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2017 Fiscal Year Annual Research Report

Innovation of Novel Adsorbents Derived from Geomimetics for Burying Radionuclides

Research Project

Project/Area Number 16H02435
Research InstitutionKyushu University

Principal Investigator

笹木 圭子  九州大学, 工学研究院, 教授 (30311525)

Co-Investigator(Kenkyū-buntansha) 平島 剛  九州大学, 工学研究院, 教授 (00175556)
出光 一哉  九州大学, 工学研究院, 教授 (10221079)
三木 一  九州大学, 工学研究院, 准教授 (10706386)
Project Period (FY) 2016-04-01 – 2019-03-31
Keywords放射性核種 / 固化埋設 / ジオミメティクス / 吸着 / 共沈
Outline of Annual Research Achievements

(1)LDHとカーボンドットとの複合体を合成し、透過型電顕像、表面電位、結晶相、赤外吸収分光により特性化するとともに、SeO42-およびSr2+の同時吸着試験をおこない反応性の評価を行った。さらに、LDHと酸化グラフェン(GO)との複合体も合成し、同様の評価によって比較した。LDH量で正規化したSeO42-の吸着量はどちらも同等のものであったが、炭素量で正規化したSr2+の吸着量は後者のほうがはるかに大きかった。Sr2+のLDH-GO複合体に対する吸着容量は、複合化しないGOに対する吸着容量よりも、GO量により正規化した上で、数倍から10倍高い値となった。LHD-カーボンドット複合体の表面電位はカーボンドットのそれに近いのに対して、LDH-GO複合体の表面電位はLDHのそれに近かった。TEM, FTIR観察から、GOはより粒子径の小さなLDHとの複合化によって層剥離が生じ、有効吸着サイト数が格段に増大し、一方LDHよりもかなり粒子径が小さいカーボンドットではその効果が生じなかった。
(2)SeO42-のエトリンガイト共沈反応において、SO42-の共存は妨害的に作用した。一方、これはそれぞれのオキソ陰イオンのエトリンガイト構造中における配位様式の差に起因していることを、FTIR、放射光分析により明らかにした。エトリンガイト中のSeO42-は外圏錯体をなすのに対し、SeO32-は内圏錯体をなすため、前者はエトリンガイトをマトリクスとする固体残渣中で安定性が劣る。これを克服するために、ガラス固化をこころみ、800°C以上の焼成により、セレンを揮発することなく、TCLP試験にも耐える安定性の高い構造に変化した。
(3)SeO42-をIO3-に置き換えてもエトリンガイトとの共沈実験後の固体残渣中では、いずれも外圏錯体を形成するものの、収着容量は後者のほうが前者よりも大きく有意差があった。

Current Status of Research Progress
Current Status of Research Progress

1: Research has progressed more than it was originally planned.

Reason

上記の実績のほか字数制限上記述していないあとの2点についても成果を挙げており、H29年度だけで、13編の再読付論文(うち12編は国際誌)を公表した。次のテーマへの発展要素も掴みつつある。

Strategy for Future Research Activity

(1)LDH-GO複合体に対して、吸着剤の再生性を検討する。吸着と脱着の過程でディラミネーションとラミネーションを反復するかどうか、他の環境材料としての発展性も見据えて検討する。
(2)IO3-イオンを取り込んだエトリンガイトは脆弱でそのままでは埋設に向かないため、固化法を検討する。熱をかけることにより揮発するヨウ素の性質があるため、熱をかけない方法、具体的には、セラミックライトや冷却等方加圧法などを検討する。
(3)陰イオンとそれを安定化するマトリクスの関係について、エトリンガイトを例として、第一原理計算による裏づけを検討する。
(4)本プロジェクトとの総括をおこなう。未公表の結果についても論文投稿の方針をまとめて早急に実施する。

  • Research Products

    (26 results)

All 2018 2017

All Journal Article (13 results) (of which Int'l Joint Research: 4 results,  Peer Reviewed: 13 results) Presentation (13 results) (of which Int'l Joint Research: 13 results,  Invited: 1 results)

  • [Journal Article] Influence of the pre-dispersion of montmorillonite on organic modification and the adsorption of perchlorate and methyl red anions2018

    • Author(s)
      Luo Wuhui、Sasaki Keiko、Hirajima Tsuyoshi
    • Journal Title

      Applied Clay Science

      Volume: 154 Pages: 1~9

    • DOI

      10.1016/j.clay.2017.12.032

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Immobilization of selenate in cancrinite using a hydrothermal method2018

