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1.
A new method has been developed at the Savannah River National Laboratory (SRNL) that can be used for the rapid determination of 226Ra in emergency urine samples following a radiological incident. If a radiological dispersive device event or a nuclear accident occurs, there will be an urgent need for rapid analyses of radionuclides in urine samples to ensure the safety of the public. Large numbers of urine samples will have to be analyzed very quickly. This new SRNL method was applied to 100 mL urine aliquots, however this method can be applied to smaller or larger sample aliquots as needed. The method was optimized for rapid turnaround times; urine samples may be prepared for counting in <3 h. A rapid calcium phosphate precipitation method was used to pre-concentrate 226Ra from the urine sample matrix, followed by removal of calcium by cation exchange separation. A stacked elution method using DGA Resin was used to purify the 226Ra during the cation exchange elution step. This approach combines the cation resin elution step with the simultaneous purification of 226Ra with DGA Resin, saving time. 133Ba was used instead of 225Ra as tracer to allow immediate counting; however, 225Ra can still be used as an option. The rapid purification of 226Ra to remove interferences using DGA Resin was compared with a slightly longer Ln Resin approach. A final barium sulfate micro-precipitation step was used with isopropanol present to reduce solubility; producing alpha spectrometry sources with peaks typically <40 keV FWHM (full width half max). This new rapid method is fast, has very high tracer yield (>90 %), and removes interferences effectively. The sample preparation method can also be adapted to ICP-MS measurement of 226Ra, with rapid removal of isobaric interferences.  相似文献   

2.
Summary The measurement of radium isotopes in natural waters is important for oceanographic studies and for public health reasons. Radium-226 (T1/2 = 1620 y) is one of the most toxic of the long-lived alpha-emitters present in the environment due to its long life and its tendency to concentrate in bones, which increases the internal radiation dose of individuals. The analysis of 226Ra and 228Ra in natural waters can be tedious and time-consuming. Different sample preparation methods are often required to prepare 226Ra and 228Ra for separate analyses. A rapid method has been developed at the Savannah River Environmental Laboratory that effectively separates both 226Ra and 228Ra (via 228Ac) for assay. This method uses MnO2 Resin from Eichrom Technologies (Darien, IL, USA) to preconcentrate 226Ra and 228Ra rapidly from water samples, along with 133Ba tracer. DGA Resinò (Eichrom) and Ln-Resinò (Eichrom) are employed in tandem to prepare 226Ra for assay by alpha-spectrometry and to determine 228Ra via the measurement of 228Ac by gas proportional counting. After preconcentration, the manganese dioxide is dissolved from the resin and passed through stacked Ln-Resin-DGA Resin cartridges that remove uranium and thorium interferences and retain 228Ac on DGA Resin. The eluate that passed through this column is evaporated, redissolved in a lower acidity and passed through Ln-Resin again to further remove interferences before performing a barium sulfate microprecipitation. The 228Ac is stripped from the resin, collected using cerium fluoride microprecipitation and counted by gas proportional counting. By using vacuum box cartridge technology with rapid flow rates, sample preparation time is minimized.  相似文献   

3.
A new method for the determination of radiostrontium in seawater samples has been developed at the Savannah River National Laboratory (SRNL) that allows rapid pre-concentration and separation of strontium and yttrium isotopes in seawater samples for measurement. The new SRNL method employs a novel and effective pre-concentration step that utilizes a blend of calcium phosphate with iron hydroxide to collect both strontium and yttrium rapidly from the seawater matrix with enhanced chemical yields. The pre-concentration steps, in combination with rapid Sr Resin and DGA Resin cartridge separation options using vacuum box technology, allow seawater samples up to 10 L to be analyzed. The total 89Sr + 90Sr activity may be determined by gas flow proportional counting and recounted after ingrowth of 90Y to differentiate 89Sr from 90Sr. Gas flow proportional counting provides a lower method detection limit than liquid scintillation or Cerenkov counting and allows simultaneous counting of samples. Simultaneous counting allows for longer count times and lower method detection limits without handling very large aliquots of seawater. Seawater samples up to 6 L may be analyzed using Sr Resin for 89Sr and 90Sr with a minimum detectable activity (MDA) of 1–10 mBq/L, depending on count times. Seawater samples up to 10 L may be analyzed for 90Sr using a DGA Resin method via collection and purification of 90Y only. If 89Sr and other fission products are present, then 91Y (beta energy 1.55 MeV, 58.5 day half-life) is also likely to be present. 91Y interferes with attempts to collect 90Y directly from the seawater sample without initial purification of Sr isotopes first and 90Y ingrowth. The DGA Resin option can be used to determine 90Sr, and if 91Y is also present, an ingrowth option with using DGA Resin again to collect 90Y can be performed. An MDA for 90Sr of <1 mBq/L for an 8 h count may be obtained using 10 L seawater sample aliquots.  相似文献   

