CN1715179A - Hydrogen isotope separating device and method - Google Patents
Hydrogen isotope separating device and method Download PDFInfo
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- CN1715179A CN1715179A CN 200510021055 CN200510021055A CN1715179A CN 1715179 A CN1715179 A CN 1715179A CN 200510021055 CN200510021055 CN 200510021055 CN 200510021055 A CN200510021055 A CN 200510021055A CN 1715179 A CN1715179 A CN 1715179A
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Abstract
The present invention provides a kind of hydrogen isotope separating apparatus and method. The hydrogen isotope separating apparatus includes several separating stages, gas transferring pump, gas flow controller, gas flow control valve, etc. cascaded in certain mode, and each of the separating stages includes several parallel separators. After mixed material gas of protium, deuterium and tritium is injected in the middle part of the separating chain, and through the superposed successive separations, deuterium and tritium gas product with very low protium content may be taken out from one end of cascade chain while taking out protium and deuterium tail gas with very low tritium content. The present invention is suitable for continuous separation of great amount of hydrogen isotopes in different fields.
Description
Technical field
The invention belongs to the hydrogen isotope separation field, be specifically related to a kind of tripping device and method of hydrogen isotope.
Background technology
Deuterium-tritium is the nuclear fuel of fusion reactor, in the fusion reactor operational process, can introduce the impurity protium inevitably, when the concentration of protium surpasses certain level, must carry out hydrogen isotope separation with remove wherein protium just can keep the fusion reaction of deuterium tritium continue carry out.On the other hand, the nuclear fuel tritium can penetrate into nuclear fuel system glove box, space air in the circulation fusion reactor operational process, considers that for personnel and environmental safety the radiation hazradial bundle of control tritium must reclaim this part tritium.And all will be referred to the separation of large-scale hydrogen isotope in these significant process.
Table 1 is in the nuclear fuel cycle process of fusion reactor, enters the composition hydrogen isotope separation operation, that need carry out several typical hydrogen isotope gas of hydrogen isotope separation.
The composition of table 1 hydrogen isotope separation operation hydrogen isotope gas
| Sequence number | Unstripped gas is formed, % | Product gas is formed, % | Remarks | ||||
| C H | C D | C T | C H | C D | C T | ||
| 1 2 3 4 | 99.95 0.5 0.5 0.5 | 0 89.8 49.5 99.5 | 0.05 9.7％ 49.5 ≤ 0.01 | 98.5 ≤ 0.05 ≤ 0.05 ≤ 0.05 | 0 90 50 100 | 1.5 10 50 ≤ 0.01 | The multiplication agent tritium extracts the major cycle of nuclear fuel major cycle nuclear fuel major cycle nuclear fuel |
The reserve of heavy water is very abundant in the seawater, and thoroughly solving human energy demand by the fusion reaction of deuterium triton is unique feasible approach.Have extensive, continuously and the hydrogen isotope separation technology of the little characteristics of the resident amount of tritium be the gordian technique of deuterium tritium fusion reactor deuterium triton Fuel cycle always, it directly determines scale of investment, operational efficiency and the economic benefit etc. of whole nuclear fuel cycle system.After in decades, promoted by triton Fuel cycle of fusion reactor deuterium and heavy water reactor tritium extraction demand, states such as U.S., day, moral, method have carried out a large amount of hydrogen isotope separation technical study, have developed the hydrogen isotope separation technology that can satisfy these Important Project project demands.At " A design study of water detritiation and hydrogenisotope separation systems for ITER " (Y.Iwai, H.Yoshida, T.Yamanishi et al.FusionEngineering Design 49-50 (2000) 847-853), " Status of the ITER Tritium plant design " (H.Yoshida, o.Kveton, J.Koonce et al.Fusion Engineering Design 39-40 (1998) 875-882) introduced low temperature fractionation hydrogen isotope separating device and the method that is used for the Fuel cycle of fusion reactor deuterium triton in, there are some inherent defectives in this isolation technique, for example, the low temperature fractionation hydrogen isotope separation must be carried out under the liquid hydrogen temperature, not only need the auxiliary construction liquid helium, liquid nitrogen supply facility, also need low temperature (20K-26K) control techniques accurately and reliably, separating technology process complexity, separation parameter is subject to the extraneous factor influence, the tritium storage allowance of separation system is big, construction and running cost are more high.; " Hydrogen isotope separation by thermal cycling adsorption process " (D ducret; ABallanger; J.Steimetz et al.Fusion Engineering Design 58-59 (2001) 417-421) introduced high low temperature sorption cycle hydrogen isotope separation (TCAP) method in; compare with cryogenic rectification method; this separation system structure and sepn process Dan Jian, construction and running cost are lower; but this separation method is a kind of semicontinuous separation method, and separating power is little more than cryogenic rectification method.Therefore, be necessary to research and develop new hydrogen isotope separation technology, to reduce the scale of investment of nuclear fuel cycle hydrogen isotope separation system, improve the operational efficiency of separation system, the security and the economy of the operation of raising system.
