Control of zeolite microenvironment for propene synthesis from methanol
| Autor: | Stewart F. Parker, Sihai Yang, Anibal J. Ramirez-Cuesta, Xue Han, Martin P. Attfield, Buxing Han, Yongqiang Cheng, Christopher M. A. Parlett, Yueming Liu, Floriana Tuna, Ivan da Silva, Luke L. Daemen, Eric J. L. McInnes, L.Y. Lin, Alena M. Sheveleva, Mengtian Fan, Chiu C. Tang, Zhimou Tang, Hamish Cavaye, Svemir Rudić, German Sastre, Joseph H. Carter |
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| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
Materials science
Science Tantalum General Physics and Astronomy chemistry.chemical_element 010402 general chemistry Photochemistry 01 natural sciences General Biochemistry Genetics and Molecular Biology Article Catalysis Propene chemistry.chemical_compound Molecule Zeolite Multidisciplinary 010405 organic chemistry General Chemistry 0104 chemical sciences chemistry Methanol Selectivity Brønsted–Lowry acid–base theory Inorganic chemistry |
| Zdroj: | Nature Communications, Vol 12, Iss 1, Pp 1-9 (2021) Lin, L, Fan, M, Sheveleva, A, Han, X, Tang, Z, Carter, J, Da Silva, I, Parlett, C, Tuna, F, Mcinnes, E, Sastre, G, Rudic, S, Cavaye, H, Parker, S F, Cheng, Y, Daemen, L L, Ramirez-Cuesta, A J, Attfield, M, Liu, Y, Tang, C C, Han, B & Yang, S 2021, ' Control of zeolite microenvironment for propene synthesis from methanol ', Nature Communications, vol. 12, 822 . https://doi.org/10.1038/s41467-021-21062-1 Digital.CSIC. Repositorio Institucional del CSIC instname Nature Communications |
| ISSN: | 2041-1723 |
| DOI: | 10.1038/s41467-021-21062-1 |
| Popis: | 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. We thank EPSRC (EP/P011632/1), the Royal Society, National Natural Science Foundation of China (21733011, 21890761, 21673076), and the University of Manchester for funding. We thank EPSRC for funding and the EPSRC National Service for EPR Spectroscopy at Manchester. A.M.S. is supported by a Royal Society Newton International Fellowship. We are grateful to the STFC/ISIS Facility, Oak Ridge National Laboratory (ORNL) and Diamond Light Source (DLS) for access to the beamlines TOSCA/MAPS, VISION and I11/I20, respectively. We acknowledge Dr. L. Keenan for help at I20 beamline (SP23594-1). UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/R026939/1, EP/R026815/1, EP/R026645/1, EP/R027129/1 or EP/M013219/1 (biocatalysis). We acknowledge the support of The University of Manchester’s Dalton Cumbrian Facility (DCF), a partner in the National Nuclear User Facility, the EPSRC UK National Ion Beam Centre and the Henry Royce Institute. We recognise Dr. R. Edge and Dr. K. Warren for their assistance during the 60Co γ-irradiation processes. We thank Prof. A. Jentys from the Technical University of Munich for the measurement of the INS spectrum of iso-butene. We thank C. Webb, E. Enston and G. Smith for help with GC–MS; Dr. L. Hughes for help with SEM and EDX; M. Kibble for help at TOSCA/MAPS beamlines. Computing resources (time on the SCARF compute cluster for some of the CASTEP calculations) was provided by STFC’s e-Science facility. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by ORNL. The computing resources at ORNL were made available through the VirtuES and the ICE-MAN projects, funded by Laboratory Directed Research and Development programme and Compute and Data Environment for Science (CADES) |
| Databáze: | OpenAIRE |
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