4.
A new rapid method for the determination of 210Po in water samples has been developed at the Savannah River National Laboratory (SRNL) that can be used for emergency response or routine water analyses. If a radiological dispersive device event or a radiological attack associated with drinking water supplies occurs, there will be an urgent need for rapid analyses of water samples, including drinking water, ground water and other water effluents. Current analytical methods for the assay of 210Po in water samples have typically involved spontaneous auto-deposition of 210Po onto silver or other metal disks followed by counting by alpha spectrometry. The auto-deposition times range from 90 min to 24 h or more, at times with yields that may be less than desirable. If sample interferences are present, decreased yields and degraded alpha spectrums can occur due to unpredictable thickening in the deposited layer. Separation methods have focused on the use of Sr Resin?, often in combination with 210Pb analysis. A new rapid method for 210Po in water samples has been developed at the SRNL that utilizes a rapid calcium phosphate co-precipitation method, separation using DGA Resin® (N,N,N′,N′ tetraoctyldiglycolamide extractant-coated resin, Eichrom Technologies or Triskem-International), followed by rapid microprecipitation of 210Po using bismuth phosphate for counting by alpha spectrometry. This new method can be performed quickly with excellent removal of interferences, high chemical yields and very good alpha peak resolution, eliminating any potential problems with the alpha source preparation for emergency or routine samples. A rapid sequential separation method to separate 210Po and actinide isotopes was also developed. This new approach, rapid separation with DGA resin plus microprecipitation for alpha source preparation, is a significant advance in radiochemistry for the rapid determination of 210Po.  相似文献   

5.
A new rapid fusion method for the determination of plutonium in large rice samples has been developed at the Savannah River National Laboratory (Aiken, SC, USA) that can be used to determine very low levels of plutonium isotopes in rice. The recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid, reliable radiochemical analyses for radionuclides in environmental and food samples. Public concern regarding foods, particularly foods such as rice in Japan, highlights the need for analytical techniques that will allow very large sample aliquots of rice to be used for analysis so that very low levels of plutonium isotopes may be detected. The new method to determine plutonium isotopes in large rice samples utilizes a furnace ashing step, a rapid sodium hydroxide fusion method, a lanthanum fluoride matrix removal step, and a column separation process with TEVA Resin? cartridges. The method can be applied to rice sample aliquots as large as 5 kg. Plutonium isotopes can be determined using alpha spectrometry or inductively-coupled plasma mass spectrometry (ICP-MS). The method showed high chemical recoveries and effective removal of interferences. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory plutonium particles are effectively digested. The MDA for a 5 kg rice sample using alpha spectrometry is 7 × 10?5 mBq g?1. The method can easily be adapted for use by ICP-MS to allow detection of plutonium isotopic ratios.  相似文献   

6.
A new approach for quantifying radium isotopes in seawater was developed in advance of the international GEOTRACES program, which has the goal of identifying processes and quantifying fluxes that control the distribution of trace elements and isotopes (TEIs) in the ocean. High-resolution water column samples were collected via a commercially available in situ pump modified to accept multiple filter media including a manganese-oxide (MnO2) impregnated acrylic cartridge for extracting dissolved radionuclides from seawater. The modifications mitigated prefilter clogging and allowed for up to 1,800 L filtrations in 4 h of pumping. Different MnO2 cartridge preparation methods were investigated to achieve maximum radium (Ra) extraction efficiency under high sample flow rates. Full-ocean depth profiles were measured for short-lived radium isotopes (223Ra and 224Ra) in shipboard laboratories using a delayed coincidence alpha scintillation counter (RaDeCC). Samples were reanalyzed 4 weeks and 2 months after collection for 228Th and 227Ac to correct for supported 224Ra and 223Ra, respectively. Finally, the cartridges were measured on a gamma-ray spectrometer for the long-lived radium isotopes (226Ra and 228Ra). Parallel 20 L samples at each pumping depth were collected from Niskin bottles and analyzed via alpha scintillation for 226Ra to determine radium extraction efficiencies for the cartridges. These modified methods will allow for increased sample throughput, and hence higher spatial resolution for radium isotopes in the ocean. Such resolution will greatly improve the determination of oceanic vertical and horizontal mixing rates over small and large scales, which in turn can be used to calculate fluxes of TEIs into the ocean.  相似文献   