    • Author(s)
      Pahlevi Niko Dian、Guo Binglin、Sasaki Keiko
    • Journal Title

      Ceramics International

      Volume: 44 Pages: 8635~8642

    • DOI

      10.1016/j.ceramint.2018.02.083

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Characterization of the intermediate in formation of selenate-substituted ettringite2017

    • Author(s)
      Guo Binglin、Sasaki Keiko、Hirajima Tsuyoshi
    • Journal Title

      Cement and Concrete Research

      Volume: 99 Pages: 30~37

    • DOI

      10.1016/j.cemconres.2017.05.002

    • Peer Reviewed
  • [Journal Article] Selenite and selenate uptaken in ettringite: Immobilization mechanisms, coordination chemistry, and insights from structure2017

    • Author(s)
      Guo Binglin、Sasaki Keiko、Hirajima Tsuyoshi
    • Journal Title

      Cement and Concrete Research

      Volume: 100 Pages: 166~175

    • DOI

      10.1016/j.cemconres.2017.07.004

    • Peer Reviewed
  • [Journal Article] Solidification of ettringite after uptaking selenate as a surrogate of radionuclide in glass-ceramics by using industrial by-products2017

    • Author(s)
      Guo Binglin、Sasaki Keiko、Hirajima Tsuyoshi
    • Journal Title

      Journal of Material Science

      Volume: 52 Pages: 12999~13011

    • DOI

      10.1007/s10853-017-1422-x

    • Peer Reviewed
  • [Journal Article] Structural transformation of selenate ettringite: a hint for exfoliation chemistry2017

    • Author(s)
      Guo Binglin、Sasaki Keiko、Hirajima Tsuyoshi
    • Journal Title

      RSC Advances

      Volume: 7 Pages: 42407~42415

    • DOI

      10.1039/c7ra08765a

    • Peer Reviewed
  • [Journal Article] Synergistic effect of Sr2+ and ReO4- adsorption on hexadecyl pyridinium-modified montmorillonite2017

    • Author(s)
      Luo Wuhui、Inoue Akihiro、Hirajima Tsuyoshi、Sasaki Keiko
    • Journal Title

      Applied Surface Science

      Volume: 394 Pages: 431~439

    • DOI

      10.1016/j.apsusc.2016.10.135

    • Peer Reviewed
  • [Journal Article] Carbon-Dot-Decorated Layered Double Hydroxide Nanocomposites as a Multifunctional Environmental Material for Co-immobilization of SeO42? and Sr2+ from Aqueous Solutions2017

    • Author(s)
      Koilraj Paulmanickam、Kamura Yuta、Sasaki Keiko
    • Journal Title

      ACS Sustainable Chemistry and Engineering

      Volume: 5 Pages: 9053~9064

    • DOI

      10.1021/acssuschemeng.7b01979

    • Peer Reviewed
  • [Journal Article] Effects of grinding montmorillonite and illite on their modification by dioctadecyl dimethyl ammonium chloride and adsorption of perchlorate2017

    • Author(s)
      Luo Wuhui、Fukumori Takeru、Guo Binglin、Osseo-Asare Kwadwo、Hirajima Tsuyoshi、Sasaki Keiko
    • Journal Title

      Applied Clay Science

      Volume: 146 Pages: 325~333

    • DOI

      10.1016/j.clay.2017.06.025

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Enhancement of fluoride immobilization in apatite by Al 3+ additives2017

    • Author(s)
      Sasaki Keiko、Nagato Shugo、Ideta Keiko、Miyawaki Jin、Hirajima Tsuyoshi
    • Journal Title

      Chemical Engineering Journal

      Volume: 311 Pages: 284~292

    • DOI

      10.1016/j.cej.2016.11.096

    • Peer Reviewed
  • [Journal Article] Quantitative analysis of radiocesium retention onto birnessite and todorokite2017

    • Author(s)
      Yu Qianqian、Ohnuki Toshihiko、Kozai Naofumi、Sakamoto Fuminori、Tanaka Kazuya、Sasaki Keiko
    • Journal Title

      Chemical Geology

      Volume: 470 Pages: 141~151

    • DOI

      10.1016/j.chemgeo.2017.09.008

    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Selective adsorption of inorganic anions on unwashed and washed hexadecyl pyridinium-modified montmorillonite2017

    • Author(s)
      Luo Wuhui、Hirajima Tsuyoshi、Sasaki Keiko
    • Journal Title

      Separation and Purification Technology

      Volume: 176 Pages: 120~125

    • DOI

      10.1016/j.seppur.2016.12.004

    • Peer Reviewed
  • [Journal Article] 過塩素酸イオン吸着済有機修飾粘土セメント固化体の特性評価2017

    • Author(s)
      INOUE Akihiro、LUO Wuhui、MORIYAMA Sayo、HIRAJIMA Tsuyoshi、SHIMADA Hideki、SASAKI Keiko
    • Journal Title

