IL46624A - Method and apparatus for separating the isotopes of a chemical element - Google Patents

Description

method aa& apparatists for se arating the isotopes of a chemical elem nt FERMI© MAR08L DBVIESrM 0/ 44594 46624/2 This invention relates to techniques for the separation of chemical compounds having molecular masses which are very close in value and especially isotopic species of the different elements. The invention applies primarily although not in any limiting sense to the separation of uranium isotopes of mass 235 and 238.

A number of methods which can be employed for separatin the isotopes of chemical elements are known at the present time and these mainly include mass spectrometry and methods which are derived from this latter, namely the so-called gaseous diffusion methods, the methods of separation by electrolysis or by dual-temperature exchange as well as the techniques of separation by ultracentrifugation. A certain number of disadvantages are attached to all these methods which have been employed at different times and for various reasons. They give rise in any case to high capital expenditure and also to practical difficulties whenever steps are taken to carry out large-scale production of chemical elements which are strongly enriched in one of the isotopes constituting the original natural element.

According to an interesting variant of the method, means are provided between two successive boxes for collecting the secondary ions of each isotopic species, each species being thus condensed in an independent accessory device.

More specifically, such an accessory device can generate a transverse electric field adapted to deflect the low-energy ions and permit to extract the latter laterally with respect to the beam.

In the very important case of separation of the uranium isotopes , enrichment by gaseous diffusion is the only technique in actual use on an industrial scale today. Specialists in this field are well aware of the fact that, although it produces remarkable results, this technique is very difficult to apply in practice from a technological standpoint and is fairly costly from an economic standpoint by reason of the very large number of microporous barriers through which uranium hexafluoride UFg has to pass in order to permit significant preferential diffusion of the isotope 235 with respect to the isotope 238 „ Furthermore, all the difficulties inherent in the actual nature of the only gaseous compound which can he employed for this purpose, namely hexafluoride UF^, are well-known ; this compound is in fact highly corrosive, highly toxic and is in the gaseous state only above approximately 65 °C The present invention relates to a method in which the isotopes of a chemical element are separated by successive filtrations of a beam of positive or negative ions, which is much more straightforward than the techniques of separation by gaseous diffusion and which provides at least equal efficiency from an economic point of view.

This method of separation essentially consists in producing a beam of positive or negative primary ions of at least one compound of said element, in accelerating said ion beam in order to pass said beam through a predetermined number of collision boxes which are open at both ends and placed one after another in series, in successively initiating within each collision box, by inelastic collisions of said ions with the molecules of a neutral target gas with which said boxes are filled at low pressure, the dissociation of a given percentage of the primary ions into at least two fragments such that one fragment is a secondary ion which appears in the form of at least two different isotopic species with respect to the element to be separated, and in choosing the potential V^ to which said collision boxes are brought in order to trap preferentially therein one of the abovementioned isotopic species which is caused to condense within each collision box, The method according to the present invention is neutral targe , gas under low pressure contained in a collision box is bombarded with, a beam of primary ions of a compound of the element whose isotopes are to be separated a given percentage of these primary ions is dissociated by inelastic collisions with the molecules of the neutral target gas and the secondary ions thus formed carry away with them in practice a kinetic energy which is proportional to their mass. In consequence, if the electric charge of the secondary fragments thus formed is known, it is possible to select a sufficiently high potential °f opposite sign to this charge and at absolute value to ensure that said secondary ions do not have the necessary kinetic energy to pass across the potential barrier corresponding to the exit of the box in which they have been formed, with the result ■■■ that they are trapped inside this latter. It is thus apparent that, if some of the dissociation fragments carry the same electric charge and appear in the form of several isotopic species, the value of the voltage "V^ to which the collision box is brought can be chosen so that the fragments corresponding to one of the isotopic species (namely the heaviest) pass to the exterior whilst the fragments corresponding to another species (namely the lightest) are on the contrary retained inside the box. Provision needs only be made in this case for a set of collision boxes placed behind each other in series and all brought to the same potential Vj, in orde to obtain from a beam of primary ions of given energy a decomposition followed by a trapping in series within each box of a certain number of secondary ions which are thus separated as a function of their respective mass, that is to say of their isotopic species in the case under of very general application and scope · the primary ions employed may with equal ease be either positive or negative and it is possible to collect at will either the heavy isotope or the light isotope as the case may be„ In. fact, if it is desired to collect the lighter compound, this latter is readily obtained by simple condensation within the boxes in which it is trapped ; on the contrary, if the heavy component is to be collected, this component is found again in the beam at the exit of each box, at which it can be extracted simply by electrostatic deflection. Moreover, it is to be understood that the process which is essentially described in this specification's being applied to isotopic separation, can be used in a manner which is evident to anyone versed in the art for the chemical separa-tion of ionized molecules having masses which are ' different and especially very close in value. .The neutral target gas employed can be as desired 5 rare gases such as argon and helium for example are wholly suitable „ In accordance with an important feature of the present invention, the voltage is chosen on the basis of information previously recorded experimentally in regard to the location and area of the different energy peaks corresponding to each of the secondary ions formed in the boxes while taking into account the fact that the chemicals-nature and the proportion of secondary ions trapped within each box are defined by the presence and the area of said peaks or portions of peaks located within the range of voltages which are lower at absolute value than the value chosen for the voltage Vg.

