CN105158790B - The Long-lived Radionuclides half-life period assay method measured based on isotopic ratio - Google Patents
The Long-lived Radionuclides half-life period assay method measured based on isotopic ratio Download PDFInfo
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Abstract
The present invention provides the Long-lived Radionuclides half-life period assay method measured based on isotopic ratio, including weighs radionuclide solution of a certain amount of half-life period more than 1 year；Radionuclide amount according to rough estimate such as increases at the natural stabilisation element of the radionuclide of magnitude in radionuclide solution, and the ratio R of radionuclide and stable isotope in solution is measured using high-precision isotope mass spectrometry1；Radionuclide solution is deposited after a period of time t, again using the ratio R of radionuclide and stable isotope in high-precision isotope mass spectrometry measurement solution2；By
Description
Technical field
The invention belongs to nuclear parameter fields of measurement, and in particular to a kind of Long-lived Radionuclides (are applied to half-life period big
In 1 year to 1 × 105In the range of year) half-life period and nucleic assay method.As a kind of Accurate measurement of nuclear parameter, it can open up
Exhibition is applied to the accurate measurement of long-lived radioactivity sample activity and the preparation of standard source.
Background technology
Nuclear parameter measurement is Nuclear Science And Engineering, the important research content in core test analysis field, at home and abroad by wide
It is general to pay attention to.
The measuring method of general Short-lived radionuclide, be by the tracking measurement to the radionuclide ray, by
The radioactive activity attenuation amplitude of nucleic calculates the half-life period of the nucleic in measuring section, and half-life period calculation formula isFor long-lived radioactivity nucleic, it is then by its radiation of the quantitative combination of its parent that its half-life period, which determines,
Property activity measurement carry out, half-life period calculation formula isIn a word, in terms of radionuclide halflife measurement,
Include the experimental procedure of activity measurement, its technological means relies primarily on radioactivity survey method, including various α, β and
γ spectral technologies.Influenceed by the partial uncertainty that the experimental procedures such as efficiency calibration in radio-analytical technique are originated, radioactivity side
The uncertainty of method measurement result is more than 0.6%, and during the half-life measurement of Long-lived Radionuclides, and activity is surveyed
Amount is more influenceed by many factors such as difficult, the radioactive background interference of weak signal measurement, and uncertainty of measurement is more up to percent
It is several or even more than more than ten percent.
The content of the invention
To solve existing radionuclide halflife assay method in continuous mode using caused by radiometric method
The high technical problem of the uncertainty of measurement result, the present invention is using the method for isotope mass spectrometry, and highest priority aims at half-life period
For 1 year to 103Year (has in the case of specific demand, it is several months or 10 that can be expanded by adjusting the resting period to half-life period4More than year)
Nucleic, Radiochemical Separation and mass spectrometric measurement technology based on mother and sons' body, by accurately determine radionuclide storage when
The interior change with other isotopic ratios, calculates the half-life period of nucleic.The present invention solution be：
The assay method of the Long-lived Radionuclides half-life period measured based on isotopic ratio, it is characterized in that：
Comprise the following steps：
1) weigh and radiated in radionuclide solution of a certain amount of half-life period more than 1 year, the radionuclide solution
Property nucleic parent and daughter mass number are unequal；
2) radionuclide amount according to rough estimate such as increases at the radionuclide of magnitude in radionuclide solution
Natural stabilisation element, the ratio of radionuclide and natural stabilisation element in solution is measured using high-precision isotope mass spectrometry
R1；
3) radionuclide solution is deposited after a period of time t, again using in high-precision isotope mass spectrometry measurement solution
The ratio R of radionuclide and natural stabilisation element2；Resting period t therein is more than the radionuclide halflife
0.3%；
4) its half-life period is calculated by following formula：