7.
A new rapid method for the determination of actinides in seawater samples has been developed at the Savannah River National Laboratory. The actinides can be measured by alpha spectrometry or inductively-coupled plasma mass spectrometry. The new method employs novel pre-concentration steps to collect the actinide isotopes quickly from 80 L or more of seawater. Actinides are co-precipitated using an iron hydroxide co-precipitation step enhanced with Ti+3 reductant, followed by lanthanum fluoride co-precipitation. Stacked TEVA Resin and TRU Resin cartridges are used to rapidly separate Pu, U, and Np isotopes from seawater samples. TEVA Resin and DGA Resin were used to separate and measure Pu, Am and Cm isotopes in seawater volumes up to 80 L. This robust method is ideal for emergency seawater samples following a radiological incident. It can also be used, however, for the routine analysis of seawater samples for oceanographic studies to enhance efficiency and productivity. In contrast, many current methods to determine actinides in seawater can take 1–2 weeks and provide chemical yields of ~30–60 %. This new sample preparation method can be performed in 4–8 h with tracer yields of ~85–95 %. By employing a rapid, robust sample preparation method with high chemical yields, less seawater is needed to achieve lower or comparable detection limits for actinide isotopes with less time and effort.  相似文献   

8.
An investigation on the distribution of 226Ra and 228Ra activity concentration in coastal surface sea water from Okha in Gujarat to Ratnagiri in Maharashtra state along the west coast of India was carried out. In-situ pre-concentration technique was used to measure radium isotopes by passing 1,000 L of seawater through MnO2 impregnated polypropylene filter cartridges at all the locations. 226Ra was estimated using gamma ray peak of its daughter radionuclides 214Bi and 214Pb. 228Ra was estimated from its daughter 228Ac. In the coastal waters, 226Ra and 228Ra activity concentration were observed to be in the range of 1.5–2.9 and 2.5–8.6 Bq m?3 with a mean of 2.2 and 4.9 Bq m?3 respectively. The activity of 228Ra was observed to be more than 226Ra in all the locations. The variation in spatial distribution of the radium isotopes activity concentration and its ratio with respect to location is discussed in the paper. The radioactive database obtained represents reference values for coastal environment of India.  相似文献   

9.
A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of 237Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry. 238U can interfere with 239Pu measurement by ICP-MS as 238UH+ mass overlap and 237Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4?C6 h, and can also be used for emergency response. 239Pu, 242Pu and 237Np were measured by ICP-MS, while 236Pu, 238Pu, and 239Pu were measured by alpha spectrometry.  相似文献   

10.
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 Resinò, TRU Resinòand Sr-Resinòcartridges 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 Resinò, (diglycolamide resin, Eichrom Technologies) to remove 225Ac and allow the separation and analysis of thorium isotopes and curium isotopes at the same time.  相似文献   

11.
A new rapid method for the determination of actinides in asphalt samples has been developed that can be used in emergency response situations or for routine analysis. If a radiological dispersive device, improvised nuclear device or a nuclear accident such as the accident at the Fukushima Nuclear Power Plant in March, 2011 occurs, there will be an urgent need for rapid analyses of many different environmental matrices, including asphalt materials, to support dose mitigation and environmental clean-up. The new method for the determination of actinides in asphalt utilizes a rapid furnace step to destroy bitumen and organics present in the asphalt and sodium hydroxide fusion to digest the remaining sample. Sample preconcentration steps are used to collect the actinides and a new stacked TRU Resin + DGA Resin column method is employed to separate the actinide isotopes in the asphalt samples. The TRU Resin plus DGA Resin separation approach, which allows sequential separation of plutonium, uranium, americium and curium isotopes in asphalt samples, can be applied to soil samples as well.  相似文献   

12.
234U, 238U, 226Ra, and 228Ra were analyzed in 14 Korean hot spring waters. Uranium was extracted with mixture of extractive scintillation cocktail containing HDEHP and 234U, 238U were analyzed with LSC. Radium isotopes were separated using Ba coprecipitation method and counted with LSC and 228Ra was also analyzed its daughter 228Ac with HPGe γ-detector. Among them 226Ra was ranged <0.01–0.155 Bq/L and 228Ra is below detection limit <0.1 Bq/L. And also, uranium content was ranged <0.01–49.7 μg/L and 234U/238U ratio was ranged 0.69–1.17.  相似文献   