An essential difference between the method separation by gaseous diffusion is immediately apparent. In the techniques just men ioned, : he enrichment is in fact progressive and' takes, place- very slowly from stage to stage through hundreds of thousands of barriers placed in series on. the c ontrary , in the case of the present invention, the physical separation phenomenon is reproduced qualitatively and identically within each of the boxes which constitute a given set. To this end, all the boxes are" brought to the same potential s Q- the ions which have not beer- dissociated withi a bo of the order JD pass out of this box and penet ate into . the following box of the order ] ;-l, "A final enrichment factor corresponding, exactly to the selected value is achieved simultaneously within, each, , collision bo and in a single step.. It then'-only remains necessary to condense on the walls of each box the material corresponding to the separated secondary ions trapped therein in order to obtain directly either the chemical compound which is enriched in one ofsits constituent elements or a mixture which contains $aid compound.

An elementary calculation makes it possible to determine the efficiency of decomposition of the incident beam of primary ions and by this very means to form an estimate of the efficiency of the process. In fact, if the initial ions conform to one decompbsition diagram alone and if the percentage ratio of this decomposition is equal to r % of the beam which enters each box, the initial io beam emerges from the nth box with an intensity ratio equal to (1 - r)n with respect to the beam which enters the first box. (Strictly speaking, this calculation presupposes that one neglects the effects of dispersion of the beam arising charges between the ions of the beam and the molecules of .the neutral target gas but it is confirmed by experience that this approximation is justified in order to obtain correct orders of magnitude).

For example, if r = 0.05 , if n. = 20, the beam emerging from the nth box represents 55 .85 % of the initial beam, the decomposition . within the boxes is 64 -.15.·!%; '·'·-. IiE it is assumed tha n = 40, the emergent beam represents in that case only 12.85 % and the decomposition is 87 .15 .

By virtue of the simplicity of the system, it is possible by. way of example to adopt a mean distance of 8 to 10 cm between the centers of the boxes and to have an apparatus having a diameter of 20 to 25 cm and a length of the order of 2 , with 20 boxes each fitted with an interchangeable liner tube in. order to permit ready collection of the ions which have been trapped and condensed oh its internal wall. If the dissociation efficiency' is' higher than j the number of boxes can be reduced. On the other hand, if the efficiency is only 2 to.5 this figure can be increased...

In accordance with a secondary feature of the method which forms the subject of the invention, the secondary ions which are not trapped in a collision box pass out of this latter with a. very low kinetic energy which is close to zero since their mass is by definition very close to that of the isotope which it has been endeavored' to trap. They can therefore very readily be extracted from the primary ion beam which continues to travel within the following collision box, as a result of simple elec rostatic deflection by means of a weak field V ) itself.

In the more general case, however, in which there are a number of diagrams of dissociation of primary ions into secondary ions, the formula given above is no longer valid since the phenomena are more complex and it is very easy to understand intuitively that the final efficiency of the desired isotopic separation is consequently reduced .

