CA1073850A - Method of separating gaseous isotope compounds and apparatus - Google Patents

Method of separating gaseous isotope compounds and apparatus

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Publication number
CA1073850A
CA1073850A CA290,493A CA290493A CA1073850A CA 1073850 A CA1073850 A CA 1073850A CA 290493 A CA290493 A CA 290493A CA 1073850 A CA1073850 A CA 1073850A
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Canada
Prior art keywords
isotope
mixture
reaction
gas
carrier gas
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired
Application number
CA290,493A
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French (fr)
Inventor
Hans-Joachim Niemann
Wolfgang Gajewski
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Kraftwerk Union AG
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Kraftwerk Union AG
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Classifications

    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D59/00Separation of different isotopes of the same chemical element
    • B01D59/34Separation by photochemical methods

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  • Life Sciences & Earth Sciences (AREA)
  • Biophysics (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Oxygen, Ozone, And Oxides In General (AREA)
  • Lasers (AREA)

Abstract

Abstract of the Disclosure Method of separating gaseous isotope compounds through selective excitation and subsequent chemical reaction with a gaseous reaction partner as well as separation of the reaction product from the remaining gas mixture, including mixing a mixture of the gaseous isotope compounds that are to be separated and the reaction partner with a neutral, multiatomic diluent gas sharply subcooled to a temperature close to the condensation temperature thereof during a time period adequate for absorption of the oscillation energy of the isotope mixture yet inadequate for affording reproduction of the original condition of this mixture, transporting the isotope mixture with a carrier gas to a beam path of a laser with a flow velocity adjusted to the excitation frequency of one of the isotope compounds, the time during which the transport occurs corresponding to the time required for absorbing the oscillation energy, and then delivering the thereby resulting chemical reac-tion product to a separation device; and apparatus for carrying out the foregoing method.

Description

l(r73~so The invention relates to method and apparatus for separating gaseous isotope compounds through selective excitation and subsequent chemical reaction with a likewise gaseous reaction partner as well as separ-ation or deposition of the preferably solid reaction product out of the remaining gas mixture. A method of this general type is known, in part, from the German Published Non-Prosecuted application DT-OS 1 959,767. It has been found, however, that in addition to the chemical reactions resulting from the selective laser excitation, which would afford a normal separation of the reaction product containing only the excited isotope, other reactions also occur which greatly impair the selectivity. This is caused initially due to the overlapping of the absorption bands so that already a selective excitation is extraordinarily hampered, and furthermore due to resonance exchange and thermally activated reactions. From German Published ~on-Prosecuted Application DT-OS 2 447,762, a method has, furthermore, become known, with the aid of which it is possible to suppress the aforementioned phenomena and to attain the desired selectivity with respect to the excit-ation of only the one isotope compound. ~his is attained through an adiabatic expansion and consequent cooling of the reaction partner to below 100 K, a process which imposes absolutely maximal demands upon the construction of the expansion nozzle.
It is accordingly an object of the invention to provide a method and apparatus for separating gaseous isotope compounds wherein the number of oscillation states are likewise drastically reduced so that the variations in the spectra of the different isotopes are visible and can be utilized for per~orming the desired excitation with the aid of laser light.
With the foregoing and other objects in view, there is provided, in accordance with the invention, a method of separating gaseous isotope compounds through selective excitation and subsequent chemical reaction with a gaseous reaction partner as well as separation of the reaction product from the remaining gas mixture, which comprises mixing a mixture of the gaseous lt)~3~5~

isotope compounds that are to be separated and the reaction partner with a neutral, multiatomic diluent gas sharply subcooled to a temperature close to the condensation temperature thereof during a time period ade~uate for absorption of the oscillation energy of the isotope mixture yet inadequate for affording reproduction of the original condition of this mixture, trans-portin~ the isotope mixture with a carrier gas to a beam path of a laser with a flow velocity adjusted to the excitation frequency of one of the isotope compounds, the time during which the transport occurs corresponding to the time required for absorbing the oscillation energy, and then delivering the thereby resulting chemical reaction product to a separation device.
The difficulty of isotope separation, especially uranium isotope separation of the compound UF6, with visible and ultraviolet light is that the electron spectra of the respective compounds are very complex.
The spectrum of this compound is not formed of a few separated oscillation bands which would permit a selective excitation through irradia-tion, for example, at the edge of the band, but rather, is formed of a great number of socalled "hot bands" which produce a quasicontinuous spectrum because of the mutual overlapping thereof. The method accordin& to the inven-tion permits a quenching or extinction of these disruptive "hot bands" and, accordingly the formation of spectra which are shifted toward one another because of the isotopy effect and are consequently selectively detectable through monochromatic laser light. These hot bands have the result that, at room temperature, over a thousand different oscillation states are occupied.
Each o~ these states has its own, relatively simple spectrum that would, in principle, afford the laser isotope separation. The number of these hot bands greatly depends upon the temperature, only for vibration temperatures below 30 K does there exist yet a single oscillation or vibration state, the basic state. For the selective excitation in the ultraviolet or W range, it is not necessary, ho~ever, to operate absolutely at such low temperatures, on the , 30 contrary, temperatures that are lower than about 150K are sufficient. The i ~ 2 -~ ' ' .