In sum, existing hydrogen isotope separation technology have mostly that device is huge, complex technical process and the too high problem of investment.
Summary of the invention
The device that existing hydrogen isotope separation technology exists is huge in order to solve, complex technical process and the high problem of investment, the invention provides a kind of than traditional hydrogen isotope separating device that the hydrogen isotope separation technical efficiency is higher, technological process is simple and running cost is low and method.
Penetration speed existed the principle of certain difference to separate when the present invention utilized protium, deuterium and tritium gas molecule to see through palladium alloy membrane at a certain temperature, made one palldium alloy hydrogen isotope separation device.With several the palldium alloy hydrogen isotope separation devices separation level that constitutes in the hydrogen isotope separation system in parallel, several separation levels are cascaded up in some way constitutes the hydrogen isotope separation cascade chain more earlier.Drop into unstripped gas from the cascade chain middle part, stack step by step by multistage hydrogen isotope separation effect, take out the very low product tritium-deuterium gas of protinium-containing amount from an end of cascade chain, take out the very low protium-deuterium tail gas of tritium-containing amount from the other end, form under certain situation in separated protium-deuterium-tritium gas, by the tritium level in protium content and the tail gas in the withdrawal ratio control product gas of control product gas and tail gas.
Hydrogen isotope separating device of the present invention comprises by the palladium alloy membrane separator and separates cascade chain, gas shifting pump, gas flow controller, gas flow control valve, temperature sensor and the pressure transmitter that the level cascade forms; Gas shifting pump and palladium alloy membrane separator separate cascade chain, gas flow controller, gas flow control valve, temperature sensor and the pressure transmitter that grade cascade forms and are connected successively.
The hydrogen isotope separation cascade chain is formed by the cascade of a plurality of separation level, separate level elder generation with adjacent two and be together in series step by step, the more in parallel and gas shifting pump of on gas circuit, connecting the gas feed that sees through pneumatic outlet and its back first step of each grade by gas feed-pneumatic outlet-gas feed mode.
The separation progression that the palladium alloy membrane separator separates institute's cascade in the level cascade chain is 1～50 better, and separating progression also can be more than 50.
Level in the hydrogen isotope separation cascade chain is to be formed in parallel by several single-stage palladium alloy membrane separators, unstripped gas import and unstripped gas inlet parallel with several single-stage palladium alloy membrane separators, see through pneumatic outlet with in parallel through pneumatic outlet, see through pneumatic outlet with not in parallel, and form gas feed, the pneumatic outlet of this separation level respectively and see through pneumatic outlet through pneumatic outlet.
The palladium alloy membrane separator is made of palldium alloy pipe, well heater and separator outer container, has the unstripped gas import, sees through pneumatic outlet and does not see through three interfaces of pneumatic outlet; Palldium alloy pipe in the separator is connect with tubulation mode series welding by several short palldium alloy tubules or is formed by connecting with spiral tube mode series welding.The palldium alloy pipe can be spirrillum or straight tube-like form.
