Activity coefficient of actinide ions in molten salts for pyroprocess

• Project/Area Number: 22360403
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Nuclear engineering
• Research Institution: Kyoto University
• Principal Investigator: YAMANA Hajimu 京都大学, 原子炉実験所, 教授 (30283683)
• Co-Investigator(Kenkyū-buntansha): FUJII Toshiyuki 京都大学, 原子炉実験所, 准教授 (10314296) ; UEHARA Akihiro 京都大学, 原子炉実験所, 助教 (30402952)
• Project Period (FY): 2010-04-01 – 2014-03-31
• Project Status: Completed (Fiscal Year 2013)
• Budget Amount: ¥18,070,000 (Direct Cost: ¥13,900,000、Indirect Cost: ¥4,170,000); Fiscal Year 2013: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000); Fiscal Year 2012: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000); Fiscal Year 2011: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000); Fiscal Year 2010: ¥11,310,000 (Direct Cost: ¥8,700,000、Indirect Cost: ¥2,610,000)
• Keywords: 乾式再処理 / 活量係数 / アクチニド / ランタニド / 溶融塩 / 錯体構造 / 電気化学 / 分光化学 / 紫外可視吸収分光 / 電気化学測定 / ラマン分光 / 塩化物溶融塩 / 紫外可視吸光分光 / ラマン分光法 / XAFS / ネオジム / サクリックボルタンメトリー / 吸収スペクトル / アルカリ塩化物 / ギブス自由エネルギー

Research Abstract

Thermodynamic stability and coordination structure of lanthanides (Ln) and actinides (An) complexes in various molten chloride mixtures were investigated by using electrochemical transient techniques and absorption spectrophotometry, respectively. It was found that the strength of Coulombic interaction between solvent cations and the Ln and An complexes is the basic factor to control the solvation effect of molten salt media on the thermodynamic stability of the complexes. It is useful information on the estimation on the thermodynamic stability of Ln depending on the composition of molten chlorides and mutual separation of Ln and An.

Research Products

• [Journal Article] Raman spectroscopic study of uranyl complex in alkali chloride melts (2013)
  • Author(s): T. Fujii, T. Uda, Y. Iwadate, T. Nagai, A. Uehara, H. Yamana
  • Journal Title: J. Nucl. Mater. Volume: 440 Issue: 1-3 Pages: 575-579
  • DOI: 10.1016/j.jnucmat.2013.04.010
  • Peer Reviewed
• [Journal Article] Reduction behavior of UO22+ in molten LiCl-RbCl and LiCl-KCl eutectics by using tungsten (2013)
  • Author(s): T. Nagai, A. Uehara, T. Fujii, H. Yamana
  • Journal Title: J. Nucl. Mater. Volume: 439 Issue: 1-3 Pages: 1-6
  • DOI: 10.1016/j.jnucmat.2013.03.078
  • Peer Reviewed
• [Journal Article] Raman spectroscopic study of uranyl complex in alkali chloride melts (2013)
  • Author(s): A. Uehara, T. Nagai, T. Fujii, O. Shirai, H. Yamana
  • Journal Title: J. Nucl. Mater. Volume: 437 Issue: 1-3 Pages: 166-170
  • DOI: 10.1016/j.jnucmat.2013.02.003
  • Peer Reviewed
• [Journal Article] Synthesis and investigation of uranyl molybdate UO2MoO4 (2013)
  • Author(s): T. Nagai, N. Sato, S. Kitawaki, A. Uehara, T. Fujii, H. Yamana, M. Myochin
  • Journal Title: J. Nucl. Mater. Volume: 433 Issue: 1-3 Pages: 397-403
  • DOI: 10.1016/j.jnucmat.2012.10.010
  • Peer Reviewed
• [Journal Article] Quantitative analysis of Eu2+ and Eu3+ in LiCl-KCl eutectic melt by spectrophotometry and electrochemistry (2013)
  • Author(s): T.-J. Kim, A. Uehara, T. Nagai, T. Fujii, H. Yamana
  • Journal Title: J. Nucl. Mater. Volume: 409(3) Issue: 3 Pages: 188-193
