Actinides in the near release from the Chernobyl NPP accident

Actinide elements concentrations in the products of near release from CNPP accident were estimated. The data on uranium,²³⁷Np,²⁴¹Am and plutonium and curium isotopes content in fuel particles are given. Sums of -emitting radionuclides and plutonium isotopes in reactor graphite particles and of uranium,²⁴²Cm,^239+240Pu isotopes in the soil and aerosol samples were also determined. By 1989 soil and dust contamination in near release of the accident is due to long-lived -emitting plutonium isotopes.     

Rapid column extraction method for actinides and 89/90Sr in water samples

Summary The SRS Environmental Laboratory analyzes water samples for environmental monitoring, including river water and ground water samples. A new, faster actinide and ^89/90Sr separation method has been developed and implemented to improve productivity, reduce labor costs and add capacity to this laboratory.This method uses stacked TEVA Resin^ò, TRU Resin^òand Sr-Resin^òcartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium, neptunium, uranium, americium, curium and thorium using a single multi-stage column combined with alpha-spectrometry. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized. The method can be used for routine analysis or as a rapid method for emergency preparedness. Thorium and curium are often analyzed separately due to the interference of the daughter of ²²⁹Th tracer, actinium (²²⁵Ac) on curium isotopes when measured by alpha-spectrometry. This new method also adds a separation step using DGA Resin^ò, (diglycolamide resin, Eichrom Technologies) to remove ²²⁵Ac and allow the separation and analysis of thorium isotopes and curium isotopes at the same time.     

Some data on transuranium element distribution in particle size fractions of Chernobyl soils

Some Chernobyl soils were collected in the north-west direction. The samples have been separated into particle size fractions 1–2; 0.5–1; 0.25–0.5; 0.16–0.25; 0.05–0.16; 0.01–0.05; 0.005–0.01; 0.002–0.005; 0.00005–0.002; and less than 0.00005 mm. The fractions were analyzed on^238,239,240Pu,²⁴¹Am,^242,244Cm content. In contrast to the global plutonium fallout, the peak of plutonium activity falls in the particle size range of 0.01–0.05 or 0.005–0.01 mm in Chernobyl soils. Transplutonium elements are more mobile in the soil. As the distance from Chernobyl increases, the trend of their distribution becomes much similar to the global fallout. It is found that the most mobile part of soil with particles of sizes less than 0.05 mm contains 55–70% of plutonium activity and 30–65% of americium and curium activity.     

Electromigration method for destructive determination of spent nuclear fuel burnup

In this report we discuss the methods and results of VVER spent fuel burnup determination by¹⁴⁶Nd content and the correlation with accumulation of some transplutonium nuclides. For separation of trivalent rare earths and transplutonium elements the method of paper electrophoresis is used. For the quantitative determination of americum and curium isotopes a modification of α-spectrometric analysis is proposed with the chemical yield control of isolated elements using²⁴⁴Cm. The amount of¹⁴³Nd is determined by the isotopic dilution method combined with mass spectrometry with¹⁴²Nd as a tracer.     

Simultaneous determination of238Pu,239+240Pu,241Pu,241Am,242Cm,244Cm,89Sr,and90Sr in vegetation samples,and application to Chernobyl-fallout contaminated grass

A radiochemical procedure is described for the simultaneous determination of²³⁸Pu,^239+240Pu,²⁴¹Pu,²⁴¹Am,²⁴²Cm,²⁴⁴Cm,⁸⁹Sr, and⁹⁰Sr in vegetation samples. The method was applied for the determination of these, radionuclides in grass, collected near Munich after the fallout from the reactor accident at Chernobyl, USSR. The specific activities observed were (in Bq kg^–1 dry weight):²³⁸Pu, 0.077;^239+240Pu, 0.15;²⁴¹Pu, 3.9;²⁴¹Am, 0.031;²⁴²Cm, 3.0;²⁴⁴Cm, 0.008;⁸⁹Sr, 2000;⁹⁰Sr, 99.     