The material composition that is used for the making of palldium alloy pipe can be Pd (23-27) %, Ag (73-77) %; Pd (6-8) %, Y (92-94) %; Pd23%, Ag3%, Au1%, among the Y73% arbitrary group.
The separation method of a kind of hydrogen isotope of the present invention is characterized in comprising following content:
300 ℃～550 ℃ of temperature, under the condition of pressure 0.1MPa～0.3MPa, feed hydrogen isotropic substance protium-deuterium-tritium mixed gas to be separated is injected by the middle part of the separation cascade chain of gas flow controller from tripping device; Through the stack step by step of stage trapping effect, the control splitting ratio; Take out the very low product deuterium-tritium gas of protinium-containing amount from an end of tripping device cascade chain, from the very low protium-deuterium tail gas of the other end taking-up tritium-containing amount of tripping device cascade chain.
Unit scale of the present invention is less, is convenient to use in the Fuel cycle of fusion reactor deuterium triton.Adopt the present invention, hydrogen isotope separation efficient is higher, technology simple, running cost is lower.
Description of drawings
Fig. 1 is the structural representation of single-stage palladium alloy membrane hydrogen isotope separation device of the present invention
Fig. 2 is the hydrogen isotope separating device structural representation with 2n separation level of the present invention
Among the figure: 1. unstripped gas 2. well heaters, 3. separator outer containers, 4. palldium alloy pipes that enter the mouth
5. see through pneumatic outlet 6. and do not see through pneumatic outlet
21. exhaust flow controller 22. temperature sensors 23. flow of feed gas amount controllers
24. exhaust flow controller 25. flow control valves 26. pressure transmitters
27. separate level 28. gas shifting pumps
Embodiment
Below in conjunction with accompanying drawing the present invention is described in detail.
1. palladium alloy membrane hydrogen isotope separation device
Fig. 1 is the structural representation of single-stage palladium alloy membrane hydrogen isotope separation device.
Among Fig. 1, this separator is made of spirrillum palldium alloy pipe 4, well heater 2 and separator outer container 3, has unstripped gas inlet 1, sees through pneumatic outlet 5 and does not see through 6 three interfaces of pneumatic outlet.
Under the working temperature, enter separator and, will have part protium-deuterium-tritium mixed gas to see through the tube wall of palldium alloy pipe, flow out from seeing through pneumatic outlet 5 never through the pneumatic outlet 6 outflow processes at the unstripped gas inlet 1 of separated unstripped gas from separator.
When protium, deuterium, tritium gas see through palladium alloy membrane, produce the hydrogen isotope separation effect owing to penetration speed is different.The size of separate effect can be used separation factor q
IjTolerance.For protium-deuterium-tritium mixed system, because q
IjAlways, concentrated, seen through the end tritium by enrichment so see through the end protium greater than 1, in other words, will be by enrichment through heavy constituent (tritium) in the end gas, light constituent (protium) will be by dilution.For single-stage separator, q
IjNot only relevant with separation temperature, also relevant with the splitting ratio of gas, the gas splitting ratio of single-stage palladium alloy membrane separator is: f=F
Unper/ F
InWherein, F
InBe the flow of the gas that enters separator, F
UnperFor not seeing through the flow of the gas of palldium alloy tube wall.Under the certain condition of palldium alloy pipe temperature and separated gas composition, reflux ratio is more little, and it is big more to separate coefficient, and still, reflux ratio is more little, and the yield of product gas (or seeing through gas) is low more.And when reflux ratio be 0 or when being 1, then can not produce the separation of isotopes effect, being equivalent to gas this moment flows out from the gas outlet end that do not see through of separator fully, or the tube wall that sees through the palldium alloy pipe fully flows out fully from seeing through end.
