Patent Number: 042785600
Section: description

DETAILED DESCRIPTION OF THE INVENTION In accordance with the invention, a uranyl nitrate solution which contains the desired gadolinium content in dissolved form is brought, together with NH.sub.3 and CO.sub.2, into precipitation apparatus which contains an aqueous body of ammonium carbonate solution with a pH-value of 9. This pH value is lowered to 8.2 during the precipitation process initiated thereby. Ammonium salts of gadolinium and uranium carbonate complexes are precipitated during the precipitation process and the precipitate, after separation from the body of solution, is converted in known manner into an oxide form that can be sintered. To illustrate the method further, reference is made to the attached drawing, which shows one form of precipitation apparatus. The precipitation vessel 1 contains a weak or dilute ammoniumcarbonate aqueous solution forming a water seal 11 with the solution having a pH of 9. A uranyl nitrate solution which contains the desired share of gadolinium in dissolved form is fed through the line 5 into, as shown in the drawing, the annulus of two vertical concentric tubes which extend down into the body of ammonium carbonate. At the same time, CO.sub.2 -gas is fed-in via the line 7 and NH.sub.3 -gas via the line 6 is fed into the annulus. Initially, the uranium and the gadolinium remain in solution. This initial solubility of the gadolinium is achieved by the alkaline ammonium carbonate seal. Thorough mixing of the fed-in materials with the ammonium carbonate solution of the water seal 11 is achieved by means of the pump 2 which withdraws a portion of the ammonium carbonate solution and recirculates it to the top of the apparatus through the mixing nozzles 4 disposed in the annulus and then down into the body of solution 11. In the precipitation process that sets in, the pH-value is allowed to fall slowly to 8.2. Thereby the gadolinium precipitates simultaneously with the uranium. Ammonium salts of uranium and gadolinium carbonate complexes are formed as precipitation products. After the precipitation process has ended, the suspension produced of precipitate in liquor is further circulated by means of the pump 2. The grain size of the precipitation products is equalized thereby. Subsequently, the pump 2 is switched off and the precipitated salts are transported via the pump 3 to a filtration device, not shown, for separation of the precipitate from the liquor. These mixed crystals, after being filtered and dried, optionally together with AUC (ammonium uranyl carbonate), converted in known manner into a oxide form that can be sintered. An appropriate method is described in detail, for example, in German Pat. No. 1 59 24 71. In another embodiment of the method shown in the drawing gaseous UF.sub.6 can be fed-in via the connecting line 7 in addition to the CO.sub.2 -gas and is then converted in the precipitation apparatus 1 into AUC. It should further be pointed out that a uranyl sulfate solution can also be used for bringing-in the gadolinium instead of a uranyl nitrate solution. The dependence of the precipitation of the gadolinium together with the uranium on the pH-value can be utilized so that the degree of gadolinium precipitation and thereby, the gadolinium content in the precipitated mixed crystals can be adjusted through control of the pH-drop from 9 to 8.2. In the extreme case, this provides the possibility of separating uranium and gadolinium if the pH is kept constant at 9. In that case, the gadolinium remains in the solution and only the uranium is precipitated. The limit for the solubility of gadolinium is then approximately 1%. Control or change of pH may be effected in the usual way by the addition of an acidic or basic substance. Ordinarily adequate control or change of pH may be accomplished simply by varying feed of CO.sub.2 and/or NH.sub.3. The method described is therefore optimally suited to precipitate uranium and gadolinium together in the form of mixed crystals and to feed them into the normal nuclear fuel production and processing, as well as for purifying uranium solutions of gadolinium.