Epoxidation of propene using Au/TiO2: on the difference between H2 and CO as a co-reactant

S. Kanungo; Y. Su; M.F. Neira d'Angelo; J.C. Schouten; E.J.M. Hensen

doi:10.1039/C7CY00525C

Epoxidation of propene using Au/TiO₂: on the difference between H₂ and CO as a co-reactant

S. Kanungo
, Y. Su
, M.F. Neira d'Angelo
, J.C. Schouten
, E.J.M. Hensen

Onderzoeksoutput: Bijdrage aan tijdschrift › Tijdschriftartikel › Academic › peer review

17 Citaten (Scopus)

207 Downloads (Pure)

Samenvatting

The role of the reducing gas in the direct epoxidation of propene to propene oxide (PO) using O₂ over a Au/TiO₂ catalyst was studied through experiments and density functional theory calculations. It was found that PO can be obtained using both H₂ and CO as co-reactants. The yield of PO was much lower with CO than that with H₂. The role of the oxygen atoms of the titania support was studied by quantum-chemical investigations, which show that the mechanism involving CO as a co-reactant should proceed via surface oxygen vacancies, whereas with H₂ the well-accepted pathway involving OOH is favored. Steady-state isotopic transient kinetic analysis experiments demonstrate that support oxygen atoms are involved in PO formation when CO is used as the co-reactant.

Originele taal-2	Engels
Pagina's (van-tot)	2252-2261
Aantal pagina's	10
Tijdschrift	Catalysis Science & Technology
Volume	7
Nummer van het tijdschrift	11
DOI's	https://doi.org/10.1039/C7CY00525C
Status	Gepubliceerd - 7 jun. 2017

Financiering

We acknowledge financial support for the research from The Netherlands Organization for Scientific Research (NWO) through project number 10017587, a VICI grant and Nuffic funding. Supercomputing facilities were funded by the NWO.

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10.1039/C7CY00525C

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abstract = "The role of the reducing gas in the direct epoxidation of propene to propene oxide (PO) using O2 over a Au/TiO2 catalyst was studied through experiments and density functional theory calculations. It was found that PO can be obtained using both H2 and CO as co-reactants. The yield of PO was much lower with CO than that with H2. The role of the oxygen atoms of the titania support was studied by quantum-chemical investigations, which show that the mechanism involving CO as a co-reactant should proceed via surface oxygen vacancies, whereas with H2 the well-accepted pathway involving OOH is favored. Steady-state isotopic transient kinetic analysis experiments demonstrate that support oxygen atoms are involved in PO formation when CO is used as the co-reactant.",

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