Background technology
Plutonium is a kind of important metallic element, and its multiple isotope has crucial application in military, economic dispatch field, and exposed plutonium metal at room temperature can react with airborne oxygen and form the oxide of plutonium, and its chemical reaction is:
Pu (s)+O
2(g) → PuO
2(s)+and Δ H (Δ H is-1056kJ/mol)
Because plutonium metal is easy to the characteristic of oxidation in air, even taked the technical matters of overlay coating (nickel-copper-nickel coating), can not guarantee definitely that plutonium metal is not oxidized.Therefore, to the differentiation of plutonium degree of oxidation with confirm just to become important.
Oxygen has multiple isotope, but stable isotope has only three kinds:
16O,
17O,
18O, it is respectively 99.757%, 0.038% in natural abundance, and 0.205%.Oxygen in the plutonium material receives the irradiation of α particle and neutron, and following physical process will take place:
17O(n,n′γ)
17O(871keV);
17O(α,α′γ)
17O(871keV);
18O(n,n′γ)
18O(1982.2keV);
18O(α,α′γ)
18O(1982.2keV);
17O (α, n)
20Ne
*(1634keV); Or
18O(α,n)
21Ne
*(350.7,1396,2438,2788.5,2794keV)
These physical processes for
16O, because
16The excitation energy of O is than higher, so in the plutonium material
16The probability that O is activated can be ignored.
17The 871keV characteristic gamma-rays of O is 1.24/10 receiving the reaction probability of α when particle excitated
6, and be 622/10 under neutron excites
6, because under the natural radiation condition, the quantity of α particle approximately is 10 of neutron quantity in the plutonium metal material
8Doubly, so the characteristic gamma-rays of the 871keV in the plutonium oxide mainly receives the particle excitated generation of α, that is:
17(α, α ' γ) for O
17O (871keV).
In the interim article " technical research of plutonium oxide property measurement " of volume the 12nd in Nuclear Technology magazine Dec in 2006 the 29th, the author has provided and has proposed to study qualitatively and discuss whether plutonium metal is oxidized through measuring 871keV characteristic gamma-rays.
But following problem but ignored in above-mentioned article, that is, because
14N (α, p)
17O (871keV) reaction also can produce the characteristic gamma-rays of 871keV, and in the production run of plutonium metal material, inevitably can introduce the N element,
14The abundance of N also can be higher, so in the gamma-rays of measuring,
14N (α, p)
17The gamma-rays that O (871keV) reaction produces also than
17(α, α ' γ) for O
17O (871keV) is higher, therefore directly utilizes
17The 871keV characteristic gamma-rays of O judges that the existence of plutonium oxide receives easily
14The interference of N.
For example, be numbered article " the The 871keV gamma ray from of " Nuclear Instruments and Methods in Physics ResearchA 474 (2001) 285-293 " at article
17O and theidentification of plutonium oxide " and article be numbered article " the THE 870.8keV GAMMA RAY FORMPuO of " Nuclear Instruments andMethods 193 (1982) 383-385 "
2" middle through thinking after the analysis, only depend on the characteristic gamma-rays of 871keV to prove existing of plutonium oxide than mistake, directly utilize
17The 871keV characteristic gamma-rays of O also is difficult to quantitative test is carried out in the existence of plutonium oxide.
Summary of the invention
The invention provides a kind of method of measuring the plutonium metal degree of oxidation, especially a kind of method of measuring plutonium metal oxidation number percent, this method can reduce or avoid problem noted earlier.
