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Impact of organic acids and carbonate ions on nuclide dissolution from fuel debris

Research Project

Project/Area Number 20H02665
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 31010:Nuclear engineering-related
Research InstitutionKyoto University

Principal Investigator

Sasaki Takayuki  京都大学, 工学研究科, 教授 (60314291)

Co-Investigator(Kenkyū-buntansha) 桐島 陽  東北大学, 多元物質科学研究所, 教授 (00400424)
秋山 大輔  東北大学, 多元物質科学研究所, 講師 (80746751)
Project Period (FY) 2020-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥18,070,000 (Direct Cost: ¥13,900,000、Indirect Cost: ¥4,170,000)
Fiscal Year 2023: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Fiscal Year 2022: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2021: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Fiscal Year 2020: ¥10,400,000 (Direct Cost: ¥8,000,000、Indirect Cost: ¥2,400,000)
Keywords燃料デブリ / 東京電力福島第一原子力発電所 / 有機酸 / 炭酸 / 溶解挙動 / 有機物 / 錯生成反応
Outline of Research at the Start

発電用原子炉の過酷事故で生じた燃料デブリの最終処分方策を考えるとき、デブリの長期安定性について検討しなければならないのは、地下水接触によりもたらされる化学影響である。デブリの構成元素(ウランや核分裂生成物、マイナーアクチニド)への有機酸や炭酸との錯生成能に着目し、事故時に発生したと考えられる燃料デブリの模擬を行うとともに、地下環境を再現した溶解実験を行う。得られた知見をもとに、デブリがどのように化学的な劣化を受けるかについて、熱力学的・分光学的に評価する。

Outline of Final Research Achievements

The chemical resistance of simulated debris to water containing organic acids and carbonic acid was investigated to consider a more realistic and feasible method for the final disposal of fuel debris w/o applying excessively conservative pretreatment. The dissolution process was evaluated thermodynamically. Focusing on the uranium-zirconium solid solutions, the uranium-iron oxide, and the uranium-calcium oxide as the simulated fuel debris, we conducted the dissolution experiment in the presence of dicarboxylic acid and/or carbonate, and analyzed the solid phase conditions and the dissolved species using various spectroscopic methods. Nuclide concentrations and dissolution rates increased with the organic acid and carbonate concentrations. Then, a new steady state between solid and liquid phases was reached due to forming a secondary solid phase on the debris surface with a redox reaction.

Academic Significance and Societal Importance of the Research Achievements

本研究は、福島第一原発事故で発生したと考えられる代表的なウラン燃料デブリやその関連物質を実験室で模擬合成し、地上地下の天然水に普遍的に含まれる有機酸や炭酸を含む水に対する化学的耐性、すなわち核種の溶解反応と溶解前後のデブリ表面の化学状態変化について実験的に評価した。この基礎知見は、進行中の廃炉事業において回収が計画されているデブリの、過度に保守的でないより安全で合理的な処理処分方策の立案に有益な情報をもたらすものである。

Report

(5 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • Research Products

    (21 results)

All 2024 2023 2022 2021 2020

All Journal Article (5 results) (of which Peer Reviewed: 5 results) Presentation (15 results) (of which Int'l Joint Research: 2 results) Book (1 results)

  • [Journal Article] Dissolution behavior and aging of iron-uranium oxide2024

    • Author(s)
      Tonna Ryutaro、Sasaki Takayuki、Okamoto Yoshihiro、Kobayashi Taishi、Akiyama Daisuke、Kirishima Akira、Sato Nobuaki
    • Journal Title

      Journal of Nuclear Materials

      Volume: 589 Pages: 154862-154862

    • DOI

      10.1016/j.jnucmat.2023.154862

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Phase analysis of simulated nuclear fuel debris synthesized using UO2, Zr, and stainless steel and leaching behavior of the fission products and matrix elements2023

    • Author(s)
      Tonna Ryutaro、Sasaki Takayuki、Kodama Yuji、Kobayashi Taishi、Akiyama Daisuke、Kirishima Akira、Sato Nobuaki、Kumagai Yuta、Kusaka Ryoji、Watanabe Masayuki
    • Journal Title

      Nuclear Engineering and Technology

      Volume: 55 Issue: 4 Pages: 1300-1309

    • DOI

      10.1016/j.net.2022.12.017

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Sorption of Cs+ and Eu3+ ions onto sedimentary rock in the presence of gamma-irradiated humic acid2022

    • Author(s)
      Zhao Qi, Saito Takeshi, Miyakawa Kazuya, Sasamoto Hiroshi, Kobayashi Taishi, Sasaki Takayuki
    • Journal Title

      Journal of Hazardous Materials

      Volume: 428 Pages: 128211-128211

    • DOI

      10.1016/j.jhazmat.2021.128211

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Phase transformation of mixed lanthanide oxides in an aqueous solution2021

    • Author(s)
      Md. Moniruzzaman, Taishi Kobayashi, Takayuki Sasaki
    • Journal Title

      Journal of Nuclear and Radiochemical Sciences

      Volume: 21 Pages: 15-27

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Solubility of Mixed Lanthanide Hydroxide and Oxide Solid Solutions2021

    • Author(s)
      Moniruzzaman Mohammad, Kobayashi Taishi, Sasaki Takayuki
    • Journal Title

      Journal of Nuclear Fuel Cycle and Waste Technology

      Volume: 19 Issue: 3 Pages: 353-366

    • DOI

      10.7733/jnfcwt.2021.19.3.353

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Presentation] U3O8-Fe2O3系共晶反応に対する酸素濃度の影響2024

