EMITTERS FOR FAST-SPECTRUM SELF-POWERED NEUTRON DETECTOR
20220155472 · 2022-05-19
Inventors
Cpc classification
G21C17/102
PHYSICS
Y02E30/30
GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
International classification
Abstract
A detector for generating an electrical current that is proportional to a flux of neutrons includes a neutron sensitive emitter, a conductive collector, an insulator between the neutron-sensitive emitter and the collector, an electrical connection to the neutron sensitive emitter, and an electrical connection to the conductive collector. The neutron sensitive emitter includes an emitter material with no more than 2 stable isotopes, and which upon impact by a neutron having an energy of from 100 keV to 1000 keV will generate electrons in proportion to the flux of neutrons in less than 10 minutes, and any generated electrons not generated in less than 10 minutes will be generated in no less than 30 days. A method of detecting neutrons generated by a nuclear reactor is also disclosed.
Claims
1. A detector for generating an electrical current that is proportional to a flux of neutrons, comprising: a neutron sensitive emitter; a conductive collector; and, an insulator between the neutron-sensitive emitter and the collector; an electrical connection to the neutron sensitive emitter; an electrical connection to the conductive collector; wherein the neutron sensitive emitter comprises an emitter material with no more than 2 stable isotopes, and which upon impact by a neutron having an energy of from 100 keV to 1000 keV will generate electrons in proportion to the flux of neutrons in less than 10 minutes, and any generated electrons not generated in less than 10 minutes will be generated in no less than 30 days.
2. The detector of claim 1, wherein the neutron-sensitive emitter comprises a Ta alloy.
3. The detector of claim 2, wherein the Ta alloy comprises ASTAR-811C.
4. The detector of claim 2, wherein the Ta alloy comprises T-111.
5. The detector of claim 2, wherein the neutron-sensitive emitter comprises at least one selected from the group consisting of .sup.181Ta, .sup.159Tb, and .sup.169Tm.
6. The detector of claim 2, wherein the neutron-sensitive emitter comprises at least one selected from the group consisting of Lu and Ir.
7. The detector of claim 6, wherein the Lu comprises in the neutron-sensitive emitter is at least one selected from the group consisting of .sup.175Lu and .sup.176Lu.
8. The detector of claim 6, wherein the Ir comprises at least one selected from the group consisting of .sup.191Ir and .sup.193Ir.
9. The detector of claim 1, wherein the detector is configured as a self-powered neutron detector (SPND).
10. The detector of claim 9, wherein the SPND is a prompt-type SPND.
11. The detector of claim 1, wherein the insulator comprises at least one selected from the group consisting of MgO, Al.sub.2O.sub.3, and vacuum.
12. The detector of claim 1, wherein the collector is a sheath with an open interior, and the emitter and the insulator are positioned within the interior.
13. The detector of claim 12, wherein the emitter material is provided on a conductive support mounted within the open interior of the collector sheath, and the insulator is positioned between the emitter material and the collector sheath.
14. The detector of claim 1, wherein the collector comprises stainless steel.
15. The detector of claim 14, wherein the stainless steel is Inconel.
16. The detector of claim 1, wherein the detector provides a signal to noise ratio of greater than 1.5 for neutrons having an energy of between 100 keV and 1000 keV.
17. The detector of claim 1, further comprising a current meter for measuring the electrical current generated by the flux of neutrons striking the emitter.
18. The detector of claim 1, further comprising a processor for relating the current measured by the current meter to the neutron flux.
19. A method of detecting neutrons generated by a nuclear reactor, comprising the steps of: providing a neutron detector comprising a neutron sensitive emitter; a conductive collector; an insulator between the neutron-sensitive emitter and the collector; an electrical connection to the neutron sensitive emitter; an electrical connection to the conductive collector; wherein the neutron sensitive emitter comprises an emitter material with no more than 2 stable isotopes, and which upon impact by a neutron having an energy of from 100 keV to 1000 keV will generate electrons in proportion to the flux of neutrons in less than 10 minutes or more than 30 days; exposing the neutron detector to neutrons having an energy of from. 100 keV to 1000 keV, wherein electrons will be generated by the emitter material in proportion to the flux in less than 10 minutes, and any generated electrons not generated in less than 10 minutes will be generated in no less than 30 days.
