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Sulfur and phosphorus co-doped FeCoNiCrMn high-entropy alloys as efficient sulfion oxidation reaction catalysts enabling self-powered asymmetric seawater electrolysis

dc.contributor.authorYu, Zhipeng
dc.contributor.authorBoukhvalov, Danil W.
dc.contributor.authorTan, Hao
dc.contributor.authorXiong, Dehua
dc.contributor.authorFeng, Chuangshi
dc.contributor.authorWang, Jingwei
dc.contributor.authorWang, Wei
dc.contributor.authorZhao, Yang
dc.contributor.authorXu, Kaiyang
dc.contributor.authorSu, Weifeng
dc.contributor.authorXiang, Xinyi
dc.contributor.authorLin, Fei
dc.contributor.authorHuang, Haoliang
dc.contributor.authorZhang, Fuxiang
dc.contributor.authorZhang, Lei
dc.contributor.authorMeng, Lijian
dc.contributor.authorLiu, Lifeng
dc.date.accessioned2024-07-01T10:06:13Z
dc.date.available2024-07-01T10:06:13Z
dc.date.issued2024
dc.description.abstractSeawater electrolysis (SWE) represents a promising approach to green hydrogen (H2) production but currently faces substantial challenges such as the interference of chlorine chemistry and high energy consumption. In this work, we demonstrate that by replacing the energy-demanding oxygen evolution reaction (OER) with the sulfion oxidation reaction (SOR) and by implementing the concept of bipolar membrane (BPM) electrolysis in an acid-base dual electrolyte system, not only can the notorious chlorine evolution reaction (CER) be completely circumvented, but the energy consumption of SWE be significantly reduced. To do so, we develop a sulfur and phosphorus co-doped FeCoNiCrMn high entropy alloy (HEA-SP) catalyst, which shows good electrocatalytic performance for the SOR in alkaline-saline water. This can be attributed to the abundant lattice defects and strains in HEA-SP, leading to a high density of active sites and an optimized electronic structure favorable for the SOR. Moreover, density functional theory calculations and in situ Raman spectroscopy characterization reveal the crucial role of imperfect sulfur coverage on the HEA in facilitating the formation of Sx clusters during the SOR. Using the HEA-SP as anode catalysts, the SOR-assisted SWE only needs electrical energy of 0.253 kWh to produce one cubic meter of H2 at 100 mA cm−2, in the presence of a BPM. Impressively, chlorine-free H2 production from seawater and upgrading of sulfions to valuable sulfur can occur simultaneously and spontaneously at 10 mA cm−2, highlighting the great potential of the HEA-SP catalysts and the asymmetric cell design to enable energy- and cost-effective seawater electrolysis.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.citationZhipeng Yu, Danil W. Boukhvalov, Hao Tan, Dehua Xiong, Chuangshi Feng, Jingwei Wang, Wei Wang, Yang Zhao, Kaiyang Xu, Weifeng Su, Xinyi Xiang, Fei Lin, Haoliang Huang, Fuxiang Zhang, Lei Zhang, Lijian Meng, Lifeng Liu, Sulfur and phosphorus co-doped FeCoNiCrMn high-entropy alloys as efficient sulfion oxidation reaction catalysts enabling self-powered asymmetric seawater electrolysis, Chemical Engineering Journal, Volume 494, 2024, 153094, ISSN 1385-8947, https://doi.org/10.1016/j.cej.2024.153094pt_PT
dc.identifier.doi10.1016/j.cej.2024.153094pt_PT
dc.identifier.issn1385-8947
dc.identifier.urihttp://hdl.handle.net/10400.22/25722
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.rights.urihttp://creativecommons.org/licenses/by-nd/4.0/pt_PT
dc.subjectHigh entropy alloyspt_PT
dc.subjectLattice defectspt_PT
dc.subjectLattice strainpt_PT
dc.subjectSeawater electrolysispt_PT
dc.subjectSulfion oxidation reactionpt_PT
dc.subjectAsymmetric acid-base electrolysispt_PT
dc.titleSulfur and phosphorus co-doped FeCoNiCrMn high-entropy alloys as efficient sulfion oxidation reaction catalysts enabling self-powered asymmetric seawater electrolysispt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.citation.titleChemical Engineering Journalpt_PT
oaire.citation.volume494pt_PT
person.familyNameMeng
person.givenNameLijian
person.identifier236430
person.identifier.ciencia-idC31B-0091-BD12
person.identifier.orcid0000-0001-6071-3502
person.identifier.scopus-author-id7202236050
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
relation.isAuthorOfPublicationcb02ae05-0786-47ff-b480-2fde7ef93e0d
relation.isAuthorOfPublication.latestForDiscoverycb02ae05-0786-47ff-b480-2fde7ef93e0d

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