~ 0~73~50 consequently existing, approximately fifty oscillation or vibration states of the UF6 and the hot bands resulting therefrom are distributed over the large range of the UV spectrum. This spectrum has a dimension of about 15,000 cm 1 ~4000 ~ to 2500 A), the bands are 20 to 30 cm 1 wide, so that approximately 500 oscillation or vibration bands are accommodated in the space without overlapping. A result thereof is that for 150K and lower temperatures, the selective excitation of a single isotope compound is possible.
As mentioned hereinbefore, such low temperatures are attainable through adiabatic cooling resulting from expansion of the gaseous UF6. For this purpose, the gas must be forced through a slot nozzle which is very difficult to manufacture and, furthermore, because of the expansion, the particle density is so low that only a relative small part of the laser light can be absorbed.
To avoid the foregoing disadvantage, in accordance with the inven-tion, the vibration temperature of the isotope compound, such as UF6, for example, is cooled off with the aid of a diluent gas which need not take part in the chemical reaction and which possesses a temperature barely above the condensation point thereof. At this low temperature, only a few vibra-tion states of this diluent, additive gas are occupied. Before mixing the isotope compound with this additive or diluent gas, the îsotope compound is mixed with the gaseous reaction partner, the temperature of this mixing being approximately at room temperature and thus higher than the temperature of the diluent gas. Through the subsequent mixing with the diluent gas, a rapid adjustment or equalization of the occupancy of the vibration state level be-tween the isotope compound and the diluent gas occurs, with a time require-ment of about 10 ys, so that the occupancy of the higher vibration level of the isotope compound is decimated or drastically reduced, while the higher vibration level of the diluent gas is only slightly excited because it exists ' in excess quantity. This diluent gas is therefore selected so that it can absorb as much as possible of the vibration or oscillation energy of the 1(~'73~50 isotope compound which, besides the selection of material, can be controlled additionally due tc the excess quantity thereof. This means, in other words, a rapid equalization of the occupation of the vibration states i.e. a rapid ; "vibration or oscillation cooling" of the isotope compound and therewith the hereinaforedescribed selective excitability due to monochromatic laser light.
The maximum of the vibration cooling is attained after a period of 40 ~s.
For the excitation operation, it is necessary, however, that these continuously, always freshly cooled molecules of the isotope compound can be detected and can then react immediately with the reaction partner. For this purpose, a carrier gas flow ~preferably, a noble gas) is supplied which tran-sport the cooled-off gas mixture through the region of laser irradiation.
The excitation by vibrations or oscillations in the cooled isotope mixture due to the kinetic energy of the carrier gas requires a time period of from 200 to 1000 ~s, but actually occurs much more slowly than the ! equalization of the vibration or oscillation level between the isotope mix-~' ture and the additive or diluent gas.
i Other features which are considered as characteristic for the '~ invention are set forth in the appended claims.
Although the invention is illustrated and described herein as em-'t~ 20 bodied in a method of separating gaseous isotope compounds and apparatus, it is nevertheless not intended to be limited to the details shown, since various modifications and structural changes may be made therein without departing from the spirit of the invention and within the scope and range of 1 equivalents of the claims.
i The construction and method of operation of the invention, however, together with additional objects and advantages thereof will be best under- ~`
stood from the following description of specific embodiments when read in connection with the accompanying drawings, in which: -, ~ Figures 1 and 2 are diagrammatic vertical and horizontal section ii 30 views, respectively, of apparatus for carrying out the method of the invention.
., .

