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Control of zeolite microenvironment for propene synthesis from methanol

DOI: 10.1038/s41467-021-21062-1 DOI Help

Authors: 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; Diamond Light Source) , Ivan Da Silva (ISIS Facility) , Christopher Parlett (Diamond Light Source; University of Manchester; University of Manchester at Harwell; UK Catalysis Hub, Research Complex at Harwell) , Floriana Tuna (University of Manchester) , Eric J. L. Mcinnes (University of Manchester) , German Sastre (UPV-CSIC Universidad Politecnica de Valencia) , Svemir Rudic (ISIS Facility) , Hamish Cavaye (ISIS Facility) , Stewart F. Parker (ISIS Facility; UK Catalysis Hub, Research Complex at Harwell) , 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 (Diamond Light Source) , Buxing Han (Institute of Chemistry, Chinese Academy of Science, Beijing) , Sihai Yang (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 12

State: Published (Approved)
Published: February 2021
Diamond Proposal Number(s): 2359

Open Access Open Access

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.

Journal Keywords: Catalysis; Inorganic chemistry

Subject Areas: Chemistry


Instruments: I11-High Resolution Powder Diffraction , I20-EDE-Energy Dispersive EXAFS (EDE)

Other Facilities: ISIS Facility; Oak Ridge National Laboratory (ORNL)

Added On: 08/02/2021 13:32

Documents:
s41467-021-21062-1.pdf

Discipline Tags:

Catalysis Inorganic Chemistry Physical Chemistry Earth Sciences & Environment Mineralogy Zeolites Chemistry

Technical Tags:

Diffraction Spectroscopy X-ray Powder Diffraction X-ray Absorption Spectroscopy (XAS)