Assessing thermal and nonthermal contributions during CO2 hydrogenation over ruthenium catalysts: effects of the illumination conditions and the nature of the support

Imizcoz Aramburu, Mikel; Pellejero, Ismael; Gandía Pascual, Luis

Assessing thermal and nonthermal contributions during CO2 hydrogenation over ruthenium catalysts: effects of the illumination conditions and the nature of the support

dc.contributor.author	Imizcoz Aramburu, Mikel
dc.contributor.author	Pellejero, Ismael
dc.contributor.author	Gandía Pascual, Luis
dc.contributor.department	Ciencias	es_ES
dc.contributor.department	Zientziak	eu
dc.contributor.department	Institute for Advanced Materials and Mathematics - INAMAT2	en
dc.contributor.funder	Universidad Pública de Navarra / Nafarroako Unibertsitate Publikoa
dc.contributor.funder	Gobierno de Navarra / Nafarroako Gobernua
dc.date.accessioned	2024-11-21T11:44:30Z
dc.date.available	2024-11-21T11:44:30Z
dc.date.issued	2024-12-05
dc.date.updated	2024-11-21T11:23:46Z
dc.description.abstract	Photothermal catalysis offers a promising approach for the clean production of carbon-neutral chemicals from CO2 through reactions with hydrogen as a renewable energy carrier. While the combined action of photons and heat from solar radiation can drive catalytic reactions, the interactions involved are very complex, depend on the catalyst composition, and often remain uncertain. Herein, we assessed the thermal and nonthermal contributions to the overall activities of a series of Ru catalysts during the photothermal hydrogenation of CO2. TiO2 (anatase/rutile mixture), anatase, ZrO2, CeO2, and SiO2 were used as supports for Ru nanoparticles (2 wt%) that were deposited using an amino-acid-assisted method. Ru@TiO2 and Ru@ZrO2 presented the best catalytic performance at relatively low reaction temperatures (220-250 °C), whereas Ru@CeO2 was the most active catalyst above 300 °C. The catalysts were tested under direct and indirect illumination conditions to assess their thermal and nonthermal contributions to the overall production of methane, with a nonthermal contribution of 60-75 % observed at the highest applied irradiance (2.2 W·cm-²). Ru@ZrO2 registered the highest nonthermal CH4 production, which is tentatively ascribable to the participation of photo-generated electrons in the catalytic reaction and the light-induced formation of oxygen vacancies. The selected catalysts were also tested under concentrated-sunlight conditions in outdoor experiments, with a maximum methane production of 200 mmolCH4·gcat-¹·h-¹ achieved over Ru@ZrO2, which resulted in 31 % CO2 conversion and 92 % selectivity for methane in a continuous flow reactor at a space velocity of 1500 mLSTP·g-¹·min-¹.	en
dc.description.sponsorship	Financial support from the Spanish Ministerio de Ciencia e Innovación and Spanish Agencia Estatal de Investigación (grants PID2019-106687RJ-I00, PID2021-127265OB-C21, PLEC2022-009221 and Beca FPU 18/01877) and from Gobierno de Navarra (PC091-092 FOREST2+) is gratefully acknowledged. Open access funding provided by Universidad Pública de Navarra.
dc.format.mimetype	application/pdf	en
dc.identifier.citation	Imizcoz, M., Pellejero, I., Gandía, L. M. (2024). Assessing thermal and nonthermal contributions during CO2 hydrogenation over ruthenium catalysts: effects of the illumination conditions and the nature of the support. Applied Catalysis B: Environmental and Energy, 358, 1-14. https://doi.org/10.1016/j.apcatb.2024.124405.
dc.identifier.doi	10.1016/j.apcatb.2024.124405
dc.identifier.issn	0926-3373
dc.identifier.uri	https://academica-e.unavarra.es/handle/2454/52555
dc.language.iso	eng
dc.publisher	Elsevier
dc.relation.ispartof	Applied Catalysis B: Environmental and Energy (2024), vol. 358, 124405
dc.relation.projectID	info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-106687RJ-I00/ES/
dc.relation.projectID	info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127265OB-C21/ES/
dc.relation.projectID	info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PLEC2022-009221/
dc.relation.projectID	info:eu-repo/grantAgreement/Gobierno de Navarra//PC091–092/
dc.relation.publisherversion	https://doi.org/10.1016/j.apcatb.2024.124405
dc.rights	© 2024 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC license
dc.rights.accessRights	info:eu-repo/semantics/openAccess
dc.rights.uri	https://creativecommons.org/licenses/by-nc/4.0/
dc.subject	Ruthenium nanoparticles	en
dc.subject	Solar CO2 conversion	en
dc.subject	Photothermal catalysis	en
dc.subject	ZrO2	en
dc.subject	CeO2	en
dc.subject	TiO2	en
dc.title	Assessing thermal and nonthermal contributions during CO2 hydrogenation over ruthenium catalysts: effects of the illumination conditions and the nature of the support	en
dc.type	info:eu-repo/semantics/article
dc.type.version	info:eu-repo/semantics/publishedVersion
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