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    Research Article

    Tuning Hierarchical ZSM-5 Zeolite for Both Gas- and Liquid-Phase Biorefining
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    • Shufang Zhao
      Shufang Zhao
      Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, Sydney Nano Institute, The University of Sydney, Sydney, New South Wales 2006, Australia
      More by Shufang Zhao
    • Wei David Wang
      Wei David Wang
      State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, Gansu 730000, China
      More by Wei David Wang
      Orcidhttp://orcid.org/0000-0003-2864-5102
    • Lizhuo Wang
      Lizhuo Wang
      Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, Sydney Nano Institute, The University of Sydney, Sydney, New South Wales 2006, Australia
      More by Lizhuo Wang
    • Wilhelm Schwieger
      Wilhelm Schwieger
      Institute of Chemical Reaction Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
      More by Wilhelm Schwieger
      Orcidhttp://orcid.org/0000-0003-4791-2667
    • Wei Wang
      Wei Wang
      State Key Laboratory of Applied Organic Chemistry, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, Gansu 730000, China
      More by Wei Wang
      Orcidhttp://orcid.org/0000-0002-9263-7927
    • Jun Huang*
      Jun Huang
      Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, Sydney Nano Institute, The University of Sydney, Sydney, New South Wales 2006, Australia
      *E-mail: [email protected]
      More by Jun Huang
      Orcidhttp://orcid.org/0000-0001-8704-605X
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    ACS Catalysis

    Cite this: ACS Catal. 2020, 10, 2, 1185–1194
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    https://doi.org/10.1021/acscatal.9b04104
    Published December 4, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    A hierarchical ZSM-5 zeolite with an adjustable mesoporous size is required for many chemical processes including the biorefining of big biomass compounds. In this research, a simple and high-efficiency hard template method has been successfully developed by adopting carbon nanoparticles obtained from carbonation of polyethylene oxide and urea. The abundant −C–O–C– groups on the surface of carbon nanoparticles provide the high hydrophilicity (from −C–O–C– to −C–O–H) in the alkaline synthetic gel solution, which promotes the synthesis of hierarchical ZSM-5 zeolite and the aluminum condensation in the silica framework to improve the Brønsted acidity. The as-synthesized hierarchical zeolites exhibited two sets of channel systems: micropores (∼0.55 nm) are from the MFI framework network, and mesopores (∼12.5 and ∼34.5 nm) result from carbon nanoparticles of 10–40 nm in size, respectively. The hierarchical ZSM-5 with minimized extraframework aluminum species showed catalytic performance with high ethanol conversion (100%) and high stability (lifetime above 30 h) in the ethanol to olefins conversion. Importantly, the diffusion efficiency in ZSM-5 with mesoporous size was remarkably improved, compared to the catalyst with mesoporous size ∼12.5 nm. As the benzylation of mesitylene with benzyl alcohol, the ZSM-5 (∼34.5 nm) sample showed the highest conversion in benzyl alcohol (82.0%) and selectivity in 2-benzyl-1,3,5-trimethylbenzene (74.3%).

    Copyright © 2019 American Chemical Society

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    • ATR-IR spectra of carbon nanoparticles, control experiment with and without the pretreatment of NaOH, NH3-TPD profiles of catalysts, the reaction results of ethanol dehydration over the regenerated catalysts, and benzylation reaction results of p-xylene/mesitylene with benzyl alcohol (PDF)

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    ACS Catalysis

    Cite this: ACS Catal. 2020, 10, 2, 1185–1194
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.9b04104
    Published December 4, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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