Separation factor q
IjAlso relevant with the total length of palldium alloy pipe in the separator.There are two kinds of methods can in limited separator space, place long palldium alloy pipe as much as possible.
A kind of method is that many short palldium alloy straight tubes are connected to a long straight tube earlier by method for welding, turns to helix again, the promptly so-called helix mode that is connected in series.
Another kind is with many short straight tubes, with a plurality of U type pipes (palldium alloy or other material are made) several palldium alloy straight tubes directly is connected in series by method for welding, the promptly so-called shell and tube mode that is connected in series.
2. palladium alloy membrane separator cascade hydrogen isotope separation chain and tripping device
Because single-stage palladium alloy membrane separator has certain hydrogen isotope separation effect, therefore multistage palladium alloy membrane separator is cascaded up in a certain way and make the stack of hydrogen isotope separation effect, just can realize that the hydrogen isotope mixed gas separates fully.
The core of separation system is to separate the cascade chain that level cascade in a certain way forms by a plurality of palladium alloy membranes.The arrow direction is the flow direction of gas in cascade chain among the figure.The cascade system of separating level is: separate level with adjacent two and be connected in series step by step by gas feed-pneumatic outlet-gas feed mode, the pneumatic outlet that sees through with each grade also connects with the gas feed of the 1st grade of its back again, and on gas circuit gas shifting pump of series connection, promptly so-calledly stride 1 grade of cascade.If separating level with adjacent two is connected in series step by step by gas feed-pneumatic outlet-gas feed mode, the pneumatic outlet that sees through with each grade also connects with the inlet mouth of the 2nd grade of its back again, and the gas shifting pump of on gas circuit, contacting, then form the so-called 2 grades of cascades of striding.Therefore, the rarest two kinds of cascade system is useful for the separation of the hydrogen isotope gas of different content respectively.The number of the single-stage palladium alloy membrane separator of each grade parallel connection is determined that by the fractional dose of separation system to medium scale separation system, the quantity of the separator of each grade parallel connection is 1-50 for little.
3. hydrogen isotope separation technological process
The example explanation separation processes process that is separated into protium-deuterium binary mixture.At first separator is heated to working temperature (400 ℃～450 ℃), observe temperature variations by temperature sensor 22, again by flow of feed gas amount controller 23 with unstripped gas from shown in Figure 2, drop into by a 2n middle part of separating the hydrogen isotope separation level catena that level constitutes, be divided into two portions in the n level, promptly see through gas and do not see through gas, wherein see through gas and turn back to the n+1 level by means of gas recycle pump; The gas that enters the n+1 level is divided into two portions again, promptly sees through gas and does not see through gas, wherein sees through gas and turns back to the n+2 level by means of gas recycle pump; Like this through the n that associates, n+1, n+2, ..., the separation step by step of 2n level, see through n, n+1, n+2 ..., the heavy isotope component in the gas of 2n level constantly removed, if n is enough big, can take out pure protium continuously from the 2n level by exhaust flow controller 21.
Because what separate the level employing shown in the accompanying drawing 2 is the mode of being connected in series, the palldium alloy pipe that is equivalent to each grade is connected into a very long palldium alloy pipe.Enter the hydrogen isotope mixed gas of 2n level, successively by n, n-1, n-2 ..., in the process that 1 grade flows to product gas collecting terminal, because light isotope component penetrated preferably palldium alloy pipe, the heavy isotope tritium is partly concentrated, through after the stage trapping, open flow control valve 25, can take out pure deuterium continuously from the 1st grade by product exhaust flow controller 24.Therefore, whole sepn process is: drop into protium-deuterium unstripped gas continuously from the n level, take out pure protium and pure deuterium continuously from the 1st grade and 2n level respectively, thereby realize separating of protium and deuterium.
In the sepn process,, can control the content of deuterium in protium content in the product gas and the tail gas by the withdrawal ratio of exhaust flow controller (24,21) control product gas and tail gas.