13.
The concentrations of radium isotopes and the progenies (226Ra; 228Ra and 228Th) in three hokutolite samples from Tamagawa hot-spring were measured. These isotopes were analyzed by a well-type HPGe γ-ray spectrometer for the 351, 911 and 583 keV γ-ray from 214Pb, 228Ac and 208Tl, respectively, each being in radioactive equilibrium with precursors. Concentration of 226Ra and 228Ra were observed to be in the range of 52–85 and 7.1–85 Bq/g, respectively. The activity ratios of 228Ra/226Ra and 228Th/226Ra provided the estimation of the growth rate (0.09–0.15 mm/y). Estimated 228Ra/226Ra activity ratios in hot-spring water from surface of three hokutolite were concordant.  相似文献   

14.
A new rapid method for the determination of 226Ra in environmental samples has been developed at the Savannah River Site Environmental Lab (Aiken, SC, USA) that can be used for emergency response or routine sample analyses. The need for rapid analyses in the event of a Radiological Dispersive Device or Improvised Nuclear Device event is well-known. In addition, the recent accident at Fukushima Nuclear Power Plant in March, 2011 reinforces the need to have rapid analyses for radionuclides in environmental samples in the event of a nuclear accident. 226Ra (T1/2?=?1,620?years) is one of the most toxic of the long-lived alpha-emitters present in the environment due to its long life and its tendency to concentrate in bones, which increases the internal radiation dose of individuals. The new method to determine 226Ra in environmental samples utilizes a rapid sodium hydroxide fusion method for solid samples, calcium carbonate precipitation to preconcentrate Ra, and rapid column separation steps to remove interferences. The column separation process uses cation exchange resin to remove large amounts of calcium, Sr Resin to remove barium and Ln Resin as a final purification step to remove 225Ac and potential interferences. The purified 226Ra sample test sources are prepared using barium sulfate microprecipitation in the presence of isopropanol for counting by alpha spectrometry. The method showed good chemical recoveries and effective removal of interferences. The determination of 226Ra in environmental samples can be performed in less than 16?h for vegetation, concrete, brick, soil, and air filter samples with excellent quality for emergency or routine analyses. The sample preparation work takes less than 6?h. 225Ra (T1/2?=?14.9?day) tracer is used and the 225Ra progeny 217At is used to determine chemical yield via alpha spectrometry. The rapid fusion technique is a rugged sample digestion method that ensures that any refractory radium particles are effectively digested. The preconcentration and column separation steps can also be applied to aqueous samples with good results.  相似文献   

15.
We developed a new method for the determination of 227Ac in geological samples. The method uses extraction chromatographic techniques and alpha-spectrometry and is applicable for a range of natural matrices. Here we report on the procedure and results of the analysis of water (fresh and seawater) and rock samples. Water samples were acidified and rock samples underwent total dissolution via acid leaching. A DGA (N,N,N′,N′-tetra-n-octyldiglycolamide) extraction chromatographic column was used for the separation of actinium. The actinium fraction was prepared for alpha spectrometric measurement via cerium fluoride micro-precipitation. Recoveries of actinium in water samples were 80 ± 8 % (number of analyses n = 14) and in rock samples 70 ± 12 % (n = 30). The minimum detectable activities (MDA) were 0.017–0.5 Bq kg?1 for both matrices. Rock sample 227Ac activities ranged from 0.17 to 8.3 Bq kg?1 and water sample activities ranged from below MDA values to 14 Bq kg?1of 227Ac. From the analysis of several standard rock and water samples with the method we found very good agreement between our results and certified values.  相似文献   

