title: Highly sensitive detection of neodymium ion in small amount of spent nuclear fuel samples using novel fluorescent macrocyclic hexadentate polyaminocarboxylate probe in capillary electrophoresis-laser-induced fluorescence detection.
abstract: A rapid and high-sensitive detection method for the total concentration of Nd ion (total Nd) in a small amount of a spent nuclear fuel sample is urgently required since the precise quantification of total Nd ion makes it possible for burnup (degree of fuel consumption) to be determined. In this work, a capillary electrophoresis-laser-induced fluorescent detection method (CE-LIF) is proposed for the analysis of total Nd in a spent fuel sample solution, with the use of a newly synthesized metal fluorescent probe which has a fluorescein and a macrocylic hexadentate chelating group, FTC-ABNOTA, for lanthanide (Ln) ions. Ln ions were derivatized to form a strongly fluorescent complex with the probe to suppress the quenching of the ligand-centered emission. The detection of Ln complexes in the CE-LIF indicated that the interaction between Ln ions and the FTC-ABNOTA was strong enough not to dissociate during migration. The mutual separation among the Ln-FTC-ABNOTA complexes in CE-LIF was achieved by pH control providing a dynamic ternary complexation (DTC) with hydroxide ions. Using the DTC separation mode, a high resolution of Nd from other Ln ions with high resolution of 1.3-1.9 and a theoretical plate number of 68,000, and a very low detection limit of 22 pM (3.2 ppt, 0.11 attomole amount basis) were successfully obtained. A simulated spent fuel sample containing various metal ions was examined in this method with a good quantification result of 102.1% recovery obtained even with a large excess of U.
authors.affiliation: Graduate School of Science and Engineering, Saitama University, 255 Shimo-Okubo, Sakura-ku, Saitama 338-8570, Japan. shingo@mail.saitama-u.ac.jp
authors.forename: Shingo
authors.initials: S
authors.lastname: Saito
authors.forename: Yoshiyuki
authors.initials: Y
authors.lastname: Sato
authors.forename: Tomoko
authors.initials: T
authors.lastname: Haraga
authors.forename: Yuta
authors.initials: Y
authors.lastname: Nakano
authors.forename: Shiho
authors.initials: S
authors.lastname: Asai
authors.forename: Yutaka
authors.initials: Y
authors.lastname: Kameo
authors.forename: Kuniaki
authors.initials: K
authors.lastname: Takahashi
authors.forename: Masami
authors.initials: M
authors.lastname: Shibukawa
mesh_terms: D019075:Electrophoresis, Capillary / Q000295:instrumentation / Q000379:methods*; D007220:Industrial Waste / Q000032:analysis*; D028581:Lanthanoid Series Elements / Q000737:chemistry; D047028:Macrocyclic Compounds / Q000737:chemistry*; D009354:Neodymium / Q000032:analysis*; D009678:Nuclear Energy; D011850:Radioactive Waste / Q000032:analysis*; D012680:Sensitivity and Specificity; D013050:Spectrometry, Fluorescence
chemical_list: D007220:Industrial Waste; D028581:Lanthanoid Series Elements; D047028:Macrocyclic Compounds; D011850:Radioactive Waste; D009354:Neodymium