Separating effect example 1 palladium alloy membrane separator carries out the separating effect of hydrogen isotope
Make single step helical shape palldium alloy pipe hydrogen isotope separation device with the Pd6.7%Y93.3% palldium alloy pipe of φ 2mm * 0.08mm.Test this kind separator separates different components H-D mixed gas under different reflux ratio conditions separation factor, the results are shown in Table 2.
The separator of two kinds of models listing in the table 2, its structure is identical, and its difference is that the total length of used spirrillum palldium alloy pipe is different, and PMS-2 is than long one times approximately of PMS-2.
The H-D separation factor of table 2 single-stage palladium alloy membrane hydrogen isotope separation device
| Type | T/K | f | q H，D |
| PMS-1 | 773 | 0.931 | 1.4 |
| 773 | 0.866 | 1.53 | |
| 873 | 0.991 | 1.43 | |
| 873 | 0.927 | 1.57 | |
| PMS-2 | 473 | 0.986 | 1.87 |
| 673 | 0.982 | 1.80 | |
| 873 | 0.953 | 1.80 |
Table 2 is the result show, this palladium alloy membrane separator has good hydrogen isotope separation ability, and separating effect can improve with the increase of the total length of used spirrillum palldium alloy pipe.Because the nucleidic mass difference between H (protium) and the T (tritium) is bigger than the nucleidic mass difference between H (protium) and the D (deuterium), under identical condition, the separation factor of H-T is more much bigger than the separation factor of H-D.
The separating effect of hydrogen isotope separation is carried out in the 2 palladium alloy membrane separator cascades of separating effect example
If the isotope separation factor of membrane separation apparatus is known, then utilize in the relevant technical literature about cascade separation of isotopes method of calculation, can more accurately estimate the separation progression of palladium alloy membrane separator cascade hydrogen isotope separation system.Hydrogen isotope separation with the extraction gas of extraction tritium from the fusion reactor tritium-breeding material is an example.Extract the 99.95%H that consists of of unstripped gas
2-0.05%T
2, if tritium level is 1.5%T in the prescribed product gas
2(be equivalent to T/H=5.2 * 10
-2), the tritium in the tail gas is 0.0002%T
2(be equivalent to T/H=2 * 10
-6), the calculation result of the change of component of gases at different levels is listed in table 3 in the then needed separation sum of series disengaging latch.In the calculating, the separation factor of getting single-stage separator is 2.5, and the gas backstreaming ratio of separator is 0.8, and the splitting ratio of product gas and tail gas gets 0.0429, and these parameters all can realize in practice.
Carrying out the hydrogen isotope separation process with level string tripping device is: separator is heated to working temperature (about 400 ℃), sends into from the middle part (3rd level) of level catena with the air demand of 18mol/h by gas flow controller and consist of 99.95%H
2-0.05%T
2Unstripped gas, more respectively by exhaust flow controller and product airshed controller, respectively with the flow of 17.22mol/h and 0.78mol/h tail gas end (the 6th grade) and product gas end (the 1st grade) extraction tail gas and product gas from the level catena.
The cascade of table 3 palladium alloy membrane separator separates H-T and separates
| Separate progression | Gas composition, tritium/protium | ||
| The first step (product gas) second stage third stage (unstripped gas) the 6th grade of level V of the fourth stage (tail gas) | Air inlet 6.09 * 10 -3 2.41×10 -3 8.56×10 -4 2.90×10 -4 7.95×10 -5 2.03×10 -5 | See through gas 3.83 * 10 -3 1.49×10 -3 5.35×10 -4 1.82×10 -4 4.96×10 -5 2.67×10 -6(extracting tail gas from here) | Do not see through gas 5.2 * 10 -2(extracting product gas from here) 6.09 * 10 -3 2.14×10 -3 7.26×10 -4 1.99×10 -4 5.07×10 -5 |
As can be seen from Table 3, send into H/T=8.56 * 10 from the 3rd level of level catena
-4Unstripped gas, can take out H/T=5.2 * 10 from the 1st grade
-2Product gas, can take out H/T=2.67 * 10 from the 6th grade
-6Tail gas.With unstripped gas relatively, the H/T of product gas has reduced by two orders of magnitude (tritium is by enrichment, and protium is by dilution), the H/T of tail gas two orders of magnitude (tritium is by dilution, and protium is by enrichment) that raise.