It is also recommended to choose a pressure of neutral gas within each collision box so as to ensure that, on the one hand, the dissociation phenomena are distributed within each of the collision boxes constituting a group and that, on the other hand, the processes of charge transfer between the incident beam of primary ions and the neutral gas molecules are not of excessive magnitude. In any case, this phenomenon can never be completely avoided but is not usually troublesome since it represents only a small fraction of the incident ions · these latter are thus converted to neutral molecules and continue to travel through all the boxes in series of a given group while being naturally lost so far as the isotopic separation and dissociation reaction is concerned.

In even more precise teims, the invention is directed to a method fo the separation of isotopes of chemical elements in which the primary incident ions of charge e and of mass M enter each collision box with the energy eV-^ and there is retained in each box at least part of the formed secondary ions of mass m and of charge e corresponding to the isotopic species to be separated by bringing each collision box to a potential "^ °f opposite si n to that of the char e e and of absolute value at leas In theory, the overall result is therefore exactly the same as if, in the case of a secondary ion having a given mass m and corresponding therefore to a predetermined isotope of the chemical element to be separated, there existed a critical value of the potential to which the different collision boxes are brought and above which all the secondary ions corresponding to the same mass are retained in the corresponding, boxes „ In the particular but very frequent case in which' he separation which is desired to carry out concerns a separation between two isotopes of the same chemical element, it should theoretically be possible to separate them by choosing for the potential of the different collision boxes a value' between the critical values corresponding to each isotopic species of the compound constituting the secondary ion of mass m„ This does not apply in practice and things are not so simple because in point of fact, by reason of the distribution of . the different energies of dissociation which are possible in the case of a given primary ion of mass about its mean theoretical value, the phenomena mentioned above are governed not by potential lines but by energy peaks of decomposition having a certain width and in which the respective areas in any case correspond approximately to the mass percentage of the different isotopes of the element considered 0 It can therefore be understood that a large number of possible cases of figures can arise : a) in the theoretical case in which the secondary ion of mass m has only two isotopic species in which the corresponding energy peaks of decomposition are completely separate* from each other,we revert to the previous case in choosing a voltage which is comprised between the two peaks 5 b) if, as is most usually the case, the energy peaks corresponding to two adjacent isotopes overlap to a partial extent or if, as is frequently the case, the diagram of decomposition into secondary ions results in a mixture of a number of isotopic fragments having different masses in which the peaks can even be placed astride of each other, the most favorable value of the voltage ^u-st "be determined empirically, precisely as a function of the total enrichment factor which it is desired to obtain 0 In some cases, this situation of partial overlap of the energy peaks can be an advantage since, by choosing precisely the value of the voltage of the collision boxes, it is sometimes possible to obtain a priori a composition of the material retained in said boxes in a predetermined isotopic ratio, that is to say to achieve a predetermined enrichment factor immediately and in a single step.

In order to apply the method according to the invention in the case in which, there is only one type of secondary ions containing the element to be separated in two isotopic species having masses rn^ and HL-,, it is convenient in practice to determine empirically between the two values the value of 1^ w ich provides the desired enrichment in one of the isotopes.

The desired enrichment can also be achieved if necessary in several steps at increasingly high factors ensure that this enrichment is not accompanied by a substantial loss of the desired isotope, which could have; been the case if it had been intended to obtain the same enrichment factor in a single step. By way of example, this makes it possible to employ primary ions which are themselves,-constituted by double isotopic mixtures (for example. UBr^, UBr^I, UCl^, UCl^I, and so forth) in which the energy peaks obtained are numerous and interlaced.

It can sometimes be an advantage to form the primary ion beam by means of a number of compounds of, the element to be enriched instead of a single compound. In all cases of application of the method, it is clearly a precise study of the diagram of decomposition in secondary ions and of the corresponding energy peaks which enables the experimenter to determine the advantage of a method of this type and the voltage V≥ which he must choose in order to obtain a predetermined enrichment factor 0 Finally, in an advantageous alternative form of the method, it can be useful to bring some boxes of a given group to slightly different potentials in order to effect simultaneous collection of mixtures at different enrichment factors determined experimentally by means of a previous study of the voltage peaks.

