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Rational design of synergistic active sites for catalytic ethene/2-butene cross-metathesis in a rhenium-doped Y zeolite catalyst

DOI: 10.1021/acscatal.1c00524 DOI Help

Authors: Pu Zhao (University of Oxford) , Lin Ye (University of Oxford) , Guangchao Li (University of Oxford; Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences) , Chen Huang (University of Oxford) , Simson Wu (University of Oxford) , Ping-Luen Ho (University of Oxford) , Haokun Wang (University of Oxford) , Tatchamapan Yoskamtorn (University of Oxford) , Denis Sheptyakov (Paul Scherrer Institute) , Giannantonio Cibin (Diamond Light Source) , Angus I. Kirkland (University of Oxford; Diamond Light Source) , Chiu C. Tang (Diamond Light Source) , Anmin Zheng (Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences) , Wenjuan Xue (Tiangong University) , Donghai Mei (Tiangong University; Pacific Northwest National Laboratory) , Kongkiat Suriye (SCG Chemicals Co., Ltd) , Shik Chi Edman Tsang (University of Oxford)
Co-authored by industrial partner: Yes

Type: Journal Paper
Journal: Acs Catalysis

State: Published (Approved)
Published: March 2021

Abstract: Synthesizing atomically dispersed synergistic active pairs is crucial yet challenging in developing highly active heterogeneous catalysts for various industrially important reactions. Here, a single molecular Re species is immobilized on the inner surface of a Y zeolite with Brønsted acid sites (BASs) within atomic proximity to form Re OMS–BAS active pairs for the efficient catalysis of olefin metathesis reactions (OMS: olefin metathesis site). The synergy within the active pairs is revealed by studying the coadsorption geometry of the olefin substrates over the active pairs by synchrotron X-ray and neutron powder diffraction. It is shown that the BAS not only facilitates olefin adsorption but also aligns the olefin molecule to the Re OMS for efficient intermediate formation. Consequently, for the cross-metathesis of ethene and trans-2-butene to propene, this catalyst shows high activity under mild reaction conditions without observable deactivation. The catalyst outperforms not only traditional ReOx-based catalysts but also the best industrially applicable WOx-based catalyst thus far that we discovered previously. The concept of using two isolated active sites of different functionalities within atomic proximity in a confined cavity can provide opportunities for designing synergistically catalytic materials.

Journal Keywords: olefin metathesis; synergistic catalysis; rhenium-based catalysts; zeolites; synchrotron X-ray and neutron diffraction

Subject Areas: Chemistry

Instruments: B18-Core EXAFS , I11-High Resolution Powder Diffraction

Other Facilities: HRPT at Swiss Spallation Neutron Source (SINQ)

Discipline Tags:

Catalysis Physical Chemistry Chemistry

Technical Tags:

Diffraction Spectroscopy X-ray Powder Diffraction X-ray Absorption Spectroscopy (XAS) Energy Dispersive EXAFS (EDE)