Adriano H Braga, Jhonatan L Fiorio, Ofelia Yang, Karla L C Silva, Tiago A Silva, Adam S Hoffman, Simon R Bare, Jefferson Bettini, Naga Vishnu V Mogili, Liane M Rossi
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引用次数: 0
Abstract
The addition of palladium (Pd) to preformed gold nanoparticles (Au NPs) enables the formation of core-shell structures with enhanced catalytic performance in oxidation reactions. However, predicting the precise palladium content required to achieve maximum catalytic activity remains difficult based on current understanding. Herein, Pd was systematically introduced onto titania-supported Au NPs (2, 6, and 10 nm) to evaluate their performance in benzyl alcohol oxidation. A volcano-like trend in catalytic activity was observed, where activity increased with Pd addition, peaked, and then declined. The Pd loading required for maximum activity depended on Au NP size: ≈40 at% Pd/Au for 2.6 nm, ≈20 at% Pd/Au for 6.4 nm, and ≈12.5 at% Pd/Au for 10.6 nm. For Au NPs > 6 nm, peak activity aligned with monolayer Pd coverage, while for smaller NPs (2-3 nm), optimal Pd content was below monolayer predictions. X-ray absorption spectroscopy revealed a core-shell structure at low Pd content, but higher Pd loadings led to Pd diffusion into the Au core. This structural transformation likely caused activity decline, indicating that AuPd alloying negatively impacts catalysis. These results highlight that core-shell Au@Pd catalysts outperform AuPd alloys and provide crucial insights for designing highly active bimetallic catalysts.
期刊介绍:
ChemPhysChem is one of the leading chemistry/physics interdisciplinary journals (ISI Impact Factor 2018: 3.077) for physical chemistry and chemical physics. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies.
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