The method in accordance with the present invention offers a large number of specific advantages over the techniques of gaseous diffusion employed up to the present time. Among these advantages can be mentioned in particular - the practical application of the invention is particularly simple since .it essentially entails the use of a series of metallic collision boxes which are all brought predetermined temperature if necessary. These boxes are supplied with a neutral target gas at low pressure and are placed within a chamber in which a secondary vacuum is maintained No new technological problem needs therefore be solved in order to put a device of this type into operation. Furthermore, a separation plant which makes use of the method can be put into operation progressively and this makes it possible to distribute capital investments in time. In fact, each collision box produces a. quantity of enriched material in a single step with a predetermined enrichment factor as desired and any increase in number of the collision boxes has the effect only of increasing the quantity of enriched material produced. This method makes it possible to obtain uranium or a uranium compound at a given enrichment between 1 and 70 %, for example, in a single operation 5 the cost price of the enrichment is substantially proportional to the enrichment factor. Should it be decided to change over from a factor of 1 % to a factor of 70 %, no modification need be made in the apparatus Starting from uranium enriched to a few per cent, it is possible to obtain uranium enriched to 99 . It is also possible to employ separation wastes and to obtain uraniuin enriched to 3 , for example.

- Fault conditions which are liable to affect either certain individual collision boxes or a group of boxes in series in an isotope separation unit do not have ■ any influence on the remainder of the installation. Each collision box in fact operates independently of adjacent boxes andj in an installation comprising a number of groups, each, group is se.lf-contained and is not dependent in any way over the method of progressive enrichment in series.

In some particularly favorable instances, total separation can be obtained in a single step^ the isotope which is not retained in the boxes being simply recovered if so desired at the end of the beam path.

- It is possible to choose in each particular case the compounds used for producing the primary ion beam and consequently to operate with compounds which are more pleasant to handle than uranium hexafluoride with all its attendant disadvantages which have already been noted.

- It is not necessary to employ substances which already have a high degree of purity since it is an objective of the method according to the invention to sort components as a function of their different masses and since the impurities modify the efficiency only in proportion to their own concentration, - The installations can be constructed in simple metal hangars and do not require a very large area for the site location. No special precaution need be taken in regard to the environment and, depending on the chemical nature of the compounds employed, pollution hazards are usually infinitely lower than in the case of handling of uranium hexafluoride .

A clearer understanding of the invention will in any case be obtained from the following description of different examples of application of the method for separating the isotopes of a chemical element and of the device for carrying out said method. These different examples will be described with reference to the accompanying figures, in which ; variation of mass dm/dV trapped within each collision box, as a function of the potential which each box is brought ; - Fig. 2 shows in sectional elevation a partial view of an isotope separation apparatus in accordance with the invention, wherein Fig. 2a shows the main body of this apparatus and Fig. 2b shows the constructional detail of one of these collision boxes 5 - Fig. 3 is an axial sectional view of an installation comprising twelve groups of collision boxes in parallel within a common vacuum chamber.

Fig. 1 serves to provide a practical illustration of the comments previously made in regard to the choice in a particular case of the voltage V2 to which each collision box is brought as a function of the isotope separation factor which it is desired to attain. In the particular example of Fig. 1, consideration has been given to the case in which two compounds of closely related isotopic composition correspond respectively to the energy peaks of decom^-position 1 and 2 centered respectively on the voltages V!2 and V"2 and in which these two voltage peaks partly overlap. This is the case for example with the separation of the uranium tri-iodide ions having the respective formulae 2¾I5 and 2¾I3 . In Fig. 1, the area of the peak S-, with respect to the area of the peak S2 has been purposely , exaggerated for the sake of enhanced clarity of the drawing but these two areas are in fact in the same ratio as the natural isotope components. When this ratio is of very small value, it can even happen in some instances that the peak of one of the compounds is not clearly discernible -Less apparent irregularity of the curve of separation of the'"" isotope which is present in the largest proportion.

The value V2 of the voltage which is really chosen for the supply of the collision boxes is materialized in the drawing by the vertical half-line 3 which delimits with the peaks 1 and 2 respectively the surface area S-^ in the case of peak 1 and the surface area S2 in the case of peak 2.

