Low-Temperature Direct Oxidation of Propane to Propylene Oxide Using Supported Subnanometer Cu Clusters
Propylene oxide, a key commodity of the chemical industry for a wide range of consumer products, is synthesized through sequential propane dehydrogenation and epoxidation reactions. However, the lack of a direct catalytic route from propane to propylene oxide reduces efficiency and represents a major challenge for catalysis science. Herein, we report the discovery of a highly active and selective catalyst, made of alumina-supported subnanometer copper clusters, which can directly convert propane to propylene oxide at temperatures as low as 150 °C. Moreover, at higher temperatures, on the same catalysts, the selectivity is switched to propylene. Accompanying theoretical calculations indicate that partially oxidized and/or hydroxylated clusters have low activation energies for both propane dehydrogenation and propylene epoxidation pathways, enabling direct conversion with very high selectivity for propylene oxide. The discovery of a low-temperature catalyst that can convert propane directly to propylene oxide provides an important opportunity for the development of energy-efficient and economic catalysts for this industrially critical process. Similarly, when operating at higher temperatures, these catalysts are posed as potent oxidative dehydrogenation catalysts.
Authors
- Anastassia N. Alexandrova (ORCID: https://orcid.org/0000-0002-3003-1911)
- Avik Halder
- Micaela Homer
- Philippe Sautet (ORCID: https://orcid.org/0000-0002-8444-3348)
- Robert E. Warburton (ORCID: https://orcid.org/0000-0002-9693-307X)
- Sönke Seifert (ORCID: https://orcid.org/0000-0003-4598-2354)
- Larry A. Curtiss (ORCID: https://orcid.org/0000-0001-8855-8006)
- Jeffrey Greeley (ORCID: https://orcid.org/0000-0001-8469-1715)
- Geng Sun (ORCID: https://orcid.org/0000-0003-2123-7464)
- Štefan Vajda (ORCID: https://orcid.org/0000-0002-1879-2099)
- Rajeev S. Assary (ORCID: https://orcid.org/0000-0002-9571-3307)
- Lei Cheng
Institutions
- Argonne National Laboratory (US)
- Davidson College (US)
- University of California, Los Angeles (US)
- Purdue University West Lafayette (US)
- University of California System (US)
- Czech Academy of Sciences, J. Heyrovský Institute of Physical Chemistry (CZ)
- Division of Materials Science and Engineering (AU)
- Advanced Photonix (United States) (US)
- Advanced Photon Source
Publication Details
- Journal
- ACS Catalysis
- Published
- 2025-03-24
- DOI
- https://doi.org/10.1021/acscatal.4c07577
- Citations
- 5
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 2.59
Funders
- European Commission
- Ministerstvo Školství, Mládeže a Tělovýchovy
- Basic Energy Sciences
- Workforce Development for Teachers and Scientists