Control of zeolite microenvironment for propene synthesis from methanol

Longfei Lin, Mengtian Fan, Alena M. Sheveleva, Xue Han, Zhimou Tang, Joseph H. Carter, Ivan Silva, Christopher M. A. Parlett, Floriana Tuna, Eric J. L. McInnes, German Sastre, Svemir Rudić, Hamish Cavaye, Stewart F. Parker, Yongqiang Cheng, Luke L. Daemen, Anibal J. Ramirez-Cuesta, Martin P. Attfield, Yueming Liu, Chiu C. Tang, Buxing Han and Sihai Yang ()
Additional contact information
Longfei Lin: University of Manchester
Mengtian Fan: University of Manchester
Alena M. Sheveleva: University of Manchester
Xue Han: University of Manchester
Zhimou Tang: East China Normal University
Joseph H. Carter: University of Manchester
Ivan Silva: STFC Rutherford Appleton Laboratory
Christopher M. A. Parlett: Harwell Science and Innovation Campus
Floriana Tuna: University of Manchester
Eric J. L. McInnes: University of Manchester
German Sastre: UPV-CSIC Universidad Politecnica de Valencia
Svemir Rudić: STFC Rutherford Appleton Laboratory
Hamish Cavaye: STFC Rutherford Appleton Laboratory
Stewart F. Parker: STFC Rutherford Appleton Laboratory
Yongqiang Cheng: Oak Ridge National Laboratory
Luke L. Daemen: Oak Ridge National Laboratory
Anibal J. Ramirez-Cuesta: Oak Ridge National Laboratory
Martin P. Attfield: University of Manchester
Yueming Liu: East China Normal University
Chiu C. Tang: Harwell Science and Innovation Campus
Buxing Han: Chinese Academy of Science
Sihai Yang: University of Manchester

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Optimising the balance between propene selectivity, propene/ethene ratio and catalytic stability and unravelling the explicit mechanism on formation of the first carbon–carbon bond are challenging goals of great importance in state-of-the-art methanol-to-olefin (MTO) research. We report a strategy to finely control the nature of active sites within the pores of commercial MFI-zeolites by incorporating tantalum(V) and aluminium(III) centres into the framework. The resultant TaAlS-1 zeolite exhibits simultaneously remarkable propene selectivity (51%), propene/ethene ratio (8.3) and catalytic stability (>50 h) at full methanol conversion. In situ synchrotron X-ray powder diffraction, X-ray absorption spectroscopy and inelastic neutron scattering coupled with DFT calculations reveal that the first carbon–carbon bond is formed between an activated methanol molecule and a trimethyloxonium intermediate. The unprecedented cooperativity between tantalum(V) and Brønsted acid sites creates an optimal microenvironment for efficient conversion of methanol and thus greatly promotes the application of zeolites in the sustainable manufacturing of light olefins.

Date: 2021
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DOI: 10.1038/s41467-021-21062-1

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