CN105425274A - Measurement and determination method for age of uranium sample - Google Patents

Measurement and determination method for age of uranium sample Download PDF

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Publication number
CN105425274A
CN105425274A CN201510870033.6A CN201510870033A CN105425274A CN 105425274 A CN105425274 A CN 105425274A CN 201510870033 A CN201510870033 A CN 201510870033A CN 105425274 A CN105425274 A CN 105425274A
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age
uranium
lysate
sample
assay method
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杨素亮
丁有钱
梁小虎
孙宏清
马鹏
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China Institute of Atomic of Energy
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China Institute of Atomic of Energy
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    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01T—MEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00—Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/36—Measuring spectral distribution of X-rays or of nuclear radiation spectrometry

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  • Physics & Mathematics (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • General Physics & Mathematics (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Molecular Biology (AREA)
  • Other Investigation Or Analysis Of Materials By Electrical Means (AREA)

Abstract

The invention relates to a measurement and determination method for an age of a uranium sample. The method comprises: dissolution of a proper number of uranium samples is carried out; 234Th in a dissolving solution is measured; a 234U in the dissolving solution is measured; radiochemical separation is carried out on thorium in the dissolving solution; the 234Th and the 234U in the separated product are measured respectively; and then the age of the uranium is calculated based on the known Bateman equation and the radioactive decay rule. With the method, the operation flow is simplified; the employed alpha spectrometer and beta spectrometer do not need detection efficiency scale; the uncertainty of the analysis result due to the detection efficiency scale of the alpha spectrometer and beta spectrometer can be avoided theoretically; and during the separation and measurement processes, no extra radioactive tracer is required.

