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Preparation of Ordered Nanoporous Indium Tin Oxides with Large Crystallites and Individual Control over Their Thermal and Electrical Conductivities

  • Yumi Saito
    Yumi Saito
    Department of Applied Chemistry, Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo 169-8555, Japan
    More by Yumi Saito
  • Takamichi Matsuno
    Takamichi Matsuno
    Department of Applied Chemistry, Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo 169-8555, Japan
  • Quansheng Guo
    Quansheng Guo
    International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
  • Takao Mori
    Takao Mori
    International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    Graduate School of Pure and Applied Sciences, University of Tsukuba, 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan
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  • Makoto Kashiwagi
    Makoto Kashiwagi
    Department of Chemistry and Biological Science, Aoyama Gakuin University, 5-10-1 Fuchinobe, Chuo-ku, Sagamihara, Kanagawa 252-5258, Japan
  • Atsushi Shimojima
    Atsushi Shimojima
    Department of Applied Chemistry, Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo 169-8555, Japan
    Kagami Memorial Research Institute for Materials Science and Technology, Waseda University, 2-8-26 Nishiwaseda, Shinjuku-ku, Tokyo 169-0051, Japan
  • Hiroaki Wada
    Hiroaki Wada
    Department of Applied Chemistry, Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo 169-8555, Japan
    More by Hiroaki Wada
  • , and 
  • Kazuyuki Kuroda*
    Kazuyuki Kuroda
    Department of Applied Chemistry, Faculty of Science and Engineering, Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo 169-8555, Japan
    Kagami Memorial Research Institute for Materials Science and Technology, Waseda University, 2-8-26 Nishiwaseda, Shinjuku-ku, Tokyo 169-0051, Japan
    *Email: [email protected]
Cite this: ACS Appl. Mater. Interfaces 2021, 13, 13, 15373–15382
Publication Date (Web):March 25, 2021
https://doi.org/10.1021/acsami.0c23133
Copyright © 2021 American Chemical Society

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    Abstract

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    Metal oxides are considered suitable candidates for thermoelectric materials owing to their high chemical stabilities. The formation of ordered nanopores within these materials, which decreases thermal conductivity (κ), has attracted significant interest. However, the electrical conductivity (σ) of reported nanoporous metal oxides is low, owing to electron scattering at the thin pore walls and many grain boundaries formed by small crystallites. Therefore, a novel synthesis method that can control pore walls while forming relatively large crystallites to reduce κ and retain σ is required. In this study, we used indium tin oxide (ITO), which is a typical example among metal oxides with high σ. Nanoporous ITOs with large crystallite sizes of several hundred nanometers and larger were successfully prepared using indium chloride as a source of indium. The pore sizes were varied using colloidal silica nanoparticles with different particle sizes as templates. The crystal phase and nanoporous structure of ITO were preserved after spark plasma sintering at 723 K and 80 MPa. The κ was significantly lower than that reported for bulk ITO due to the phonon scattering caused by the nanoporous structure and thin pore walls. There was a limited decrease in σ even with high porosity. These findings show that κ and σ are independently controllable through the precise control of the structure. The control of the thickness of the pore walls at tens of nanometers was effective for the selective scattering of phonons, while almost retaining electron mobility. The remarkable preservation of σ was attributed to the large crystallites that maintained paths for electron conduction and decreased electron scattering at the grain boundaries.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c23133.

    • Details of the experimental procedures and calculations; SEM images and nitrogen adsorption–desorption isotherms of SCCs; SEM images, TEM images, ED patterns, and XRD patterns of ITO-76-L; XRD pattern and nitrogen adsorption–desorption isotherms of the ITO-76-L pellet; XRD pattern, SAXS patterns, and SEM images of the ITO-76-S pellet; |S| and ZT values of the pellet samples (PDF)

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    Cited By

    This article is cited by 8 publications.

    1. Huijuan Wu, Lili Chen, Suiting Ning, Xiaodie Zhao, Shuping Deng, Ning Qi, Feng Ren, Zhiquan Chen, Jing Tang. Extremely Low Thermal Conductivity and Enhanced Thermoelectric Performance of Porous Gallium-Doped In2O3. ACS Applied Energy Materials 2021, 4 (11) , 12943-12953. https://doi.org/10.1021/acsaem.1c02585
    2. Yi Han, Zu-Gang Li, Tinghua Li, Wei Zhao, Xiao-Wei Gong, Zhen-Hua Ge. Heating properties of ITO ceramics with different Sn/In ratios. Modern Physics Letters B 2024, 38 (13) https://doi.org/10.1142/S0217984924500994
    3. Jun Fang, Hong Cheng, Desong Fan. Enhanced heat transfer using wafer-scale crack-free well-ordered porous structure surface. International Communications in Heat and Mass Transfer 2023, 148 , 107018. https://doi.org/10.1016/j.icheatmasstransfer.2023.107018
    4. Ting Liu, Zhucheng Jiang, Jiaxiang Liu. Novel seed-assisted synthesis of indium tin oxide submicro-cubes and their resistivity. Frontiers of Chemical Science and Engineering 2023, 17 (5) , 557-569. https://doi.org/10.1007/s11705-022-2249-9
    5. F. Giovannelli, E. Sabarthes, F. Delorme. Thermoelectric properties of La7Mo7O30 sintered by reactive spark plasma sintering. Ceramics International 2023, 49 (8) , 11921-11925. https://doi.org/10.1016/j.ceramint.2022.12.040
    6. Yuta Shimasaki, Takamichi Matsuno, Quansheng Guo, Atsushi Shimojima, Hiroaki Wada, Takao Mori, Kazuyuki Kuroda. Preparation of mesoporous nitrogen-doped titania comprising large crystallites with low thermal conductivity. Nanoscale Advances 2022, 4 (11) , 2509-2520. https://doi.org/10.1039/D2NA00083K
    7. Matthew Hadden, David Martinez-Martin, Ken-Tye Yong, Yogambha Ramaswamy, Gurvinder Singh. Recent Advancements in the Fabrication of Functional Nanoporous Materials and Their Biomedical Applications. Materials 2022, 15 (6) , 2111. https://doi.org/10.3390/ma15062111
    8. Ting Liu, Zhucheng Jiang, Jiaxiang Liu. Novel Seed-Assisted Synthesis of Ito Submicro-Cubes and Their Resistivity. SSRN Electronic Journal 2022, 443 https://doi.org/10.2139/ssrn.4020113

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