Self‐Stabilized Heterometallic Pair Sites for Selective Ethanol Dehydrogenation on Pt–Cr–Ag Alloy Catalysts
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<sub>x</sub>Cr<sub>x</sub>Ag<sub>1-2x</sub> (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)
- Jason F. Weaver (ORCID: https://orcid.org/0000-0002-6777-4727)
- 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
- 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 International Edition
- Published
- 2025-10-14
- DOI
- https://doi.org/10.1002/anie.202513844
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- National Science Foundation
- U.S. Department of Energy
- University of Pennsylvania
- VINNOVA
- Svenska Forskningsrådet Formas
- Vetenskapsrådet
- Office of Science
- Materials Research Science and Engineering Center, Harvard University
- Division of Materials Research
- Division of Chemical, Bioengineering, Environmental, and Transport Systems
- Division of Chemistry
- Basic Energy Sciences
- Lawrence Livermore National Laboratory
- Brookhaven National Laboratory
- SLAC National Accelerator Laboratory