~1738SO

It will be noted that in the description of the drawing presented hereinafter additional details of the method o~ the invention will be men-tioned.
For use with the apparatus of Figures 1 and 2, UF6 has been selected as the isotope compound A. The apparatus per se is formed of a supply vessel 1 for carrier gas C which is conducted through a valve 2 into a distributor chamber or plenum 3. Upon leaving the chamber 3, the gas C is accelerated in a conventional manner to a velocity of about 500 meters per second (m/s).
One possible manner of effecting this, would be for example, to heat the carrier gas C to a higher temperature and bring it up to the required flow velocity through a simple nozzle.
A mixing tube 5 is connected to the distributor chamber 3 by a nozzle 4, the isotope compound A and the reaction partner D, on the one hand, as well as diluent gas B, on the other hand being fed to the mixing tube 5 -through a multiplicity of respective inlet openings 7 and 8. As is apparent from Figure l, the multiplicity of inlet openings 7 and 8 are so disposed as to direct the respective gases A, B and D into the mixing tube 5 at an angle to the axis thereof. The reaction partner enters through a tube 71 into the opening 7 and mixes with the isotope gas A before passing into the mixing tube 5. The carrier gas C then meets with the mixed gases A and D as well as the diluent gas B in the mixing tube 5. The carrier gas C has a velocity of about 500 m/s as it enters the mixing tube 5. The openings 7 and 8 through which the other gases A, D and B are fed into the mixing tube 5 have a respective diameter of about 0.1 mm. The temperature of the gases A and D
is also like that of the gas C, namely about 300K, however, the pressure thereof is 0.1 Torr. The temperature of the diluent gas B, on the other hand, is only 100~K, and the pressure thereof 1 Torr.
The mixing time for these gases is about l0 to 30 microseconds (~s) and the gas mixture covers a distance of from 0.5 to 1.5 cm in this period of time along a path 51 in the tube 5. After the mixing process has been . : , . : . , : ~, . .... : . .. . . . ....... . . .

1(~ 350 completed, irradiation of the mixture is effected by a non-illustrated laser light source. An irradiation chamber 52 is therefore connec~ed to the end of the path 51. The irradiation chamber 52 is laterally defined by two Brewster windows 53 formed of CaF2 which permit the laser beam to pass therethrough practically without loss. It is advantageous to arrange this irradiation chamber 52 so that it is shiftable or displaceable. It can then be shifted from a point about 1 cm behind the nozzles 7 and 8 to about 10 cm behind those nozzles together with the non-illustrated laser device, and adjusted in such a manner that the laser beam strikes the gas mixture at the maximum of the "oscillation cooling of the isotope gas A which is reached after about 40 ~s."
A reaction chamber 54 having the same cross section as that of the irradiation chamber 52 is connected to the latter. In the pa~h through this reaction chamber 54, the chemical reaction between the supplied reaction partner D and the excited isotope compound A occurs. In a condensation chamber 6 connected to the reaction chamber 54 and provided with water-cooled ~ walls, the reaction product separates out or dPposits preferably in solid - form, the remainder gases being discharged through a suction outlet opening 62 with the aid of a non-illustrated pump, The throughput or flow rate of the isotope compound A, for a velo-'' 20 city of the carrier gas C of 0.5 ~ lO cm/s, is 3 105 cm3/s. For the here-inaforementioned pressure of 0.1 Torr, this corresponds to a quantity of 1.75 mMol/s or 0.1 Mol/min. If the isotope that is to be selectively excited is present in a relation or proportion of 0.7% in the isotope mixture (this is the pereentage of the fissionable uranium isotope U235 in the natural uranium), light in an amount of 0.75 . 10l9 photons/s must be'beamed in for the purpose of exciting each molecule of this isotope. This corresponds to a laser powder of about 5 Watt for a wavelength of 300 ~ = 3000 A.
For the isotope compound UF6, hereinaforementioned in this example, and hydrogen as reaction partner, the following chemical process then occurs in the reaction path of the chamber 54:

.. . .

~73~50
2 UF6 + H2 s 2 UF5 ~ 2 HF
UF5 is a solid and deposits as dust in the condensation chamber 6.
When using C0 as reaction partner, the following reaction occurs:
UF6 + CO ~ UF5 + CF0 ~ UF4 + CF2 0 When using CH4 as reaction partner, the chemical reaction reads as follows: ~ ~
UF6 + C~4 ~ UF5 + C2H6 ~ CH3F + HF -SF6, C0 or CH4 can be used as diluent gas. The cooling thereof can be effected in a conventional manner, for example, through heat exchangers, the primary circulatory loop of which is traversed, for example, by liquid ~;
helium. Since the diluent gas is present in considerably greater quantity than the isotope gas, it remains also in the reaction path 54 at a relatively lower temperature so that it practically does not take part in the chemical reaction with the excited isotope compound. The reaction gas must, therefore, be separately mixed with the isotope gas even if it is of a type that is the same as the diluent gas.
Noble gases i.e. monatomic gases, are chiefly employed as the carriergasessince they are not able to absorb large amounts or parts of oscil-latlon energy. Indeed, it would also be possible to use hydrogen as carrier gas. In such a case, the supply line 71 for the reaction partner D could be dîspensed with.
It should also be noted that the irradiation chamber 52 can be dis-posed in a conventional manner between two resonator mirrors so that the laser beam reflects therebetween and is amplified to a maximal extent so that only the pure absorption losses within the gas mixture must be replaced by the laser. It is also possible to achieve, in a conventional manner, through other mirror systems, the passage of the laser beam through the gas mixture ~' in the irradiation chamber 52 along many, practically parallel paths, and thereby increase the excitation efficiency.
The hereinaforementioned device for carrying out the method of the , ~, , , , :
~, . ~ . . . ' ' , ' ' '' ~(~73~5() invention may, of course, be modified in many respects, and the construction :
thereof must depend especially upon the laser that is to be used. The frequency of the laser should particularly be adjustable or tunable so that final tuning or adjustment for the excitatîon can be determined empirically.

