CN115094351B - Depleted uranium-based hydrogen absorption and storage alloy and method - Google Patents
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Abstract
The invention discloses a depleted uranium-based hydrogen absorption and storage alloy and a method thereof, wherein the hydrogen absorption and storage alloy is prepared by doping gamma-phase depleted uranium with nickel, and the content of U in the uranium-nickel hydrogen storage alloy is as follows: the Ni atomic ratio is 7: (1-3), the doping sites of the Ni atoms comprise the interior and the face center of the uranium-depleted super-cell, and the ratio of U: the Ni atomic ratio is 8: (0.5-1.5), the doping sites of Ni atoms are in the depleted uranium super-crystal cells, and the hydrogen absorption and storage alloy has excellent hydrogen storage and storage isotope properties, not only plays a role in promoting the development of hydrogen energy, but also plays a role in promoting the development and progress of a large-scale hydrogen isotope storage and supply system in a nuclear fusion reactor; meanwhile, the invention realizes resource utilization of a large amount of depleted uranium generated in the nuclear fuel industry, and makes a contribution to sustainable green development of nuclear energy.
Description
Technical Field
The invention belongs to the technical field of hydrogen energy and nuclear waste treatment, and particularly belongs to a depleted uranium-based hydrogen absorption and storage alloy and a method.
Background
Depleted uranium is a by-product of nuclear fuel production processes, and because of its radioactivity, its handling and storage is a recognized problem. Along with the popularization and development of nuclear power technology. The demand for nuclear fuel has increased and a large accumulation of by-product depleted uranium has occurred. The resource utilization of the depleted uranium is an effective means for treating the depleted uranium byproduct.
The uranium can react with hydrogen and isotopes thereof to produce uranium hydride at normal temperature, so that the uranium can be used as a solid-state hydrogen storage material. The hydrogen storage method has certain advantages when being applied to hydrogen storage, such as low hydrogen adsorption pressure, high hydrogen absorption rate and capability of realizing higher volume hydrogen storage, and the volume hydrogen storage is almost more than twice of that of a liquid hydrogen storage mode. The uranium material can simultaneously realize the storage of hydrogen and isotopes thereof, and the decomposition temperatures of hydrides of the hydrogen and the isotopes thereof have differences, so that the purification and separation of the hydrogen and the isotopes thereof can be realized based on the differences; although the application of the depleted uranium to the solid-state hydrogen storage material has great advantages, the depleted uranium has certain disadvantages, hydride of the depleted uranium is easy to pulverize, the volume expansion rate before and after hydrogen absorption and storage is up to more than 75%, and the working temperature of hydrogen release is also high, so that a scheme for improving the performance of the depleted uranium-based hydrogen absorption and storage alloy needs to be researched.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides a depleted uranium-based hydrogen absorption and storage alloy and a method thereof.
In order to achieve the purpose, the invention provides the following technical scheme: a depleted uranium-based hydrogen storage alloy prepared by doping a gamma-phase depleted uranium with nickel, U: the Ni atomic ratio is 7: (1-3) the doping sites of the Ni atoms comprise the inner part and the face center of the uranium-depleted super cell.
Further, in the hydrogen absorption and storage alloy, the ratio of U: the Ni atomic ratio is 7:3.
the invention also provides a depleted uranium-based hydrogen absorption and storage alloy which is prepared by doping gamma-phase depleted uranium with nickel, wherein U: the Ni atomic ratio is 8: (0.5 to 1.5) the doping site of the Ni atom is inside the uranium-depleted super cell.
Further, in the hydrogen absorption and storage alloy, the ratio of U: the Ni atomic ratio is 8:1.
the invention also discloses a design method of the depleted uranium-based hydrogen absorption and storage alloy, and the structure of the uranium-nickel alloy is designed and calculated through a first principle.