For addressing the above problem, the present invention proposes a kind of method of measuring plutonium metal oxidation number percent, said method comprising the steps of:
A, be 100 gram standard testing samples with pure zirconia plutonium powder and simple metal plutonium powder mixes; Carry out 871keV characteristic gamma-rays peak position count value and measure, obtain having the plutonium metal 871keV characteristic gamma-rays peak position count value w1 of this plutonium oxide of confirming percentage by weight;
B, the said 100 gram standard testing samples in the steps A are added outer source irradiates; Carry out 871keV characteristic gamma-rays peak position count value simultaneously and measure, obtain having plutonium metal 871keV characteristic gamma-rays peak position count value w2 under the source irradiates condition outside adding of this plutonium oxide of confirming percentage by weight;
C, the 871keV characteristic gamma-rays peak position count value w2 under the source irradiates condition outside adding that obtains among the step B is deducted the 871keV characteristic gamma-rays peak position count value w1 that obtains in the steps A, can obtain having this confirm percentage by weight the plutonium metal of plutonium oxide in
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 that O (871keV) reaction is taken place;
D, with reference to steps A-C, measure in the plutonium metal of plutonium oxide of Different Weight number percent
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 that O (871keV) reaction is taken place simulates plutonium oxide percentage by weight 0-100%'s in the 100 gram standard testing sample plutonium metals
17(n, n ' γ) for O
17O (871keV) reaction 871keV characteristic gamma-rays peak position count value typical curve;
E, get the plutonium metal sample of 100 grams degree of oxidation to be measured, carry out 871keV characteristic gamma-rays peak position count value and measure, obtain its 871keV characteristic gamma-rays peak position count value w1 ';
F, the plutonium metal sample that said 100 in the step e restrained degree of oxidation to be measured add the source irradiates described in the outer above-mentioned steps B; Carry out 871keV characteristic gamma-rays peak position count value simultaneously and measure, obtain plutonium metal sample 871keV characteristic gamma-rays peak position count value w2 ' under the source irradiates condition outside adding of said 100 grams degree of oxidation to be measured;
G, the 871keV characteristic gamma-rays peak position count value w2 ' under the source irradiates condition outside adding that obtains in the step F is deducted the 871keV characteristic gamma-rays peak position count value w1 ' that obtains in the step e, can obtain in the plutonium metal sample of said 100 grams degree of oxidation to be measured
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 ' that O (871keV) reaction is taken place;
H, the typical curve described in the said count value w3 ' that obtains among the step G and the step D is compared, can obtain the plutonium oxide percentage by weight in the plutonium metal sample of said 100 grams degree of oxidation to be measured.
Preferably, the pure zirconia plutonium powder in the 100 gram standard testing samples was respectively 1: 9,2: 8,3: 7,4: 6,5: 5,6: 4,7: 3,8: 2,9: 1 with simple metal plutonium powder weight ratio described in the step D.
Preferably, said outer neutron source is the 5MKev ra-Be neutron source.
A kind of method of measuring plutonium metal oxidation number percent provided by the present invention is measured under the oxidized plutonium metal sample natural radiation condition earlier
17(α, α ' γ) for O
17O (871keV) and
14N (α, p)
17The 871keV characteristic gamma-rays peak position count value that is taken place of O (871keV) reaction is utilized then
17(n, n ' γ) for O
17O (871keV) reaction through adding outer source irradiates, strengthens in the plutonium metal sample to be tested
17(n, n ' γ) for O
17The ability of O (871keV) reaction; Record outside adding the 871keV characteristic gamma-rays peak position count value of oxidized plutonium metal sample under the source irradiates condition; Will be outside adding under the source irradiates condition measured 871keV characteristic gamma-rays peak position count value deduct 871keV characteristic gamma-rays peak position count value measured under the natural radiation condition, can obtain in the oxidized plutonium metal sample
17The 871keV characteristic gamma-rays peak position count value that O contributed so just can effectively be avoided
14N (α, p)
17The gamma-ray interference of 871keV characteristic that O (871keV) reaction is produced, the plutonium metal sample that also just can treat the oxygen determination degree carries out quantitative test.
Embodiment
To understand in order technical characterictic of the present invention, purpose and effect being had more clearly, to contrast description of drawings embodiment of the present invention at present.Wherein, identical parts adopt identical label.
Specify according to a kind of method of measuring the plutonium metal degree of oxidation of the present invention especially a kind of implementation step and principle thereof of measuring the method for plutonium metal oxidation number percent with reference to the accompanying drawings.
A kind of method of measuring plutonium metal oxidation number percent provided by the present invention said method comprising the steps of:
A, be 100 gram standard testing samples with pure zirconia plutonium powder and simple metal plutonium powder mixes; Carry out 871keV characteristic gamma-rays peak position count value and measure, obtain having the plutonium metal 871keV characteristic gamma-rays peak position count value w1 of this plutonium oxide of confirming percentage by weight;
B, the said 100 gram standard testing samples in the steps A are added outer source irradiates; Carry out 871keV characteristic gamma-rays peak position count value simultaneously and measure, obtain having plutonium metal 871keV characteristic gamma-rays peak position count value w2 under the source irradiates condition outside adding of this plutonium oxide of confirming percentage by weight;
C, the 871keV characteristic gamma-rays peak position count value w2 under the source irradiates condition outside adding that obtains among the step B is deducted the 871keV characteristic gamma-rays peak position count value w1 that obtains in the steps A, can obtain having this confirm percentage by weight the plutonium metal of plutonium oxide in
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 that O (871keV) reaction is taken place;
D, with reference to steps A-C, measure in the plutonium metal of plutonium oxide of Different Weight number percent
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 that O (871keV) reaction is taken place simulates plutonium oxide percentage by weight 0-100%'s in the 100 gram standard testing sample plutonium metals
17(n, n ' γ) for O
17O (871keV) reaction 871keV characteristic gamma-rays peak position count value typical curve;
E, get the plutonium metal sample of 100 grams degree of oxidation to be measured, carry out 871keV characteristic gamma-rays peak position count value and measure, obtain its 871keV characteristic gamma-rays peak position count value w1 ';
F, the plutonium metal sample that said 100 in the step e restrained degree of oxidation to be measured add the source irradiates described in the outer above-mentioned steps B; Carry out 871keV characteristic gamma-rays peak position count value simultaneously and measure, obtain plutonium metal sample 871keV characteristic gamma-rays peak position count value w2 ' under the source irradiates condition outside adding of said 100 grams degree of oxidation to be measured;
G, the 871keV characteristic gamma-rays peak position count value w2 ' under the source irradiates condition outside adding that obtains in the step F is deducted the 871keV characteristic gamma-rays peak position count value w1 ' that obtains in the step e, can obtain in the plutonium metal sample of said 100 grams degree of oxidation to be measured
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 ' that O (871keV) reaction is taken place;
H, the typical curve described in the said count value w3 ' that obtains among the step G and the step D is compared, can obtain the plutonium oxide percentage by weight in the plutonium metal sample of said 100 grams degree of oxidation to be measured.
