Abstract：To fill the lack of background data of 238Pu in terrestrial environment of China, the surface soil samples collected from different locations were analyzed for the plutonium isotopes content (238Pu, 239+240Pu). The results showed that the specific activities of 238Pu in samples were very low, in range of 0.007~0.045Bq/kg and the activity ratios of 238Pu/239+240Pu were in range of 0.032~0.041, similar to the reported data from neighboring countries and other mid-latitude locations in the northern hemisphere. A binary model was employed to attribute the origin of 238Pu in the environment, and the results suggested that the origin of 238Pu in surface soils be related most of all to nuclear weapon fallout and SNAP-9A fallout.
Browne E, Tuli J K. Nuclear data sheets for A=234[J]. Nuclear Data Sheets, 2007,108(3):681-772.
[2]
Qiao J X, Hou X L, Miro M, et al. Determination of plutonium isotopes in waters and environmental solids:A review[J]. Analytica Chimica Acta, 2009,652(1/2):66-84.
[3]
Hardy E P, Krey P W, Volchok H L. Global inventory and distribution of fallout plutonium[J]. Nature, 1973,241(5390):444-445.
[4]
UNSCEAR. Sources and effects of ionizing radiation. Volume II:effect[R]. Vienna, Austria:United Nations Scientific Committee on the Effects of Atomic Radiation, 2000:519.
[5]
Yamamoto M, Sakaguchi A, Ochiai S, et al. Isotopic Pu, Am and Cm signatures in environmental samples contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident[J]. Journal of Environmental Radioactivity, 2014,132:31-46.
[6]
Turner M, Rudin M, Cizdziel J, et al. Excess plutonium in soil near the Nevada Test Site, USA[J]. Environmental Pollution, 2003,125(2):193-203.
[7]
Ollui Mboulou M, Hurtgen C, Hofkens K, et al. Vertical distributions in the Kapachi soil of the plutonium isotopes (238Pu, 239,240Pu, 241Pu), of 241Am, and of 243,244Cm, eight years after the Chernobyl Accident[J]. Journal of Environmental Radioactivity, 1998,39(3):231-237.
[8]
Pittet P, Josset M, Boilley D, et al. Origin and age of an ongoing radioactive contamination of soils near La hague reprocessing plant based on 239+240Pu/238Pu and 241Am/241Pu current ratios and 90Sr and Ln(III) soil contents[J]. Chemosphere, 2021,270.
[9]
Wu J W, Sun J, Xiao X Y. An overview of current knowledge concerning the inventory and sources of plutonium in the China Seas[J]. Marine Pollution Bulletin, 2020,150.
[10]
Huang Y, Tims S G, Froehlich M B, et al. The 240Pu/239Pu atom ratio in Chinese soils[J]. Science of the Total Environment, 2019,678:603-610.
[11]
Dong W, Tims S G, Fifield L K, et al. Concentration and characterization of plutonium in soils of Hubei in central China[J]. Journal of Environmental Radioactivity, 2010,101(1):29-32.
[12]
黄亚楠,潘少明,肖智,等.中国表层土壤中239+240Pu的空间分布与变异性研究[J]. 中国环境科学, 2020,40(6):2554-2564. Huang Y N, Pan S M, Xiao Z, et al. Spatial distribution and variability of 239+240Pu in surface soil of China[J]. China Environmental Science, 2020,40(6):2554-2564.
[13]
黄亚楠,潘少明,张威,等.中国大陆土壤中239+240Pu的来源与背景值研究[J]. 中国环境科学, 2018,38(12):4608-4616. Huang Y N, Pan S M, Zhang W, et al. The source and reference inventory of 239+240Pu in the soil of China[J]. China Environmental Science, 2018,38(12):4608-4616.
[14]
黄亚楠,吴孟孟,肖智.中国西北地区环境中239+240Pu的来源与成因分析[J]. 中国环境科学, 2021,41(11):5334-5344. Huang Y N, Wu M M, Xiao Z. Source of 239+240Pu in the environment of Northwest China and its causes[J]. China Environmental Science, 2021,41(11):5334-5344.
[15]
Xu Y H, Qiao J X, Hou X L, et al. Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements[J]. Talanta, 2014,119:590-595.
[16]
伊小伟,李冬梅,徐江,等.242Pu同位素稀释剂的标定[J]. 核化学与放射化学, 2007,29(4):216-219. Yi X W, Li D M, Xu J, et al. Determination of the specific activity and isotope ratios of 242Pu spike solution[J]. Journal of Nuclear and Radiochemistry, 2007,29(4):216-219.
[17]
伊小伟,李冬梅,党海军,等.UTEVA萃取色层分离超铀元素的性能研究[J]. 核化学与放射化学, 2010,32(1):22-26. Yi X W, Li D M, Dang H J, et al. Separation of transuranium elements with UTEVA extraction chromatography[J]. Journal of Nuclear and Radiochemistry, 2010,32(1):22-26.