Further, the specific design steps are as follows:
s1, determining the atomic ratio of U and Ni, carrying out cell expansion based on a U unit cell to obtain a super unit cell, and carrying out Ni atom doping at different positions around the U atom to obtain an initial structure of a target alloy;
s2, the initial structure of the target alloy is subjected to relaxation and electronic static self-consistency, and the total energy is selected to be less than 1.0 multiplied by 10 -6 eV/atom, stress per atom lower than
The structure of (2) is used as an optimized structure of the uranium nickel alloy;
s3, screening the optimized structure under the same atomic ratio to obtain uranium-nickel alloy and uranium-nickel alloy hydride with the optimized structure under the atomic ratio;
s4, screening the uranium-nickel alloy with the optimal structure under different atomic proportions, selecting the uranium-nickel alloy as the hydrogen absorption and storage alloy, wherein the formation energy of the uranium-nickel alloy is less than 0.2, the volume expansion rate of the uranium-nickel alloy after hydrogen absorption is less than that of pure uranium after hydrogen absorption, and the uranium-nickel alloy with the reduced hydrogen release thermodynamic equilibrium temperature of the uranium-nickel alloy hydride is used as the hydrogen absorption and storage alloy.
Further, the volume expansion rate η of the hydrogen absorption and storage alloy is calculated according to the following formula:
wherein, V hydrid Volume, V, of uranium alloy/pure uranium hydride alloy,metak Representing the volume of uranium alloy/pure uranium.
Further, the suctionThermodynamic equilibrium temperature T of hydrogen storage alloy d Is represented as follows:
T d ＝ΔH/ΔS
where Δ H is the enthalpy change of the dehydrogenation reaction and Δ S is the entropy change of the dehydrogenation reaction.
Compared with the prior art, the invention has at least the following beneficial effects:
the invention provides a depleted uranium-based hydrogen absorption and storage alloy and a method, which realize the resource utilization of gamma-phase depleted uranium generated in the nuclear fuel industry and make contribution to the sustainable green development of nuclear energy, wherein after Ni is doped in a gamma-phase uranium crystal, the unit cell volume is reduced, the size of a lattice gap is reduced, the stability of hydrogen in the gap is reduced, and the dissociation equilibrium pressure is increased, so that the hydrogen release is facilitated, and the doping of Ni does not cause the huge change of the electronic structure of uranium, so that the hydrogen absorption capacity of the uranium is maintained; the Ni element is low in price, and the doping of the Ni element can effectively reduce the volume expansion rate and reduce the thermodynamic equilibrium temperature; therefore, the hydrogen absorbing and storing alloy has excellent hydrogen storing and hydrogen storing isotope performance, not only plays a role in promoting the development of hydrogen energy, but also plays a role in promoting the development and progress of a large-scale hydrogen isotope storage and supply system in a nuclear fusion reactor.
The invention provides a depleted uranium-based hydrogen absorption and storage alloy and a method, wherein the optimal atomic ratio of a uranium-nickel alloy is 7:3 or 8:1, the doping amounts of Ni in the two proportions are greatly different, but the volume expansion rate and the hydrogen release temperature are both obviously reduced, compared with a pure uranium material with the same uranium content, the uranium-nickel alloy with the atomic ratio of 7:3 has the advantages that the volume expansion rate is obviously reduced to 43.5 percent, and the thermodynamic equilibrium temperature of hydrogen release is as low as 541K; compared with a pure uranium material with the same uranium content, the uranium-nickel alloy with the atomic ratio of 8:1 has the volume expansion rate of 52.9 percent, the thermodynamic equilibrium temperature of hydrogen release is as low as 543K, the uranium-nickel alloy shows excellent hydrogen storage and storage performance, and has wide application prospects in hydrogen storage and hydrogen isotopes.
Drawings
FIG. 1 is a diagram showing the relationship between the volume expansion rate and the hydrogen storage capacity of a uranium nickel alloy with the atomic ratio of U to Ni of 8:1.
FIG. 2 is a graph showing the relationship between the volume expansion rate and the hydrogen storage capacity of a uranium nickel alloy with the atomic ratio of U to Ni of 7:3.
In FIG. 3, the hydrogen release temperature Td of the uranium alloy with different hydrogen absorption amounts is shown.
FIG. 4 is a structural diagram of a micro crystal of a uranium nickel alloy with the atomic ratio of U to Ni of 7:3.
Detailed Description
The invention is further described with reference to the following figures and detailed description.
