CN116487079B - Method for qualitatively testing nuclear fuel microcell burnup based on electronic probe - Google Patents

Method for qualitatively testing nuclear fuel microcell burnup based on electronic probe Download PDF

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CN116487079B
CN116487079B CN202310343900.5A CN202310343900A CN116487079B CN 116487079 B CN116487079 B CN 116487079B CN 202310343900 A CN202310343900 A CN 202310343900A CN 116487079 B CN116487079 B CN 116487079B
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burnup
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CN116487079A (en
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斯嘉轩
伍晓勇
方忠强
滕常青
毛建军
李佳文
张伟
吴璐
温榜
王桢
辛虹阳
何文
孔祥刚
信天缘
宋小蓉
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Nuclear Power Institute of China
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    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21CNUCLEAR REACTORS
    • G21C17/00Monitoring; Testing ; Maintaining
    • G21C17/06Devices or arrangements for monitoring or testing fuel or fuel elements outside the reactor core, e.g. for burn-up, for contamination
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N23/00Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00
    • G01N23/22Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material
    • G01N23/225Investigating or analysing materials by the use of wave or particle radiation, e.g. X-rays or neutrons, not covered by groups G01N3/00 – G01N17/00, G01N21/00 or G01N22/00 by measuring secondary emission from the material using electron or ion
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    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract

The invention discloses a qualitative test method for nuclear fuel microcell burnup based on an electronic probe, which comprises the following steps: obtaining the burnup of a nuclear fuel sample; measuring the content of fission element neodymium in at least two areas to be measured on the surface of the nuclear fuel sample based on an electronic probe, counting to obtain the average neodymium content of the nuclear fuel sample, and establishing the association relation between the burnup of the nuclear fuel sample and the average neodymium content; on the basis, the neodymium content of the micro-area on the surface of the nuclear fuel sample is measured through an electronic probe, and the burnup of the micro-area can be calculated according to the association relation. The neodymium content of the micro-area of the nuclear fuel can accurately respond to the burnup of the micro-area, the electronic probe has high test precision, no damage to a sample and short test time, so that the method can accurately, conveniently and efficiently obtain the micro-area burnup of the nuclear fuel.

Description

Method for qualitatively testing nuclear fuel microcell burnup based on electronic probe
Technical Field
The invention relates to a technology for testing nuclear fuel burnup after irradiation, in particular to a method for qualitatively testing nuclear fuel microcell burnup based on an electronic probe.
Background
Currently the dominant types of nuclear fuels are dispersion fuels and rod fuels. For the dispersion fuel, the mixing is uneven in the manufacturing process, the volume difference of local fuel phases is larger, and the aggregation of fuel particles is further aggravated in the rolling process, so that the neutron flux is unevenly distributed in space in the service period, and the burning of different micro areas in the fuel is different. This can result in the burnup at some locations having exceeded the design threshold being a weak point of the fuel, even though the overall burnup of the fuel is low. For pressurized water reactor rod fuels, the microcell burnup of the pellet edge fuel is much higher than the center region of the pellet due to neutron space self-shielding effect. The burnup at the micro-area in the fuel after irradiation is directly related to the micro-morphology, composition, structure and performance of the micro-area, so that the method has important significance in testing the burnup at the micro-area of the fuel.
However, the existing burnup test method comprises the steps of firstly obtaining a fuel surface identification fissile nuclide counting distribution diagram through gamma scanning, then cutting a plurality of samples with different counts on the fuel, dissolving the samples with acid, adopting a mass spectrometry method to test the accurate content of the fissile nuclides, further obtaining the burnup of the samples, establishing the association relation between the burnup of the samples and the average value of the count of the samples, and finally calculating the burnups of other positions according to the association relation and the count values at other positions. However, the range of the gamma scanning acquisition signal is large, the testing precision is low (millimeter level), the testing requirement of the micro-area burnup cannot be met, and no practical method for acquiring the nuclear fuel micro-area burnup after irradiation is available at present.
Disclosure of Invention
The invention aims to provide a qualitative test method for nuclear fuel microcell burnup based on an electronic probe, which solves the problem that the practical method for obtaining the nuclear fuel microcell burnup after irradiation is not available at present.
