UiO-66 MOF-Derived Ru@ZrO2 catalysts for photo-thermal CO2 hydrogenation

Almazán, Fernando; Lafuente, Marta; Echarte Villeras, Amaya; Imizcoz Aramburu, Mikel; Pellejero, Ismael; Gandía Pascual, Luis

Publication:
UiO-66 MOF-Derived Ru@ZrO2 catalysts for photo-thermal CO2 hydrogenation

dc.contributor.author	Almazán, Fernando
dc.contributor.author	Lafuente, Marta
dc.contributor.author	Echarte Villeras, Amaya
dc.contributor.author	Imizcoz Aramburu, Mikel
dc.contributor.author	Pellejero, Ismael
dc.contributor.author	Gandía Pascual, Luis
dc.contributor.department	Institute for Advanced Materials and Mathematics - INAMAT2	en
dc.contributor.funder	Universidad Pública de Navarra / Nafarroako Unibertsitate Publikoa	es
dc.date.accessioned	2023-10-16T10:10:45Z
dc.date.available	2023-10-16T10:10:45Z
dc.date.issued	2023
dc.date.updated	2023-10-16T09:42:24Z
dc.description.abstract	The use of metal–organic frameworks (MOFs) as templates or precursors in the manufacture of heterogeneous catalysts is highly attractive due to the transfer of MOFs’ inherent porosity and homogeneous metallic distribution to the derived structure. Herein, we report on the preparation of MOF-derived Ru@ZrO2 catalysts by controlled thermal treatment of zirconium-based MOF UiO66 with ruthenium moieties. Ru3+ (3 or 10 mol%) precursor was added to UiO-66 synthesis and, subsequently, the as-synthesized hybrid structure was calcined in flowing air at different temperatures (400–600 ◦C) to obtain ZrO2 -derived oxides doped with highly dispersed Ru metallic clusters. The materials were tested for the catalytic photo-thermal conversion of CO2 to CH4 . Methanation experiments were conducted in a continuous flow (feed flow rate of 5 sccm and 1:4 CO2 to H2 molar ratio) reactor at temperatures from 80 to 300 ◦C. Ru0.10@ZrO2 catalyst calcined at 600 ◦C was able to hydrogenate CO2 to CH4 with production rates up to 65 mmolCH4·gcat. –1 ·h –1, CH4 yield of 80% and nearly 100% selectivity at 300 ◦C. The effect of the illumination was investigated with this catalyst using a high-power visible LED. A CO2 conversion enhancement from 18% to 38% was measured when 24 sun of visible LED radiation was applied, mainly due to the increase in the temperature as a result of the efficient absorption of the radiation received. MOF-derived Ru@ZrO2 catalysts have resulted to be noticeably active materials for the photo-thermal hydrogenation of CO2 for the purpose of the production of carbon-neutral methane. A remarkable effect of the ZrO2 crystalline phase on the CH4 selectivity has been found, with monoclinic zirconia being much more selective to CH4 than its cubic allotrope.	en
dc.description.sponsorship	Financial support was obtained from Spanish Agencia Estatal de Investigación and Spanish Ministerio de Ciencia e Innovación MCIN/AEI/10.13039/501100011033/ and FEDER “Una manera de hacer Europa” (grants PID2019-106687RJ-I00/AEI/ 10.13039/501100011033 and PID2021-127265OB-C21), as well as from Plan de Recuperación, Transformación y Resiliencia and NextGenerationEU (grants PLEC2022-009221 and TED2021-130846B-100), which is gratefully acknowledged. M.L. and M.I. thank Spanish Ministerio de Universidades and Unión Europea-NextGenerationEU for the postdoctoral ¨Margarita Salas¨ and FPU 18/01877 grants, respectively. A.E. thanks Universidad Pública de Navarra for the predoctoral fellowship. L.M.G. thanks the Banco de Santander and Universidad Pública de Navarra for their financial support under “Programa de Intensificación de la Investigación 2018” initiative.	en
dc.format.mimetype	application/pdf	en
dc.format.mimetype	application/zip	en
dc.identifier.citation	Almazán, F., Lafuente, M., Echarte, A., Imizcoz, M., Pellejero, I., & Gandía, L. M. (2023). UiO-66 MOF-Derived Ru@ZrO2 Catalysts for Photo-Thermal CO2 Hydrogenation. Chemistry, 5(2), 720–729. https://doi.org/10.3390/chemistry50200511.	en
dc.identifier.doi	10.3390/chemistry5020051
dc.identifier.issn	2624-8549
dc.identifier.uri	https://academica-e.unavarra.es/handle/2454/46528
dc.language.iso	eng	en
dc.publisher	MDPI	en
dc.relation.ispartof	Chemistry 2023, 5, 720–729	en
dc.relation.projectID	info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-106687RJ-I00/ES/	en
dc.relation.projectID	info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127265OB-C21	en
dc.relation.projectID	info:eu-repo/grantAgreement/AEI//PLEC2022-009221	en
dc.relation.projectID	info:eu-repo/grantAgreement/AEI//TED2021-130846B-100	en
dc.relation.publisherversion	https://doi.org/10.3390/chemistry5020051
dc.rights	© 2023 by the authors. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license.	en
dc.rights.accessRights	info:eu-repo/semantics/openAccess
dc.rights.uri	http://creativecommons.org/licenses/by/4.0/
dc.subject	Calcination	en
dc.subject	Carbon neutral fuels	en
dc.subject	CO<sub>2</sub> hydrogenation	en
dc.subject	MOF-derived catalyst	en
dc.subject	Photo-thermal catalysis	en
dc.subject	UiO-66	en
dc.subject	Zirconia	en
dc.title	UiO-66 MOF-Derived Ru@ZrO2 catalysts for photo-thermal CO2 hydrogenation	en
dc.type	info:eu-repo/semantics/article
dc.type.version	Versión publicada / Argitaratu den bertsioa	es
dc.type.version	info:eu-repo/semantics/publishedVersion	en
dspace.entity.type	Publication
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