Self‐Stabilized Heterometallic Pair Sites for Selective Ethanol Dehydrogenation on Pt–Cr–Ag Alloy Catalysts
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.
Authors
- Prahlad K. Routh (ORCID: https://orcid.org/0000-0002-0629-3743)
- Johan Zetterberg (ORCID: https://orcid.org/0000-0002-0882-1482)
- M. M. Montemore (ORCID: https://orcid.org/0000-0002-4157-1745)
- Jan Knudsen (ORCID: https://orcid.org/0000-0002-8280-7638)
- Andrea Grespi (ORCID: https://orcid.org/0000-0003-3132-4318)
- Esteban L. Fornero
- Lindsay R. Merte (ORCID: https://orcid.org/0000-0002-3213-4199)
- John S. Miller (ORCID: https://orcid.org/0000-0002-1164-9249)
- Anatoly I. Frenkel (ORCID: https://orcid.org/0000-0002-5451-1207)
- Lisa Rämisch (ORCID: https://orcid.org/0000-0002-4738-8247)
- J. Biener
- J. Anibal Boscoboinik (ORCID: https://orcid.org/0000-0002-5090-7079)
- Eric A. Stach (ORCID: https://orcid.org/0000-0002-3366-2153)
- Shuting Xiang (ORCID: https://orcid.org/0000-0001-9423-3347)
- E. Charles H. Sykes (ORCID: https://orcid.org/0000-0002-0224-2084)
- Harald Wallander (ORCID: https://orcid.org/0000-0002-4691-1606)
- Jovenal Jamir
- Rajeev Kumar (ORCID: https://orcid.org/0000-0002-2248-7601)
- Ulrike Küst (ORCID: https://orcid.org/0009-0009-0056-3165)
- Shengjie Zhang (ORCID: https://orcid.org/0000-0003-4158-9010)
- Jason F. Weaver
- Steven Arias
Institutions
- Tulane University (US)
- Tufts University (US)
- Lawrence Livermore National Laboratory (US)
- Malmö University (SE)
- Lund University (SE)
- Brookhaven National Laboratory (US)
- University of Florida (US)
- Instituto de Desarrollo Tecnológico para la Industria Química (AR)
- MAX IV Laboratory (SE)
- Stony Brook University (US)
- University of Pennsylvania (US)
Publication Details
- Journal
- Angewandte Chemie
- Published
- 2025-10-14
- DOI
- https://doi.org/10.1002/ange.202513844
- Primary Topic
- Catalysts for Methane Reforming
- Type
- article
- Field-Weighted Citation Impact
- 0.00