The invention provides a method for qualitatively testing nuclear fuel microcell burnup based on an electronic probe, which comprises the following steps:
obtaining the burnup of a nuclear fuel sample;
measuring the neodymium content of at least two areas to be measured in a fuel phase on the surface of the nuclear fuel sample based on the electronic probe, and counting to obtain the average neodymium content of the nuclear fuel sample, so as to obtain the ratio of the burnup of the nuclear fuel sample to the average neodymium content;
and measuring the neodymium content of the micro-zone on the surface of the nuclear fuel sample based on the electronic probe, and calculating the burnup of the micro-zone according to the ratio and the neodymium content of the micro-zone. The specific calculation formula is shown as formula (1):
wherein: BU is micro-area burnup; BU (BUs) S Average neodymium content of the sample; w (Nd) S Average burn-up for the sample; w (Nd)) Is the neodymium content at the micro-region.
The invention has the beneficial effects that:
1. the fission product neodymium element basically does not migrate in the fuel, does not volatilize, and is thermally neutron-induced in the nuclear fuel 239 Pu、 241 Pu、 235 Caused by U fission and fast neutrons 238 The U fission can generate neodymium, so that the neodymium content of the fission product can accurately reflect the burnup of the irradiated nuclear fuel micro-region, and meanwhile, the fission yield of neodymium element is high, so that the detection is convenient, and the burnup of the nuclear fuel is obtained by detecting the neodymium element.
2. Because the electronic probe has high test precision, no damage to the sample and short test time, the micro-area burnup of the nuclear fuel can be accurately, conveniently and efficiently obtained.
3. The area of the X-ray excitation area of the electronic probe can be as small as 1 square micron, so that the acquisition scale of burnup is greatly reduced.
As a possible preferred way, the sum of the areas to be measured covers 50% of the surface area of the fuel phase of the nuclear fuel sample, in which a spot is tested at 50 μm intervals, further ensuring the accuracy of the measurement results.
As a possible preferred mode, each area to be tested only covers the fuel phase matrix of the nuclear fuel sample, so that the influence of grain boundaries, air holes, cracks and the like on the detection result is avoided, and the accuracy of the detection result is ensured.
As one possible implementation, the electronic probe test employs spot scanning. The fuel phase matrix is subjected to point scanning under the conditions of the amplification factor of 9000-11000X, the accelerating voltage of 15-25 Kv and the beam current of 150-200 nA, and the point scanning test time is 4-6 min.
As a possible implementation, when the nuclear fuel is in a rod shape, one test point is selected at intervals of 100-150 μm from the center of the sample to the edge of the sample along the radial direction of the nuclear fuel sample. In particular, a scanning point is selected every 30-50 μm in the heavy structure area at the edge of the pellet, so as to ensure that the relatively accurate average neodymium content of the rod-type fuel sample is obtained.
As a possible implementation manner, when the nuclear fuel is in a dispersion type, 4-6 fuel particles are selected at the peripheral edges of the nuclear fuel sample, 6-8 fuel particles are selected in the central region of the sample according to the interval distance of 400-600 mu m, and an electronic probe point scanning test is performed on the central position of each fuel particle and the position 8-10 mu m away from the edges of the fuel particles, so that the relatively accurate average neodymium content of the dispersion type fuel sample is ensured.
The diameter of the micro-regions is in the order of micrometers.
As a possible implementation manner, obtaining burnup of the nuclear fuel sample specifically includes:
acquisition of the nuclear fuel fissile nuclides by gamma scanning 137 Characteristic gamma count profile of Cs;
cutting at least 2 samples of nuclear fuel from the nuclear fuel with different average gamma counts;
after each of the nuclear fuel samples is dissolved with an acid, the fissile nuclides are tested by a mass spectrometer (fissile nuclides are typically selected from 145 Nd、 146 Nd、 148 Nd or 235 U) accurate content, and further obtaining the burnup of the known counting nuclear fuel sample;
establishing nuclear fuel burn-up 137 The correspondence between the characteristic gamma counts of Cs;
and cutting a sample from the nuclear fuel again, and calculating to obtain the burnup of the nuclear fuel sample according to the average gamma count of the nuclear fuel sample and the corresponding relation.
Drawings
FIG. 1 is a graph showing a gamma scanning count profile of a U-Mo dispersion fuel in an example;
FIG. 2 is a schematic illustration of fuel particles selected for electron probe testing in a U-Mo dispersion fuel core of an example;
FIG. 3 is a plot of electron probe spot scanning test areas within U-Mo fuel particles in an example.
Detailed Description
In order to make the technical problems, technical schemes and beneficial effects to be solved more clear, the invention is further described in detail below. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the scope of the invention.
The inventor of the invention finds that when the existing burnup test method is adopted, the burnup in the micrometer scale range of the nuclear fuel cannot be effectively obtained due to the large range of the gamma scanning acquisition signal and low test precision (millimeter level).