Description

The assay method at a kind of uranium sample age
Technical field
The invention belongs to radiochemicak analysis field, be specifically related to the assay method at a kind of uranium sample age, be applicable to Enriched Uranium sample and depleted nuclear fuel sample.
Background technology
Age of uranium sample refers to that its concentrated or Chemical Decomposition is for the last time to the time interval measuring the moment, and it is the dynamic fingerprint of nuclear material, is that one of its important evidence of originating is traced or examined in international nuclear safeguards.Diffusion method or centrifuge method is no matter used to produce enriched uranium, all with gaseous state UF 6for raw material, product is also in UF 6state.UF 6triple point low, about 57 DEG C of gasifications.And the fluoride gasification point temperature of the elements such as decay daughter Pa and Th of uranium is all higher, as ThF 4boiling point be 1782 DEG C, PaF 4and PaF 5boiling point also all higher than 500 DEG C.Therefore, after transforming and be concentrated, the daughter nuclides such as Pa and Th in product enriched uranium and tailing depleted nuclear fuel all can be thought just to grow out after concentration.These daughter nuclides and parent nucleus be not before reaching balance, and its content is along with time growth, and this is the theoretical foundation of uranium sample age determination.
The age determination method of uranium material comprises gamma energy spectrum method and radiochemical method.Wherein gamma energy spectrum method is applicable to 234the high-enriched uranium sample that U abundance is higher.Principle is measured by high resolution gamma-ray spectrometer 214bi with 234the activity ratio of U determines the age of sample.The method is without the need to carrying out chemical treatment to sample, relatively fast and simple.But because sample source and scale merit source are difficult to completely the same in the space distribution etc. of γ particle energy, geometric condition (size, shape, density) and nucleic, cause detection efficiency uncertainty comparatively large, corresponding analysis result uncertainty is also larger.In addition, 234u arrives 214gaseous species in Bi decay chain 222whether Rn overflows also can impact analysis result.Therefore, gamma energy spectrum method is not suitable for the higher sample analysis of accuracy requirement.Radiochemical method measures the age of uranium, can measure 230th and its parent nucleus 234the activity ratio of U, also can measure 231pa and its parent nucleus 235the activity ratio of U.With 230th with 234the activity ratio pH-value determination pH of U is example, by Bei Teman equation and Law of radioactive decay, can be able to lower relational expression: t=1.09 × 10 after calculating 5× A ( 230th) t/ A ( 234u) t.Wherein, t be sample age (unit is a), A ( 230th) t/ A ( 234u) tfor in sample 230th with 234the activity ratio of U.Radiochemical method applicability is comparatively strong, and result uncertainty is relatively little, is the method often selected in uranium age analysis.But traditional radiochemical method separation process length, complex operation, workload are large; And detection efficiency calibration must be carried out to the gamma ray spectrometer used and alpha spectrometer, except need using a lot of expensive radioactivity standard material, also can bring larger uncertainty to analysis result.
In view of above-mentioned defect, creator of the present invention, through long research and practice, obtains the assay method at uranium sample age of the present invention.
Summary of the invention
For the defect existed in prior art, the invention provides the assay method at a kind of uranium sample age, ensure that alpha spectrometer and gamma ray spectrometer are all without the need to scale detection efficiency, avoid the uncertainty brought to analysis result by alpha spectrometer and gamma ray spectrometer detection efficiency calibration; Be separated and all do not need extra radiotracer in measuring process; Method of operating is simple.
For reaching above object, the technical solution used in the present invention is: the assay method providing a kind of uranium sample age, comprises the steps:
1) uranium sample is dissolved;
2) in lysate 234th measures;
3) in lysate 234u measures;
4) Radiochemical Separation is carried out to thorium in lysate;
5) in products of separated 234th and 230th measures respectively;
6) known Bei Teman equation and Law of radioactive decay is utilized to calculate the age of uranium.
Further, in step 1) in, uranium sample is dissolved in nitric acid.
Further, in step 2) in, take appropriate lysate and prepare flat source, utilize high-purity oleic acid to measure wherein 234th.
Further, step 3) in, get appropriate lysate, add appropriate nitric acid and again dilute, take appropriate dilution, behind electro-deposition source, utilize alpha spectrometer to measure in dilution 234u.
Further, in step 4) in, the Radiochemical Separation of described thorium takes appropriate lysate, and by the anion exchange resins chromatograph post of this lysate by having crossed with nitric acid pre-equilibration, hydrochloric acid desorb, collects stripping liquid and weigh.
Further, in step 5) in, get appropriate stripping liquid, prepare flat source, use high-purity oleic acid to measure wherein 234th; Source processed after remaining stripping liquid electro-deposition after preparing flat source, uses alpha spectrometer to measure 230th.
Further, in step 6) in, the computing formula of described Bei Teman equation and Law of radioactive decay is:
t＝1.09×10 5×A( 230Th)t/A( 234U)t
Wherein, t be sample age (unit is a), A ( 230th) t/A ( 234u) t is in sample 230th with 234the activity ratio of U.
