Nickel promotes selective ethylene epoxidation on silver
Over the last 80 years, chlorine (Cl) has been the primary promoter of the ethylene epoxidation reaction valued at ~40 billion USD per year, providing a ~25% selectivity increase over unpromoted silver (Ag) (~55%). Promoters such as cesium, rhenium, and molybdenum each add a few percent of selectivity enhancements to achieve 90% overall, but their codependence on Cl makes optimizing and understanding their function complex. We took a theory-guided, single-atom alloy approach to identify nickel (Ni) as a dopant in Ag that can facilitate selective oxidation by activating molecular oxygen (O<sub>2</sub>) without binding oxygen (O) too strongly. Surface science experiments confirmed the facile adsorption/desorption of O<sub>2</sub> on NiAg, as well as demonstrating that Ni serves to stabilize unselective nucleophilic oxygen. Supported Ag catalyst studies revealed that the addition of Ni in a 1:200 Ni to Ag atomic ratio provides a ~25% selectivity increase without the need for Cl co-flow and acts cooperatively with Cl, resulting in a further 10% initial increase in selectivity.
Authors
- Elizabeth E. Happel
- M. M. Montemore (ORCID: https://orcid.org/0000-0002-4157-1745)
- Laura A. Cramer (ORCID: https://orcid.org/0000-0001-5600-8317)
- Adam S. Hoffman (ORCID: https://orcid.org/0000-0002-7682-4108)
- Phillip Christopher (ORCID: https://orcid.org/0000-0002-4898-5510)
- Iradwikanari Waluyo (ORCID: https://orcid.org/0000-0002-4046-9722)
- Adrian Hunt (ORCID: https://orcid.org/0000-0002-5283-9647)
- E. Charles H. Sykes (ORCID: https://orcid.org/0000-0002-0224-2084)
- Anika Jalil (ORCID: https://orcid.org/0000-0001-9581-731X)
Institutions
- Tulane University (US)
- Tufts University (US)
- University of California, Santa Barbara (US)
- Brookhaven National Laboratory (US)
- SLAC National Accelerator Laboratory (US)
Publication Details
- Journal
- Science
- Published
- 2025-02-20
- DOI
- https://doi.org/10.1126/science.adt1213
- Citations
- 37
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 19.16