The inventor of the present invention found in searching for a device capable of measuring the burnup of a nuclear fuel that neodymium (Nd) element, which is a product of fission of the nuclear fuel, is mainly dissolved in the nuclear fuel in an oxidized state, ignoring movement caused by non-thermal influence such as cracking fragments and neutron collisions during irradiation, nd does not migrate or volatilize in the nuclear fuel, and is also contained in the nuclear fuel due to thermal neutrons 239 Pu、 241 Pu、 235 Caused by U fission and fast neutrons 238 Nd can be generated by U fission, so that Nd element can accurately reflect burnup of nuclear fuel; the inventors of the present invention have therefore set out how to accurately measure Nd element content in a nuclear fuel micro-region to obtain burnup at the nuclear fuel micro-region. The inventor finds that the electron probe can be used for accurately measuring the neodymium content in the micro-area of the nuclear fuel, the diameter of the micro-area which can be tested by the electron probe is smaller than 1 micron, the nuclear fuel sample is not damaged, the test time is short, and the micro-area burnup of the nuclear fuel can be accurately, conveniently and efficiently obtained.
The invention discloses a qualitative test method for nuclear fuel micro-area burnup based on an electronic probe, wherein the micro-area refers to an area with a diameter of micron order; as used herein, the term "burnup" refers to the amount of nuclear fuel consumed during operation of the reactor, and as used herein, the term "amount" refers to 235 U、 239 Atomic number of fissionable nuclides such as Pu.
A qualitative test method for nuclear fuel microcell burnup based on an electronic probe comprises the following steps:
s1, acquiring the burnup of a nuclear fuel sample;
in the invention, the specific method for obtaining the burnup of the nuclear fuel sample can be as follows:
s1-1: acquisition ofThe nuclear fuel 137 The Cs fissile nuclide gamma counting distribution map can be obtained by adopting a gamma scanning method;
s1-2: selecting and cutting at least 2 nuclear fuel samples with different average gamma count values from the nuclear fuel, dissolving and measuring the burnup of the nuclear fuel samples, and establishing a relation between the burnup and the average gamma count values;
in the invention, at least 2 nuclear fuel samples with different average gamma count values can be selected and obtained by cutting according to the obtained gamma count distribution map. In view of the radioactivity problems during subsequent dissolution and burn-up by mass spectrometry, the sample needs to be as small as possible, suitably the length, width and height of the sample may be 3mm x 2mm.
In the present invention, the dissolution is to measure burnup of the nuclear fuel sample, and the dissolution agent may be aqua regia (concentrated hydrochloric acid: concentrated nitric acid=3:1 (volume ratio)).
In the present invention, the nuclear fuel sample may be tested for fissile nuclides using ICP-MS mass spectrometry (generally selected from 145 Nd、 146 Nd、 148 Nd or 235 And U) accurate content, and further calculating to obtain the burnup of the nuclear fuel sample.
And establishing a corresponding relation between the burnup and the average gamma count value.
S1-3: and then 1 nuclear fuel sample is selected and cut from the nuclear fuel for the electron probe micro-area burnup test.
The length, width and height of the nuclear fuel sample can be 2-4 mm, 3-6 mm and 1-3 mm respectively. Suitably may be 3mm by 6mm by 2mm.
S2, measuring the neodymium content of at least two areas to be measured on the surface of the nuclear fuel sample based on an electronic probe, and counting to obtain the average neodymium content of the nuclear fuel sample, so as to obtain the ratio of the burnup of the nuclear fuel sample to the average neodymium content;
in the invention, before the nuclear fuel sample is measured by adopting the electronic probe, the nuclear fuel sample can be inlaid and then subjected to grinding, polishing and vacuum coating processing, wherein the technological parameters in the grinding, polishing and vacuum coating processing processes are conventional numerical values or can be obtained by a person skilled in the art without the need of creative labor, so that the nuclear fuel sample is not described in detail herein; and fixing the processed nuclear fuel sample on the electronic probe sample holder through conductive adhesive.
In the invention, the sum of areas of the areas to be measured covers 50% of the fuel phase surface area of the nuclear fuel sample, and in the area to be measured, one point is measured at intervals of 50 mu m, thereby being beneficial to improving the measurement accuracy.
In the invention, when selecting the region to be measured, the regions such as grain boundary, air hole, crack and the like are preferably avoided so as not to have adverse effect on the measurement result, namely, the substrate of the nuclear fuel is preferably only subjected to electron probe test, and the measured result can be corrected by adopting ZAF (atomic number effect, absorption effect and fluorescence excitation effect coverage) correction theory.
