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Template-strategy of atomic arrangement in layered double hydroxides

Research Project

Project/Area Number 21K14404
Research Category

Grant-in-Aid for Early-Career Scientists

Allocation TypeMulti-year Fund
Review Section Basic Section 26020:Inorganic materials and properties-related
Research InstitutionThe University of Tokyo (2022)
Shinshu University (2021)

Principal Investigator

Sudare Tomohito  東京大学, 大学院理学系研究科(理学部), 特任助教 (40783923)

Project Period (FY) 2021-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000)
Fiscal Year 2022: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
Fiscal Year 2021: ¥2,730,000 (Direct Cost: ¥2,100,000、Indirect Cost: ¥630,000)
Keywordsトポケミカル反応 / 層状複水酸化物 / 硝酸イオン / トポケミカル法 / イオン吸着 / Rietveld解析 / X線吸収微細構造 / ナノ空間 / 原子配列 / XAFS / 吸着等温線 / 第一原理計算 / 水素結合 / イオン交換 / RDF解析
Outline of Research at the Start

2021年度前半は,原子配列テンプレート法による新奇原子配列をもつLDHsの作製を実施する。歪みの規則配列化に着目し,JT活性イオン(Ni3+,Co2+,Fe3+(HS),Fe4+(LS),Mn4+)とJT不活性イオン(Ni2+,Co3+,Fe4+(HS),Mn3+)の混合組成からなるLDHsを作製する。
2021年度後半~2022年度は,LDHsの原子配列を解明するために,平均構造と局所構造からの解析を試みる。ラボでの粉末X線回折測定および放射光粉末X線回折測定,X線微細構造スペクトル測定と解析による平均・局所構造の解析をルーチンワーク的に実施する。

Outline of Final Research Achievements

We aimed to fabricate layered double hydroxides (LDHs) with novel atomic arrangements. Through the establishment of a method for controlling the atomic arrangement of LDHs based on topochemical reactions, and evaluation of the performance of ion adsorption and elucidation of the adsorption mechanism, we aimed to obtain a guiding principle for the selective adsorption and separation of ions by inorganic adsorbents. As a result, it was found that the LDHs synthesized by topochemical reactions have a solid solution composition that exceeds the conventional solid solution limit and a high symmetry atomic arrangement. Furthermore, these LDHs showed high fluoride ion selectivity and high adsorption capacity for nitrate ions, indicating for the first time that atomic arrangement, i.e., the geometry of adsorption sites, is the key to the adsorption separation of ions.

Academic Significance and Societal Importance of the Research Achievements

反応性窒素の人為活動による生産量は年々増加している。特に、施肥や産業、生活によって生成され、環境中の水への排出される硝酸イオンの量は、化石燃料の消費による放出量や農地による固定量をはるかに上回っており、窒素の地球科学的循環に向けた選択的な分離・濃縮技術が求められている。分子科学の観点でも、平面分子内に電荷共鳴構造をもつため、電荷密度や求核性が極めて小さく、一般に、物質との相互作用が小さい。そのため、吸着材による水中からの分離が極めて難しい。それに対して、今回開発したLDHsは極めて高い硝酸イオン吸着能をもつため、環境問題の解決に資するのみでなく、吸着科学の学理構築に資するものである。

Report

(3 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • Research Products

    (7 results)

All 2023 2022 2021

All Journal Article (5 results) (of which Peer Reviewed: 5 results,  Open Access: 1 results) Presentation (2 results) (of which Int'l Joint Research: 1 results,  Invited: 2 results)

  • [Journal Article] Layer-Stacking Sequence Governs Ion-Storage in Layered Double Hydroxides2023

    • Author(s)
      Sudare Tomohito、Ueda Mizuki、Yamaguchi Takuro、Tipplook Mongkol、Tanaka Hideki、Hayashi Fumitaka、Teshima Katsuya
    • Journal Title

      The Journal of Physical Chemistry Letters

      Volume: 14 Issue: 2 Pages: 584-591

    • DOI

      10.1021/acs.jpclett.2c03553

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Extended Solid-Solubility Limit in Layered Double Hydroxides: Tuning the Anion-Adsorption Selectivity2022

    • Author(s)
      Sudare Tomohito、Kawaguchi Kenta、Yamaguchi Kazuse、Hirono Kazuki、Tipplook Mongkol、Tanaka Hideki、Hayashi Fumitaka、Teshima Katsuya
    • Journal Title

      Chemistry of Materials

      Volume: 34 Issue: 23 Pages: 10681-10690

    • DOI

      10.1021/acs.chemmater.2c02829

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Critical role of water structure around interlayer ions for ion storage in layered double hydroxides2022

    • Author(s)
      Sudare Tomohito、Yamaguchi Takuro、Ueda Mizuki、Shiiba Hiromasa、Tanaka Hideki、Tipplook Mongkol、Hayashi Fumitaka、Teshima Katsuya
    • Journal Title

      Nature Communications

      Volume: 13 Issue: 1 Pages: 6448-6448

    • DOI

      10.1038/s41467-022-34124-9

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Charge Distribution Controls On‐Target Separation of Low Nucleophilicity Anions in Layered Double Hydroxides2022

    • Author(s)
      Sudare Tomohito、Tamura Shuhei、Kashiwazaki Maru、Nakamura Yuki、Kawaguchi Kenta、Shiiba Hiromasa、Fujisawa Kazunori、Tipplook Mongkol、Tanaka Hideki、Hayashi Fumitaka、Teshima Katsuya
    • Journal Title

      Advanced Materials Interfaces

      Volume: 9 Issue: 31 Pages: 2201484-2201484

    • DOI

      10.1002/admi.202201484

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Single-Step Topochemical Synthesis of NiFe Layered Double Hydroxides for Superior Anion Removal from Aquatic Systems2021

    • Author(s)
      Mongkol Tipplook, Tomohito Sudare, Hiromasa Shiiba, Arisa Seki, and Katsuya Teshima
    • Journal Title

      ACS Appl. Mater. Interfaces.

      Volume: 13 Issue: 43 Pages: 51186-51197

    • DOI

      10.1021/acsami.1c13706

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Presentation] Engineering cation atomic arrangement in layered hydroxide for nitrate adsorption from water2021

    • Author(s)
      T. Sudare
    • Organizer
      MRM 2021
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] 層状複水酸化物における陰イオンの選択的な吸着・分離~原子配列から層間水のはたらきまで~2021

    • Author(s)
      簾智仁
    • Organizer
      表面技術協会 関東支部第99回講演会
    • Related Report
      2021 Research-status Report
    • Invited

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Published: 2021-04-28   Modified: 2024-01-30  

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