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Entrapped Single Tungstate Site in Zeolite for Cooperative Catalysis of Olefin Metathesis with Brønsted Acid Site

DOI: 10.1021/jacs.8b03012 DOI Help

Authors: Pu Zhao (University of Oxford) , Lin Ye (University of Oxford) , Zhenyu Sun (University of Oxford) , Benedict T. W. Lo (University of Oxford) , Harry Woodcock (University of Oxford) , Chen Huang (University of Oxford) , Chiu Tang (Diamond Light Source) , Angus I. Kirkland (University of Oxford; Diamond Light Source) , Donghai Mei (Physical and Computational Sciences Directorate & Institute for Integrated Catalysis, Pacific Northwest National) , Shik Chi Edman Tsang (University of Oxford)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of The American Chemical Society

State: Published (Approved)
Published: April 2018

Abstract: Industrial olefin metathesis catalysts generally suffer from low reaction rates and require harsh reaction conditions for moderate activities. This is due to their inability to prevent metathesis active sites (MAS) from aggregation and their intrinsic poor adsorption and activation of olefin molecules. Here, isolated tungstate species as single molecular MAS is immobilized inside zeolite pores by Brønsted acid sites (BAS) on the inner surface. It is demonstrated for the first time that unoccupied BAS in atomic proximity to MAS enhance olefin adsorption and greatly facilitate the formation of metallocycle intermediates in a stereospecific manner. Thus, effective cooperative catalysis takes place over the BAS-MAS pair. In consequence, for the cross-metathesis of ethene and trans-2-butene to propene, under the same mild reaction conditions, the propene production rate over WOx/USY is ca. 7,300 times that over the industrial WO3/SiO2 based catalyst. A propene yield up to 79% (80% selectivity) without observable deactivation was obtained over WOx/USY for a wide range of reaction conditions.

Subject Areas: Chemistry

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