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Synthesis of reaction‐adapted zeolites as methanol-to-olefins catalysts with mimics of reaction intermediates as organic structure‐directing agents

Nature Catalysisvolume 1pages547554 (2018) | Download Citation

Abstract

Catalysis with enzymes and zeolites have in common the presence of well-defined single active sites and pockets/cavities where the reaction transition states can be stabilized by longer-range interactions. We show here that for a complex reaction, such as the conversion of methanol-to-olefins (MTO), it is possible to synthesize reaction-adapted zeolites by using mimics of the key molecular species involved in the MTO mechanism. Effort has focused on the intermediates of the paring mechanism because the paring is less favoured energetically than the side-chain route. All the organic structure-directing agents based on intermediate mimics crystallize cage-based small-pore zeolitic materials, all of them capable of performing the MTO reaction. Among the zeolites obtained, RTH favours the whole reaction steps following the paring route and gives the highest propylene/ethylene ratio compared to traditional CHA-related zeolites (3.07 and 0.86, respectively).

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Acknowledgements

This work was supported by the European Union through ERC-AdG-2014-671093 (SynCatMatch), the Spanish Government-MINECO through Severo Ochoa (SEV-2016-0683) and MAT2015-71261-R. The Electron Microscopy Service of the Universitat Politècnica de València (UPV) is acknowledged for their help in sample characterization. C.L. acknowledges the China Scholarship Council for a PhD fellowship.

Author information

Author notes

  1. These authors contributed equally: Chengeng Li, Cecilia Paris.

Affiliations

  1. Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, València, Spain

    • Chengeng Li
    • , Cecilia Paris
    • , Joaquín Martínez-Triguero
    • , Mercedes Boronat
    • , Manuel Moliner
    •  & Avelino Corma

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Contributions

A.C. conceived and directed the project. M.M. and A.C. designed the synthesis and M.M. directed the zeolite synthesis work. C.P. carried out the synthesis of the organic molecules. C.L. performed the zeolite synthesis. C.L. and J.M.-T. performed the MTO catalytic experiments. M.B. carried out the theoretical calculations. M.M., M.B. and A.C. wrote the manuscript. C.L., C.P., J.M.-T., M.B., M.M. and A.C. participated in the discussion and interpretation of the experimental data.

Competing interests

The authors declare no competing interests.

Corresponding author

Correspondence to Avelino Corma.

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    Supplementary Figures 1–24, Supplementary Tables 1–6, Supplementary Methods, Supplementary References

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DOI

https://doi.org/10.1038/s41929-018-0104-7

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