Claims (10)
1, a kind of hydrogen isotope separating device is characterized in that: described tripping device comprises that the palladium alloy membrane separator separates cascade chain, gas shifting pump, gas flow controller, gas flow control valve, temperature sensor and pressure transmitter that the level cascade forms; Gas shifting pump and palladium alloy membrane separator separate cascade chain, gas flow controller, gas flow control valve, temperature sensor and the pressure transmitter that grade cascade forms and are connected successively.
2, hydrogen isotope separating device according to claim 1, it is characterized in that: described hydrogen isotope separation cascade chain is formed by the cascade of a plurality of separation level, separate level elder generation with adjacent two and be together in series step by step, the more in parallel and gas shifting pump of on gas circuit, connecting the gas feed that sees through pneumatic outlet and its back first step of each grade by gas feed-pneumatic outlet-gas feed mode.
3, hydrogen isotope separating device according to claim 1 and 2 is characterized in that: the separation progression that described palladium alloy membrane separator separates institute's cascade in the level cascade chain is 1～50.
4, according to claim 1,2 or 3 arbitrary described hydrogen isotope separating devices, it is characterized in that: the level in the described hydrogen isotope separation cascade chain is formed in parallel by several single-stage palladium alloy membrane separators, unstripped gas import and unstripped gas inlet parallel with several single-stage palladium alloy membrane separators, see through pneumatic outlet with in parallel through pneumatic outlet, see through pneumatic outlet with not in parallel, and form gas feed, the pneumatic outlet of this separation level respectively and see through pneumatic outlet through pneumatic outlet.
5, according to the arbitrary described hydrogen isotope separating device of claim 1～4, it is characterized in that: described palladium alloy membrane separator is made of spirrillum palldium alloy pipe, well heater and separator outer container, has the unstripped gas import, sees through pneumatic outlet and does not see through three interfaces of pneumatic outlet; Spirrillum palldium alloy pipe in the separator is fixedly connected in the serial connection mode.
6, according to the arbitrary described hydrogen isotope separating device of claim 1～4, it is characterized in that: described palladium alloy membrane separator is made of straight tube-like palldium alloy pipe, well heater and separator outer container, has the unstripped gas import, sees through pneumatic outlet and does not see through three interfaces of pneumatic outlet; Straight tube-like palldium alloy pipe in the separator is fixedly connected in the serial connection mode.
7, according to the arbitrary described hydrogen isotope separating device of claim 1～4, it is characterized in that: the described material that is used for the making of palldium alloy pipe consists of Pd (23-27) %, Ag (73-77) %.
8, according to the arbitrary described hydrogen isotope separating device of claim 1～4, it is characterized in that: the described material that is used for the making of palldium alloy pipe consists of Pd (6-8) %, Y (92-94) %.
9, according to the arbitrary described hydrogen isotope separating device of claim 1～4, it is characterized in that: the described material that is used for the making of palldium alloy pipe consists of Pd23%, Ag3%, Au1%, Y73%.
10, a kind of separation method of hydrogen isotope is characterized in that comprising following content:
300 ℃～550 ℃ of temperature, under the condition of pressure 0.1MPa～0.3MPa, feed hydrogen isotropic substance protium-deuterium-tritium mixed gas to be separated is injected by the middle part of the separation cascade chain of gas flow controller from tripping device; Through the stack step by step of stage trapping effect, the control splitting ratio; Take out the very low product deuterium-tritium gas of protinium-containing amount from an end of tripping device cascade chain, from the very low protium-deuterium tail gas of the other end taking-up tritium-containing amount of tripping device cascade chain.
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