• 专利附录
  • 专利说明
  • 权利要求
  • 类似技术
  • 同族专利
  • 引用文献
  • 法律状态
  • 优先权
    • 专利摘要:
    The invention relates to methods and devices for the separation of hydrogen isotopes using chemical isotope exchange. The purpose of the invention is to increase the degree of separation of hydrogen isotopes. The method involves directing hydrogen isotopes in a stream of inert carrier gas countercurrently to a stream of water vapor with an inert carrier gas. The streams are separated by a metal membrane of palladium or palladium-silver alloy. The partial pressure of hydrogen on both sides of the membrane is maintained the same and not exceeding 10 4 Pa, and the process is carried out at a temperature of 120-300 ° C. Due to the isotopic exchange between the isotopes of hydrogen and water vapor and the equality of the partial pressures of hydrogen through the membrane, selective diffusion of molecules containing deuterium and tritium occurs. The device includes isotope exchange reactors 1 with a metal membrane 12 made of palladium or palladium-silver alloy, chambers 2 for recovering hydrogen isotopes from water, pipelines 8.9 for supplying inert carrier gas, pipelines 3 for supplying hydrogen isotopes from chambers 2 to reactors 1 , water evaporators 7, pipelines 4 for supplying water to reactors, water vapor condenser 26, oxidizing chambers 14 with a metal membrane 16 made of palladium or palladium alloy with silver and a layer of metal oxide 18. 2 p.p. 7 hp f-ly, 1 ill., 1 tab.
    公开号:SU1507206A3
    申请号:SU823445697
    申请日:1982-06-04
    公开日:1989-09-07
    发明作者:Иниотакис Николаос；Фон Дер Декен Клаус-Бенедикт
    申请人:Кернфоршунгсанлаге Юлих, Гмбх (Фирма)；
    IPC主号:
    专利说明:

    rum. The partial pressure of hydrogen on both sides of the membrane is maintained at the same and not exceeding 10 Pa, and the process is carried out at a temperature of 120-300 ° C. Due to the isotopic exchange between hydrogen isotopes and water vapor and the equality of the partial pressures of hydrogen through the membrane, containing deuterium and tritium. The device includes isotope exchange reactors 1 with a metal membrane 12 made of palladium or palladium alloy with
    silver, chambers 2 for the recovery of hydrogen isotopes from water, pipelines 8 and 9 for supplying inert carrier gas, pipelines 3 for supplying water isotopes from chambers 2 to reactors 1, evaporators codes 7, pipelines A for supplying water to reactors, water condenser steam 26, oxidation chambers 14 with a metal membrane 16 made of palladium or an alloy. palladium with silver and a layer of metal oxide 18. 2 sec. 7 hp ff, 1 ill., 1 tab.
    The invention relates to methods and devices for the separation of hydrogen isotopes using chemical isotope exchange and can be used in the preparation of deuterium and tritium, as well as in the purification of tritium products involved in nuclear reactors.
    The aim of the invention is to increase the degree of separation of hydrogen isotopes.
    Due to the countercurrent direction of isotopes of hydrogen and water vapor in a stream of inert carrier gas on opposite sides of the metal membrane permeable to hydrogen isotopes and maintaining the same hydrogen partial pressure on both sides of the membrane due to the isotope exchange between hydrogen isotopes and water vapor, selective diffusion of molecules containing deuterium and tritium isotopes.
    The drawing is a flow chart illustrating the operation of the method and apparatus for separating hydrogen isotopes in a two-stage cascade plant.
    The method of separating hydrogen isotopes involves the reduction of water of the initial isotopic composition with the formation of hydrogen protons, contacting the formed hydrogen isotopes with water vapor by directing the flow of hydrogen isotopes countercurrently to water vapor and diverting a stream of water vapor enriched with hydrogen protons. Foot steam is mixed with inert gas5
    0
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    e-carriers along different sides of a hydrogen-permeable palladium metal membrane or a palladium alloy with -silver. The partial pressure of hydrogen on both sides of the membrane is maintained the same and not exceeding U Pa, and the contact of hydrogen isotopes with water vapor is carried out at 120-300 ° C.
    In particular, a stream of water vapor can form from water of the same composition from which hydrogen isotopes are obtained. Thereby, the degree of isotope separation can be increased. Hydrogen and water isotope streams can pass in a mixture with the same carrier gas, which simplifies the process. A portion of the inert carrier gas withdrawn from the membrane, after purification from isotopes of hydrogen and water vapor, can be reused as carrier gas, which is economically advantageous.
