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Rational Design of Fe Single Sites Supported on Hierarchical Zeolites via Atomic Layer Deposition for Few-Walled Carbon Nanotube Production

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Mater. Interfaces 2024, 16, 26, 33590-33600
    Energy, Environmental, and Catalysis Applications

    Rational Design of Fe Single Sites Supported on Hierarchical Zeolites via Atomic Layer Deposition for Few-Walled Carbon Nanotube Production
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    • Peeranat Chaipornchalerm
      Peeranat Chaipornchalerm
      Department of Chemical and Biomolecular Engineering, School of Energy Science and Engineering, Vidyasirimedhi Institute of Science and Technology, Rayong 21210, Thailand
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    • Watinee Nunthakitgoson
      Watinee Nunthakitgoson
      Department of Chemical and Biomolecular Engineering, School of Energy Science and Engineering, Vidyasirimedhi Institute of Science and Technology, Rayong 21210, Thailand
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      Orcidhttps://orcid.org/0000-0003-1864-7534
    • Poobodin Mano
      Poobodin Mano
      National Nanotechnology Center, National Science and Technology Development Agency, Pathum Thani 12120, Thailand
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    • Pinit Kidkhunthod
      Pinit Kidkhunthod
      Synchrotron Light Research Institute (Public Organization), Nakhon Ratchasima 30000, Thailand
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    • Alejandro Montoya
      Alejandro Montoya
      School of Chemical and Bimolecular Engineering, The University of Sydney, Sydney, New South Wales 2006, Australia
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      Orcidhttps://orcid.org/0000-0003-3514-9262
    • Supawadee Namuangruk
      Supawadee Namuangruk
      National Nanotechnology Center, National Science and Technology Development Agency, Pathum Thani 12120, Thailand
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      Orcidhttps://orcid.org/0000-0003-2087-6707
    • Chularat Wattanakit*
      Chularat Wattanakit
      Department of Chemical and Biomolecular Engineering, School of Energy Science and Engineering, Vidyasirimedhi Institute of Science and Technology, Rayong 21210, Thailand
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0003-3419-9874
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2024, 16, 26, 33590–33600
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    https://doi.org/10.1021/acsami.4c06105
    Published June 20, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Metal single-site catalysts have recently played an essential role in catalysis due to their enhanced activity, selectivity, and precise reaction control compared to those of conventional metal cluster catalysts. However, the rational design and catalytic application of metal single-site catalysts are still in the early stages of development. In this contribution, we report the rational design of Fe single sites incorporated in a hierarchical ZSM-5 via atomic layer deposition (ALD). The designer catalysts demonstrated highly dispersed Fe species, predominantly stabilized by oxygen atoms in the zeolite framework at terminal, isolated, and vicinal silanol groups within the micropores and external surfaces of the zeolite. The successful incorporation of highly thermally stable and uniform Fe single sites into hierarchical zeolite through ALD represents a significant advancement in few-walled carbon nanotube production. The inner and outer diameters of produced CNTs are approximately 4.4 ± 2.4 and 8.6 ± 1.8 nm, respectively, notably smaller than those produced via traditional impregnated catalysts. This example emphasizes the concept of rational design of a single Fe site dispersed on a hierarchical ZSM-5 surface, which is anticipated to be a promising catalyst for advancing catalytic applications.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.4c06105.

    • XRD patterns, N2 adsorption–desorption isotherm, HAADF-STEM images, TEM images, NH3-TPD profiles of catalysts, Raman spectra of spent catalysts, elemental compositions of catalysts, Fe K-edge fit parameters, possible configuration of catalysts according to the computational study, and catalytic activity of the catalysts for ethanol dehydration and the CNT growth process (PDF)

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2024, 16, 26, 33590–33600
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.4c06105
    Published June 20, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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