Highly selective CO formation via CO2 hydrogenation over novel ceria-based high-entropy oxides (HEOs)

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dc.contributor.authorCortázar, María
dc.contributor.authorLafuente Adiego, Marta
dc.contributor.authorNavarro Puyuelo, Andrea
dc.contributor.authorGarcía, Xènia
dc.contributor.authorLlorca Piqué, Jordi
dc.contributor.authorReyero Zaragoza, Inés
dc.contributor.authorBimbela Serrano, Fernando
dc.contributor.authorGandía Pascual, Luis
dc.contributor.departmentCienciases_ES
dc.contributor.departmentZientziakeu
dc.contributor.departmentInstitute for Advanced Materials and Mathematics - INAMAT2en
dc.contributor.funderUniversidad Pública de Navarra / Nafarroako Unibertsitate Publikoa
dc.date.accessioned2025-03-19T12:26:11Z
dc.date.available2025-03-19T12:26:11Z
dc.date.issued2025-03-01
dc.date.updated2025-03-19T12:15:41Z
dc.description.abstractIn the present study, new ceria-based high-entropy oxides (HEOs) were investigated as CO2 hydrogenation catalysts. The nominal composition was (Ce0.5Ni0.1Co0.1Cu0.1Zn0.1Mg0.1)Ox and the synthesis was accomplished through the citrate complexing sol-gel method. Characterization techniques utilized including ICP-AES, in situ XRD and in situ XPS, SEM-EDS, HR-TEM and HAADF-STEM, Raman spectroscopy, H2-TPR, CO2-TPD and N2 physical adsorption. The physicochemical characterization and the catalytic results revealed that the conditions of the thermal treatments at which the oxides were subjected critically determined the catalytic performance, especially the CO2 hydrogenation products selectivities. Calcination in air and/or reduction in hydrogen conducted at temperatures below 500 °C led to active but poorly selective catalysts that produced both methane and CO with significant yields. This was mainly attributed to the presence of metallic Cu, Ni and Co on the catalysts that appeared to be supported on ceria doped with the rest of the formulation elements. In contrast, thermal treatments at 750 °C favored the formation of a rocksalt entropy-stabilized (NiCoCuZnMg)Ox HEO supported on ceria that has stood out for showing an excellent selectivity towards the reverse water¿gas shift (RWGS) reaction. This catalyst led to CO selectivities of almost 100 % over a very wide range of reaction temperatures (300-700 °C). Long-term stability tests (100 h) showed only a slight decrease in CO2 conversion, while CO selectivity remained stable at nearly 100 % at 400 °C. XRD characterization of the used catalysts evidenced that, whereas the basic catalyst structure remained, some metallic copper exsolved during reduction and reaction period. These results are relevant and very promising, opening a door to the development of new catalysts for the valorization of CO2 through the RWGS reaction, thus expanding the low-temperature limit at which this process can be carried out selectively.en
dc.description.sponsorshipAuthors wish to thank the Spanish Agencia Estatal de Investigaci´on (AEI) and Ministerio de Ciencia e Innovaci´on (MCIN), the European Regional Development Fund (ERDF/FEDER), the European Union¿s NextGenerationEU funds for their financial support. In particular, this work was partially funded by the following research projects: TED2021- 130846B-I00 (MULTIeFUEL project), PID2021-127265OB-C21 (SOLFUEL project), PLEC2022-009221 (Panel-to-Fuel project), PID2021- 124572OB-C31, and CEX2023-001300-M. M. Cortazar and M. Lafuente also thank Ministerio de Universidades (Spain) and NextGenerationEU funds for their ¨Margarita Salas¨postdoctoral grants. JL is a Serra Húnter Fellow and is grateful to ICREA Academia program. Open access funding provided by Universidad Pública de Navarra.
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dc.identifier.citationCortazar, M., Lafuente, M., Navarro-Puyuelo, A., Garcia, X., Llorca, J., Reyero, I., Bimbela, F., Gandía, L. M. (2025). Highly selective CO formation via CO2 hydrogenation over novel ceria-based high-entropy oxides (HEOs). Chemical Engineering Journal, 507, 1-15. https://doi.org/10.1016/j.cej.2025.160706.
dc.identifier.doi10.1016/j.cej.2025.160706
dc.identifier.issn1385-8947
dc.identifier.urihttps://academica-e.unavarra.es/handle/2454/53775
dc.language.isoeng
dc.publisherElsevier
dc.relation.ispartofChemical Engineering Journal (2025), vol. 507, 160706
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/TED2021-130846B-I00/
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127265OB-C21/ES/
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PLEC2022-009221/ES/
dc.relation.projectIDinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-124572OB-C31/ES/
dc.relation.projectIDinfo:eu-repo/grantAgreement/MCIN/Plan Estatal de I+D+i 2021-2023/CEX2023-001300-M/
dc.relation.publisherversionhttps://doi.org/10.1016/j.cej.2025.160706
dc.rights© 2025 The Authors. This is an open access article under the CC BY-NC-ND license.
dc.rights.accessRightsinfo:eu-repo/semantics/openAccess
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/
dc.subjectCarbon dioxideen
dc.subjectCarbon monoxideen
dc.subjectEntropy-stabilized oxidesen
dc.subjectMethanationen
dc.subjectReverse water-gas shift (RWGS)en
dc.titleHighly selective CO formation via CO2 hydrogenation over novel ceria-based high-entropy oxides (HEOs)en
dc.typeinfo:eu-repo/semantics/article
dc.type.versioninfo:eu-repo/semantics/publishedVersion
dspace.entity.typePublication
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