20. The method of claim 17, wherein electrons are generated in less than 5 minutes.
21. The method of claim 18, wherein any electron not generated in less than 5 minutes will be generated in no less than 72 days.
22. The method of claim 17, wherein the nuclear reactor is configured as a fast-spectrum nuclear reactor.
23. The method of claim 17, wherein the detector provides a signal to noise ratio of greater than 1.5 for neutrons having an energy of between 100 keV and 1000 keV.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
[0024] There are shown in the drawings embodiments that are presently preferred it being understood that the invention is not limited to the arrangements and instrumentalities shown, wherein:
[0025]
[0026]
[0027]
[0028]
[0029]
[0030]
[0031]
[0032]
[0033]
[0034]
[0035]
[0036]
[0037]
[0038]
[0039]
[0040]
[0041]
[0042]
[0043]
[0044]
[0045]
[0046]
[0047]
[0048]
[0049]
[0050]
[0051]
[0052]
[0053]
[0054]
DETAILED DESCRIPTION OF THE INVENTION
[0055] A detector for generating an electrical current that is proportional to a flux of neutrons includes a neutron sensitive emitter, a conductive collector, an insulator between the neutron-sensitive emitter and the collector, an electrical connection to the neutron sensitive emitter, and an electrical connection to the conductive collector. The neutron sensitive emitter includes an emitter material with no more than 2 stable isotopes, and which upon impact by a neutron having an energy of from 100 keV to 1000 keV will generate electrons in proportion to the flux of neutrons in less than 10 minutes, and any generated electrons not generated in less than 10 minutes will be generated in no less than 30 days. The detector can be configured as a self-powered neutron detector (SPND). The SPND can be a prompt-type SPND.
[0056] The neutron-sensitive emitter can include a Ta alloy. The Ta alloy can be ASTAR-811C. The Ta alloy can be T-111. The neutron-sensitive emitter material can include at least one selected from the group of .sup.181Ta, .sup.159Tb, and .sup.169Tm.
[0057] The neutron-sensitive emitter can also include at least one selected from the group of Lu and Ir. The Lu in the neutron-sensitive emitter can include at least one selected from the group of .sup.175Lu and .sup.176Lu. The Ir can include at least one selected from the group of .sup.191Ir and .sup.193Ir.
[0058] The insulator can include at least one selected from the group of MgO, Al.sub.2O.sub.3, and vacuum. Other insulators are possible.
[0059] The collector can be configured as a sheath with an open interior, and the emitter and the insulation can be positioned within the interior. The emitter material can be provided on a conductive support mounted within the open interior of the collector sheath, and the insulator can be positioned between the emitter material and the collector sheath. The collector can be made of any suitable material. The collector can be made of stainless steel. The stainless steel can be Inconel.
[0060] The detector can provide a signal to noise ratio of greater than 1.5 for neutrons having an energy of between 100 keV and 1000 keV.
[0061] A method of detecting neutrons generated by a nuclear reactor includes the step of providing a neutron detector comprising a neutron sensitive emitter; a conductive collector; an insulator between the neutron-sensitive emitter and the collector; an electrical connection to the neutron sensitive emitter; and an electrical connection to the conductive collector. The neutron sensitive emitter comprises an emitter material with no more than 2 stable isotopes, and upon impact by a neutron having an energy of from 100 keV to 1000 keV will generate electrons in proportion to the flux of neutrons in less than 10 minutes or more than 30 days. The neutron detector is exposed to neutrons having an energy of from 100 keV to 1000 keV. Electrons will be generated by the emitter material in proportion to the flux in less than 10 minutes, and any generated electrons not generated in less than 10 minutes will be generated in no less than 30 days. The electrons generated by the emitter in proportion to the neutron flux can be generated in less than 1 s, 2 s, 3 s, 4 s 5 s, 6 s, 7 s, 8 s, 9 s, 10 s, 20 s, 30 s, 40 s, 50 s, 1 min, 2 min, 3 min, 4, min, 5, min, 6 min, 7 min, 8 min, 9 min, or 10 min, or within a range of any high value and low value selected from these values. Any electron not generated in less than 10 minutes will be generated in no less than 30 days. Any electron not generated in less than 10 min will be generated in no less than 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 49, 50, 51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67, 68, 69, 70, 71, 72 days, or within a range of any high value and low value selected from these values.
