title: Simultaneous determination of radiocesium ((135)Cs, (137)Cs) and plutonium ((239)Pu, (240)Pu) isotopes in river suspended particles by ICP-MS/MS and SF-ICP-MS.
abstract: Due to radioisotope releases in the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, long-term monitoring of radiocesium ((135)Cs and (137)Cs) and Pu isotopes ((239)Pu and (240)Pu) in river suspended particles is necessary to study the transport and fate of these long-lived radioisotopes in the land-ocean system. However, it is expensive and technically difficult to collect samples of suspended particles from river and ocean. Thus, simultaneous determination of multi-radionuclides remains as a challenging topic. In this study, for the first time, we report an analytical method for simultaneous determination of radiocesium and Pu isotopes in suspended particles with small sample size (1-2g). Radiocesium and Pu were sequentially pre-concentrated using ammonium molybdophosphate and ferric hydroxide co-precipitation, respectively. After the two-stage ion-exchange chromatography separation from the matrix elements, radiocesium and Pu isotopes were finally determined by ICP-MS/MS and SF-ICP-MS, respectively. The interfering elements of U ((238)U(1)H(+) and (238)U(2)H(+) for (239)Pu and (240)Pu, respectively) and Ba ((135)Ba(+) and (137)Ba(+) for (135)Cs and (137)Cs, respectively) were sufficiently removed with the decontamination factors of 1-8×10(6) and 1×10(4), respectively, with the developed method. Soil reference materials were utilized for method validation, and the obtained (135)Cs/(137)Cs and (240)Pu/(239)Pu atom ratios, and (239+240)Pu activities showed a good agreement with the certified/information values. In addition, the developed method was applied to analyze radiocesium and Pu in the suspended particles of land water samples collected from Fukushima Prefecture after the FDNPP accident. The (135)Cs/(137)Cs atom ratios (0.329-0.391) and (137)Cs activities (23.4-152Bq/g) suggested radiocesium contamination of the suspended particles mainly originated from the accident-released radioactive contaminates, while similar Pu contamination of suspended particles caused by the accident could be neglected as the (240)Pu/(239)Pu atom ratios (0.182-0.208) were within the range of global fallout.
authors.affiliation: Biospheric Assessment for Waste Disposal Team & Fukushima Project Headquarters, National Institute of Radiological Sciences, National Institutes for Quantum and Radiological Science and Technology, Anagawa 4-9-1, Inage, Chiba 263-8555, Japan; School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023, China.
authors.forename: Liguo
authors.initials: L
authors.lastname: Cao
authors.affiliation: Biospheric Assessment for Waste Disposal Team & Fukushima Project Headquarters, National Institute of Radiological Sciences, National Institutes for Quantum and Radiological Science and Technology, Anagawa 4-9-1, Inage, Chiba 263-8555, Japan. Electronic address: jzheng@nirs.go.jp.
authors.forename: Jian
authors.initials: J
authors.lastname: Zheng
authors.affiliation: Institute of Environmental Radioactivity, Fukushima University, 1 Kanayagawa, Fukushima-City 960-1296, Japan.
authors.forename: Hirofumi
authors.initials: H
authors.lastname: Tsukada
authors.affiliation: School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023, China.
authors.forename: Shaoming
authors.initials: S
authors.lastname: Pan
authors.affiliation: Biospheric Assessment for Waste Disposal Team & Fukushima Project Headquarters, National Institute of Radiological Sciences, National Institutes for Quantum and Radiological Science and Technology, Anagawa 4-9-1, Inage, Chiba 263-8555, Japan.
authors.forename: Zhongtang
authors.initials: Z
authors.lastname: Wang
authors.affiliation: Biospheric Assessment for Waste Disposal Team & Fukushima Project Headquarters, National Institute of Radiological Sciences, National Institutes for Quantum and Radiological Science and Technology, Anagawa 4-9-1, Inage, Chiba 263-8555, Japan.
authors.forename: Keiko
authors.initials: K
authors.lastname: Tagami
authors.affiliation: Biospheric Assessment for Waste Disposal Team & Fukushima Project Headquarters, National Institute of Radiological Sciences, National Institutes for Quantum and Radiological Science and Technology, Anagawa 4-9-1, Inage, Chiba 263-8555, Japan.
authors.forename: Shigeo
authors.initials: S
authors.lastname: Uchida
keywords: ICP-MS; Ion-exchange chromatography; Multi-radionuclide determination; Plutonium; Radiocesium; Suspended particle