Regional distribution of Chernobyl-derived plutonium deposition in Finland

The Chernobyl nuclear power plant accident in April 1986 caused a widely spread plume of radionuclides containing, amongst other materials, plutonium isotopes. The regional deposition of these nuclides in Finland has been assessed, based on samples of lichen, peat, precipitation, surface soil and grass. Unlike the deposition of transuranium elements from the weapons tests in the 1950"s and the 1960"s, the deposition in Finland from the Chernobyl accident was very unevenly distributed. Even then, the Chernobyl-derived deposition of ^239,240Pu in the most contaminated regions of Finland was only around 10% of the global fallout from weapons tests. The total amount of ^239,240Pu deposited in Finland was 1^.10¹¹ Bq (»25 g), i.e., approximately half of a percent of the activity deposited in the 1950"s and the 1960"s. In addition to the alpha-emitting Pu isotopes, the Chernobyl plume also contained a significant amount of the beta-emitting ²⁴¹Pu, which is the precursor of the long-lived alpha-emitter ²⁴¹Am. The highest plutonium deposition values were found in a relatively narrow swath from the southwestern coast of Finland northeastwards across the country. This is related to the calculated route of the air parcel trajectory associated with the initial explosion of the Chernobyl reactor. The high deposition values found in the northeastern part of the plume route over Finland can be attributed to the simultaneous occurrence of precipitation. The relatively high plutonium deposition in the southwestern part of Finland occurred, however, without concurrent precipitation. This indicates that the plutonium was at least partly associated with relatively large particles having a substantial deposition velocity due to gravitational setting     

Use of alcoholic solutions for the isolation and purification of americium and curium with anion-exchangers

The sorption of transplutonium (TPE), rare-earth (RE) and other elements by anion-exchangers (Dowex 1 type) from aqueous alcoholic solutions of nitric acid and ammonium thiocyanate was investigated. This investigation allowed the development of simple and effective methods of americium—curium separation from frradiated plutonium. Plutonium, TPE (in a +3 oxidation state) and RE are firmly sorbed by the anion-exchanger from 1 M HNO₃ in 90% alcohol, Fe, Al and fission products Cs, Sr, Nb, Zr, and Ru pass through the column under these conditions. The RE separation from TPE is achieved by washing the column with 0.5M NH₄SCN in 80% alcohol. The column is then washed with 0.5 M HNO₃ in 85% alcohol, and americium—curium separation proceeds. Use of this method for recovery of an irradiated plutonium target containing 100 mg Pu, Am and Cm is described.     

Determination of plutonium,americium and curium in airborne effluents of nuclear power plants

A radiochemical method has been developed for the determination of²³⁸Pu,^{239, 240}Pu,²⁴¹Am,²⁴²Cm and²⁴⁴Cm in airborne effluents of nuclear power plants. The method involves conversion of transuranium elements to acid-soluble forms, dissolution, purification, electrodeposition and alpha spectrometric determination. Final recovery ranged from 69.0 to 75.4% for plutonium and from 26.8 to 68.3% for americium and curium.     

Plutonium and cesium isotopes in river waters in Japan

Concentrations of cesium isotopes and plutonium in river water samples in Japan, collected during the period from June 1985 to February 1987, have been measured. The total¹³⁷Cs concentrations in the Japanese river waters ranged from 0.063 to 1.89 mBq·l^–1. The portion of particulate¹³⁷Cs to total was observed to be less than 10 to 35%. The total^239,240Pu concentrations ranged from 0.56 to 1.93 Bq·l^–1. Particulate^239,240Pu occupied 13 to 95% of the total. After the Chernobyl fallout, elevated¹³⁷Cs concentrations were observed in the Japanese river waters as well as the detection of¹³⁴Cs, whereas there was no effect on the river plutonium from the Chernobyl fallout. The partition coefficients of¹³⁷Cs and plutonium between suspended particulate and dissolved phases in the Japanese rivers were determined: from 1.0·10⁴ to 3.2·10⁵ and from 4.1·10⁴ to 2.3·10⁶ for¹³⁷Cs and plutonium, respectively. The result suggests that these radionuclides, especially plutonium, are tightly associated with soil particles and/or suspended matter.     

Radionuclides in macro algae at Monaco following the Chernobyl accident

Samples of macro algae,Codium tomentosum (green),Corallina mediterranea (red),Sphaerococcus coronopifolius (red) andDictyota dichtoma (brown), were collected off Monaco during 1984 and 1988 and analyzed for gamma-emitting radionuclides and transuranium elements. Due to the Chernobyl accident, increased radioactivity in the atmosphere at Monaco was recorded on 30 April 1986 with maximal activity concentrations on 2–3 May. The maximal activity concentrations in sea water occurred on 5–6 May and in the algae on 11 May. The decrease of activity concentrations can be described after May 11 as a single exponential relationship, where elimination rates for different radionuclides and different species specific to the environment can be calculated.The elimination rates thus observed correspond to mean residence times between 70 and 370 days corrected for physical decay. The concentration factors were also estimated and the highest values were found for¹³¹I,¹²⁹Te^m, and 110 Ag^m and lowest for radiocaesium and¹⁴⁰Ba. The red algaeSphaerococcus coronopifolius showed generally higher concentration factors than green and brown algae.Regarding transuranium elements, a theoretical contribution from the Chernobyl accident can be made but only²⁴²Cm was detected in the algae above previous levels before the accident, due to the relatively small fallout of transuranics.     