[0062] The detector can further include a current meter for measuring the electrical current generated by the flux of neutrons striking the emitter. The detector can further include a processor for relating the current measured by the current meter to the neutron flux.
[0063] For a given neutron to be captured by a nucleus, the nucleus must have a “target” resonance equal to the total neutron energy to which it can excite. If it is desired to maximize the capture of a spectrum of neutrons, it is beneficial that the nuclei have many closely grouped states providing a range of suitable targets at energies that coincide with the peak of the neutron spectrum.
[0064] Nuclear level structure is the macroscopic result of the summation of all possible microscopic couplings of the nucleon wave functions, and an increase in nucleon number (A) will likely result in heightened density of states. A notable exception to the correlation between higher A nuclei and level density occurs around magic numbers because these nuclei are heavily structural in nature. Additionally, odd, especially odd proton number (Z), nuclei are likely to present with increased level densities because the odd nucleon effectively occupies a single particle state above an even-even “core,” forming a valence wave function with more options for coupling. Nuclei with A>150 are likely to be deformed. Deformation also adds to the complexity of the nuclear wave function as it breaks nuclear spherical symmetry, introducing a new quantum number. This new quantum number provides more modes by which nucleons can couple, resulting in level splitting and thus increased level density. It can thus be concluded that suitable emitters are likely to be found in stable, mid-shell, odd Z nuclei located in the region between double magic .sup.132Sn and .sup.208Pb, as highlighted in
[0065] The following equation can be used to calculate the energy group cross sections:
where σ.sup.g.sub.ξ is the microscopic group cross section for energy group g for reaction type ξ, σ.sub.ξ(E) is the microscopic cross section for reaction type (as a function of energy, E.sub.gϵ[E.sub.g-1, E.sub.g] is the corresponding energy range for the analysis domain, and ϕ(E) is the scalar flux. The dominant reaction types are absorption and scattering. The absorption process includes radiative capture and fission reactions, and scattering includes elastic and inelastic scattering.
[0066]
[0067] The macroscopic group cross section for a homogeneous material for reaction ξ, Σ.sup.g.sub.ξ is then calculated via the following expression:
Σ.sub.ξ.sup.g=Nσ.sub.ξ.sup.g, (2)
where N is the atomic number density of the material. For materials with multiple isotopes, this expression is carried out individually for each isotope, and then the cross section is the sum of all corrected by natural abundance percentages. Here, the total macroscopic cross section represents the probability of all possible interactions that neutrons can undergo per unit path length traveled in the medium.
[0068] The reaction rate of type ξ for energy group g as a function of time is calculated by using the following expression:
where N(t) is the atomic number density for the material, and ϕ(E, t) is the scalar flux, both as a function of time. Similarly, the time-dependent burnup rate, b(t), of the emitter material at a given time t is defined as
where σ.sub.a(E) is the neutron absorption cross section for the emitter material. Likewise, the time-integrated burnup, B(t), of the emitter material at a given t is calculated by
[0069] To tune the SPND design for use in a fast reactor and maximize overall detector sensitivity, a generic neutron flux spectrum from an SFR from Verma et al. was used to calculate group microscopic (n,γ) cross sections from ENDF data for a wide range of nuclei. V. Verma, “Self powered neutron detectors as in-core detectors for sodium cooled fast reactors”, Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment 860 (2017) 6-12. Datasets were taken preferentially from ENDF/B-VII.1, ENDF/B-VIII.0, and JEFF-3.3 databases in that order, depending on availability. An example of the result of the process is shown in
[0070] Both full-group (i.e., across the full energy of the reactor neutron spectrum) and fast-group (0.5-2.0 MeV) microscopic and macroscopic cross sections were calculated, as demonstrated in Eq. (1) and Eq. (2), respectively. The reaction rate, as shown in Eq. (3), and burnup per month, as shown in Eq. (5), for the full- and fast-groups was also calculated. The calculated burnup rate for a commonly used emitter material, .sup.103Rh, in a thermal neutron flux was compared to that in literature. The calculated burnup rate was 0.39%, which matched the published value exactly.
