Patent Number: 042242584
Section: summary

The invention relates to the production of uniform spherical particles of nuclear fuel or breeder materials from drops of aqueous solutions of nitrates of uranium, plutonium, or thorium, or mixtures of them, in which the solution is subdivided into drops by means of a vibrator and the drops fall into an ammonia solution for the precipitation of the corresponding oxide or oxides, after which the particles formed are dried and sintered. The invention particularly concerns the production of such materials in which the drops of the starting solution, before falling into the ammonia solution, first pass through a space free of ammonia gas of such magnitude that the drops attain their spherical form before they pass out of that space, and then pass through a second space through which ammonia gas flows, for stabilizing the spherical shape of the drops. The ammonia gas in such cases is introduced through one or more injection tubes and the space containing ammonia gas through which the drops pass before reaching the ammonia solution is designed to provide for sufficient hardening of the spherical drops to prevent their deformation in subsequent treatement. The invention also concerns an apparatus for carrying out the process in question. A process and apparatus for such a purpose is already known from German published patent application AS No. 24 59 445. Such nuclear fuel or breeder particles are used principally for production of fuel or breeder elements for high temperature reactors. For such purposes, it is important that the particles should be produced in as uniform size as possible and that they should have a good spherical shape. In the present state of the art, it is known to produce such nuclear fuel or breeder particles by first providing a nitrate solution and then subdividing it into drops and solidifying the drops by passing them first through a gaseous ammonia phase and, finally, introducing them into a liquid ammonia phase (solution). It occurs often that a part of this solidification process is frustrated by the addition of ammonia to the nuclear fuel or nuclear breeder solution before the separation into drops of the solution. In order to subdivide the solution of nuclear fuel or breeder material into drops and carry out the solidification, a process has been devised known from the article "SNAM Process for the Preparation of Ceramic Nuclear Fuel Microspheres" by G. Brambilla, P. Gerontopulos, and D. Neri in laboratory studies published in "energia nucleare" in April 1970, Issue 4, Vol. 17., and, likewise from the above-named German published patent application (AS No. 24 59 445). In this process the starting solution goes vertically through a gaseous ammonia phase (the second gas-filled space through which the particles pass) and a liquid (aqueous) ammonia phase both contained in a solidifcation column at the top of which nozzles are provided by which the stream flowing out of them is divided into separate drops by vibration. In order to provide that in these drops a shell of sufficient solidity is formed so that they can be subjected to the impact on the liquid ammonia phase without permanent deformation and, of course, without shattering, the drops of fuel or breeder material solution are first allowed to pass through a gaseous ammonia phase. It has been found in this case that the spacing between the drops is so much reduced with increasing frequency of drop formation (greater than 400 Hz) that eventually insufficient ammonia gas reaches the mutually facing sides of the individual drops of such a succession of drops. There is present a NH.sub.3 concentration decrease in a radial direction, so that the solidification and thereby the prehardening of the drops is produced nonuniformly in the ammonia gas phase. In consequence, upon impact of the drops on the aqueous ammonia solution, nonuniform distortion of the drops is produced. The process known from the above-mentioned "energia nucleare" article also discloses the introduction of the ammonia gas by a laterally disposed gas supply tube. It is also known from the above-mentioned German published patent application to utilize an ammonia gas stream directed on the chain of drops with a component opposing the direction of the movement of the drops while feeding the gas from the side. This effect (i.e., flow of gas with upward component) is produced with a nozzle arranged parallel to the direction in which the drops fall, by reversing the gas flow by deflection on the surface of the ammonia solution. In spite of the utilization of these arrangements, it has, however, not been possible to prevent the occurrence of nonuniformities in the producition of spherical particles. THE PRESENT INVENTION It is an object of this invention to provide a method and apparatus for the production of spherical particles of nuclear fuel and breeder materials of uniform size, and in particular in a process in which nonuniformities of the particles can be prevented. Briefly, the ammonia gas in the second part of the gas phase through which the drops pass is directed obliquely to the direction of movement of the drops and is introduced with a component of motion in the direction of the movement of the drops. In this manner, the result is obtained that as the drops, during their passage through the space containing the ammonia gas, are uniformly enveloped in the flow of ammonia gas and are, therefore, also uniformly solidified. Thus, in the desired flowing of ammonia gas past the drops, entrainment of air between the drops as they penetrate into the space containing the ammonia gas is prevented and the drops do not fall in a zone within the path of fall which is impoverished in its ammonia gas content. When a good flushing of the drops with ammonia gas is provided, the quantity of ammonia gas to be supplied in the path of fall can be better fitted to the requirements and, thereby, a saving in ammonia gas may be obtained. In consequence, the amount of waste resulting from the process is reduced. It is particularly effective for the direction of flow of the ammonia gas to form an angle in the range from 30.degree. to 60.degree. with the direction of movement of the drops at the place where the gas impinges on the drops and for the speed of flow of the gas to be 10 to 20 times as great as the average velocity of the drops. A useful modification of the process of the invention, for the case in which the ammonia gas is directed at the drops in more than one stream, is for the places of impingement of these streams to be spaced from each other. The apparatus of the invention, accordingly comprises a first container for holding the aqueous solution of a ammonia and for confining above it a space in which ammonia gas flows, a second container for the nitrate solution provided with a nozzle for dispensing the solution in the forming of a sequence of drops and a supply tube system for supplying ammonia gas to the space above the ammonia solution with at least one nozzle for the ammonia gas so disposed with reference to the nozzle that dispenses the liquid to be converted into drops and, ultimately, into particle spheres, that the ammonia gas is directed at the drops in a stream that is oblique to the direction of motion of the drops and has a component of motion in the direction of the drops. Again, it is advantageous for the nozzle for introduction of ammonia gas to be so disposed that the ammonia gas impinges on the stream of drops so as to form an angle in the range from 30.degree. to 60.degree. with the drop stream. It is useful to provide more than one nozzle for introduction of ammonia gas so disposed that the places of impingement of the respective ammonia gas streams are spaced from each other. A spacing of a few millimeters is preferred. As a further development of the invention, it is useful for the nozzles for the production of ammonia gas to be in the form of flat nozzles, which is to say that the stream is in the form of a blade or fan rather than in the form of a needle or a pencil, in which case the long dimension of the opening cross-section of the nozzle is disposed perpendicular to the plane in which the cooperating nozzles for the liquid and for the ammonia gas lie (i.e., the plane in which the axes of the gas nozzle under consideration and of the solution nozzle with which it cooperates lie).