2026-05-17T12:18:04Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:0n7bp-3dg82 2025-07-18T08:25:50Z openaire_data community-mcarchive

Lustemberg, Pablo G. Ganduglia-Pirovano, M. Verónica Rodríguez, José A. Fernández Villanueva, Estefanía Ramírez, Pedro J. Lustemberg, Pablo G. Pérez, Rubén Ganduglia-Pirovano, M. Verónica Rodríguez, José A. 2025-07-18 <p>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<sub>2</sub> 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<sub>0.3</sub>Au<sub>0.7</sub>/CeO<sub>2</sub> catalyst, which predominantly exposes isolated Pd atoms, achieves remarkable methanol selectivity (∼80%) at 500 K with a 1:1 methaneto-water ratio. While Pd/CeO<sub>2 </sub>efficiently activates methane, its tendency for overreaction leads to complete methanol decomposition, thereby limiting selectivity. Alloying Pd withAu on ceria mitigates this over-reactivity, preventing methanol degradation while maintaining sufficient catalytic activity. The PdAu/CeO<sub>2</sub> 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<sub>2</sub> 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.</p> application/gzip text/markdown text/plain https://doi.org/10.24435/materialscloud:nc-b8 oai:materialscloud.org:0n7bp-3dg82 mcid:2025.111 eng Materials Cloud https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:4y-bf info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode Computational chemistry Heterogeneous catalysis Methane to methanol CH4 CH3OH Gold Palladium CeO2 ceria Alloy Bimetallic Nanoparticle DFT GOFEE Engineering PdAu/CeO2 alloy/oxide interfaces for selective methane-to-methanol conversion with water info:eu-repo/semantics/other