Advantageous Effects of the present invention is: (1) Radiochemical Separation flow operations of the present invention relative ease; (2) alpha spectrometer used and gamma ray spectrometer are all without the need to scale detection efficiency; (3) uncertainty brought to analysis result by alpha spectrometer and gamma ray spectrometer detection efficiency calibration is avoided in theory; (4) be separated and all do not need extra radiotracer in measuring process.
Accompanying drawing explanation
Fig. 1 is the process flow diagram of uranium sample age determination method of the present invention.
Embodiment
Below in conjunction with accompanying drawing, the specific embodiment of the present invention is described in further detail.
As shown in Figure 1, be the assay method at uranium sample age of the present invention, the method comprises the steps:
(1) dissolving of uranium sample.Get appropriate enriched uranium or depleted nuclear fuel sample (wherein uranium content is generally not more than 1g, 234u content is generally not less than 5.0 × 10 3bq), be dissolved in 10mL8mol/L nitric acid;
(2) in lysate 234the measurement of Th.Take appropriate lysate and prepare flat source, high-purity oleic acid is measured wherein 234th;
(3) in lysate 234the measurement of U.Take about 0.1mL lysate, again weigh with after appropriate 0.01mol/L nitric acid dilution; Take appropriate dilution (volume is not more than 0.1mL, and uranium-bearing is not more than 50 μ g), behind electro-deposition source, alpha spectrometer is measured wherein 234u;
(4) Radiochemical Separation of thorium.Take appropriate lysate, the anion exchange resins chromatograph post crossed by 8mol/L nitric acid pre-equilibration, 8mol/L nitric acid washing about 20 column volumes (yellow colour band disappears completely to post), the 6mol/L hydrochloric acid desorb of 5 column volumes, every column volume Fractional Collections stripping liquid is also weighed, and NaI gamma ray spectrometer is measured;
(5) in products of separated 234the measurement of Th.After being merged by stripping liquid higher for thorium content, the flat source of sampling preparation, measures wherein under using step (2) same spectrometer the same terms 234th;
(6) in products of separated 230the measurement of Th.Behind stripping liquid electro-deposition source higher for remaining thorium content after the flat source of preparation, the same probe of step (3) same alpha spectrometer is used to measure under the same conditions 230th.
Be described below by specific embodiment:
Analytic target is certain depleted nuclear fuel sample, and chemical species is nitric hydrate uranyl, and reagent product batch number is 8901, factory of China Nuclear Industry Corporation 404 product.
Take this sample 2.1g in glass small beaker, adding about 11mL concentration is the salpeter solution of 8mol/L, and glass bar is stirred to and dissolves completely.Take this lysate 0.16204g, prepare flat source, the surface location of popping one's head at BE3830 molded breadth energy high-purity oleic acid (U.S. Ortec Products) is measured, and counting rate is 1.1407cps.Separately take about 0.1mL (0.13821g) to dodge in pipe in 20mL liquid, take 20mL0.01mol/L nitric acid (20.059g) and dilute.Take dilution 0.1mL (0.11072g), α measurement source is prepared in molecule electro-deposition, and (electrodeposition efficiency is 99.9%, and measuring source activity district area is 2cm 2), 7200-08 type alpha spectrometer (U.S. Canberra Products) is measured, and source pitch of fins probe 11mm, records 234the counting rate of U is 0.037718cps.
Take 13.485g lysate (as calculated, wherein 234the gross-count rate of U is 671.33cps) with anion exchange resins chromatograph post (Dowex1 × 4 anion exchange resins, 75-120 order, the U.S. Rhom and Hass product of the flow velocity of about 0.3mL/min by having crossed with 8mol/L nitric acid pre-equilibration; Post bed specification is Φ 5 × 75mm), 8mol/L nitric acid washing about 20 column volumes (yellow colour band disappears completely to post), the 6mol/L hydrochloric acid desorb of 5 column volumes, the stripping liquid every column volume of weighed tubule collects 1 pipe, measures after again weighing with 3MW3/LP type NaI gamma ray spectrometer.Wherein 234what Th content was higher is the 2nd pipe stripping liquid, and stripping liquid quality is 1.7068g.Take this stripping liquid 0.16204g and prepare flat source, and measure with the same high-purity oleic acid measuring lysate gamma spectrum, measuring position is similarly detecting head surface, and counting rate is 1.1407cps.Be corrected to the moment before upper prop, in the 2nd pipe stripping liquid 234the counting rate of Th is 84.384cps, and namely the chemical yield of flow process thorium is 88.89%.Take this stripping liquid 1.3884g, behind electro-deposition source (deposition is 98.9%), measure at same position with the same probe of the same spectrometer measuring lysate alpha energy spectrum, counting rate is 0.12444cps.Correct through sampling coefficient and chemical yield, can be regarded as in upper prop feed liquid 230the gross-count rate of Th is 0.17404cps.
Finally, by t=1.09 × 10 5× A ( 230th) t/ A ( 234u) t(wherein t is the age of sample, A ( 230th) t/ A ( 234u) tfor 230th with 234the activity ratio of U) calculate, and by " JJF1135-2005 People's Republic of China (PRC) national measurement technical specification, chemical analysis evaluation of uncertainty in measurement " uncertainty evaluation is carried out to result, obtain the age of this sample for (28.2 ± 0.9) a, Coverage factor k=2.
The assay method at uranium sample age of the present invention is not limited to above-mentioned embodiment, and those skilled in the art's technical scheme according to the present invention draws and other embodiment belongs to technological innovation scope of the present invention equally.

