Self‐Stabilized Heterometallic Pair Sites for Selective Ethanol Dehydrogenation on Pt–Cr–Ag Alloy Catalysts
Abstract
Abstract 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 Pt x Cr x Ag 1‐2x ( 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.
Article Details
Authors (22)
Jason F. Weaver
Department of Chemical Engineering University of Florida Gainesville FL 32611 USA
Shuting Xiang
Department of Materials Science and Chemical Engineering
Jovenal Jamir
Department of Chemical Engineering University of Florida Gainesville FL 32611 USA
Ulrike Küst
Lisa Rämisch
Division of Synchrotron Radiation Research
Andrea Grespi
Division of Synchrotron Radiation Research and NanoLund Department of Physics Lund University Lund SE‐22100 Sweden
Harald Wallander
Materials Science and Applied Mathematics
Johan Zetterberg
Division of Combustion Physics
Steven Arias
Center for Functional Nanomaterials Brookhaven National Laboratory Upton New York 11973 USA
Esteban L. Fornero
Instituto de Desarrollo Tecnológico para la Industria Química Universidad Nacional del Litoral (UNL) y CONICET Güemes 3450 Santa Fe 3000 Argentina
Prahlad K. Routh
Department of Materials Science and Chemical Engineering
Shengjie Zhang
Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics
John S. Miller
Materials Science Division Physical and Life Sciences Directorate Lawrence Livermore National Laboratory 7000 East Ave Livermore CA 94550 USA
Rajeev Kumar Rai
Department of Materials Science and Engineering University of Pennsylvania Philadelphia PA 19104 USA
Eric A. Stach
Department of Materials Science and Engineering, University of Pennsylvania, 3231 Walnut Street, Philadelphia, Pennsylvania 19104, United States
J. Anibal Boscoboinik
Matthew M. Montemore
Department of Chemical and Biomolecular Engineering
E. Charles H. Sykes
Department of Chemistry Tufts University Medford MA 02155 USA
Jan Knudsen
Jürgen Biener
Materials Science Division Physical and Life Sciences Directorate Lawrence Livermore National Laboratory 7000 East Ave Livermore CA 94550 USA
Lindsay R. Merte
Materials Science and Applied Mathematics
Anatoly I. Frenkel
Department of Materials Science and Chemical Engineering