16.
An isotopic dilution method has been developed for the determination of 226Ra and 228Ra in sea water and sediments with 223Ra as a yield tracer. An alternative procedure which obviates the need for 223Ra is demonstrated for sediments by the assay of 224Ra and 228Th which occur naturally in sediments. In addition, a direct method for β-counting 228Ra–228Ac is proposed. Radium, polonium, thorium and uranium isotopes and 210Pb are coprecipitated from sea water with aluminum phosphate carrier. The radium and lead-210 are coprecipitated with lead nitrate in sediment leachings. All radium procedures utilize identical chemical isolation and the cathodic electrodeposition of radium. Subsequently, the α-radiation emitted by 226Ra, 223Ra and 224Ra is determined by pulse-height analysis: the 228Ra-228Ac and 210Pb-210Bi are measured by low background anticoincidence β-counting techniques. This method was used for samples containing 10-11–0.5 · 10-12 g of 226Ra and 10-13–10-15 g of 228Ra and gave a precision of 3–6% and 5–10% respectively, even though radium levels an order of magnitude less can be measured. The 226Ra method is applicable to all environmental samples, whereas 228Ra determinations are limited to applications where the 228Ra226Ra activity ratio is greater than 0.1. This method is especially attractive for studies of parent-daughter disequilibria.  相似文献   

17.
To facilitate the use of225Ra as a yield tracer in radiochemical assays of226Ra and228Ra, growth and decay tables for225Ra, and its daughter225Ac, have been computed.  相似文献   

18.
A procedure for the analysis of228Ra in drinking water has been developed. The procedure involves separation of radium by an initial coprecipitation with lead sulfate. The isolated Pb(Ra)SO4 is then dissolved in sodium diethylenetriamine pentaacetate (DTPA). Radium-228 is co-precipitated from this solution with barium sulfate while the DTPA supernate which contains pre-existing228Ac is discarded. The purified Ba(Ra)SO4 precipitate is then allowed to ingrow, generating228Ac, which is then dissolved in DTPA, isolating both226Ra and228Ra in the precipitate while228 Ac remains in the aqueous supernate. The supernate is partitioned against di-(2-ethylhexyl phosphoric acid), HDEHP, dissolved in n-heptane, which retains the228Ac. Actinium-228 is then stripped from the organic phase by partitioning against 1M HNO3. Finally, the228Ac is coprecipitated onto cerium oxalate. The precipitate is collected on a filter and counted in a low-background beta counter. Radium-228 standards with concentrations ranging from 0.044 to 1.6 Bq were used to establish the detector counting efficiency for228Ac in cerium oxalate samples, as well as monitoring the chemical yield and absorption factors. The resultant average value of 30.3±2.1 cpm/Bq (uncertainty given at 95% level of confidence) was obtained. Various228Ra cross checks from U. S. Environmental Protection Agency (EPA) with concentrations of 0.063–0.52 Bq/l were analyzed in order to assess the performance of the procedure. The minimum detectable concentration (MDC) of228Ra in water with this procedure is 0.015 Bq/l. This is based on a one liter aliquot of sample, a 100 min couting period, and a 3 hour decay interval between the end of228Ac ingrowth and midpoint of counting. Decontamination factor studies were performed to determine the extent of the carry-over of238U,226Ra,210Po, and90Sr into the final fraction.  相似文献   

19.
This research was dedicated to the study of the background levels of 210Po and natural gamma emitters as 40K, 214Pb, 214Bi, 228Ac, 212Pb and 212Bi in coffee powder and in coffee beverage; also the artificial 137Cs was determined. In the coffee powder the mean 210Po activity resulted 7.25 ± 2.25 × 10?2 Bq kg?1. 40K showed a mean activity of 907.4 ± 115.6 Bq kg?1. The mean activity concentration of 214Pb and 214Bi, indicators of 226Ra, given as mean value of the two radionuclides, resulted 10.61 ± 4.02 Bq kg?1. 228Ac, 228Ra indicator, showed a mean activity concentration of 13.73 ± 3.20 Bq kg?1. The mean activity concentration of 212Pb, 224Ra indicator, was 8.28 ± 2.88 Bq kg?1. 208Tl, 224Ra indicator, presented a mean activity concentration of 11.03 ± 4.34 Bq kg?1. In all samples, the artifical 137Cs resulted below the detection limit (2.0 Bq kg?1). The arithmetical mean value of percentage of 210Po extraction in coffee beverage resulted 20.5 ± 6.9. The percentage of transfer of gamma emitters,40K, 214Pb, 214Bi, 228Ac, 212Pb, 208Tl resulted of 80.0, 33.5, 24.7, 30.0, 35.1 and 53.5 % for 40K, 214Pb, 214Bi, 228Ac, 212Pb and 208Tl respectively.  相似文献   

20.
Alpha spectrometry is proposed for the quantitative analysis of227Ac and228Th in irradiated226Ra targets. The chemical separation and the radiochemical determination is described.  相似文献   

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