Patent Number: 045227691
Section: summary

FIELD OF THE INVENTION This invention relates generally to the ceramic art and the formation of sintered bodies from particulate oxide materials. It is particularly concerned with a process for producing consolidated units of particulate ceramic materials including the compressing of such particles into coherent and handleable compacts for subsequent sintering to integrated bodies. The invention is specifically directed to the manufacture of nuclear fuel products from particulate materials containing uranium dioxide. CROSS-REFERENCE This invention is related to that disclosed and claimed in U.S. patent application Ser. No. 331,492 filed Dec. 17, 1981, in the names of George L. Gaines, Jr., Patricia A. Piacente, William J. Ward III, Peter C. Smith, Timothy J. Gallivan, and Harry M. Laska; and to Ser. No. 273,900 filed June 15, 1981, in the names of George L. Gaines, Jr. and William J. Ward III, now U.S. Pat. No. 4,389,341 . Both of said applications are assigned to the same assignee as this application, and are incorporated herein by reference. BACKGROUND OF THE INVENTION Fissionable nuclear fuel for nuclear reactors comprises a variety of compositions and forms of fissionable materials, including ceramic compounds of uranium, plutonium and thorium. Fuel compounds for commercial power generating reactors typically comprise oxides of uranium, plutonium and thorium, and mixtures thereof. The generally most suitable and commonly used fuel for such commercial nuclear reactors is uranium dioxide, which can be combined with minor amounts of other fuel materials including neutron flux controlling additives such as gadolinium. Commercially produced uranium dioxide is a fine, fairly porous powder, a form which is not suitable as such for use as fuel in commercial reactors. A number of means have been developed and used to convert powdered uranium dioxide into a form suitable for use as a fuel for in power generating nuclear reactors. One commonly used technique has been to sinter appropriately sized bodies of the powdered uranium dioxide material at high termperatures to develop strong diffusion bonds between the individual powder particles. However, the sintering technique requires a preliminary forming of the loose powder into a shaped, and self-retaining, body of particles of sufficient strength and integrity to survive handling and the sintering procedure. The operation of consolidating fine particles into a body or coherent compact with acceptable low levels of rejects, and the strength and uniformity for enduring subsequent handling and firing has been a subject of considerable concern and investigation in the nuclear fuel industry. Conventional organic or plastic binders commonly used in powder fabrication have been considered to be unsuitable in nuclear fuel processing operations. Entrainment of any binder residues such as carbon within the sintered nuclear fuel product is unacceptable in reactor service. Moreover, the presence of any organic binder among the particles inhibits the formation during sintering of strong diffusion bonds between the particles, and adversely affects the density of the sintered product. The complete removal of binders, or their decomposition products, prior to sintering is especially difficult, and usually requires a costly additional operation in the fuel manufacture. Accordingly, a common method has been to die press uranium dioxide powder into appropriately sized "green" (unfired) compacts without the assistance of any binder. This approach however has resulted in very costly high rates of rejects and scrap material recycling because of the weakness of green, binder-free compacts of powder. U.S. Pat. No. 4,061,700, issued Dec. 6, 1977, to Gallivan, and assigned to the same assignee as this application, discloses a distinctive group of fugitive binders that improved the production of sintered pellets of particulate nuclear fuel materials for nuclear reactors. The fugitive binders of this patent function without contaminating the resulting fuel products, and they permit the formation of strong bonds between sintered particles during firing without deleteriously affecting the desired porosity of the sintered pellet. The disclosure of the said U.S. Pat. No. 4,061,700 and of U.S. Pat. Nos. 3,803,273; 3,923,933; and 3,927,154, also assigned to the same assignee as the instant application, and relating to significant aspects in the subject field of producing nuclear fuel pellets from particulate fissionable ceramic material for reactor service, are all incorporated hereby by reference. The prior art techniques or means such as disclosed in U.S. Pat. No. 4,061,700, have been found wanting in some conditions and circumstances. For instance it has been observed that the fugitive binders of the aforesaid patent do not provide consistent results as to pellet strength and integrity irrespective of the blending conditions and particle characteristics of the uranium dioxide powder. Specifically the severity of agitation in blending, relative humidity and temperature, and duration of storage, as well as the uranium oxide powder properties such as size, surface area and moisture content are all factors that apparently can detract from the uniformity of the physical attributes provided by such fugitive binders. The amine-type of fugitive binder of the aforesaid applications Ser. Nos. 331,492 and 273,900 have been found to provide significant improvements in the processing characteristic of particulate ceramic materials comprising uranium dioxide and in the physical properties of compacts formed therefrom. Nevertheless, the foregoing prior art measures have not sufficiently overcome the inherent brittle nature of some ceramic materials comprising uranium dioxide powder and imparted therein a degree of plasticity to enable their consistent and rapid consolidation to coherent compacts having high resistance to fracture. This invention deals with the typical brittle nature of ceramic materials and problems imposed thereby when compression molding such in materials in particulate form and also occurring in the resulting molded product. As is well known, ceramic materials are generally of a relatively brittle consistency as opposed to a plastic conformable consistency. Thus, rather than gradually deforming over a period of progressively increasing applied compressive stress approaching the breaking point as is the case with a plastic material, ceramics tend to rigidly resist substantially all deformation until the breaking point is reached whereupon they abruptly fracture with the resulting fissure or fissures instantly progressing through the mass fragmenting it. An apt illustration of this brittle and unyielding property and the facture characteristics of a ceramic is the crushing of a glass marble. On the other hand, a plastic material will gradually yield and deform with progressively increasing compressive stress until reaching its breaking point and rupturing, and commonly the propagation of the resulting fracture is of a slower rate and does not continue to the extent of fragmenting the mass. Thus, a plastic type of material is more amenable to compression molding than the brittle type of materials. This inherent brittle characteristic in uranium dioxide powder, or its lack of plasticity, constitutes a significant shortcoming in compression molding operations and in the properties of the molded products. SUMMARY OF THE INVENTION This invention comprises a method of producing coherent compacts from particulate ceramic material wherein the ceramic material is rendered more plastic, or less brittle, while undergoing compression molding by providing a novel binder system including a multifunctional primary amine with carbon dioxide gas. Thus the invention entails a process comprising a combination of operations acting upon the specified ingredients, including the essential provision of carbon dioxide gas for the amine compound contained in the particulate ceramic nuclear fuel material. OBJECTS OF THE INVENTION It is a primary object of this invention to provide an improved method for rendering particulate ceramic material more amenable to compression molding. It is another object of this invention to provide means for overcoming the brittle nature of ceramic particles and to impart plasticity to such a material whereby it can be compression molded under essentially all compacting conditions and at high rates with a lower level of rejects. A further object of this invention is to provide a method for improving the compression molding of particulate ceramic materials comprising uranium dioxide powder into coherent compacts and increasing the resistance of such compacts of ceramic materials to fracture and fissure propagation during compression molding and thereafter, including the sintered products of the molded material. A still further object of this invention is to provide a method of producing nuclear fuel pellets comprising uranium dioxide from particulate ceramic material wherein the particulate ceramic is compression molded to a coherent compact at fast rates with minimal rejects due to fractures in either the unfired coherent compact or in its sintered product.