The isotopic proportion of the compounds in the mixture retained in the different collision boxes is equal to the ratio of the two areas and S2 corresponding to each of the two isotopes to be separated.

In some cases , it is advantageous to improve the efficiency of the condensation of trapped secondary ions which, in view of an insufficient deceleration, might tend to leave the collision boxes. To that end, and according to the invention, means for collecting the secondary ions can be provided between two successive boxes. By way of example, such means can consist in a plurality of grids (in equal numbers with the isotopic species to be separated) , brought to potentials that are slightly positive (if positive ions are involved) and that are increasing in the path direction, which permits to exert a strict control of the deceleration of the ions to be trapped. Each secondary ion species can thus be trapped in an independent accessing device, adapted in particular to generate a local transverse electric field for extracting the law-energy ions laterally with respect to the beam.

It can therefore be readily seen that, depending on the position chosen for the straight line 3, that is to say finally according to the value of V2 , it is possible to obtain either the first isotope in the pure state or a mixture of these two isotopes in predetermined proportions. It is also evident that there is no advantage whatever to be gained by giving V2 a value which is higher than V "2 above which both isotopes would then be trapped within the boxes, that is to say above which the original isotopic composition would finally be found once again.

In Fig. 2b, at the output of box 12 is shown, in diagrammatic form, a device which can prove of interest, in some specific cases, for improving the condensation, of secondary ions, should the latter, in view of an insufficient deceleration, would tend to leave the box.

To that end, deflector 19 comprises two grids 33 and 34 brought to retarding potentials , between which are generated, by known means such as plates 35, transverse electric fields E1 and E2 adapted to provide the lateral extraction of low-energy secondary ions. These fields of low intensity have substantially no effect on the non decomposed primary ions Anyone versed in the art can readily generalize the reasoning drawn from this figure 1 to the case in which the energy peaks of the different masses are more than two in number and may even relate to a plurality of chemical compounds of one and the same element which is present in the form of several isotopic species. It needs only be considered in fact that the total masses retained in each box have a chemical nature and a proportion in the overall mixture which are represented by the presence of the different decomposition peaks and the sum of the areas of f the different peaks located on the left-hand side of the straight line 3 in Fi . 1. In each particular case, anyone versed in the art who has studied the decomposition diagrams and drawn up the chart of the separation peaks will he able to choose the abscissa "V^ of the straight line 3, that is to say the potential of the collision boxes as a function of the desired result.

Referring now to Fig. 2, there will be described in greater detail an apparatus in accordance with the invention for carrying out the method. This apparatus essentially comprises a frame 4 on which is mounted a tubular chamber 5 hermetically closed at one end on an ion source 6 and at the other end by a detachable cover 7° This tubular chamber 5 is provided with a lateral opening .8 of ' large size for putting said chamber into communication with a secondary-vacuum pumping system comprising a first primary-vacuum pump 9 completed by a second secondary-vacuum pump 10. The combined assembly of the two pumps 9 and 10 as shown diagrammatically serves to maintain a vacuum of the order , of 10 torr within the tubular chamber 5.

In accordance with the invention, there is removably and slidably mounted within said tubular chamber 5 a cylindrical liner tube 11 on which are fixed in axial alignment the different collision boxes such as 12, 13, 14, 15 and 16. These different collision boxes are of metal and brought to the same potential V2 by means of the electric conductor 17 which supplies them in parallel ; furthermore, these collision boxes 12 to 16 are also supplied in parallel via the pipe 18 with a neutral gas such as argon or helium -3 for exam le at a low ressure of the order of 10 torr. 16 for an electrostatic deflector, five of which are shown in this example and designated respectively by the reference numerals 19, 20, 21, 22 and 23, As explained earlier, these deflectors are intended to cause the isotope compounds of mass m which have not been trapped within the collision boxes to be deflected towards the walls of the cylindrical liner tube 11 on which they are condensed „ To this end and as already explained in the foregoing, a very low voltage is sufficient since, by definition, these secondary ions are discharged with a kinetic energy which is either close to zero or very weak and it is therefore possible to separate them from the primary ion beam without thereby resulting ±Q any appreciable disturbance of this latter.

