Engineering PdAu/CeO2 Alloy/Oxide Interfaces for Selective Methane-to-Methanol Conversion with Water
The direct conversion of methane-to-methanol remains a critical challenge in methane valorization. In this study, we unveil the crucial role of PdAu/CeO<inf>2</inf> catalysts in enabling selective methane transformation under mild conditions, using only water as the sole oxidant. Through...
| Autores: | , , , , , |
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| Tipo de recurso: | artículo |
| Estado: | Versión publicada |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositorio: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/413992 |
| Acceso en línea: | http://hdl.handle.net/10261/413992 https://www.scopus.com/inward/record.uri?eid=2-s2.0-105011850710&doi=10.1002%2Fanie.202505716&partnerID=40&md5=c71819158074fd21064dd6514ef06428 |
| Access Level: | acceso abierto |
| Palabra clave: | Alloy–oxide interface DFT calculations Methane-to-methanol conversion PdAu/CeO2 catalyst XPS characterization |
| Sumario: | The direct conversion of methane-to-methanol remains a critical challenge in methane valorization. In this study, we unveil the crucial role of PdAu/CeO<inf>2</inf> catalysts in enabling selective methane transformation under mild conditions, using only water as the sole oxidant. Through a combination of experimental techniques, including XPS and catalytic testing, alongside density functional theory (DFT) calculations, we demonstrate that a Pd<inf>0.3</inf>Au<inf>0.7</inf>/CeO<inf>2</inf> catalyst, which predominantly exposes isolated Pd atoms, achieves remarkable methanol selectivity (∼80%) at 500 K with a 1:1 methane-to-water ratio. While Pd/CeO<inf>2</inf> efficiently activates methane, its tendency for overreaction leads to complete methanol decomposition, thereby limiting selectivity. Alloying Pd with Au on ceria mitigates this over-reactivity, preventing methanol degradation while maintaining sufficient catalytic activity. The PdAu/CeO<inf>2</inf> composite exhibits a synergistic effect: Pd in contact with the ceria support facilitates methane activation and water dissociation, while Au fine-tunes reactivity to promote methanol formation. DFT calculations confirm that isolated Pd sites at the PdAu/CeO<inf>2</inf> interface play a key role in balancing activity and selectivity. This work underscores the importance of alloy/oxide interfaces in controlling selective methane conversion with water and offers valuable insights for designing highly efficient catalysts for methanol synthesis. © 2025 The Author(s). Angewandte Chemie International Edition published by Wiley-VCH GmbH. |
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