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Abnormally High Graphitic Crystallization of Cellulose Nanocrystals

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Mater. Interfaces 2024, 16, 20, 26580-26589
    Functional Nanostructured Materials (including low-D carbon)

    Abnormally High Graphitic Crystallization of Cellulose Nanocrystals
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    • Jung-Eun Lee
      Jung-Eun Lee
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Jung-Eun Lee
      Orcidhttps://orcid.org/0000-0003-2692-2356
    • Woo Cheol Jeon
      Woo Cheol Jeon
      Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
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    • Yea Eun Kim
      Yea Eun Kim
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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    • Ga-Hyeun Lee
      Ga-Hyeun Lee
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Ga-Hyeun Lee
      Orcidhttps://orcid.org/0000-0003-3933-8466
    • Juyoung Kim
      Juyoung Kim
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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    • Min Jeong Kim
      Min Jeong Kim
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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    • Seung Min Lee
      Seung Min Lee
      School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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    • Seong Hyeon Kweon
      Seong Hyeon Kweon
      School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
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    • Sang Kyu Kwak*
      Sang Kyu Kwak
      Department of Chemical and Biological Engineering, Korea University, Seoul 02841, Republic of Korea
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0002-0332-1534
    • Han Gi Chae*
      Han Gi Chae
      Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      *Email: [email protected]
      More by Han Gi Chae
      Orcidhttps://orcid.org/0000-0003-2196-0986
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2024, 16, 20, 26580–26589
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    https://doi.org/10.1021/acsami.4c04015
    Published May 11, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Cellulose nanocrystals (CNCs) are currently of great interest for many applications, such as energy storage and nanocomposites, because of their natural abundance. A number of carbonization studies have reported abnormal graphitization behavior of CNCs, although cellulose is generally known as a precursor for hard carbon (nongraphitizable carbon). Herein, we report a spray-freeze-drying (SFD) method for CNCs and a subsequent carbonization study to ascertain the difference in the structural development between the amorphous and crystalline phases. The morphological observation by high-resolution transmission electron microscopy of the carbonized SFD-CNC clearly shows that the amorphous and crystalline phases of CNC are attributed to the formation of hard and soft carbon, respectively. The results of a reactive molecular dynamics (RMD) study also show that the amorphous cellulose phase leads to the formation of fewer carbon ring structures, indicative of hard carbon. In contrast, the pristine crystalline cellulose phase has a higher density and thermal stability, resulting in limited molecular relaxation and the formation of a highly crystalline graphitic structure (soft carbon).

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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.4c04015.

    • Characterization of pristine CNC including product specification, elemental composition, XRD, and DSC; cellulose polymer chain and model systems of crystalline cellulose and amorphous cellulose; porosity characterization of spray-freeze-dried CNCs; SEM images; HRTEM observation of amorphous and turbostratic/graphitic components in carbonized CNCs; molecular dynamics simulations of cellulose decomposition, potentials, radial distribution functions, diffusion coefficients, carbonization intermediates, and gas formation; comparison of d-spacing and crystal sizes from WAXD and Raman deconvolution; electrical resistivity comparison to carbon blacks (PDF)

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2024, 16, 20, 26580–26589
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.4c04015
    Published May 11, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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