Alloying is an effective scheme for improving the performance of the uranium material, and can effectively improve the corrosion resistance of the material and the dimensional stability; the gamma-phase uranium alloy has a highly symmetrical body-centered cubic structure, has isotropy, has good thermal conductivity in all directions, and is an ideal state for synthesizing the hydrogen storage material, but the gamma-phase uranium cannot stably exist at room temperature; the depleted uranium-based hydrogen storage alloy provided by the invention adopts depleted uranium as a raw material and is doped with nickel elements, and the obtained uranium-nickel hydrogen storage alloy has the following characteristics that (1) nickel is a metal with abundant reserves, low price and better corrosion resistance, can form an alloy with various elements, and has extremely high solid solubility in gamma-phase uranium: the Ni atomic ratio is 7: (1 to 3) or 8: (0.5-1.5), the uranium nickel alloy can overcome the problems and defects of expansion and pulverization and the like of pure uranium hydrogen storage, and is suitable for storing hydrogen and hydrogen isotopes as the hydrogen storage alloy.
Preferably, the atomic radius of nickel is 0.123nm, the atomic radius of uranium is 0.156nm, and as the radius of Ni atoms is smaller than that of U atoms, the atomic ratio of U is 8:1, the Ni atoms are doped in the superlattice of U atoms in a gap doping mode, and the doping sites are positioned inside the depleted uranium superlattice; under the atomic ratio of U to Ni of 7:3, ni atoms are doped in the U atom super-crystal cell in a mode of combined action of gap doping and substitution doping, and doping sites comprise the inner part and the face center of the uranium-depleted super-crystal cell.
Preferably, interstitial doping is the insertion of nickel atoms directly into interstitial sites in the uranium unit cell, with tetrahedral sites and octahedral sites being common doping sites.
The invention also discloses a design method of the depleted uranium-based hydrogen absorption and storage alloy, and particularly relates to a method for designing and calculating based on a first nature principle, wherein the first nature calculation is based on the interaction between atomic nucleus and electrons, and a microstructure is obtained by solving Schrodinger wave equation from the basic principle of quantum mechanics, so that the physical properties and the chemical properties of a system are obtained through other treatments. Because the direct solution of the multi-electron system Schrodinger equation has great solution difficulty, the direct solution of the multi-electron system Schrodinger equation is simplified to finally form a density functional theory, and the design of the depleted uranium-based hydrogen absorption and storage alloy is carried out on the basis of the density functional theory, and the design method comprises the following steps:
1. firstly, cell expansion is carried out according to the atomic ratio of a target alloy, a gamma-phase uranium crystal is BCC (body centered cubic) structure, and a Supercell is obtained through cell expansion of 2 x 1.
Determining the number and the types of U atoms at different sites in the super cell, adjusting the size of the crystal lattice of the gamma-uranium 2 x 1 super cell, and doping Ni atoms at different positions around the U atoms to obtain an initial structure.
2. Selecting proper parameters according to the material properties, the basic principle of quantum mechanics and the required experimental precision, and performing relaxation and electronic static self-consistency on the initial structure of the target alloy obtained in the step 1 by using VASP software to obtain the total energy less than 1.0 multiplied by 10 -6 eV/atom, each atom being subjected to a force lower than
The optimized structure of the target alloy of (1);
3. screening the optimized structures in the same atomic ratio to obtain the optimal structures in the atomic ratio, optimizing and calculating the hydride of the uranium-nickel alloy with the optimal structure to obtain the uranium-nickel alloy and the hydride of the uranium-nickel alloy with the optimal structures in the same atomic ratio;
preferably, the optimized structures under the same atomic proportion are screened according to the energy minimum principle;
4. screening the uranium-nickel alloy with the optimal structure under different atomic proportions, and selecting the uranium-nickel alloy as the hydrogen absorption and storage alloy, wherein the formation energy of the uranium-nickel alloy is less than 0.2, the volume expansion rate of the uranium-nickel alloy after hydrogen absorption is less than that of pure uranium after hydrogen absorption, and the uranium-nickel alloy with the reduced hydrogen release thermodynamic equilibrium temperature of the hydride of the uranium-nickel alloy is used as the hydrogen absorption and storage alloy.
5. The volume expansion rate and the hydrogen storage and release performance of the obtained hydrogen absorption and storage alloy are verified:
the thermodynamic property of the hydrogen storage alloy for storing and releasing hydrogen passes through the thermodynamic equilibrium temperature T d (hydrogen evolution initiation temperature/K) is expressed as:
T d ＝ΔH/ΔS
where Δ H is the enthalpy change of the dehydrogenation reaction and Δ S is the entropy change of the dehydrogenation reaction.
