51978089, the Natural Science Foundation of Sichuan Province of China Grant No. 2023NSFSC1967, the Innovation Team of Chengdu Normal University Grant number CSCXTD2020B09, and Indoor Space Layout Optimization and Safety Guarantee Sichuan University Key Laboratory Open Project (SNKJ202501, SNKJ202504, SNKJ202505, SNKJ202506). L. Yang is grateful for the project (Grant MSSB-2024-02) funed by Key Laboratory of Pattern Recognition and Intelligent Information Processing, Institutions of Higher Education of Sichuan Province. It was also funded by the China Postdoctoral Science Foundation (Project No. 2023MD734228). ICN2 acknowledges funding from Generalitat de Catalunya 2021SGR00457. The authors thank the Shiyanjia Lab (www.shiyanjia.com) for conducting the XPS analysis. This study is part of the Advanced Materials programme and was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17·I1) and by Generalitat de Catalunya (In-CAEM Project). The authors thank support from the project AMaDE (PID2023-149158OB-C43), funded by MCIN/ AEI/10.13039/501100011033/ and by “ERDF A way of making Europe”, by the “European Union”. ICN2 is supported by the Severo Ochoa program from Spanish MCIN/AEI (Grant No.: CEX2021-001214-S) and is funded by the CERCA Programme/Generalitat de Catalunya. Part of the present work has been performed in the framework of Universitat Autònoma de Barcelona Materials Science PhD program. JY has received funding from the CSC-UAB PhD scholarship program. ICN2 is founding member of e-DREAM.With funding from the Spanish government through the "Severo Ochoa Centre of Excelence" accreditation (CEX2021-001214-S)Peer reviewedElsevierNational Natural Science Foundation of ChinaNatural Science Foundation of Sichuan ProvinceChengdu UniversitySichuan UniversityChina Postdoctoral Science FoundationGeneralitat de CatalunyaMinisterio de Ciencia e Innovación (España)Agencia Estatal de Investigación (España)European CommissionUniversidad Autónoma de BarcelonaChinese Academy of SciencesArbiol, Jordi [0000-0002-0695-1726]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202520252025info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10261/397783https://api.elsevier.com/content/abstract/scopus_id/105011680941reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2023-149158OB-C43info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/CEX2021-001214-SThe underlying dataset has been published as supplementary material of the article in the publisher platform at DOI 10.1016/j.jcis.2025.138535https://doi.org/10.1016/j.jcis.2025.138535Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3977832026-05-22T06:33:51Z
score 15.812429

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