[0071] Potential emitter materials were chosen based on several general criteria before being further down-selected by nuclear-physics driven constraints that determine the SPND type. The results from this stage of the analysis indicated rhenium, iridium, osmium, europium, lutetium, tantalum, gadolinium, terbium, tungsten, platinum, palladium, silver, rhodium, technetium, thallium, thulium, ytterbium, erbium, dysprosium, and hafnium as possible candidates. A comparison of the fast-group (n, γ) macroscopic cross sections for a unit volume of material is shown in
[0072] The materials were then selected for survivability within the environment, limiting to materials with melting points above 1,000° C., which eliminated europium and ytterbium. Additionally, elements with one or two stable isotopes were found to render enrichment of emitter materials unnecessary and minimize the complexity of the FS-SPND fabrication. This process further eliminated palladium, osmium, gadolinium, tungsten, erbium, dysprosium, platinum, and hafnium. Platinum as noted is already used as an emitter in SPGDs deployed in CANDU reactors. The final general constraints were that all emitter materials must be available, and readily machinable. The latter criterion excluded highly poisonous materials, such as thallium, and radioactive materials, such as technetium leaving rhenium, iridium, lutetium, tantalum, terbium, silver, rhodium, and thulium, as possible candidates.
[0073] To minimize background noise in prompt-type SPNDs, the reaction product of the neutron-capture reaction in the emitter must have a sufficiently long β decay half-life, preferably at least 30-72 days, to not compete with the primary (γ, e.sup.−) reaction channel. Any β.sup.− decay will introduce a comparatively slow detector response that is effectively an ever-building background component to the signal responding to changes in neutron flux but on a slow enough time scale as to be undesirable. An emitter with a large proportion of nuclei with β decay half-lives of sufficiently short duration could eventually introduce enough background noise that the desired signal could be over-whelmed. Additionally, all prompt-type emitters should have large proton numbers (Z) to maximize the number of electrons available in the material for the signal-producing reaction.
[0074] Alternatively, it is desired that products of the (n, β.sup.−) reaction in delayed-type emitters have as short a β decay half-life as possible preferably less than 10 min. The preference is for a β decay half-life on the order of seconds because the response time of the detector to changes in neutron flux is directly related to the duration of the β decay half-life of the reaction product. The β decay daughter of the reaction product should be stable because, similarly to the prompt-type SPND, β.sup.− decay at this stage would introduce an undesired background noise component to the overall detector response and could dampen the detector response time. Because signal in SPNDs is only produced when electrons reach the collector, it is desirable to elect materials likely to produce higher energy and thus more penetrating β.sup.− particles. For delayed-type SPNDs, this is accomplished by selecting emitter materials with (n, β.sup.−) reaction products that have a large amount of energy available to be released via β.sup.− decay, a factor represented by a high Q.sub.β value, and strong feeding to the ground and lowly-excited states in their respective β− decay daughters.
[0075] These constraints removed rhenium from the list of candidates. As shown in
[0076] Electrical current in both SPND types is also produced through a (γ, e.sup.−) reaction due to interactions with prompt γ flux and γ rays from neutron scattering reactions, the detector response to which is always immediate. To include the effect of these prompt signal components in the emitter selection process, a model of an SPND by using the Monte Carlo simulation toolkit, Geant4 version 10.6.1 was generated. The Geant4 model uses the following physics packages: G4HadronPhysicsQGSP_BIC_HP, G4IonElasticPhysics, G4IonPhysicsXS, G4StoppingPhysics, G4EmStandardPhysics_option4, G4Decay Physics, and G4RadioactiveDecayPhysics.