If the radionuclidic parents are equal with daughter mass number, the either pure γ radiation of certain gamma activity is included
Property nucleic, then based on isotopic ratio measure Long-lived Radionuclides half-life period assay method, it is characterized in that：
Comprise the following steps：
1) radionuclide solution of a certain amount of half-life period more than 1 year is weighed；Radiated in the radionuclide solution
Property nucleic parent is equal with daughter mass number；
2) radionuclide amount according to rough estimate such as increases at the radioactive nucleus of magnitude in the radionuclide solution
The natural stabilisation element of element, carries out Radiochemical Separation and removes decay daughter, is measured in solution and radiated using high-precision isotope mass spectrometry
Property nucleic and natural stabilisation element ratio R1；
3) solution is deposited after a period of time t, Radiochemical Separation is carried out again and removes decay daughter, using the same position of high accuracy
The ratio R of radionuclide and natural stabilisation element in quality spectrometry solution2；Resting period t therein is more than the radioactivity
The 0.3% of nucleic half-life period；
4) its half-life period is calculated by following formula：
It is an advantage of the invention that：
1st, the present invention uses mass spectrographic method, avoided the processes such as ratio, the efficiency correction of radioactive ray point there may be
Uncertainty.By the high accuracy analysis to Long-lived Radionuclides and other isotopic ratios, its half-life period is measured, is put
The dependence to radioactive assays has been taken off, the degree of accuracy of part radionuclide halflife measurement can be improved.With reference to parent nucleus
Accurate quantitative result, can be applied to the accurate calibration of long-lived radioactivity source degree activity, uncertainty level can by 0.6% with
On be down to less than 0.3% level, the uncertainty to most of nucleic half-life measurement is better than 0.5%, preferably can as little as 0.1%
Level.
2nd, the present invention is few to part Long-lived Radionuclides sample for analysis amount, and measuring technology is not related to activity, penetrated
The radioassays such as line.It is high based on mass spectrographic method of testing sensitivity, it is more than more than 10 years Radionuclide analysis for half-life period and tests
Radioactive assays consumption is considerably less than with sample operation amount, personnel's radiation risk and testing cost is reduced.
Embodiment
Below with151Sm analyze and229Exemplified by Th, its half-life period assay method and calculation formula are introduced.
Embodiment 1:Half-life period method is determined without the isotopic ratio of chemical sample preparation
229Th is233U decay daughter, determines the fields such as year, core test in geology division of history into periods U-Th and is used widely.229Th
Main to occur alpha-decay, half-life period is 7880 ± 120 years, and relative uncertainty degree is 1.5%.
Buying229Th standard liquids (or from233Extracted in U solution229Th) about 8 × 10-7G, addition230Th/232Th is about 0.1
Thorium enriched isotope solutions (wherein232Th is about 4 × 10-6G) and U500 isotope abundances standard liquid (235U/238U=
0.999698) about 4 × 10-6G, about 15g is diluted to by solution uranium, thorium mixed solution, and the solution is used into hot surface MALDI-MS
Analyzed, used235U/238U=0.999698 corrections Th mass discrimination influence, determines Th isotopes229Th/232Th ratios
Value R1, cooling 6 years after again by the solution use hot surface MALDI-MS, and with same uranium isotope ratio correction Th quality
Discriminate against effects measurement Th isotopes229Th/232Th ratio Rs2, byCalculate Th half-life period.In half-life period
In calculating, R1And R2The uncertainty of the correction factor of isotopic ratio measurement is cancelled out each other, and the uncertainty of measurement result is main
The experimental standard deviation (being better than 6e-6) measured from isotopic ratio, this method pair is thought in initial analysis229Th half-life period surveys
It is about 0.78% to measure uncertainty.
Embodiment 2:Isotopic ratio determines half-life period method after chemical separation and purification
151Sm is important nuclear material fission product, in necks such as spentnuclear fuel post processing, radioactive environment monitoring and nuclear tests
Domain is received significant attention.151Sm half-life period is (89 ± 8) year, and its relative uncertainty degree is about 9%, far can not meet kernel analysis
Deng area research demand.