Wherein,, can use low background HpGe gamma ray spectrometer to measure for the measurement of gamma-rays peak position count value, such as, can measure as testing tool with the GEM-30185-P detector and the DESPEC numeral multichannel analyzer of ORTEC company.
Said outer neutron source can be that the gamma ray that radium or the decay of other metals are sent comes the irradiation beryllium to produce neutron perhaps directly by californium source given-ioff neutron.
In a preferred embodiment, said outer neutron source is the 5MKev ra-Be neutron source.
Through above-mentioned steps A-D, can obtain having 871keV characteristic gamma-rays peak position count value typical curve without 100 gram plutonium metal specimen of the plutonium oxide of percentage by weight.
In a preferred embodiment, the pure zirconia plutonium powder in the 100 gram standard testing samples was respectively 1: 9,2: 8,3: 7,4: 6,5: 5,6: 4,7: 3,8: 2,9: 1 with simple metal plutonium powder weight ratio described in the step D.
Such as; According to pure zirconia plutonium powder and simple metal plutonium powder weight ratio is preparation in 1: 9 100 gram standard testing samples; That is to say and use 10 gram pure zirconia plutonium powder and 90 gram simple metal plutonium powder; After it is fully mixed in beaker; Put into low background HpGe gamma ray spectrometer, it is carried out 871keV characteristic gamma-rays peak position count value mensuration under the natural radiation condition, Fig. 1 is a kind of 871keV characteristic gamma-rays peak position count value test result synoptic diagram of measuring the method for plutonium metal degree of oxidation according to a specific embodiment of the present invention.As shown in Figure 1; Through said low background HpGe gamma ray spectrometer; Can record pure zirconia plutonium powder is the 100 871keV characteristic gamma-rays peak position count value w1s of gram standard testing sample under the natural radiation condition of preparation in 1: 9 with simple metal plutonium powder weight ratio, and this 871keV characteristic gamma-rays peak position count value w1 has comprised under the natural radiation condition
17(α, α ' γ) for O
17O (871keV) reaction with
14N (α, p)
17The 871keV characteristic gamma-rays peak position count value that O (871keV) reaction is taken place.
After 871keV characteristic gamma-rays peak position count value under the natural radiation condition is measured completion, be that the 100 gram standard testing samples of preparing at 1: 9 shine to said pure zirconia plutonium powder and simple metal plutonium powder weight ratio through neutron source outside low background HpGe gamma ray spectrometer adds.
Outside adding under the source irradiates condition; Through said low background HpGe gamma ray spectrometer; Can record pure zirconia plutonium powder is the 871keV characteristic gamma-rays peak position count value w2 of 100 gram standard testing samples of preparation in 1: 9 with simple metal plutonium powder weight ratio, and this 871keV characteristic gamma-rays peak position count value w2 had both comprised under the natural radiation condition
17(α, α ' γ) for O
17O (871keV) reaction with
14N (α, p)
17The 871keV characteristic gamma-rays peak position count value that O (871keV) reaction is taken place has also comprised after the neutron irradiation
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value that O (871keV) reaction is taken place, wherein, neutron irradiation excites down the gamma-rays peak position count value that produces can not produce any influence for α under the natural radiation condition, and
14N can not excite at neutron yet and produce extra 871keV characteristic gamma-rays peak position count value down.
Therefore said 871keV characteristic gamma-rays peak position count value w2 is deducted said 871keV characteristic gamma-rays peak position count value w1, can be with under the natural conditions
17(α, α ' γ) for O
17O (871keV) reaction with
14N (α, p)
17The 871keV characteristic gamma-rays peak position count value that O (871keV) reaction is taken place balances out, and only obtains after the neutron irradiation
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 that O (871keV) reaction is taken place.