  • DOI: 10.1016/j.jnucmat.2010.12.004
  • Peer Reviewed
• [Journal Article] Raman Spectroscopic Study of Rare Earth Chlorides in Alkali Chloride Eutectic Melts (2013)
  • Author(s): T. Uda,T. Fujii,Y. Iwadate,A. Uehara, H. Yamana
  • Journal Title: Zeitschrift fur anorganische und allgemeine Chemie Volume: 639 Issue: 5 Pages: 765-769
  • DOI: 10.1002/zaac.201200480
  • Peer Reviewed
• [Journal Article] Electrochemical deposition of uranium oxide in highly concentrated calcium chloride (2012)
  • Author(s): A. Uehara, O. Shirai, T. Fujii, T. Nagai, H. Yamana
  • Journal Title: J Appl Electrochem Volume: 42 Issue: 6 Pages: 455-461
  • DOI: 10.1007/s10800-012-0420-6
  • Peer Reviewed
• [Journal Article] Thermodynamic properties of trivalent lanthanide and actinide ions in molten mixtures of LiCl and KCl (2012)
  • Author(s): K. Fukasawa, A. Uehara, T. Nagai, N. Sato, T. Fujii., H. Yamana
  • Journal Title: Journal of Nuclear Materials Volume: 424 Issue: 1-3 Pages: 17-22
  • DOI: 10.1016/j.jnucmat.2012.01.009
  • Peer Reviewed
• [Journal Article] Absorption spectra and cyclic voltammograms of uranium species in molten lithium molybdate-sodium molybdate eutectic at 550 ◦C (2011)
  • Author(s): T. Nagai A. Uehara, M. Fukushima, M. Myochin, T. Fujii, N. Sato, and H. Yamana
  • Journal Title: Proc. Radiochim. Acta Volume: 1 Issue: 1 Pages: 151-155
  • DOI: 10.1524/rcpr.2011.0028
  • Peer Reviewed
• [Journal Article] Electrochemical and spectrophotometric study on trivalent neodymium ion in molten binary mixtures of LiCl and alkali earth chlorides (2011)
  • Author(s): K. Fukasawa, A. Uehara, T. Nagai, T. Fujii, H. Yamana
  • Journal Title: J. Nucl. Mater Volume: 414 Issue: 2 Pages: 265-269
  • DOI: 10.1016/j.jnucmat.2011.04.002
  • Peer Reviewed
• [Journal Article] Okamoto, EXAFS analysis of uranium(IV) and thorium(IV) complexes in concentrated CaCl2 solutions (2011)
  • Author(s): A. Uehara, T. Fujii, H. Matsuura, N. Sato, T. Nagai, K. Minato, H. Yamana and Y
  • Journal Title: Proc. Radiochim. Acta Volume: 1 Issue: 1 Pages: 161-165
  • DOI: 10.1524/rcpr.2011.0030
  • Peer Reviewed
• [Journal Article] Electrochemical behavior and electronic absorption spectra of uranium trivalent ions in molten LiCl-CsCl mixtures (2011)
  • Author(s): T. Nagai, A. Uehara, T. Fujii, N. Sato, and H. Yamana
  • Journal Title: J. Nucl. Mater Volume: 414 Issue: 2 Pages: 226-231
  • DOI: 10.1016/j.jnucmat.2011.03.048
  • Peer Reviewed
• [Journal Article] Separation of Nd metal by using disproportionation reaction of Nd(II) in molten chlorides (2011)
  • Author(s): A. Uehara, K. Fukasawa, T. Nagai, T. Fujii, and H. Yamana
  • Journal Title: J. Nucl. Mater Volume: 414 Issue: 2 Pages: 336-339
  • DOI: 10.1016/j.jnucmat.2011.05.004
  • NAID: 130007036105
  • Peer Reviewed
• [Journal Article] Electrochemical and spectrophotometric study on neodymium ions in molten alkali chloride mixtures J (2011)
  • Author(s): K. Fukasawa, A. Uehara, T. Nagai, T. Fujii, H. Yamana
  • Journal Title: Alloys and Compds Volume: 509 Issue: 16 Pages: 5112-5118
  • DOI: 10.1016/j.jallcom.2011.01.192
  • Peer Reviewed
• [Journal Article] Coordination characteristics of trivalent lanthanides and actinides in molten hydrate salts of Ca(NO3)2 and CaCl2 (2011)