Claims (7)

1. the assay method at uranium sample age, comprises the steps:
1) uranium sample is dissolved;
2) in lysate 234th measures;
3) in lysate 234u measures;
4) Radiochemical Separation is carried out to thorium in lysate;
5) in products of separated 234th and 230th measures respectively;
6) known Bei Teman equation and Law of radioactive decay is utilized to calculate the age of uranium.
2. the assay method at a kind of uranium sample age as claimed in claim 1, is characterized in that: in step 1) in, uranium sample is dissolved in nitric acid.
3. the assay method at a kind of uranium sample age as claimed in claim 1, is characterized in that: in step 2) in, take appropriate lysate and prepare flat source, utilize high-purity oleic acid to measure wherein 234th.
4. the assay method at a kind of uranium sample age as claimed in claim 1, is characterized in that: in step 3) in, get appropriate lysate, add appropriate nitric acid and again dilute, take appropriate dilution, behind electro-deposition source, utilize alpha spectrometer to measure in dilution 234u.
5. the assay method at a kind of uranium sample age as claimed in claim 1, it is characterized in that: in step 4) in, the Radiochemical Separation of described thorium, take appropriate lysate, by the anion exchange resins chromatograph post of this lysate by having crossed with nitric acid pre-equilibration, hydrochloric acid desorb, collects stripping liquid and weighs.
6. the assay method at a kind of uranium sample age as claimed in claim 1, is characterized in that: in step 5) in, get appropriate stripping liquid, prepare flat source, use high-purity oleic acid to measure wherein 234th; Source processed after remaining stripping liquid electro-deposition after preparing flat source, uses alpha spectrometer to measure 230th.
7. the assay method at a kind of uranium sample age as claimed in claim 1, is characterized in that: in step 6) in, according to the formula that Bei Teman equation and Law of radioactive decay are extrapolated be:
t＝1.09×10 5×A( 230Th) t/A( 234U) t
Wherein, t is the age of sample, A ( 230th) t/ A ( 234u) tfor in sample 230th with 234the activity ratio of U.
CN201510870033.6A 2015-12-02 2015-12-02 Measurement and determination method for age of uranium sample Pending CN105425274A (en)

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Publication number Priority date Publication date Assignee Title
CN106872556A (en) * 2017-01-05 2017-06-20 中国原子能科学研究院 A kind of measuring method of uranium product production time
CN108459070A (en) * 2018-02-11 2018-08-28 中国科学院地质与地球物理研究所 A kind of diluent free measures apatite (U-Th)/He and determines year method
CN109342641A (en) * 2018-11-05 2019-02-15 中国原子能科学研究院 The measuring method at the age of particle containing plutonium
CN109490935A (en) * 2018-11-12 2019-03-19 西北核技术研究所 The filter sample γ measurement source method and device extracted based on particulate matter
CN111426764A (en) * 2020-04-09 2020-07-17 中国科学院地质与地球物理研究所 Method for testing age of hydrothermal sulfide in quaternary seabed

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Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN106872556A (en) * 2017-01-05 2017-06-20 中国原子能科学研究院 A kind of measuring method of uranium product production time
CN108459070A (en) * 2018-02-11 2018-08-28 中国科学院地质与地球物理研究所 A kind of diluent free measures apatite (U-Th)/He and determines year method
CN109342641A (en) * 2018-11-05 2019-02-15 中国原子能科学研究院 The measuring method at the age of particle containing plutonium
CN109342641B (en) * 2018-11-05 2020-11-10 中国原子能科学研究院 Method for measuring age of plutonium-containing fine particles
CN109490935A (en) * 2018-11-12 2019-03-19 西北核技术研究所 The filter sample γ measurement source method and device extracted based on particulate matter
CN109490935B (en) * 2018-11-12 2020-06-26 西北核技术研究所 Filtering material sample gamma measurement source preparation method and device based on particulate matter extraction
CN111426764A (en) * 2020-04-09 2020-07-17 中国科学院地质与地球物理研究所 Method for testing age of hydrothermal sulfide in quaternary seabed

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Application publication date: 20160323