Fig. 2b shows on a larger scale the constructional detail of a collision box such as the box 12 provided with' a body 24 and with two screwed-in covers 25 and 26 each having a central aperture 2 and 28 for the passage of the beam ; the cylindrical body 2A is also provided with a terminal lug 29 for bringing the unit to the desired potential V2 and with a nozzle 30 which is connected to the pipe 18 and thus serves to maintain a low pressure of neutral gas within the box 12. This neutral gas therefore escapes continuously through the apertures such as 27 and 28 of each collision box towards the interior of the tubular chamber 5 from which it is continuously extracted by the pumps 9 and 10.

When this proves necessary, it is also possible to cool the walls of each of the chambers 12 to 16 in order to cause the condensation of the gaseous material corre-sponding to the secondary ions formed and retained within readily be constructed and has not been illustrated for the sake of enhanced simplification of the drawing of Fig. 2.

In order to give a clear idea in regard to the possible orders of magnitude of an installation in accordance with the description of Fig. 2 , there is commonly employed a group of 10. collision boxes each having a diameter of 3 cm and a length of 6 to 12 cm. A space of 2 cm is maintained between two consecutive boxes and the cylindrical liner tube 11 has a diameter of 15 cm.

When the apparatus has operated for a sufficient period of time to produce by condensation within each collision box the requisite masses of either pure or enriched isotopic compound, it is then only necessary to withdraw the removable cylindrical liner tube 11 from the tubular chamber 5 in simple translational motion, whereupon the material obtained can be collected directly from the internal walls of each collision box. It should- be noted that this apparatus also makes it possible to recover the portion of the mass corresponding to the secondary ions which have not been trapped within the boxes and which has become attached to the cold internal walls of the removable liner tube 11 during the performance of the process.

Fig. 3 shows, within a cylindrical chamber 29 formed by two half-shells 9a and 29b , a series of twelve separation units such as 30 which are held in position by means of metallic spacer members 31 = This arrangement makes it possible to optimize the overall size of an apparatus comprising a plurality of separation units in the smallest possible volume. In order to carry out dis-charging operations, the two half-shells 29a and 29b o en By way of example, the apparatus described above can be employed for separating the uranium isotopes from uranium tetraiodide having the formula UI^ by adopting the two following decomposition diagrams which are observed simultaneously in the most frequent case · UI^ ~— UIj I and UI* — UlJ + ∑2 w th respective yields of 8.3 % and 1.2 % of UI^ and UI2 secondary ions formed with respect to the UI^ primary ions.

Under these conditions, a source of UI^ primary ions is employed for the 'purpose of producing the beam which is propagated through the different collision boxes which are filled with an inert gas such as argon or helium. The UIj secondary ion then appears in two different species namely and 2^¾ΊΪ which correspond respectively to decomposition ratios mM having values In order to carry out the separation of these two ions by preferential trapping of the ion in the different collision boxes, it is only necessary to apply to each box a voltage comprised between the two calculated values V'2 and V"2 which are given by the following formulae : - xl Vl 1 - x, - x2 1 - 2 - 4.8503 and - 4.8740 V-,_ ; the first of these two voltages corresponds to the summit of the peak of the compound and the second voltage corresponds to the summit of the peak of the compound 2^¾Ί^.

If the decomposition and the parasitic phenomena are not of excessive magnitude, the energy peaks are completely separated although superposition of the two peaks may occur in the majority of cases as a result of the decomposition energy. Depending on the desired degree of enrichment, a voltage comprised between the two values Vl2 and V"2 s adopted for the box B2, If V-j^ = 2000 volts is adopted, the voltage V2 therefore caused to vary between - 9700 volts and - 9748 volts. When the conditions of decomposition are known, the voltage V2 cari 0I" course be determined empirically in order to produce a given value of enrichment.

If ten collision boxes are employed in series, the total decomposition of the beam is 1 - (1 - r)10 = 1 - 1 - (0.083 -i- 0.012)j10 = 1 - (0.905)10 = 1 - 0.369 = J 0.631.