  • Author(s): T. Fujii, G. Okude, A. Uehara, S. Sekimoto, H. Hayashi, M. Akabori, K. Minato, H. Yamana
  • Journal Title: J. Radioanal. Nucl. Chem Volume: 288 Issue: 1 Pages: 181-187
  • DOI: 10.1007/s10967-010-0907-8
  • NAID: 120003087950
  • Peer Reviewed
• [Journal Article] Coordination characteristics of trivalent lanthanides and actinides in molten hydrate salts of Ca(NO_3)_2 and CaCl_2 (2011)
  • Author(s): T.Fujii, G.Okude, A.Uehara, S.Sekimoto, H.Hayashi, M.Akabori, K.Minato, H.Yamana
  • Journal Title: J.Radioanal.Nucl.Chem. Volume: 288 Pages: 181-187
  • Peer Reviewed
• [Journal Article] Electrochemical Study of Neodymium Ions in Molten Chlorides (2010)
  • Author(s): K. Fukasawa, A. Uehara, T. Nagai, T. Fujii and H. Yamana
  • Journal Title: Green Energy and Technology Pages: 330-333
  • DOI: 10.1007/978-4-431-99779-5_53
  • ISBN: 9784431997788, 9784431997795
  • Peer Reviewed
• [Journal Article] Am/Cm Separation in Molten Chloride Melt Utilizing the Divalency of Am (2010)
  • Author(s): H. Yamana, A. Uehara, T. Nagai1, K. Fukasawa, and T. Fujii
  • Journal Title: IOP Conf. Series : Materials Science and Engineering Volume: 9 Pages: 12069-12069
  • DOI: 10.1088/1757-899x/9/1/012069
  • Peer Reviewed
• [Journal Article] Study on Coordination Characteristics of Neptunium and Uranium Ions in Calcium Nitrate Hydrate Melt by Raman Spectrometry and UV/Vis/NIR Spectrometry (2010)
  • Author(s): T. Fujii, G. Okude, A. Uehara, and H. Yamana
  • Journal Title: IOP Conf. Series : Materials Science and Engineering Volume: 9 Pages: 012061-012061
  • DOI: 10.1088/1757-899x/9/1/012061
  • Peer Reviewed
• [Journal Article] Electronic absorption spectra of U3+ and U4+ in molten LiCl-RbCl eutectic (2010)
  • Author(s): T. Nagai1, A. Uehara, T. Fujii, N. Sato and H. Yamana
  • Journal Title: IOP Conf. Series : Materials Science and Engineering Volume: 9 Pages: 012050-012050
  • DOI: 10.1088/1757-899x/9/1/012050
  • Peer Reviewed
• [Journal Article] Electrochemical characteristics of uranium ions in calcium chloride hydrate melts (2010)
  • Author(s): A Uehara, T Fujii, T Nagai, O Shirai, N Sato and H Yamana
  • Journal Title: IOP Conf. Series : Materials Science and Engineering Volume: 9 Pages: 12080-12080
  • DOI: 10.1088/1757-899x/9/1/012080
  • Peer Reviewed
• [Journal Article] Electrochemical characteristics of uranium ions in calcium chloride hydrate melts (2010)
  • Author(s): A.Uehara, T.Fujii, T.Nagai, O.Shirai, N.Sato, H.Yamana
  • Journal Title: IOP Conf.Series : Materials Science and Engineering Volume: 9
  • Peer Reviewed
• [Journal Article] Electronic absorption spectra of U^<3+> and U^<4+> in molten LiCl-RbCl eutectic (2010)
  • Author(s): T.Nagai1, A.Uehara, T.Fujii, N.Sato, H.Yamana
  • Journal Title: IOP Conf.Series : Materials Science and Engineering Volume: 9
  • Peer Reviewed
• [Journal Article] Unique extraction behavior of americium and curium in a system of TBP and calcium nitrate hydrate melt (2010)
  • Author(s): G.Okude, T.Fujii, A.Uehara, S.Sekimoto, K.Minato, H.Yamana
  • Journal Title: IOP Conf.Series : Materials Science and Engineering Volume: 9
  • Peer Reviewed
• [Presentation] 溶融LiCl-KCl浴中のネオジムカチオン周りの局所構造に及ぼすフッ化物添加効果 (2013)
