Photo-thermal Catalytic CO2 Methanation by RuO x @MIL-101(Cr) with 9.2% Apparent Quantum Yield under Visible Light Irradiation
[EN] Solar-assisted gaseous CO2 hydrogenation to CH4 is a potential strategy for favoring the transition to net zero emissions. Here, we report the development of a series of efficient metal-organic frameworks with MIL-101(Cr or Fe) topology decorated with RuOx nanoparticles (ca. 0.2-2 wt %) as hete...
| Autores: | , , , , , , , , , , , |
|---|---|
| Tipo de recurso: | artículo |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Universitat Politècnica de València (UPV) |
| Repositorio: | RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia |
| Idioma: | inglés |
| OAI Identifier: | oai:riunet.upv.es:10251/228376 |
| Acceso en línea: | https://riunet.upv.es/handle/10251/228376 |
| Access Level: | acceso abierto |
| Palabra clave: | Photo-thermal catalysis Metal-organic frameworks MIL-101(Cr) RuOx nanoparticles CO2 methanation |
| Sumario: | [EN] Solar-assisted gaseous CO2 hydrogenation to CH4 is a potential strategy for favoring the transition to net zero emissions. Here, we report the development of a series of efficient metal-organic frameworks with MIL-101(Cr or Fe) topology decorated with RuOx nanoparticles (ca. 0.2-2 wt %) as heterogeneous photocatalysts for the selective methanation of CO2 by H-2 under simulated sunlight irradiation. The activity of RuOx(1 wt %)@MIL-101(Cr) is between 3 and 50 times higher than related MOF-based photocatalysts under similar reaction conditions. Among the different photocatalysts, the optimized RuOx(2 wt %)@MIL-101(Cr) photocatalyst showed 98.1% CO2 conversion with 98.8% CH4 selectivity reaching a production rate of 7.85 mmol g(-1) h(-1) with 720 mW cm(-2) at 200 degrees C. Further, this photocatalyst exhibited a record apparent quantum yield of 9.2% at 600 nm and 200 degrees C after subtracting thermal activity contribution compared to any previous MOF- or other heterogeneous-based photocatalyst reported so far. The photocatalyst retained its activity and integrity upon reuse for about 110 h. Transient photocurrent, electrochemical impedance, photoluminescence, and laser flash photolysis spectroscopies together with additional photocatalytic experiments suggest the occurrance of dual photochemical and photothermal reaction pathways. The photocatalytic CO2 methanation reaction mechanism was further investigated using operando Fourier transform infrared spectroscopy. |
|---|