In ac ual fact and under ordinary experimental conditions, there is found a not-negligible proportion of UIj, (nearly 20 % in the source beam), the decomposition diagrams of which are as follows · UI — UI2 + I UI -—> UI+ ÷ i2 The decomposition yields with respect to the initial ion beam which enters each collision box are 0.7 and 0,3 % respectively. the voltage In the case under consideration, both experience and a study of the energy peaks of UI^, UI^ and UI* lead to the choice of V2 = - 9720 volts instead of - 9724- volts for example (this value corresponds to V' + V» ) if it is desired to obtain an enrichment of 3 % in a single step.

In this example of application, the collision boxes can be cooled to approximately 150° C if necessary in orde to cause the condensation of UI^ on the walls* Other halogenated .oompounds of uranium are equally well suited to the separation of the uranium-235 isotope ;· by the method accordin to the invention 5 among these can be mentioned by way of example the bromides UBr^, U r^I and UBr^^ s:nd. the chlorides UCT^,; UCl^Br. and UCl^I.

In the case of the derivatives UBr^, ■ UBr^I or UCl^I, the formation of the secondary ion results in the loss of an atom of Br in the- first case and in the loss of an iodine atom in the last two cases and the corresponding energy peaks are often interlaced. Under these conditions. optimization must be sought by making a judicious choice of the voltage between two generally contradictory objectives, namely the achievement of a predetermined and relatively high enrichment factor in a single step or the desire to avoid excessive loss of U-235 in. compounds having a mass of higher value than that of the compounds which are retained in the boxes.

In the case of the bromide UB ^, the decomposition reaction employed corresponds to the diagram ; U 8½r3 7¾r+ -→ U 81Br÷ ,· 7¾r 481 .. n 478 in the case of the isotope 235 of U, x2 = ~ = = O.858I If = 2000 V is adopted, we obtain V' = ~ xli—Vl±- = - 1209 volts 1 - ¾ V"2 = " X2≤—Vl±- = - 1217 volts 1 - x2 By choosing V2 = ~ 12 120 volts, a study of the energy peaks shows that there is a 10 % enrichment in Since the probability of existence of the compound U the real enrichment will in fact be only 3/16 x 10 % - 1,8 5 . If it is desired as a final objective to obtain a real enrichment of 3 , two successive operations are therefore required in order to achieve this result.

In each particular case, the choice of the use of either one, two or a number of operations is governed only by the objective to be gained. 46624/2 ,^

Claims (4)

1. A method for separating the isotopes of a chemical element, wherein said method consists in producing a beam of positive or negative primary ions of at least one compound of said element, in accelerating said ion beam in order to pass said beam through a predetermined number of collision boxes which are open at both ends and placed one after another in series, in successively initiating within each collision box, by inelastic collisions of said ions with the molecules of a neutral target gas with which said boxes are filled at low pressure, the dissociation of a given percentage of the primary ions into at least two fragments such that one fragment is a secondary ion which appears in the form of at least two different isotopic species with respect to the element to be separated, and in choosing the potential V2 to which said collision boxes are brought in order to trap preferentially therein one of the isotopic species aforesaid which is caused to condense within each collision box.

2. A method for separating isotopes according to Claim 1, wherein means are provided between two successive boxes for collecting the secondary ions of each isotopic species, each species being thus condensed in an independent accessory device.

3. A method according to Claim 1 for separating the isotopes of a chemical element, wherein the voltage is chosen on the basis of information previously · recorded experimentally in regard to the location and area of the different energy peaks corresponding to each of the secondary ions formed in the boxes while taking into account the fact that the chemical nature and the proportion of secondary ions trapped within each box are defined by the presence and the area of said peaks or portions of peaks located within the range of 46624/2