Fig. 2 is for plutonium oxide percentage by weight 0-100%'s in the 100 gram standard testing sample plutonium metals of the method for measuring the plutonium metal degree of oxidation according to a specific embodiment of the present invention a kind of
17(n, n ' γ) for O
17O (871keV) reaction 871keV characteristic gamma-rays peak position count value typical curve synoptic diagram.Transverse axis is represented plutonium oxide percentage by weight in the 100 gram standard testing sample plutonium metals among the figure, and the longitudinal axis is illustrated in and adds 871keV characteristic gamma-rays peak position count value under the outer source irradiates condition.
With reference to Fig. 2, corresponding pure zirconia plutonium powder and simple metal plutonium powder weight ratio are 100 gram standard testing samples of preparation in 1: 9, that is to say on the transverse axis that the plutonium oxide percentage by weight is in the 100 gram standard testing sample plutonium metals at 10% o'clock, its
17(n, n ' γ) for O
17O (871keV) reaction 871keV characteristic gamma-rays peak position count value is the 871keV characteristic gamma-rays peak position count value w3 that uses preceding method to calculate.
Equally, be respectively 2: 8,3: 7,4: 6,5: 5,6: 4,7: 3,8: 2,9: 1 o'clock corresponding to the pure zirconia plutonium powder in the 100 gram standard testing samples and simple metal plutonium powder weight ratio
17(n, n ' γ) for O
17The also available said method test of O (871keV) reaction 871keV characteristic gamma-rays peak position count value draws, and therefore also just can obtain among Fig. 2 on the transverse axis 100 and restrain that the plutonium oxide percentage by weight is to be respectively in the standard testing sample plutonium metals at 20%, 30%, 40%, 50%, 60%, 70%, 80%, 90% o'clock
17(n, n ' γ) for O
17O (871keV) reaction 871keV characteristic gamma-rays peak position count value.Therefore (n, n ' γ) 17O (871keV) react 871keV characteristic gamma-rays peak position count value typical curve also just can to simulate the 17O of plutonium oxide percentage by weight 0-100% in the 100 gram standard testing sample plutonium metals shown in Figure 2.
In the time need testing to the plutonium metal of unknown degree of oxidation, can take out the plutonium metal sample of 100 grams degree of oxidation to be measured, record the plutonium metal sample of said degree of oxidation to be measured according to the method for step e-G
17(n, n ' γ) for O
17The 871keV characteristic gamma-rays peak position count value w3 ' that O (871keV) reaction is taken place; Said 871keV characteristic gamma-rays peak position count value w3 ' is compared with said typical curve; Can find corresponding plutonium oxide percentage by weight; Just obtain the transverse axis coordinate on the pairing said typical curve of ordinate of orthogonal axes w3 ', this transverse axis coordinate is the plutonium oxide percentage by weight of the plutonium metal of said unknown degree of oxidation just.
A kind of method of measuring the plutonium metal degree of oxidation provided by the present invention is measured under the oxidized plutonium metal sample natural radiation condition earlier
17(α, α ' γ) for O
17O (871keV) and
14N (α, p)
17The 871keV characteristic gamma-rays peak position count value that is taken place of O (871keV) reaction is utilized then
17(n, n ' γ) for O
17O (871keV) reaction through adding outer source irradiates, strengthens in the plutonium metal sample to be tested
17(n, n ' γ) for O
17The ability of O (871keV) reaction; Record outside adding the 871keV characteristic gamma-rays peak position count value of oxidized plutonium metal sample under the source irradiates condition; Will be outside adding under the source irradiates condition measured 871keV characteristic gamma-rays peak position count value deduct 871keV characteristic gamma-rays peak position count value measured under the natural radiation condition, can obtain in the oxidized plutonium metal sample
17The 871keV characteristic gamma-rays peak position count value that O contributed so just can effectively be avoided
14N (α, p)
17The gamma-ray interference of 871keV characteristic that O (871keV) reaction is produced, the plutonium metal sample that also just can treat the oxygen determination degree carries out quantitative test.
Describing according to the mode of a plurality of embodiment though it will be appreciated by those skilled in the art that the present invention, is not that each embodiment only comprises an independently technical scheme.Narration like this only is for the sake of clarity in the instructions; Those skilled in the art should do instructions as a wholely to understand, and regard technical scheme related among each embodiment as the mode that can be combined into different embodiment each other understand protection scope of the present invention.
The above is merely the schematic embodiment of the present invention, is not in order to limit scope of the present invention.Any those skilled in the art, revises and combines the equivalent variations of under the prerequisite that does not break away from design of the present invention and principle, being done, and all should belong to the scope that the present invention protects.