Determination of 135Cs and 135Cs/137Cs Atomic Ratio in Environmental Samples by Combining Ammonium Molybdophosphate (AMP)-Selective Cs Adsorption and Ion-Exchange Chromatographic Separation to Triple-Quadrupole Inductively Coupled Plasma-Mass Spectrometry

被引:76
作者
Zheng, Jian [1 ]
Bu, Wenting [1 ,2 ]
Tagami, Keiko [1 ]
Shikamori, Yasuyuki [3 ]
Nakano, Kazumi [3 ]
Uchida, Shigeo [1 ]
Ishii, Nobuyoshi [1 ]
机构
[1] Natl Inst Radiol Sci, Res Ctr Radiat Protect, Inage Ku, Chiba 2638555, Japan
[2] Peking Univ, State Key Lab Nucl Phys & Technol, Sch Phys, Beijing 100871, Peoples R China
[3] Agilent Technol Japan Ltd, Applicat Ctr, Hachioji, Tokyo 1928510, Japan
关键词
CESIUM ISOTOPE RATIOS; RADIOACTIVE CONTAMINATION; NUCLEAR; PLANT; RADIONUCLIDES; RELEASE; CHEMISTRY; TOOL; GAS;
D O I
10.1021/ac501712m
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
Since the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident in 2011, the activity ratio of Cs-134/Cs-137 has been widely used as a tracer for contamination source identification. However, because of the short half-life of Cs-134 (2.06 y), this tracer will become unavailable in the near future. This article presents an analytical method for the determination of the long-lived Cs-135 (t(2/1) = 2 x 10(6) y) and the atomic ratio of Cs-135/Cs-137, as a promising geochemical tracer, in environmental samples. The analytical method involves ammonium molybdophosphate (AMP)-selective adsorption of Cs and subsequent two-stage ion-exchange chromatographic separation, followed by detection of isolated radiocesium isotopes via triple-quadrupole inductively coupled plasma-mass spectrometry (ICP-MS/MS). The AMP-selective adsorption of Cs and the chromatographic separation system showed high decontamination factors (10(4)-10(5)) for interfering elements, such as Ba, Mo, Sb, and Sn. Using ICP-MS/MS, only selected ions enter the collision/reaction cell to react with N2O, reducing the isobaric interferences (Ba-135(+) and Ba-137(+)) and polyatomic interferences ((MoAr+)-Mo-95-Ar-40, (MoAr)-Mo-97-Ar-40, (SnO+)-Sn-119-O-16, and (SbO+)-Sb-121-O-16) produced by sample matrix ions. The high abundance sensitivity (10(-9) for the Cs-135/Cs-133 ratio) provided by ICP-MS/MS allowed reliable analysis of Cs-135 and Cs-137 isotopes with the lowest detection limits ever reported by mass counting methods (0.01 pg mL(-1) and 0.006 pg mL(-1), respectively). The developed analytical method was successfully applied to the determination of Cs-135 and Cs-137 isotopes in environmental samples (soil, litter, and lichen) collected after the FDNPP accident for contamination source identification.
引用
收藏
页码:7103 / 7110
页数:8
相关论文
共 34 条
[1]   Impacts of the Fukushima Nuclear Power Plants on Marine Radioactivity [J].
Buesseler, Ken ;
Aoyama, Michio ;
Fukasawa, Masao .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2011, 45 (23) :9931-9935
[2]   Determination of (135) Cs by neutron activation analysis [J].
Chao, JH ;
Tseng, CL .
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION A-ACCELERATORS SPECTROMETERS DETECTORS AND ASSOCIATED EQUIPMENT, 1996, 372 (1-2) :275-279
[3]  
Chen HW, 2008, CHINESE J PHYS, V46, P560
[4]  
Crouch E. A. C., 1977, Atomic Data and Nuclear Data Tables, V19, P417, DOI 10.1016/0092-640X(77)90023-7
[5]   On-line ion chemistry for the AMS analysis of 90Sr and 135,137Cs [J].
Eliades, J. ;
Zhao, X-L ;
Litherland, A. E. ;
Kieser, W. E. .
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS, 2013, 294 :361-363
[6]   Collision cell chemistry for the analysis of radioisotopes by inductively coupled plasma mass spectrometry [J].
Epov, VN ;
Taylor, V ;
Lariviere, D ;
Evans, RD ;
Cornett, RJ .
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY, 2003, 258 (03) :473-482
[7]  
Fryer F., 2013, PUBLICATION, V5991-2802EN, P55
[8]   Cs-Ba separation using N2O as a reactant gas in a Multiple Collector-Inductively Coupled Plasma Mass Spectrometer collision-reaction cell: Application to the measurements of Cs isotopes in spent nuclear fuel samples [J].
Granet, M. ;
Nonell, A. ;
Favre, G. ;
Chartier, F. ;
Isnard, H. ;
Moureau, J. ;
Caussignac, C. ;
Tran, B. .
SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY, 2008, 63 (11) :1309-1314
[9]   Critical comparison of radiometric and mass spectrometric methods for the determination of radionuclides in environmental, biological and nuclear waste samples [J].
Hou, Xiaolin ;
Roos, Per .
ANALYTICA CHIMICA ACTA, 2008, 608 (02) :105-139
[10]   Assessment of individual radionuclide distributions from the Fukushima nuclear accident covering central-east Japan [J].
Kinoshita, Norikazu ;
Sueki, Keisuke ;
Sasa, Kimikazu ;
Kitagawa, Jun-ichi ;
Ikarashi, Satoshi ;
Nishimura, Tomohiro ;
Wong, Ying-Shee ;
Satou, Yukihiko ;
Handa, Koji ;
Takahashi, Tsutomu ;
Sato, Masanori ;
Yamagata, Takeyasu .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2011, 108 (49) :19526-19529