    • Author(s)
      岩原 聖樹, 秋山 大輔, 桐島 陽
    • Organizer
      2B06, 日本原子力学会2024年春の年会, 近畿大学
    • Related Report
      2023 Annual Research Report
  • [Presentation] Dissolution and aging of metal monouranates: Simulated debris of Fukushima Daiichi Nuclear Power Station2023

    • Author(s)
      T. Sasaki, Y. Kato, R. Tonna, T. Kobayashi, Y. Okamoto
    • Organizer
      Migration 2023, Nantes, France
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] (U,Zr)O2の水への溶解メカニズムに関する考察2023

    • Author(s)
      頓名龍太郎,小林大志,佐々木隆之
    • Organizer
      1D05, 日本原子力学会 2023年秋の大会, 名古屋大学
    • Related Report
      2023 Annual Research Report
  • [Presentation] ZrO2の溶解反応における固相表面に関する考察2023

    • Author(s)
      花房拓豊,小林大志,佐々木隆之
    • Organizer
      1D06, 日本原子力学会 2023年秋の大会, 名古屋大学
    • Related Report
      2023 Annual Research Report
  • [Presentation] 不活性雰囲気下でのU-Fe-O系模擬燃料デブリの相関係に関する研究2023

    • Author(s)
      井野 広海, 秋山 大輔, 桐島 陽
    • Organizer
      2E13, 日本原子力学会2023年秋の大会, 名古屋大学
    • Related Report
      2023 Annual Research Report
  • [Presentation] CaUO4の炭酸存在下での溶解挙動2022

    • Author(s)
      加藤 雄斗、小林 大志、佐々木 隆之
    • Organizer
      日本原子力学会 2022年秋の大会, 1A01
    • Related Report
      2022 Annual Research Report
  • [Presentation] 鉄-ウラン系酸化物固相の溶解反応2022

    • Author(s)
      頓名龍太郎、小林大志、佐々木隆之、秋山大輔、桐島陽、佐藤修彰、岡本芳浩
    • Organizer
      日本地球惑星科学連合2022年大会, MAG39-11
    • Related Report
      2022 Annual Research Report
  • [Presentation] Dissolution Behavior and Aging of Iron-uranium Oxide; Simulated Debris of Fukushima Daiichi Nuclear Power Plant (1F)2022

    • Author(s)
      Ryutaro Tonna, Takayuki Sasaki, Taishi Kobayashi, Yoshihiro Okamoto, Daisuke Akiyama, Akira Kirishima, Nobuaki Sato
    • Organizer
      IYNC2022, Koriyama
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] UFeO4固相溶解に関する熱力学的考察2021

    • Author(s)
      頓名龍太郎, 小林大志, 佐々木隆之, 秋山大輔, 桐島陽, 佐藤修彰
    • Organizer
      2021年日本原子力学会春の年会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 5価ウラン-鉄酸化物の溶解メカニズムに関する考察2021

    • Author(s)
      頓名龍太郎, 小林大志, 佐々木隆之, 秋山大輔, 桐島陽, 佐藤修彰
    • Organizer
      2021年日本原子力学会秋の大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Gamma-irradiation-induced molecular-weight-dependent distribution of humic acid complexed with metal ions2021

    • Author(s)
      Zhao Qi, Kobayashi Taishi, Saito Takeshi, Sasaki Takayuki
    • Organizer
      2021年日本原子力学会春の年会
    • Related Report
      2021 Annual Research Report
  • [Presentation] UFeO4主固相とする模擬デブリの熱中性子照射および核種溶出挙動2021

    • Author(s)
      頓名龍太郎, 佐々木隆之, 小林大志, 関本俊
    • Organizer
      第55回京都大学複合原子力科学研究所学術講演会
    • Related Report
      2020 Annual Research Report
  • [Presentation] UFeO4固相溶解に関する熱力学的考察2021

    • Author(s)
      頓名龍太郎, 小林大志, 佐々木隆之, 秋山大輔, 桐島陽, 佐藤修彰
    • Organizer
      日本原子力学会2021年春の年会, 3I13
    • Related Report
      2020 Annual Research Report
  • [Presentation] Characterization of the solubility controlling solid phases of mixed lanthanide oxides (L1,L2,L3,)2O3 (L1,L2,L3= La,Nd,Eu,Tm)2021

    • Author(s)
      Md Moniruzzaman, Taishi Kobayashi, Takayuki Sasaki
    • Organizer
      AESJ 2021 Spring Meeting
    • Related Report
      2020 Annual Research Report
  • [Presentation] Characterization and solubility of mixed lanthanide oxides, (L1,L2)2O3 (L1,L2=La,Nd,Eu,Tm)2020

    • Author(s)
      Md Moniruzzaman, Taishi Kobayashi, Takayuki Sasaki
    • Organizer
      AESJ 2020 Fall Meeting
    • Related Report
      2020 Annual Research Report
  • [Book] 燃料デブリ化学の現在地2023

    • Author(s)
      佐藤修彰、桐島陽、佐々木隆之、高野公秀、熊谷友多、佐藤宗一、田中康介
    • Total Pages
      180
    • Publisher
      東北大学出版会
    • ISBN
      9784861633904
    • Related Report
      2023 Annual Research Report

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Published: 2020-04-28   Modified: 2025-01-30  

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