    The device for separating hydrogen isotopes contains successively connected reactors 1 and 1a of isotopic exchange between hydrogen isotopes and water vapor, chambers 2 and 2a for recovering hydrogen isotopes from water, pipelines 3 and 3, for supplying hydrogen isotopes from reducing chambers to reactors, pipelines 4 and 4a for supplying water to reactors 1 and 1a, pipelines 5 and 5a for removing steam from reactors and feeding it to chambers 2 and 2a for reducing hydrogen isotopes and pipelines 6 and 6a for withdrawing hydrogen isotopes from reactors. The device also contains evaporators 7 and 7a connected to
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    pipelines D and 4a for supplying water to the reactors, and pipelines 8.8a and 9.9a for supplying an inert carrier gas, connected to pipelines 3.3a and 4.4a for supplying isotopes of hydrogen and water to the reactors. Reactors 1 and 1a are made in the form of chambers divided into two cavities 10, 11 and 10a, 11a by metal membranes 12 and 12a on palladium or palladium-silver alloy and separating a stream of hydrogen isotopes with an inert carrier gas from the stream water vapor with inert carrier gas.
    The hydrogen isotope separation device may contain additional pipes 13 and 13a with flow regulators connecting pipes 6 and 6a for removing hydrogen isotopes and pipelines A and 4a for supplying water to the reactors. The device may contain oxidizing chambers 14 and 14a communicating with pipelines 6 and 6a for diverting hydrogen isotopes from reactors 1 and 1a, and also pipelines 15 and 15a for connecting oxidizing chambers to pipelines 8 and 8a for supplying inert carrier gas .
    Oxidation chambers 14 and 14a, as well as reactors 1 and 1a, can be divided into two cavities with metal membranes 16 and 16a made of palladium or palladium-silver alloy and provided with conduits 17 and 17a for draining the reaction products in a stream of inert carrier gas.
    As an oxidizing agent, metal oxide layer 18 and 18a can be placed in chambers 14 and 14a.
    The device comprises a water storage device 19, a pipeline 20 for supplying water to chamber 2, a cylinder 21 for an inert carrier gas. Valves 22 and 23 serve to regulate the consumption of isotopes of hydrogen and water vapor, respectively, and valve 24 to regulate the flow of carrier gas. The conduit 25 serves to supply the mixture to the capacitor 26, and the conduit 27 to discharge water from the condenser 26.
    The device that implements the method for the separation of hydrogen isotopes, works as follows.
    . Water from accumulator 19 is supplied via conduit 20 to chamber 2 to recover hydrogen isotopes from water. Alternate hydrogen isotopes
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    the water 3 is directed to the cavity 10 of the reactor 1. At the same time, an inert carrier gas is fed from the cylinder 21 through line 8 to the cavity 10. On the other hand, water vapor in a mixture with an inert carrier gas is directed into the cavity 11 of the reactor 1. Water vapor is obtained in the evaporator 7 by evaporation of water coming from storage device 19 through pipelines 4 and 4a. Thus, two countercurrent flows are formed on the membrane 12 of the reactor 1: a stream of hydrogen isotopes with a carrier gas and a stream of 41st water with a carrier gas. The flow rate of hydrogen isotopes and water vapor is controlled by valves 22 and 23, as well as by means of the flow rate of the carrier gas by valve 24.
    In the reactor 1, from the cavity 10, hydrogen isotopes through the membrane 12 diffuse into the cavity 11, where they are isotope exchanged with water vapor. As a result of the reaction, a part of deuterium and tritium atoms from ND and NT molecules are bound in the form of NDO and NTR molecules, respectively. The fluxes of hydrogen isotopes, water vapor, and carrier gas in cavities 10 and 11, as well as the temperature, are chosen in such a way that the partial pressure of hydrogen in them is the same and does not exceed 10 Pa. Limiting the partial pressure is necessary to prolong the operating period of the metallic membranes. The equality of the partial pressure of hydrogen on both sides of the membrane 12 is necessary so that only a stream of deuterium and tritium isotopes exist through the membrane and there is no flow of hydrogen. Thus, in this case, the membrane, practically not being in the usual conditions selective with respect to hydrogen isotopes, due to the equality of the partial pressures of hydrogen and the reaction of isotopic metabolism, is capable of selectively passing deuterium and trit isotopes. The degree of separation of hydrogen isotopes, determined by the relative content of deuterium or tritium in relation to the content of all its isotopes on both sides of the membrane, is noticeably higher than in the case of only the isotope exchange reaction, when the separation effect at each stage is equal to the equilibrium reaction constant.
    The operating temperature in reactors 1 and 1a should be maintained in the range of 120-300 ° C. At these temperatures, the equilibrium constants of isotopic exchange for deuterium and tritium turn out to be quite large. For example, for the equilibrium constant exchange of tritium with hydrogen is K 3.6, and deuterium with hydrogen K0 is 2.46. The temperature can be set by means of appropriate heating of the carrier gas.
