Control of zeolite microenvironment for propene synthesis from methanol View Full Text


Ontology type: schema:ScholarlyArticle      Open Access: True


Article Info

DATE

2021-02-05

AUTHORS

Longfei Lin, Mengtian Fan, Alena M. Sheveleva, Xue Han, Zhimou Tang, Joseph H. Carter, Ivan da 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, Sihai Yang

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. More... »

PAGES

822

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/s41467-021-21062-1

DOI

http://dx.doi.org/10.1038/s41467-021-21062-1

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1135139516

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/33547288


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