In the invention, when the nuclear fuel sample is in a rod shape, in order to obtain more accurate neodymium content, a scanning point is selected from the center of the nuclear fuel sample to the edge of the nuclear fuel sample at intervals of 100-150 mu m, and a scanning point is selected from a heavy structure area at the edge of the nuclear fuel sample at intervals of 30-50 mu m.
In the invention, when the nuclear fuel sample is in a dispersion type, in order to obtain more accurate Nd content, 4-6 fuel particles are respectively selected at the inner peripheral edge of the nuclear fuel sample, 6-8 fuel particles are selected in the central region of the core body according to the interval distance of 100-150 mu m, and an electronic probe point scanning test is carried out on the central position of each fuel particle and the position 8-10 mu m away from the edge of the fuel particle.
In the invention, the electron probe can be spot scanning, the amplification factor of the electron probe is 9000-11000, suitably 10000, the acceleration voltage is 15-25 Kv, suitably 20Kv, the beam current is 150-200 nA, suitably 200nA, and the counting time is 4-6 min, suitably 5min.
S3, measuring the neodymium content of the micro-zone on the fuel phase surface of the nuclear fuel sample based on an electronic probe, and calculating the burnup of the micro-zone according to the ratio and the neodymium content of the micro-zone.
And (3) calculating the burnup of the micro-area according to the ratio obtained in the step (S2) and the neodymium content of the micro-area, wherein the detailed calculation formula is shown in the formula (1).
The method for qualitatively testing the fuel consumption of the nuclear fuel micro-area based on the electronic probe has the characteristics of high measurement precision, short required time and no damage to the nuclear fuel sample, and has good application prospect in the nuclear fuel field.
Example 1
The method for qualitatively testing the nuclear fuel microcell burnup based on the electronic probe comprises the following steps:
(1) Gamma scanning is carried out on the irradiated U-Mo dispersed fuel to obtain a gamma counting distribution diagram of the fuel, as shown in figure 1;
(2) According to the gamma scanning result, two samples with different average gamma counts (the size is 3mm multiplied by 2mm, for convenience of description, the samples are marked as a sample No. 1 and a sample No. 2) are selected and cut, and after the samples are dissolved by aqua regia, ICP-MS mass spectrometry is adopted to test the burnup, and in addition, a piece of 3mm multiplied by 6mm multiplied by 2mm is selected and cut for testing the micro-area burnup by an electronic probe (for convenience of description, the samples are marked as a sample No. 3);
(3) According to the average gamma counts of the samples 1 and 2 and the burnup, establishing a relation between the burnup and the average gamma count value, wherein the gamma count 63 represents the burnup of 5.0%;
(4) According to the relation obtained in the step (3), since the average gamma count of the sample No. 3 is known to be 48, the burnup of the sample No. 3 can be calculated from the relation in the step (3) to be 3.81%;
(5) After embedding the sample No. 3, grinding, polishing and vacuum coating, and fixing the sample on an electronic probe sample holder through conductive adhesive for detection;
(6) Adopting an electronic probe to respectively select 4 fuel particles in a sample No. 3 near the peripheral edge, selecting 6 fuel particles in the central area of the core body according to the interval of 150 mu m, carrying out Nd element test by the electronic probe, and distributing 10 fuel particles as shown in figure 2;
(7) The center position of each fuel particle and the position at an arbitrary distance of 10 μm from the edge of the particle were respectively subjected to a point scan, as shown in fig. 3, the parameters of the point scan were as follows: the accelerating voltage is 20Kv, the beam current is 200nA, the counting time is 5min, the testing process needs to avoid the areas such as grain boundary, air hole, crack and the like, only the fuel matrix is tested, the obtained semi-quantitative result is corrected by ZF4 to obtain Nd content test values, all Nd content test values are averaged, and the average Nd content of a sample is 1.08wt%;
(8) Nd content at any micro-region on sample No. 3 surface was then tested using an electron probe and found to be 1.02wt%. The micro-zone burnup of 3.60% at the position is calculated according to the ratio of the average Nd content of 1.08wt% of the sample to the sample burnup of 3.81%, and the specific calculation formula is as follows:
wherein: BU is micro-area burnup; BU (BUs) S Average neodymium content (1.08 wt%) of the sample; w (Nd) S Average burn-up for sample (3.81%); w (Nd) is the neodymium content (1.02 wt%) at the domain.