    Water enriched in deuterium and tritium, mixed with gaseous hydrogen isotopes and carrier gas from cavity 11 of reactor 1, is passed through chambers 2a to recover hydrogen and, after adding the required amount of carrier gas, to reactor 1a, where the cycle is repeated, and the degree of separation, calculated with respect to the content of hydrogen isotopes in the water of the initial composition, increases even more,
    Water for the initial isotopic composition can be used to obtain water vapor in evaporators 7 and 7a. In this case, the degree of separation into the second (and subsequent) stages of the cascade increases.
    Using the same inert carrier gas in all parts of the process chain is most beneficial. For this purpose, 11 pipelines 9.9a, 13.1 per, 15, and 15a are used. In particular, to reduce the flow rate of the carrier gas, a portion of the gas through the lines 13 and 13a can be rotated into a cycle for mixing with water vapor.
    A carrier gas for the purpose of its purification from hydrogen isotopes can be fed into oxidizing chambers 14 and 14a. Oxidation chambers may be similar in structure to reactors 1 and 1a and contain a membrane 16 (1b) of palladium or palladium-silver alloy. In this case, the oxidizer in the form of a metal oxide (in particular, copper oxide) should be contained on the secondary side of the membrane. Hydrogen isotopes, diffused through membranes 16 and 16a, react with metal oxide to form water. I feed 1 iiHi pTiUiii carrier gas through pipelines 15 and 13a, and Q
    5 0 5
    ABOUT
    .
    5 o 5 5
    products withdrawn By pipelines 17
    and 17a.
    Using membranes 16 and 16a
    in the oxidation chambers 14 and 14e, the resistance to the passage of carrier gas through the installation can be reduced.
    From the last stage, through pipeline 25, a mixture of water vapor with a carrier gas can be fed to a condenser 26, from which water enriched in deuterium and tritium can be removed through pipeline 27 and the carrier gas will be recycled.
    The table shows the data on the degree of separation of deuterium, obtained for three different temperatures t 120,200 and 300 ° C, in an installation of two stages. Helium was used as a carrier gas with a flow rate in each reactor of about 2.5 kg / s. The data correspond to two cases: water vapor for reactors 1 and 1a is formed from water, obtained 1 1 in evaporators 7 and 7a (case I), and water vapor formed from water of initial isotopic composition (case II):
     The table shows that already at two stages the degree of separation according to the proposed method and device noticeably exceeds the equilibrium constant K, which determines the degree of separation at each stage under the condition that only the isotope exchange reaction takes place.
    权利要求:
    Claims (9)
    [1]
    Invention Formula
    1. A method for separating hydrogen isotopes, including reducing hydrogen isotopes from water of initial isotopic composition, contacting formed hydrogen isotopes with water by directing the flow of hydrogen isotopes countercurrently to the flow of water and diverting a stream of water enriched with hydrogen isotopes, characterized in that the separation, the flow of water is used in the form of a stream of water vapor, the flows of isotopes of hydrogen and water vapor are directed in a mixture with inert carrier gases along different sides n metal membrane made of palladium or palladium-silver alloy, with the partial density of hydrogen on both sides of the memorial being the same and not iipepi.i and 10 Pa,
    while hydrogen isotopes are contacted with iodine vapor at 120,.
    [2]
    2. The method according to claim 1, about tl and h and yugts and the fact that a stream of water vapor form from the water of the initial isotopic composition.
    [3]
    3. Method according to paragraphs. 1 and 2, about t of l and. This is due to the fact that the flows of hydrogen and water vapor tops are mixed with the same inert carrier gas.
    [4]
    4. Method according to paragraphs. 1-3, which is based on the fact that a part of the inertial flow ratio that connects pipelines for the removal of hydrogen isotopes and pipelines for supplying feed to the reactors.
    25
    Its carrier gas discharged from the membrane is purified from hydrogen isotopes and water vapor and used as a carrier gas for mixing with hydrogen and water vapor 20 isotopes directed to the membrane.
    [5]
    5. A device for the separation of hydrogen isotopes containing successively connected isotopic exchange reactors between hydrogen isotopes and water, chambers for reducing hydrogen isotopes from water, pipelines for supplying hydrogen isotopes from reducing chambers to reactors, pipelines for feeding feeds to reactors, pipelines for draining water from reactors and its supply to reduction chambers and pipelines for removal of hydrogen isotopes from reactors, characterized in that, in order to increase the degree of separation, it also contains vaporizers connected to pipelines to supply water to the reactors, and pipelines to supply an inert carrier gas, .-.
    thirty
    35
    7. The device according to paragraphs. 5 and 6, that is, it contains oxidizing chambers, communicates with pipelines for the removal of hydrogen isotopes and reactors, and pipelines for connecting oxidizing chambers with pipelines for supplying an inert carrier gas.
    8. The device according to claim 7, characterized in that the oxidation chambers are separated by metal membranes of palladium or palladium-silver alloy into two cavities and are provided with pipelines for supplying an inert carrier gas and discharging the reaction products in the carrier gas stream.