[0077] Because many of the required cross section data were not in Geant4's G4NDL database, the nuclear cross section database based on ENDF/B-VII.1 data generated for Geant4 were used. This database was expanded by using the AMPX-6 code to broaden the afore-mentioned cross section data for temperatures ranging from 22 to 750° C. to allow an irradiation temperature to be set within the simulation space. The appropriate cross section database, and thus the irradiation temperature, was selected at runtime through the G4NEUTR0NHPDATA environmental variable.
[0078] The Geant4 model was validated by using a rhodium SPND with the detector dimensions shown in Table 1.
TABLE-US-00001 TABLE 1 Dimensions of rhodium SPND used for validation. Component Material R.sub.in (mm) R.sub.out (mm) Length (mm) Emitter .sup.103Rh 0 23 200 Insulator MgO 23 23.25 200 Collector Inconel 600 23.25 23.5 200
[0079] An irradiation temperature of 400° C. was selected, and an impulse beam (released at T=0) of 10.sup.8 thermal neutrons was directed at the emitter. The results showed that 15% of the signal was prompt, falling within the typical range of 7-15% expected for a rhodium SPND.
[0080] Additionally, the response time of the detector was simulated. Because rhodium SPNDs are a delayed-type detector, this quantity is driven by the β decay half-life of .sup.104Rh, which is produced by neutron capture on .sup.103Rh. The delayed portion of response, shown in
[0081] SPNDs with a generic geometry were simulated, assuming natural elemental abundances for each material and an irradiation temperature of 400° C. The insulator and collectors remained unchanged for each simulation, and comprised MgO and Inconel 600, respectively. The detector was set in a simulated pipe filled with magnesium salt. The primary, or incident, particles in the simulation were a spectrum of neutrons and γ rays derived from the neutron flux and prompt γ field for an SFR. Primary particles were formed into a beam and aimed at the emitter to maximize the likelihood of interaction with the emitter of the simulated detector. All particles were emitted as a simulated reactor impulse produced at time T=0 in the simulation space. Reaction products, including reaction chains in cases such as double neutron-capture, were allowed to grow in and decay out within the simulation. The end result of the simulation is a tally of the total number of electrons generated in the emitter. Comparing this number across the selected candidates provides a measure of the relative merit of each material. No attempt to sum electrons in the collector was made because each material will produce a different electron spectrum. As such, the number of electrons that can escape the emitter and travel to the collector will highly depend on emitter and insulator thicknesses and must be optimized for each material.
[0082] Five emitter candidates were identified for prompt-type SPNDs, four of which, are new, and two candidates for delayed-type SPNDs, both of which are currently used emitter materials. The prompt-type emitter materials are shown in Table 2, and the delayed-type materials are shown in Table 3. The results are listed in order of judged suitability based on the fast-group macroscopic (n, γ) cross section, the number and relative abundance of stable isotopes, the β decay half-lives of the reaction products, and expected reaction and burnup rates. Iridium is the only known, if rarely used, emitter in this table. Table 2 includes top emitter candidates for prompt-type SPNDs listed in order of suitability. Σ.sub.γ is the fast-group (n, γ) cross section (0.5-2.0 MeV). T.sub.1/2 represents the β decay half-life of the reaction product, and burnup (B) is calculated at a neutron flux of φ¢=5×10.sup.15 n/cm.sup.2 s for neutron energies between 0.5-2.0 MeV.
TABLE-US-00002 TABLE 2 Isotope
[0083] The burnup rate, b, of the emitter is a strong indicator of the sensitivity of the detector. The B/month from fast-group neutrons with energies between 0.5-2.0 MeV, as shown in Table 2, are comparable with those of rhodium in a thermal neutron field (0.39%). Rhodium is a high-sensitivity emitter when operating in a thermal reactor; thus, the emitter materials are similarly sensitive when operating in a fast-spectrum reactor.