. ~:
:
:

,, , .. , : . . , , ' :.

Claims (6)

THE EMBODIMENTS OF THE INVENTION IN WHICH AN EXCLUSIVE
PROPERTY OR PRIVILEGE IS CLAIMED ARE DEFINED AS FOLLOWS:
1. Method of separating gaseous isotope compounds through selective exci-tation and subsequent chemical reaction with a gaseous reaction partner as well as separation of the reaction product from the remaining gas mixture, which comprises mixing a mixture of the gaseous isotope compounds that are to be separated and the reaction partner with a neutral, multiatomic diluent gas sharply subcooled to a temperature close to the condensation temperature thereof during a time period adequate for absorption of the oscillation energy of the isotope mixture yet inadequate for affording reproduction of the original condition of this mixture, transporting the isotope mixture with a carrier gas to a beam path of a laser with a flow velocity adjusted to the excitation frequency of one of the isotope compounds, the time during which the transport occurs corresponding to the time required for absorbing the oscillation energy, and then delivering the thereby resulting chemical reac-tion product to a separation device.
2. Method according to claim 1 which comprises initally heating the carrier gas to a higher temperature and then passing the heated carrier gas through a simple nozzle to impart the flow velocity thereto.
3. Method according to claim 1 wherein the gaseous isotope compound is UF6, the reaction partner H2, CO or CH4, the diluent gas SF6, CH4, or CO and the carrier gas Ar, He, Kr or Xe.
4. Method according to claim 3 wherein the carrier gas and the reaction partner are both H2, and wherein the mixing thereof with the isotope compound is effected at a time before the diluent gas is fed to the mixture.
5. Device for carrying out a method of separating gaseous isotope com-pounds according to claim 1 comprising a supply vessel for carrier gas, a heating device connected to said supply vessel for heating the carrier gas, said heating device being formed with a slot-like accelerating nozzle, a mixing tube chamber portion communicating through said nozzle with said heat-ing device, feed lines for isotope compound, reaction partner and diluent gas terminating in said mixing tube chamber portion, an irradiating chamber communicating with and adjustably spaceable from said mixing tube chamber portion, said irradiating chamber having Brewster windows for affording ac-cess to the interior thereof of a laser beam, a reaction chamber communica-ting with said irradiation chamber, and a collecting chamber constructed as a cooled condensation chamber and, in turn, communicating with said reaction chamber, said condensation chamber having connected thereto suction means for removing remainder gas therefrom.
6. Device according to claim 5 including first pipelines for supplying the reaction partner to said mixing tube chamber portion, and second pipe-lines for supplying the isotope compound to said mixing tube chamber portion, said first and second pipelines being connected to the respective feed lines therefor directly before inlet thereof to said mixing tube chamber portion.
CA290,493A 1976-11-10 1977-11-09 Method of separating gaseous isotope compounds and apparatus Expired CA1073850A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE19762651306 DE2651306A1 (en) 1976-11-10 1976-11-10 PROCESS FOR THE SEPARATION OF GASEOUS ISOTOPE COMPOUNDS

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CA1073850A true CA1073850A (en) 1980-03-18

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JP (1) JPS5360493A (en)
AU (1) AU510304B2 (en)
CA (1) CA1073850A (en)
DE (1) DE2651306A1 (en)
FR (1) FR2370507A1 (en)
GB (1) GB1560980A (en)
IL (1) IL53294A (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2900689C2 (en) * 1979-01-10 1984-09-20 Deutsche Forschungs- und Versuchsanstalt für Luft- und Raumfahrt e.V., 5300 Bonn Use of a device with a mixing body for mixing a gaseous isotope mixture with an additional gas during isotope separation by selective laser excitation

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2447762C2 (en) * 1974-10-07 1987-10-01 Kraftwerk Union AG, 4330 Mülheim Method and device for separating mixtures of substances and application of the same for the production of chemical compounds
DE2458563A1 (en) * 1974-12-11 1976-06-16 Uranit Gmbh PROCESS FOR ISOTOPE SEPARATION BY USING LASER

Also Published As

Publication number Publication date
AU510304B2 (en) 1980-06-19
FR2370507B1 (en) 1980-10-10
IL53294A (en) 1980-11-30
JPS5360493A (en) 1978-05-31
FR2370507A1 (en) 1978-06-09
AU3034577A (en) 1979-05-10
DE2651306A1 (en) 1978-05-11
GB1560980A (en) 1980-02-13

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