  • Author(s): 藤田一宏,根津篤,津野聡,山城龍太郎,赤塚洋,山名元,藤井俊行,松浦治明
  • Organizer: 電気化学会春の大会
  • Place of Presentation: 東北大学（宮城県）
• [Presentation] 種々の溶融塩化物浴中におけるネオジムカチオンの局所構造解析 (2012)
  • Author(s): 松浦治明、根津篤、塩飽秀啓、矢板毅、山名元、藤井俊行、深澤一仁、宇多健詞、土原章寛
  • Organizer: 2012年電気化学会春の大会
  • Place of Presentation: アクトシティ浜松(静岡県)
  • Year and Date: 2012-03-29
• [Presentation] 溶融塩化物系におけるランタニドおよびアクチニドの熱力学的安定性 (2012)
  • Author(s): 深澤一仁、永井崇之、佐藤修彰、上原章寛、藤井俊行、山名元
  • Organizer: 日本原子力学会2012年春の年会
  • Place of Presentation: 福井大学文京キャンパス(福井県)
  • Year and Date: 2012-03-21
• [Presentation] Raman spectroscopic study of uranyl complex in alkali chloride melts (2012)
  • Author(s): T. Fujii, T. Uda, Y. Iwadate, T. Nagai A. Uehara, H. Yamana
  • Organizer: Nuclear Materials 2012
  • Place of Presentation: 大阪国際交流センター（大阪府）
• [Presentation] On the Utilization of the Divalency of Actinides and Lanthanides for their Effective Separation (2011)
  • Author(s): H. Yamana, K. Fukasawa, T. Fujii, T. Nagai, and A. Uehara
  • Organizer: Global 2011
  • Place of Presentation: Japan, Makuhari
  • Year and Date: 2011-12-11
• [Presentation] Thermodynamic Properties of Trivalent Lanthanide and Actinide Ions in Alkali Chloride and Alkaline Earfh Chloride Mixtures (2011)
  • Author(s): T.Fujii, A.Uehara, K.Fukasawa, T.Uda, T.Nagai, N.Sato, H.Yamana
  • Organizer: International symposium on molten salts and ionc liquids
  • Place of Presentation: カンクン(メキシコ)
  • Year and Date: 2011-11-29
• [Presentation] Thermodynamic Properties of Trivalent Lanthanide and Actinide Ions in Alkali Chloride and Alkaline Earth Chloride Mixtures (2011)
  • Author(s): T. Fujii, A. Uehara, K. Fukasawa, T. Uda, T. Nagai, N. Sato, and H. Yamana
  • Organizer: International symposium on molten salts and ionc liquids 2011
  • Place of Presentation: Mexico, Cancun
  • Year and Date: 2011-11-27
• [Presentation] 溶融塩化物中におけるU(III)イオンの電気化学的および分光学的研究 (2011)
  • Author(s): 深澤一仁、永井崇之、上原章寛、藤井俊行、山名元
  • Organizer: 日本原子力学会2011年秋の大会
  • Place of Presentation: 北九州国際会議場(福岡県)
  • Year and Date: 2011-09-22
• [Presentation] On the Utilization of the Divalency of Actinides and Lanthanides for their Effective Separation (2011)
  • Author(s): H.Yamana, K.Fukasawa, T.Fujii, T.Nagai, A.Uehara
  • Organizer: Gloval 2011
  • Place of Presentation: 幕張(千葉県)
  • Year and Date: 2011-09-04
• [Presentation] Thermodynamic stability of Nd(III) complex in ternary mixtures of molten alkali chlorides (2011)
  • Author(s): K.Fukasawa, A.Uehara, T.Nagai, T.Fujii, H.Yamana
  • Organizer: G-COE International Symposium "ZERO CARBON ENERGY 2011"
  • Place of Presentation: Ajou University(韓国)
  • Year and Date: 2011-08-19
• [Presentation] Formation of Uranium Fluoride Complex by Addition of Fluoride Ion to Molten NaCl-CsCl Eutectic (2011)
  • Author(s): A. Uehara, O. Shirai, T. Fujii, T. Nagai, N. Sato, H. Yamana
  • Organizer: MS 9
  • Place of Presentation: Norway Trondheim
  • Year and Date: 2011-06-11
• [Presentation] 溶融塩化物中でのランタニドイオンの化学特性 (2011)
  • Author(s): 深澤一仁, 上原章寛, 藤井俊行, 山名元, 永井崇之
  • Organizer: 日本原子力学会2011年春の年会
  • Place of Presentation: 福井大学
  • Year and Date: 2011-03-30
• [Presentation] 溶融塩中のNd(II)の不均化反応を利用したNd の分離 (2011)
  • Author(s): 上原章寛, 藤井俊行, 山名元, 深澤一仁,(JAEA) 永井崇之
