Adjusting the Chemical Reactivity of Oxygen for Propylene Epoxidation on Silver by Rational Design: The Use of an Oxyanion and Cl
[1];
[1];
[4];
[6]
- Catalysis for Energy, CE-GKAT, Energy Materials In-situ Laboratory (EMIL), BESSY II, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Straße 15, 12489 Berlin, Germany, Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany
- Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany
- Catalysis for Energy, CE-GKAT, Energy Materials In-situ Laboratory (EMIL), BESSY II, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Straße 15, 12489 Berlin, Germany, Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany
- CNR-IOM DEMOCRITOS, Consiglio Nazionale delle Ricerche─Istituto Officina dei Materiali, c/o SISSA, Via Bonomea 265, 34136 Trieste, Italy
- Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany, Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, Mülheim an der Ruhr 45470, Germany
- Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany, Theoretical Division, Los Alamos National Lab, Los Alamos, New Mexico 00000, United States
The development of catalysts for propylene oxide production from direct epoxidation using propylene and oxygen remains a challenge. Compared to ethylene epoxidation, where selectivity on silver catalysts is high, the low selectivity to produce propylene oxide over silver is partially attributed to the lack of electrophilic oxygen under propylene epoxidation reaction conditions. Here, we investigate how to mediate the chemical reactivity of oxygen by theory-inspired experiments for propylene epoxidation. We show how adding electrophilic-O via SO4 oxyanions to the surface of silver increases epoxide selectivity. Moreover, we show how the addition of Cl to the SO4-modified catalyst activates the oxyanion, giving a more than 4-fold increase in selectivity to propylene oxide. Finally, we explore different systems using DFT and draw a picture on how the next catalyst/co-catalyst systems should be tuned to design a catalyst with high selectivity for direct propylene oxidation.
- Research Organization:
- Helmholtz-Zentrum Berlin fur Materialien und Energie GmbH (Germany); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- 89233218CNA000001
- OSTI ID:
- 1972747
- Alternate ID(s):
- OSTI ID: 1972666; OSTI ID: 1973822
- Report Number(s):
- LA-UR-23-23269
- Journal Information:
- ACS Catalysis, Journal Name: ACS Catalysis Vol. 13 Journal Issue: 9; ISSN 2155-5435
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Similar Records
Reaction Mechanism for Direct Propylene Epoxidation by Alumina-Supported Silver Aggregates. The Role of the Particle / Support Interface
Increased Silver Activity for Direct Propylene Epoxidation via Subnanometer Size Effects