      J. MMIJ

      Volume: 133 Pages: 235~240

    • DOI

      10.2473/journalofmmij.133.235

    • Peer Reviewed
  • [Presentation] Effects of precursors on the photocatalytic activities of graphitic carbon nitride in hexavalent chromium reduction and rhodamine B degradation under visible light irradiation2018

    • Author(s)
      Chitiphon Chuaicham, Keiko Sasaki
    • Organizer
      ACS spring 2018
    • Int'l Joint Research
  • [Presentation] Suppression mechanism of anionic pollutants released from fly ash by Ca additives2018

    • Author(s)
      Shingo Nakama, Quanzhi Tian, Binglin Guo, Niko Dian Pahlevi, Zhaochu Hu, Keiko Sasaki
    • Organizer
      ACS spring 2018
    • Int'l Joint Research
  • [Presentation] Geomimetics for chemical separation of anionic radionuclides toward long term storage2017

    • Author(s)
      Keiko Sasaki
    • Organizer
      ACS Asia-Pasific International Chapters Conference (APICC)
    • Int'l Joint Research / Invited
  • [Presentation] Eco-friendly alkali free amino acid-assisted hydrothermal synthesis of different divalent cations containing layered double hydroxide and their chromate adsorption efficiency2017

    • Author(s)
      Paulmanickam Koilraj, Keiko Sasaki
    • Organizer
      ACS Asia-Pasific International Chapters Conference (APICC)
    • Int'l Joint Research
  • [Presentation] Synthesis of amorphous carbon-doped mixed oxyhydroxides and their dual performance for arsenite and fluoride uptake performance from binary mixture solution2017

    • Author(s)
      Muthu Prabhu, Paulmanickam Koilraj, Keiko Sasaki
    • Organizer
      ACS Asia-Pasific International Chapters Conference (APICC)
    • Int'l Joint Research
  • [Presentation] Facile synthesis of ZnTi mixed metal oxide/C3N4 composites for photocatalytic decolorization of rhodamine B under visible light2017

    • Author(s)
      Chitiphon Chuaicham, Keiko Sasaki
    • Organizer
      ACS Asia-Pasific International Chapters Conference (APICC)
    • Int'l Joint Research
  • [Presentation] Immobilization of borate and arsenate from geothermal waters by co-precipitation with hydroxyapatite2017

    • Author(s)
      Keiko Sasaki, Yoshikazu Hayashi, Binglin Guo
    • Organizer
      Goldschmidt 2017
    • Int'l Joint Research
  • [Presentation] Immobilization Process of Selenate in Cancrinite by Hydrothermal Method2017

    • Author(s)
      Niko Dian Pahlevi, Binglin Guo, Keiko Sasaki
    • Organizer
      EARTH 2017
    • Int'l Joint Research
  • [Presentation] Immobilization of borate from the discharged water in mining activity by co-precipitation with hydroxyapatite2017

    • Author(s)
      Yoshikazu Hayashi, Binglin Guo, Keiko Sasaki
    • Organizer
      EARTH 2017
    • Int'l Joint Research
  • [Presentation] Removal of borate by co-precipitation with hydroxyapatite in the geothermal drainage from mining activity in lab and pilot scales2017

    • Author(s)
      Yoshikazu HAYASHI, Binglin GUO, Tsuyoshi HIRAJIMA, Tatsuya ITO, Takeshi NAKAMURA, Keiko SASAKI
    • Organizer
      CINEST2017
    • Int'l Joint Research
  • [Presentation] Co-immobilization of 79SeO42- and 90Sr2+ on the layered double hydroxide/carbon material composites2017

    • Author(s)
      Yuta Kamura, Paulmanickam Koilraj, Keiko Sasaki
    • Organizer
      CINEST2017
    • Int'l Joint Research
  • [Presentation] Affecting Factors to the Phase Matrix to Immobilize Selenate in Hydrothermal Co-Precipitation with Sodalite/Cancrinite2017

    • Author(s)
      Niko Dian PAHLEVI, Binglin GUO, Tsuyoshi HIRAJIMA, and Keiko SASAKI
    • Organizer
      CINEST2017
    • Int'l Joint Research
  • [Presentation] Synergistic adsorption of Sr2+ and ClO4ー on encapsulated organo-montmorillonite in alginate2017

    • Author(s)
      Wuhui Luo, Keiko Sasaki
    • Organizer
      Hybrid Materials 2017
    • Int'l Joint Research

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Published: 2018-12-17  

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