UH 3 After the small atomic radius Ni is dissolved in the medium solid solution, the unit cell volume is reduced, the size of a crystal lattice gap is reduced, the stability of hydrogen in the gap is reduced, the dissociation equilibrium pressure is increased, the hydrogen release is facilitated, and the doping of the Ni element does not cause the huge change of the electronic structure of the uranium element and simultaneously maintains the hydrogen absorption capacity of the uranium element.
The volume expansion ratio of the hydrogen absorbing alloy is described by the following formula:
wherein eta represents the volume expansion rate of the alloy, V hydrid Volume, V, of uranium alloy/pure uranium hydride alloy,metal Representing the volume of uranium alloy/pure uranium.
The hydrogen absorbing and storing alloy is based on the gamma-phase uranium, an ideal structure is finally obtained through cell expansion, ni doping, structure optimization and static self-consistency, the uranium nickel alloy with lower volume expansion rate and hydrogen releasing temperature is used as the hydrogen absorbing and storing alloy, and the problems of high volume expansion rate, easy pulverization, high hydrogen releasing temperature and the like of the depleted uranium hydrogen storage are solved.
Example 1
Designing an atomic ratio U, wherein Ni is 7:3, doping Ni in uranium unit cells by using the combined action of interstitial doping and substitutional doping as shown in figure 4 to obtain a hydrogen absorption and storage alloy, and as shown in figure 2, actually calculating and analyzing the volume expansion rate of hydrogen absorption H/U =3 to be as low as 43.5% and the hydrogen release temperature to be as low as 541K; u shape 7 Ni 3 The proportion of the medium Ni element is higher, and the volume expansion rate of the medium Ni element is higherThe number of the reduction is more desirable. This will effectively ameliorate the problem of uranium alloy dusting during application due to volume expansion.
Example 2
The atomic ratio U is designed, ni is 7:2, the uranium unit cell is doped with Ni by gap doping, the hydrogen absorption and storage alloy is obtained, the volume expansion rate of the hydrogen absorption amount H/U =3 can be as low as 56.3% by actual calculation and analysis, and the hydrogen release temperature is as low as 338K. Doping ratio of Ni element U 7 Ni 3 Less. Compared with the atomic ratio 7:3, the volume expansion rate is larger, but the hydrogen releasing temperature is lower, and the working environment is more ideal.
Example 3
The atomic ratio U is designed, ni is 7:1, the uranium unit cell is doped with Ni instead of doping to obtain the hydrogen absorption and storage alloy, the hydrogen absorption amount H/U =3.1 volume expansion rate is 65.4% through actual calculation and analysis, and the hydrogen release temperature is as low as 398K. At stoichiometry 7:1, the trend is similar to 7:2. However, compared with the typical mixture ratio 7:3, the volume expansion rate is reduced, but the performance is poor compared with 7:3. The hydrogen release temperature is obviously reduced, and certain advantages are achieved.
Example 4
The atomic ratio U is designed, ni is 8:1, the uranium unit cell is doped with Ni by gap doping, and the hydrogen absorption and storage alloy is obtained, as shown in figure 1, the volume expansion rate of the hydrogen absorption amount H/U =3 can be as low as 52.9% through actual calculation and analysis, and the hydrogen release temperature is as low as 543K.
Example 5
The atomic ratio U is designed to be 8.5, ni is doped in uranium unit cells by gap doping to obtain the hydrogen absorption and storage alloy, the hydrogen absorption amount H/U =3 volume expansion rate is 67.4% by actual calculation and analysis, and the hydrogen release temperature is as low as 555K.
Example 6
The atomic ratio U to Ni is designed to be 8, ni is doped in uranium unit cells by gap doping to obtain the hydrogen absorption and storage alloy, the volume expansion rate of the hydrogen absorption amount H/U =3 can be as low as 62.7% by actual calculation and analysis, and the hydrogen release temperature is as low as 382K.
As shown in fig. 3, the hydrogen desorption temperature of the uranium nickel alloy of the invention is lower than that of pure uranium under a certain hydrogen absorption amount.