    9. A device according to claim 8, characterized in that a layer of metal oxide is placed in the oxidation chambers.
    connected to pipelines for supplying hydrogen and water isotopes to reactors, the reactors being made in the form of chambers divided into two cavities by metal membranes made of palladium or palladium-silver alloy and separating hydrogen isotopes with an inert carrier gas from an inert gas stream carrier gas.
    [6]
    6. The device according to claim 5, characterized in that it contains an additional pipeline with pe
    [7]
    7. The device according to paragraphs. 5 and 6, that is, it contains oxidizing chambers, communicates with pipelines for the removal of hydrogen isotopes and reactors, and pipelines for connecting oxidizing chambers with pipelines for supplying an inert carrier gas.
    [8]
    8. The device according to claim 7, characterized in that the oxidation chambers are separated by metal membranes of palladium or palladium-silver alloy into two cavities and are provided with pipelines for supplying an inert carrier gas and discharging the reaction products in the carrier gas stream.
    [9]
    9. A device according to claim 8, characterized in that a layer of metal oxide is placed in the oxidation chambers.
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    同族专利:
    公开号 | 公开日
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    DE3123860A1|1983-01-27|
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    US4687644A|1987-08-18|
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    引用文献:
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    RU2648263C1|2014-08-18|2018-03-23|Де Нора Пермелек Лтд|Method for treatment of raw water, which contains tritium water|US2690379A|1942-11-21|1954-09-28|Harold C Urey|Process for production of deuterium oxide as a source of deuterium|
    CA907292A|1970-01-28|1972-08-15|H. Stevens William|Process and catalyst for enriching a fluid with hydrogen isotopes|
    US3981976A|1970-01-28|1976-09-21|Atomic Energy Of Canada Limited|Process for hydrogen isotope concentration between liquid water and hydrogen gas|
    US3789112A|1970-10-28|1974-01-29|Gulf Research Development Co|Process for obtaining deuterium from hydrogen-containing components and the production of heavy water therefrom|
    US4053576A|1975-05-19|1977-10-11|The Regents Of The University Of Minnesota|System for obtaining hydrogen and oxygen from water using solar energy|
    CA1072720A|1976-06-25|1980-03-04|John P. Butler|Process for the exchange of hydrogen isotopes using a catalyst packed bed assembly|
    US4190515A|1978-05-18|1980-02-26|Atomic Energy Of Canada Limited|Apparatus for removal and recovery of tritium from light and heavy water|
    US4191626A|1978-05-22|1980-03-04|Atomic Energy Of Canada Limited|Apparatus for finishing and upgrading of heavy water|
    DE2854682C2|1978-12-18|1985-08-14|Kernforschungsanlage Jülich GmbH, 5170 Jülich|Method and device for hydrogen isotope separation|
    US4399120A|1979-12-26|1983-08-16|Union Carbide Corporation|Hydrogen-water isotopic exchange process|US4659554A|1984-06-04|1987-04-21|Allied Corporation|Low-energy process for separation of hydrogen isotopes|
    JPH03503521A|1988-03-31|1991-08-08|
    US4996033A|1988-03-31|1991-02-26|Molecular Technology Corporation|Catalytic method for concentrating isotopes|
    US5154878A|1990-04-30|1992-10-13|Anthony Busigin|Process and apparatus for tritium recovery|
    US5468462A|1993-12-06|1995-11-21|Atomic Energy Of Canada Limited|Geographically distributed tritium extraction plant and process for producing detritiated heavy water using combined electrolysis and catalytic exchange processes|
    US5451322A|1994-06-03|1995-09-19|Battelle Memorial Institute|Method and apparatus for tritiated water separation|
    US6348153B1|1998-03-25|2002-02-19|James A. Patterson|Method for separating heavy isotopes of hydrogen oxide from water|
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    US9150610B2|2009-11-16|2015-10-06|Biomotif Ab|Method and apparatus to perform hydrogen-deuterium exchange|
    US8597471B2|2010-08-19|2013-12-03|Industrial Idea Partners, Inc.|Heat driven concentrator with alternate condensers|
    US8470073B2|2010-09-15|2013-06-25|Savannah River Nuclear Solutions, Llc|Apparatus and process for separating hydrogen isotopes|
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    RU2647040C1|2017-02-03|2018-03-13|Федеральное государственное бюджетное образовательное учреждение высшего образования "Российский химико-технологический университет имени Д.И. Менделеева"|Method of gas purification from tritiaded water vapor|
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    法律状态:
    优先权:
    申请号 | 申请日 | 专利标题
    DE3123860A|DE3123860C2|1981-06-16|1981-06-16|Method and device for the gradual enrichment of deuterium and / or tritium by isotope exchange|
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