4. - A method according to claim 1 for separating the.' · isotopes of a chemical^ element, wherein all the collision boxes forming part of any one assembly are brought to the same potential V2.„ ■ 5„ A method according to claim 1 for "separating the isotopes' of a chemical element, wherein at least a number .( of boxes of any one assembly are brought to slightly ' different potentials in order to collect mixtures having J isotopic compositions which are also different. · ,6, A method according to claim 1 for separating the, isotopes of a chemical element, wherein the primary incident ions of charge e and of mass M pass into' each . :< 'collision box with the energy eV^ and there is retained in .! e*ach box at least part of the formed secondary ions of mass j. m and of charge e by bringing each collision box to a . ·! potential V2 of opposite §ign to that of the charge e and of absolute value at least >equal to mV-j/(M ~ m) subject ,to ..· deviations arising from the distribution of the ion dissociation energies about said value. .•'7. A method according to claim 1 for separating the isotopes of a chemical element, wherein the primary ... incident ions of charge e and of mass M enter each collision box with the energy eV^ and produce by dissociation' a secondary ion of charge e which exists in two isotopic species having respective masses rn^ and m2 (m^ ir,) and ■ at least part .of the ions of mass rn^ is trapped preferen- ' tially within each collision box by bringing each box to a vpotential V of opposite sign to th of the- charge e and; ■ a-nd eviations 46624/2 arising from the distribution of the ion dissociation energies about these two values, 8,· A method according to any one of claims 1 to T>9 wherein the untrapped secondary' ions are eliminated from the beam between two consecutive boxes by means of a weak electrostatic field which produces practically no action on ; the primary ion beam. . j 9".„ A method according to any one of claims 1 to 7, wherein the collision boxes are cooled so as to ensure trapping of the ions retained by condensation on the walls. 10. A method according to any one of claims 1 to 7? wherein the collision boxes are filled with a target gas 'i under a pressure of the order of 10 torr. j 11.,· A method according to claimiO, wherein the target j gas is a rare gas selected from the group comprising argon, i and helium. 12, A method according to claim 1 for separating the ■uranium isotopes 258 and 235» wherein a beam of uranium. iodide ions UI^ is caused to pass through a predetermined number of collision boxes filled with argon under low pressure by employing the decomposition reaction , UI^ —> UIj ·!· I and by choosing the potential of each collision box aforesaid such that at least part of the 23*5 ·+ "TJIj- ions thus produced does not have a sufficient kinetic energy to. leave the box in which they are' formed. ' 13.» A method according to -claim 1 for separating the ' uranium isotopes 238 and 235 s wherein a beam of uranium iodide ions UI^ is caused to pass through a predetermined number of collision boxes filled with argon under low pressure by employing the decomposition reaction TTI^ —> UI*^' -:- I and wherein the degree of enrichment in 46624/2 -¾ of the ions trapped in each box is adjusted by adopting for Vg a value comprised between the energy peaks 235 + corresponding respectively to the trapping of UI^ and of 23¾i|. '■'.14. method according to claim 1 for separating the uranium isotopes 238 and 235 > wherein halogenated compounds ! of uranium are employed as primary' ions and selected from . the. roup comprising the bromides UB ^, UBr^I, UBrglg an& the chlorides UCl^ and UCl^Br, Ϊ5, A method according to claim l for separating the uranium isotopes 238 and 235? wherein use is made of the decomposition reaction 2¾ 81Br^ ¾r+ → 25% 81Β^ 7%r„ | ■■■.. 'δ, . An apparatus for carrying out the method of separation of isotopes according to any one of claims 1 to wherein said, apparatus comprises within a cylindrical j liner tube an assembly of 'metallic collision boxes aligned alohg the common axis thereof and each pierced by a beam' entrance aperture, and a beam exit aperture, means for carry-, ing out in parallel a supply of neutral gas at low pressure within each box, means for bringing each of said boxes in parallel to a commo electric potential Vg* means for cooling said boxes and a deflecting electrode between each box, said liner tube being removably mounted in sliding motion within ■ ■a fixed tubular chamber which is closed at one end' by an ion source whose axis coincides with the common axis of the collision boxes and at the other end by an impervious cover, said tubular chamber being adapted to communicate through a wide lateral opening with a secondary-vacuum pumping system. ■ : 17. ■ A method according to claim' 1 for. separating the . isotopes of a chemical element, substantially as hereinbefore described. 46624/2 IS1., An apparatus for carrying out the method of separation of isotopes according to claim 1, substantially as hereinbefore described with reference to and as illustrated' in the accompanying drawings. For the Applicants PARTNERS B.5219