The foregoing description of the embodiments has been provided for the purpose of illustrating the general principles of the invention, and is not meant to limit the scope of the invention, but to limit the invention to the particular embodiments, and any modifications, equivalents, improvements, etc. that fall within the spirit and principles of the invention are intended to be included within the scope of the invention.

Claims (6)

1. A method for qualitatively testing nuclear fuel microcell burnup based on an electronic probe, the method comprising:
the burnup of the nuclear fuel sample is obtained, and the method is as follows:
obtaining nuclear fuel by gamma scanning method 137 Cs fissile nuclide gamma count profile;
selecting and cutting at least 2 nuclear fuel samples with different average gamma count values according to the obtained gamma count distribution map, dissolving and measuring the exact fissile nuclide content of the nuclear fuel samples tested by adopting an ICP-MS mass spectrometry, further calculating and obtaining the burnup of the nuclear fuel samples, and establishing the relation between the burnup and the average gamma count values; the dissolving agent used in the dissolution is aqua regia, and the aqua regia consists of concentrated hydrochloric acid and concentrated nitric acid with the volume ratio of 3:1;
measuring the neodymium content of at least two areas to be measured in a fuel phase on the surface of the nuclear fuel sample based on an electronic probe, and counting to obtain the average neodymium content of the nuclear fuel sample, so as to obtain the ratio of the burnup of the nuclear fuel sample to the average neodymium content;
measuring the neodymium content of the micro-area on the surface of the nuclear fuel sample based on an electronic probe, and calculating the burnup of the micro-area according to the ratio and the neodymium content of the micro-area;
the specific calculation formula of the micro-area burnup is shown as the formula (1):
wherein: BU is micro-area burnup; BU (BUs) S Average neodymium content of the sample; w (Nd) S Average burn-up for the sample; w (Nd) is the Nd content at the micro-region.
2. The method for qualitatively testing nuclear fuel micro-zone burnup based on an electronic probe according to claim 1, wherein the electronic probe test is: the fuel phase matrix is subjected to point scanning under the conditions of the amplification factor of 9000-11000X, the accelerating voltage of 15-25 Kv and the beam current of 150-200 nA, and the point scanning time is 4-6 min.
3. The method for qualitatively testing nuclear fuel micro-zone burnup based on an electronic probe according to claim 1, wherein when the nuclear fuel is in a rod shape, one test point is selected from the center of the sample to the edge of the sample at intervals of 100-150 μm along the radial direction of the nuclear fuel sample; the region of the heavy structure at the edge of the pellet is selected as a scan spot every 30-50 μm apart.
4. The method for qualitatively testing nuclear fuel micro-zone burnup based on an electronic probe according to claim 1, wherein when the nuclear fuel is in a dispersion form, 4-6 fuel particles are selected at the peripheral edges of the nuclear fuel sample, 6-8 fuel particles are selected at the central area of the sample according to the interval distance of 400-600 μm, and an electronic probe point scan test is performed on the central position of each fuel particle and the position 8-10 μm away from the edges of the fuel particles.
5. The method for qualitatively testing nuclear fuel micro-segment burnup based on electronic probes according to claim 1, wherein the micro-segment has a diameter of micron order.
6. The method for qualitatively testing nuclear fuel micro-zone burnup based on an electronic probe according to claim 1, wherein the specific burnup method for obtaining a nuclear fuel sample comprises the following steps:
acquisition of the nuclear fuel fissile nuclides by gamma scanning 137 Characteristic gamma count profile of Cs;
cutting at least 2 samples of nuclear fuel from the nuclear fuel with different average gamma counts;
after each nuclear fuel sample is dissolved by acid, testing the accurate content of fissile nuclides by a mass spectrometer, and further obtaining the burnup of the known count nuclear fuel sample;
establishing nuclear fuel burn-up 137 The correspondence between the characteristic gamma counts of Cs;
and cutting a sample from the nuclear fuel again, and calculating to obtain the burnup of the nuclear fuel sample according to the average gamma count of the nuclear fuel sample and the corresponding relation.
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朱荣保,杨留成,吕峰,张琴芬.由~(137)Cs,~(144)Ce和~(148)Nd为监测体测定燃耗中的辐照史校正方法.原子能科学技术.1985,(第03期),全文. *
燃料元件破坏性燃耗测量过程的质量控制;梁帮宏;苏冬萍;张劲松;陈云明;李兵;李顺涛;冯伟伟;;原子能科学技术(第04期);全文 *
秦山核电站考验元件燃耗的辐照史校正计算;杨留成, 朱荣保, 金华晋, 朱焕南, 江金才;原子能科学技术(第04期);全文 *

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