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Title: Low-Temperature Direct Oxidation of Propane to Propylene Oxide Using Supported Subnanometer Cu Clusters

Journal Article · · ACS Catalysis
 [1]; ORCiD logo [2];  [3]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [5]
  1. Argonne National Laboratory (ANL), Argonne, IL (United States)
  2. Purdue University, West Lafayette, IN (United States); Case Western Reserve University, Cleveland, OH (United States)
  3. University of California, Los Angeles, CA (United States)
  4. Purdue University, West Lafayette, IN (United States)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States); Czech Academy of Sciences, Prague (Czech Republic)

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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); Czech Academy of Sciences (CAS), Prague (Czech Republic)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)
Grant/Contract Number:
AC02-06CH11357; SC0014664; SC0019152
OSTI ID:
2537948
Journal Information:
ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 7 Vol. 15; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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