Rapid column extraction method for actinides in soil

Summary The determination of actinides in environmental soil and sediment samples is very important for environmental monitoring as well as for emergency preparedness. A new, rapid actinide separation method has been developed and implemented that provides total dissolution of large soil samples, high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin^ò, TRU Resin^ò and DGA-Resin^ò cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium, neptunium, uranium, americium, and curium using a single multi-stage column combined with alpha-spectrometry. The method combines a rapid fusion step for total dissolution to dissolve refractory analytes and matrix removal using cerium fluoride precipitation to remove the difficult soil matrix. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.     

Intermetallics and alloys of transplutonium elements with metals of the platinum group

Americium and curium alloys with palladium and platinum containing up to 20% of actinide were prepared by the coupled reduction technique. The alloys obtained were investigated by X-ray, differential thermal analysis and metallography. Phase diagram sections for Pd–Am, Pd–Cm, Pt–Am and Pt–Cm systems have been constructed. Intermetallics Pt₅An (An=²⁴³Am,²⁴⁴Cm,²⁴⁹Bk,²⁴⁹Cf), Ir₂ ²⁴⁹Bk and Rh₃ ²³⁹Bk were obtained as thin layers on the surfaces of metallic substrates. X-ray investigation has shown that Pt₅An compounds have hexagonal structures of the Cu₅Ca-type, Ir₂Bk- cubic lattice of the Cu₂Mg-type and Rh₃Bk intermetallic has fcc lattice of the Cu₃Au-type. The influence of intensive -decay of transplutonium nuclides on the crystal structure of the intermetallics prepared has been investigated.     

ICP-MS analysis of plutonium activities and <Superscript>240</Superscript>Pu/<Superscript>239</Superscript>Pu ratio in alpha spectrometry planchet deposits

Plutonium isotopes were measured by alpha-spectrometry and ICP-MS in sediment samples from two European lakes: Blelham Tarn in U.K. and Stechlin lake in Germany. The ICP-MS measurements were made after alpha-spectrometry counting of the planchets. The planchets were prepared by traditional electrodeposition method after radiochemical extraction, separation and purification of the Pu fraction. A short radiochemical separation using plutonium selective resin, between the two spectrometry measures, is presented. The results show that these two complementary methods are in good agreement, the plutonium activity concentrations are the same. Alpha-spectrometry allows the ²³⁸Pu determination and ICP-MS individual measurement of ²³⁹Pu and ²⁴⁰Pu. ²³⁸Pu/^239+240Pu and ²⁴⁰Pu/²³⁹Pu ratios are calculated to determine the plutonium contamination source. With the results of these two techniques, it could be demonstrate that the plutonium is of global fallout origin.     

Plutonium isotopes in the surface air at Vinča-Belgrade site in May 1986

Surface air concentrations of plutonium isotopes at the Vinca-Belgrade site for the period May 1–15, 1986, are reported. The increase in²³⁸Pu/^239,240Pu ratios confirms that the source of plutonium in surface air was the Chernobyl accident.     

Estimation of244Cm intake by bioassay measurements following a contamination incident

An employee was contaminated with radioactive material consisting primarily of²⁴⁴Cm and²⁴⁶Cm as a consequence of handling a curium nitrate solution at a reprocessing facility.In vivo gamma analysis andin vitro (urine and fecal) analysis were initiated soon after the incident. Furtherin vivo measurements were performed regularly through hour 528, andin vitro bioassay measurements were obtained through day 74. A sample of the curium solution from the workplace was obtained to confirm that the nitrate was the chemical form in question and to identify the isotopes of curium present. The mass ratio of²⁴⁴Cm/²⁴⁶Cm was determined to be 91 to 7. Diethylenetriaminepentaacetate (DTPA) was administered on hours 33 and 71. Observed excretion rates were consistent with available information on curium. In this paper, the results of thein vivo andin vitro measurements are presented and intake estimates for the incident are developed using various excretion rate functions.     

