Angewandte Chemie (International ed. in English) · 2025
Self-Stabilized Heterometallic Pair Sites for Selective Ethanol Dehydrogenation on Pt-Cr-Ag Alloy Catalysts.
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Weaver Jason F, Xiang Shuting, Jamir Jovenal, Küst Ulrike, Rämisch Lisa, Grespi Andrea, Wallander Harald, Zetterberg Johan, Arias Steven, Fornero Esteban L, Routh Prahlad K, Zhang Shengjie, Miller John S, Rai Rajeev Kumar, Stach Eric A, Boscoboinik J Anibal, Montemore Matthew M, Sykes E Charles H, Knudsen Jan, Biener Jürgen, Merte Lindsay R, Frenkel Anatoly I
Аннотация
Self-stabilized, heterometallic pair-sites can enable fine-tuning of catalytic functionality while also mitigating dynamic structural changes that degrade catalytic performance. This study demonstrates the development and characterization of trimetallic PtxCrxAg1-2x (x ≤ 0.1) alloys with active Pt-Cr pair-ensembles for non-oxidative ethanol dehydrogenation, leveraging predictions that favorable bonding stabilizes Pt-Cr pairs diluted in Ag. Operando X-ray absorption spectroscopy confirms the preferential formation and stability of Pt-Cr pairings dispersed throughout the Ag matrix, and ambient-pressure X-ray photoelectron spectroscopy shows that Pt-Cr sites have significant activity for ethanol dehydrogenation, while suppressing reaction processes that deactivate binary Pt-Ag and Cr-Ag alloys. This work demonstrates that stabilizing heterometallic pair sites within trimetallic alloys provides a new avenue for designing catalysts with discrete active sites that are durable and highly selective.