Buying151Sm standard liquids (or by concentrating150The irradiation generation of Sm isotope production reactors151Sm) it is used for the test of half-life period.Under
Two kinds of technological approaches based on boron isotopic abundance ratio are introduced respectively and are determined in face151The method of Sm half-life period.
Take about 20kBq's respectively according to certificate concentration151Sm solution, natural Sm concentration mark is weighed with ten a ten thousandth balances
The accurate natural Sm containing about 7 micrograms, is added to151In Sm solution.Through rock, stand etc. step to make Sm exchange it is uniform after, put down
It is divided into two parts of solution.1 part151Sm solution removes the interference nucleic such as Eu through chemical separation and purification respectively, using high-precision isotope
Mass spectrum receives inductivity coupled plasma mass spectrometries (hot surface MALDI-MS also can) analytical technology more as, by147Sm/149Sm=
1.084746 correcting Sm mass fractionation, determine151Sm/150Sm isotopic ratios R1；By second part of natural Sm concentration standard of addition
Solution151After Sm stands 2 years, the impurity species such as Eu are removed through same experimental procedure, including chemical separation and purification, by147Sm
/149Sm=1.084746 corrects Sm mass fractionation, determines151Sm/150Sm isotopic ratios R2, byCalculate151Sm half-life period.In half-life period calculates, R1And R2The uncertainty of the correction factor of isotopic ratio measurement is cancelled out each other,
The uncertainty of measurement result is mainly derived from the experimental standard deviation (being better than 3e-5) of isotopic ratio measurement, and initial analysis is recognized
For this method pair151Sm half-life measurement uncertainties are about 0.67%.
Claims (2)
1. the assay method of the Long-lived Radionuclides half-life period measured based on isotopic ratio, it is characterised in that：Including with
Lower step：
1) radioactive nucleus in radionuclide solution of a certain amount of half-life period more than 1 year, the radionuclide solution is weighed
Plain parent and daughter mass number are unequal；
2) radionuclide amount according to rough estimate such as increases at the day of the radionuclide of magnitude in radionuclide solution
Right stable element, the ratio R of radionuclide and natural stabilisation element in solution is measured using high-precision isotope mass spectrometry1；
3) radionuclide solution is deposited after a period of time t, again using radiation in high-precision isotope mass spectrometry measurement solution
Property nucleic and natural stabilisation element ratio R2；Resting period t therein is more than the 0.3% of the radionuclide halflife；
4) its half-life period is calculated by following formula：
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2. the assay method of the Long-lived Radionuclides half-life period measured based on isotopic ratio, it is characterised in that：Including with
Lower step：
1) radionuclide solution of a certain amount of half-life period more than 1 year is weighed；Radioactive nucleus in the radionuclide solution
Plain parent is equal with daughter mass number；
2) radionuclide amount according to rough estimate such as increases at the radionuclide of magnitude in the radionuclide solution
Natural stabilisation element, carries out Radiochemical Separation and removes decay daughter, radioactive nucleus in solution is measured using high-precision isotope mass spectrometry
The ratio R of element and natural stabilisation element1；
3) solution is deposited after a period of time t, Radiochemical Separation is carried out again and removes decay daughter, using high-precision isotope matter
The ratio R of radionuclide and natural stabilisation element in spectrometry solution2；Resting period t therein is more than the radionuclide
The 0.3% of half-life period；
4) its half-life period is calculated by following formula：
<mrow>
<msub>
<mi>T</mi>
<mrow>
<mn>1</mn>
<mo>/</mo>
<mn>2</mn>
</mrow>
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<mo>=</mo>
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1
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| Title |
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| 《Half-life measurements of long-lived radionuclides—New data analysis and systematic effects》;H. Schrader;《Applied Radiation and Isotopes》;20100831;第68卷(第7-8期);全文 * |
| 《在大量同质异位素干扰下的同位素稀释质谱法测定173Lu 和174Lu》;徐江等;《核化学与放射化学》;20070228;第29卷(第1期);全文 * |
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