[0084] Table 3 includes top emitter candidates for delayed-type SPNDs listed in order of suitability. Σ.sub.γ, is the fast-group (n,γ) cross section (0.5-2.0 MeV). T.sub.1/2 represents the β decay half-life of the reaction product, and burnup (B) is calculated at the thermal neutron flux of φ=5×10.sup.15 n/cm.sup.2 s for neutron energies between 0.5-2.0 MeV.
TABLE-US-00003 TABLE 3 Nucleus
[0085] The results of the Geant4 simulation that show the number of electrons produced in the emitter in each material per 10.sup.9 events are provided in
[0086] Tantalum produces many electrons per unit volume and is readily available. It is an ideal prompt-type candidate because it has one naturally occurring isotope, .sup.181Ta. The β decay half-life of the (n, γ) reaction product, .sup.182Ta, is 114 days, which is sufficiently long to minimize β− decay as a source of background noise in the detector response function.
[0087] Terbium has one stable isotope, .sup.159Tb, and the neutron-capture reaction product, .sup.160Tb, has a β decay half-life of 72 days with a 100% β.sup.− decay branching ratio, as shown in
[0088] Like tantalum and terbium, thulium is readily available, machinable, and has only one stable isotope, .sup.169Tm. The neutron-capture reaction product, .sup.170Tm, has a suitably long β decay half-life of 128 days.
[0089] Although iridium produces more electrons per unit volume in the expected reactor flux than tantalum, it has two stable isotopes, .sup.191Ir and .sup.193Ir. The reaction chains and relative abundances are shown in
[0090] Lutetium appears to be similar to iridium because it has two stable isotopes: Lu, which is 97.4% abundant, and .sup.176Lu, which is 2.6% abundant.
[0091] The two delayed-type candidates, rhodium and silver, produce a lower number of electrons per unit volume than most of the other prompt-type emitter materials. They are less desirable for use in a fast-nuclear reactor than the prompt-type candidates outlined previously.
[0092] Rhodium is a common emitter in thermal nuclear reactors due to its high sensitivity, and thus it is thoroughly characterized.
[0093] Rhodium has only one stable isotope: .sup.103Rh; the decay chain is shown in
[0094] Silver not only produces less electrons per unit volume but it also has two stable isotopes, .sup.107Ag and .sup.109Ag, as shown in
[0095] Through a thorough analysis of ENDF cross section data, five prompt-type candidate emitter materials were determined as suitable for fast-spectrum reactors: tantalum, terbium, thulium, lutetium, and iridium. Iridium is a previously known, although rarely used, emitter. The most promising candidates are tantalum, terbium, and thulium, listed in order of suitability. Also identified were two commonly used delayed-type emitters as suitable for use in a fast-reactor spectrum: rhodium and silver. Calculations indicate that the prompt-type emitters described herein outperform the delayed-type.
[0096] The calculated burn up rates and Geant4 simulations for the chosen prompt-type emitter candidates in a fast reactor flux are comparable with those of existing high-sensitivity emitters operating in thermal-neutron fluxes. Therefore, it is expected that each of the identified prompt-type candidates to produce a suitably sensitive detector for the application.
[0097] There is shown in
[0098] A schematic circuit diagram is shown in
[0099] There is shown in
[0100] The invention as shown in the drawings and described in detail herein disclose arrangements of elements of particular construction and configuration for illustrating preferred embodiments of structure and method of operation of the present invention. It is to be understood however, that elements of different construction and configuration and other arrangements thereof, other than those illustrated and described may be employed in accordance with the spirit of the invention, and such changes, alternations and modifications as would occur to those skilled in the art are considered to be within the scope of this invention as broadly defined in the appended claims. In addition, it is to be understood that the phraseology and terminology employed herein are for the purpose of description and should not be regarded as limiting.