[18]
杜丽丽,代义华,张海涛,等.水溶液中Np、Pu、Am和Cm同时电沉积制备α测量源[J]. 核化学与放射化学, 2018,40(3):145-150. Du L L, Dai Y H, Zhang H T, et al. Simutaneous electrodeposition procedure of transuranic elements Np, Pu, Am and Cm for alpha spectrometric measurement[J]. 核化学与放射化学, 2018,40(3):145-150.
[19]
徐江,李志明,施艳梅,等.钚材料4条衰变链的年龄诊断方法研究[J]. 分析化学, 2013,41(11):1675-1680. Xu J, Li Z M, Shi Y M, et al. Study of plutonium age diagnosis method from 4 decay chain[J]. Chinese Journal of Analytical Chemistry, 2013,41(11):1675-1680.
[20]
Dai X X. Isotopic uranium analysis in urine samples by alpha spectrometry[J]. Journal of Radioanalytical and Nuclear Chemistry, 2011,289(2):595-600.
[21]
Aggarwal S K, Chitambar S A, Kavimandan V D, et al. Precision and accuracy in the determination of 238Pu/(239Pu+240Pu) a activity ratio by alpha spectrometry[J]. Radiochimica Acta, 1980,27(1):1-6.
[22]
Moreno J, Vajda N, Danesi P R, et al. Combined procedure for the determination of 90Sr, 241Am and Pu radionuclides in soil samples[J]. Journal of Radioanalytical and Nuclear Chemistry, 1997,226(1/2):279-284.
[23]
Hrnecek E, Jakopic R, Wallner A, et al. A combined method for the determination of the isotopic vector of plutonium isotopes in environmental samples[J]. Journal of Radioanalytical and Nuclear Chemistry, 2008,276(3):789-793.
[24]
Jia G G, Testa C, Desideri D, et al. Sequential separation and determination of plutonium, americium-241and strontium-90 in soils and sediments[J]. Journal of Radioanalytical and Nuclear Chemistry, 1998,230(1/2):21-27.
[25]
Kim C S, Lee M H, Kim C K, et al. 90Sr, 137Cs, 239,240Pu and 238Pu concentrations in surface soils of Korea[J]. Journal of Environmental Radioactivity, 1998,40(1):75-88.
[26]
Holgye Z, Schlesingerova E, Tecl J, et al. 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in soils around nuclear research centre Rez, near Prague[J]. Journal of Environmental Radioactivity, 2004,71(2):115-125.
[27]
Bunzl K, Kracke W. Cumulative deposition of 137Cs, 238Pu, 239+240Pu and 241Am from global fallout in soils from forest, grassland and arable land in Bavaria (FRG)[J]. Journal of Environmental Radioactivity, 1988,8(1):1-14.
[28]
Danesi P R, Bleise A, Burkart W, et al. Isotopic composition and origin of uranium and plutonium in selected soil samples collected in Kosovo[J]. Journal of Environmental Radioactivity, 2003,64(2/3):121-131.
[29]
Belyaev B N, Domkin V D, Ivanova L M, et al. Plutonium contamination level and isotopic composition in soils around St. Petersburg[J]. Radiochemistry, 2001,43(2):203-206.
[30]
Al Hamarneh I, Wreikat A, Toukan K. Radioactivity concentrations of 40K, 134Cs, 137Cs, 90Sr, 241Am, 238Pu and 239+240Pu radionuclides in Jordanian soil samples[J]. Journal of Environmental Radioactivity, 2003,67(1):53-67.
[31]
Figueira R C L, Tessler M G, de Mahiques M M, et al. Distribution of 137Cs, 238Pu and 239+240Pu in sediments of the southeastern Brazilian shelf-SW Atlantic margin[J]. Science of the Total Environment, 2006,357(1):146-159.
[32]
Bouisset P, Nohl M, Bouville A, et al. Inventory and vertical distribution of 137Cs, 239+240Pu and 238Pu in soil from Raivavae and Hiva Oa, two French Polynesian islands in the southern hemisphere[J]. Journal of Environmental Radioactivity, 2018,183:82-93.
[33]
Roos P, Holm E, Persson R B R, et al. Deposition of 210Pb, 137Cs, 239+240Pu, 238Pu, and 241Am in the Antarctic Peninsula area[J]. Journal of Environmental Radioactivity, 1994,24(3):235-251.
[34]
Yamamoto M, Hoshi M, Takada J, et al. Distributions of Pu isotopes and 137Cs in soil from Semipalatinsk Nuclear Test Site detonations throughout southern districts[J]. Journal of Radioanalytical and Nuclear Chemistry, 2004,261(1):19-36.
[35]
Komosa A. Study on plutonium isotopes determination in soils from the region of Lublin (Poland)[J]. Science of the Total Environment, 1996,188(1):59-62.
