Control of zeolite microenvironment for propene synthesis from methanol

Longfei Lin, Mengtian Fan, Alena Sheveleva, Xue Han, Zhimou Tang, Joseph Carter, Ivan Da Silva, Christopher Parlett, Floriana Tuna, Eric Mcinnes, Germán Sastre, Svemir Rudic, Hamish Cavaye, Stewart F. Parker, Yongqiang Cheng, Luke L Daemen, Anibal J. Ramirez-Cuesta, Martin Attfield, Yueming Liu, Chiu C. TangBuxing Han, Sihai Yang

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Abstract

Optimising the balance in “propene selectivity-propene/ethene ratio-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 pore 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 hours) 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.
Original languageEnglish
Article number822
JournalNature Communications
Volume12
DOIs
Publication statusPublished - 5 Feb 2021

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