Claims (8)
1. A design method of a depleted uranium-based hydrogen absorption and storage alloy is characterized by comprising the following specific design steps:
s1, determining the atomic ratio of U and Ni, performing cell expansion based on a U unit cell to obtain a super unit cell, and performing Ni atom doping at different positions around the U atom to obtain an initial structure of a target alloy;
s2, the initial structure of the target alloy is subjected to relaxation and electronic static self-consistency, and the total energy is selected to be less than 1.0 multiplied by 10 -6 The structure with stress of each atom lower than 0.01 eV/A is used as the optimized structure of the uranium nickel alloy;
s3, screening the optimized structures in the same atomic ratio to obtain uranium-nickel alloy and uranium-nickel alloy hydride in the optimized structures in the atomic ratio;
s4, screening the uranium-nickel alloy with the optimal structure under different atomic proportions, selecting the uranium-nickel alloy as a hydrogen absorption and storage alloy, wherein the formation energy of the uranium-nickel alloy is less than 0.2, the volume expansion rate of the uranium-nickel alloy after hydrogen absorption is less than that of pure uranium after hydrogen absorption, and the uranium-nickel alloy with the reduced hydrogen release thermodynamic equilibrium temperature of a uranium-nickel alloy hydride is taken as the hydrogen absorption and storage alloy;
u: the Ni atomic ratio is 7: (1~3) or 8: (0.5 to 1.5).
2. The method for designing the depleted uranium-based hydrogen storage alloy according to claim 1, wherein the depleted uranium-based hydrogen storage alloy is designed and calculated by a first principle.
3. The method of claim 1 wherein the volume expansion of the hydrogen occluding alloy is low
The calculation formula of (a) is as follows:
wherein the content of the first and second substances,
representing the volume of uranium alloy/pure uranium hydride,
representing the volume of uranium alloy/pure uranium.
4. The method for designing the depleted uranium-based hydrogen absorption and storage alloy according to claim 1, wherein the thermodynamic equilibrium temperature of the hydrogen absorption and storage alloy
Is represented as follows:
wherein the content of the first and second substances,
is the change in enthalpy of the dehydrogenation reaction,
is the entropy change of the dehydrogenation reaction.
5. A depleted uranium-based hydrogen storage alloy according to any one of claims 1~4, produced by doping a gamma phase depleted uranium with nickel, U: the Ni atomic ratio is 7: (1~3) the doping sites for the Ni atoms include the interior of the uranium depleted super cell and the face center.
6. The depleted uranium based hydrogen storage alloy according to claim 5, wherein the ratio of U: the Ni atomic ratio is 7:3.
7. a depleted uranium-based hydrogen storage alloy according to any one of claims 1~4, produced by doping a gamma phase depleted uranium with nickel, U: the Ni atomic ratio is 8: and (0.5-1.5) the doping site of the Ni atom is in the uranium-depleted super-crystal cell.
8. The depleted uranium based hydrogen storage alloy according to claim 7, wherein the ratio of U: the Ni atomic ratio is 8:1.
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Citations (6)
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| US2692823A (en) * | 1947-08-07 | 1954-10-26 | Marion E Cieslicki | Uranium-nickel metal alloy |
| FR1303032A (en) * | 1961-07-21 | 1962-09-07 | Commissariat Energie Atomique | Uranium-molybdenum alloy and its manufacturing process |
| US4383853A (en) * | 1981-02-18 | 1983-05-17 | William J. McCollough | Corrosion-resistant Fe-Cr-uranium238 pellet and method for making the same |
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| JPH0891801A (en) * | 1994-09-26 | 1996-04-09 | Michio Yamawaki | Storing method of hydrogen by using uranium |
| CN1350896A (en) * | 2000-10-31 | 2002-05-29 | 韩国原子力研究所 | Method and apparatus for manufacturing uranium foils containing fine crystals |
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Patent Citations (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| US2692823A (en) * | 1947-08-07 | 1954-10-26 | Marion E Cieslicki | Uranium-nickel metal alloy |
| FR1303032A (en) * | 1961-07-21 | 1962-09-07 | Commissariat Energie Atomique | Uranium-molybdenum alloy and its manufacturing process |
| GB950163A (en) * | 1961-07-21 | 1964-02-19 | Commissariat Energie Atomique | Improvements in or relating to uranium/molybdenum alloys |
| US4383853A (en) * | 1981-02-18 | 1983-05-17 | William J. McCollough | Corrosion-resistant Fe-Cr-uranium238 pellet and method for making the same |
| US4650518A (en) * | 1983-12-22 | 1987-03-17 | Nukem Gmbh | Container for the final storage of radioactive wastes |
| JPH0891801A (en) * | 1994-09-26 | 1996-04-09 | Michio Yamawaki | Storing method of hydrogen by using uranium |
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