  • Organizer: 日本原子力学会2011年春の年会
  • Place of Presentation: 福井大学
  • Year and Date: 2011-03-30
• [Presentation] 溶融塩化物中におけるU(III)イオンの電気化学的および分光学的研究 (2011)
  • Author(s): 深澤一仁, 上原章寛, 藤井俊行, 山名元, (JAEA) 永井崇之
  • Organizer: 日本原子力学会2011年秋の大会
  • Place of Presentation: 福井大学
  • Year and Date: 2011-03-30
• [Presentation] Separation by Using NdCl2 Reduced from NdCl3 in Molten Chlorides (2010)
  • Author(s): A. Uehara, K. Fukasawa, T. Nagai, T. Fujii, H. Yamana
  • Organizer: Nuclear Materials 2010, Karlsruhe Germany
  • Year and Date: 2010-10-04
• [Presentation] Electrochemical and Spectrophotometrical Study of Neodymium Trivalent Ion in Molten Binary Mixtures of LiCl and Alkali Earth Chlorides (2010)
  • Author(s): K. Fukasawa, A. Uehara, T. Nagai, T. Fujii, H. Yamana
  • Organizer: Nuclear Materials
  • Place of Presentation: Karlsruhe Germany
  • Year and Date: 2010-10-04
• [Presentation] 塩化物溶融塩中でのアクチニドオキソイオンの還元反応に関する基礎研究;(1)溶融塩中ウラニルイオンのウランイオンへの還元方法の検討 (2010)
  • Author(s): 永井崇之、平野弘康、上原章寛、藤井俊行、山名元、深澤一仁
  • Organizer: 日本原子力学会秋の大会
  • Place of Presentation: 北海道大学
  • Year and Date: 2010-09-17
• [Presentation] 溶融塩化物中でのネオジムイオンの化学特性に関する実験的および計算化学的研究 (2010)
  • Author(s): 深澤一仁、上原章寛、藤井俊行、山名元、永井崇之
  • Organizer: 日本原子力学会秋の大会
  • Place of Presentation: 北海道大学
  • Year and Date: 2010-09-17
• [Presentation] 塩化物溶融塩中でのアクチニドオキソイオンの還元反応に関する基礎研究 (2010)
  • Author(s): 永井崇之, 平野弘康, 上原章寛,藤井俊行, 山名元, 深澤一仁
  • Organizer: 日本原子力学会2010年秋の大会
  • Place of Presentation: 北海道大学
  • Year and Date: 2010-09-15
• [Presentation] 溶融塩化物中でのネオジムイオンの化学特性に関する実験的および計算化学的研究 (2010)
  • Author(s): 深澤一仁, 上原章寛, 藤井俊行, 山名元, 永井崇之
  • Organizer: 日本原子力学会2010年秋の大会
  • Place of Presentation: 北海道大学
  • Year and Date: 2010-09-15
• [Presentation] 濃厚電解質溶液中でのウランイオンの溶存状態と電気化学的挙動 (2010)
  • Author(s): 上原章寛、藤井俊行、山名元、永井崇之、白井理
  • Organizer: 日本分析化学会秋の年会
  • Place of Presentation: 東北大学
  • Year and Date: 2010-09-15
• [Presentation] 溶融塩化物中でのランタニドイオンの化学特性 (2010)
  • Author(s): 深澤一仁、上原章寛、永井崇之、藤井俊行、山名元
  • Organizer: 溶融塩討論会
  • Place of Presentation: ロワジールホテル函館
  • Year and Date: 2010-09-09
• [Presentation] アルカリ塩化物溶融塩中でのウランイオンの溶解度測定 (2010)
  • Author(s): 上原章寛,藤井俊行,永井崇之,深澤一仁,山名 元
  • Organizer: 日本原子力学会2010年春の年会
  • Place of Presentation: 茨城大学
  • Year and Date: 2010-03-26
• [Presentation] Separation by Using NdCl_2 Reduced from NdCl_3 in Molten Chlorides (2010)
  • Author(s): A.Uehara, K.Fukasawa, T.Nagai, T.Fujii1, H.Yamana
  • Organizer: Nuclear Materials 2010
  • Place of Presentation: Karlsruhe Germany
• [Presentation] Electrochemical and Spectrophotometrical Study of Neodymium Trivalent Ion in Molten Binary Mixtures of LiCl and Alkali Earth Chlorides (2010)
  • Author(s): K.Fukasawa, A.Uehara, T.Nagai, T.Fujii, H.Yamana
  • Organizer: Nuclear Materials 2010
  • Place of Presentation: Karlsruhe Germany
• [Presentation] Electrochemical Behavior and Electronic Absorption Spectra of Uranium Ions in Molten LiCl-CsCl Mixtures (2010)
  • Author(s): T.Nagai, A.Uehara, T.Fujii, N.Sato, H.Yamana
  • Organizer: Nuclear Materials 2010
  • Place of Presentation: Karlsruhe Germany
• [Patent(Industrial Property Rights)] 溶融塩中の酸塩化物及び酸化物並びにこれら化合物イオンの塩化処理方法 (2011)
  • Inventor(s): 永井崇之, 山名元, 藤井俊行, 上原章寛
  • Industrial Property Rights Holder: 永井崇之
  • Filing Date: 2011-02-22