Radiochemical determination of the yields of transuranium nuclides produced from natural uranium irradiated in a reactor

Transuranium nuclides were produced by irradiating a pellet of natural uranium sulfide in the Japan Material Testing Reactor (JMTR). After irradiation, a successive separation of uranium, plutonium, americium and curium was carried out. The fractional concentrations of the nuclides²³⁸Pu,²³⁹Pu,²⁴⁰Pu,²⁴¹Am,²⁴³Am,²⁴²Cm and²⁴⁴Cm were determined by α-ray spectrometry, and those of²⁴¹Pu and^242mAm were estimated from the build-up of α-emitting daughters,²⁴¹Am and²⁴²Cm, respectively. As the yield of²⁴²Pu was too slight to be detected by α-counting, the neutron activation analysis of the plutonium fraction based on the²⁴²Pu(n, γ)²⁴³Pu reaction was carried out by γ-ray spectrometry, and it was shown that a few pg of²⁴²Pu could be determined. A burn-up of²³⁵U was also estimated by neutron activation analysis. The experimental results are compared with the calculated ones.     

Determination of the plutonium concentration by isotope dilution mass spectrometry using239Pu as a spike

A method is described for the determination of plutonium concentration in the presence of a bulk of other impurities by isotope dilution mass spectrometry /IDMS/ using²³⁹Pu as a spike. The method involves the addition of²³⁹Pu spike / 90 atom%/ to samples with²³⁹Pu / 70 atom%/ and vice versa. After ensuring chemical exchange between the sample and the spike isotopes, plutonium is purified by conventional anion exchange procedure in 7M HNO₃ medium.²³⁹Pu/²⁴⁰Pu atom ratio in the purified spiked sample is determined with high precision /better than 0.1%/ using a thermal ionization mass spectrometer. Concentration of plutonium in the sample is calculated from the changes in²³⁹Pu/²⁴⁰Pu atom ratio in the spiked mixture. Results obtained on different plutonium samples using²³⁹Pu as a spike are compared with those obtained by the use of²⁴²Pu spike. Precision and accuracy comparable to those achieved by using²⁴²Pu are demonstrated. The method provides an alternative in the event of non-availability of enriched²⁴²Pu or²⁴⁴Pu required in IDMS of plutonium and at the same time, offers certain advantages over the use of²⁴²Pu or²⁴⁴Pu spike.     

Fallout of transuranium elements following the Chernobyl accident

The deposition of transuranium elements in Sweden following the Chernobyl accident was investigated through the analysis of carpets of lichen-and moss-samples and also air-filters and precipitation. The impact of transuranium elements was small compared to that of radiocesium. The deposition of^239+240Pu was, as for other actinides, inhomogeneously distributed and ranged from 0.1% to 100% of the inventory in 1986 from nuclear detonation tests. The activity ratio of^239+240Pu/¹³⁷Cs was between 10^–3 and 10^–6 in comparison to 10^–2 for nuclear test fallout. The activity ratios of²⁴¹Pu,²⁴²Cm,²³⁸Pu,^243+244Am and^239+240Pu were about 86, 14, 0.47, 0.14, and 0.13 respectively, but large variations were observed. The results from Sweden were compared with those found in South Finland, Denmark and Southern Europe. The deposition over Scandinavia originated from the initial explosion at Chernobyl, which contained relatively higher amounts of actinide elements than the second emission, which occurred a few days later and was a result of actions taken to bring the fire under control.     

Plutonium isotopes in the surface air in Japan: Effect of Chernobyl accident

Plutonium isotope concentrations in the surface air at Tsukuba, Japan are reported during the period from 1981 to the end of 1986. The^239,240Pu concentration in the surface air, which showed a marked seasonal variation with a spring maximum and fall minimum, decreased until the end of 1985 according to the stratospheric residence time of 1.15 years. In May 1986, elevated^239,240Pu concentrations with high²³⁸Pu/^239,240Pu activity ratios were observed. The serial trend of plutonium concentration in the surface air is similar to the concentrations of the Chernobyl-released radionuclides. These findings suggest that a significant part of the plutonium in the surface air in May 1986 was due to the Chernobyl fallout. The size distribution of plutonium bearing particles indicates that plutonium isotopes were mechanically released in the Chernobyl accident. The surface air concentration of plutonium from the Chernobyl accident was much lower than the concentrations of the volatile fission products, and increased the monthly mean^239,240Pu concentration by only 0.03 Bqm^–3.