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United States Patent [19] [11] Patent Number: 4,492,764 Watanabe Et Al

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United States Patent [19] [11] Patent Number: 4,492,764 Watanabe Et Al United States Patent [19] [11] Patent Number: 4,492,764 Watanabe et al. [45] Date of Patent: Jan. 8, 1985 [54] SINTERED CERAMIC BODY CONTAINING 4.022.584 5/1977 Rudy ................. .. Sol/98 4.145.213 3/1979 Oskarsson et al 75/238 TITANIUM CARBONITRIDE 4.268.582 5/1981 Hale el al. ........................... .. 75/238 [75] Inventors: Tadahiko Watanabe, Saga; Yuko Primary Exam1'ner——Mark Bell Tsuya, Tokyo; Yuji Enomoto. Attorney. Agenl. 0r Firm-—Brisebois & Kruger Sakura, all of Japan [57] ABSTRACT [73] Assignee: Agency of Industrial Science and Technology, Tokyo. Japan A refractory ceramic body having excellent bending strength and high hardness and with little porosity is [21] Appl. No.: 475,976 ‘ obtained by sintering a powdery mixture comprising 5 [22] Filed: Mar. 16, 1983 to 95% by weight of a titanium carbonitride and 95 to [30] Foreign Application Priority Data 5% by weight ofa metal boride such as metal diborides, e.g. titanium diboride, W3B5 and M0385 at a tempera Jul. 12, 1982 [JP] Japan .............................. .. 57-121748 ture of 1700m to 1800° C. Further improvements can be [51] Int. Cl.3 ..................... .. C04B 35/56; C048 35/58 obtained by partial replacement of the above mentioned [52] US. Cl. .................................... .. 501/87; 501/96 components with elementary boron, titanium carbide or [58] Field of Search .................... .. 501/87. 96; 75/238. titanium nitride or when the titanium carbonitride com ‘ 75/244 ponent is a combination of at least two kinds oftitanium carbonitrides having different chemical compositions [56] References Cited relative to the proportion of the carbon and nitrogen. U.S. PATENT DOCUMENTS 3.741.733 6/1973 Kieffer ................................ .. 75/238 16 Claims, N0 Drawings 4,492,764 1 2 titanium carbide TiC, titanium nitride TiN or elemen SINTERED CERAMIC BODY CONTAINING tary boron. When elementary boron is added to the TITANIUM CARBONITRIDE powdery mixture, the amount thereof should not ex ceed 10% by weight. 7 BACKGROUND OF THE INVENTION 5 The admixture of the titanium carbide or nitride to The present invention relates to a novel sintered ce the binary mixture of the titanium carbonitride and the ramic body based on or containing a titanium carboni metal boride has an effect to impart a further improved tride or. more particularly, to a sintered ceramic body Hp hardness of, for example, 2500 kg/mm2 or higher at containing a titanium carbonitride and a metal boride room temperature to the sintered body in comparison and having excellent bending strength and hardness as with the sintered bodies prepared from binary mixtures well as outstandingly high density. of the components (a) and (b) alone. Similar improve Titanium carbonitrides are promising as a material for ment in the hardness of the sintered body is also ob various sintered ceramic bodies usable as a cutting tool, tained when the component (a) is a mixture composed parts of heavy-duty machines and the like since the of at least two kinds of titanium carbonitrides having sintered ceramic body based on or containing titanium different chemical compositions relative to the propor carbonitride is excellent in the high melting point, hard tions of carbon and nitrogen. ' ness and tenacity as well as the remarkable resistance against oxidation when used in a high temperature oxi DETAILED DESCRIPTION OF THE dizing atmosphere. PREFERRED EMBODIMENTS Notwithstanding the above mentioned advantages, 20 The first of the essential components, i.e. component titanium carbonitride-containing sintered ceramic bod (a), in the powdery mixture to be sintered is a titanium ies are currently not used in the industry at least as a carbonitride which is a chemical entity expressed by the refractory material because a sintered ceramic body formula Ti(CaN,3), in which the ratio of (1:8 should be prepared from a titanium carbonitride alone is relatively in the range from 10:90 to 90:10 or each of the values of brittle and has an unsatisfactorily low bending strength 25 a and ,B should be in the range from 0.1 to 0.9, n+3 while this problem of brittleness and poor bending being approximately equal to l. The titanium carboni strength cannot be overcome even by the attempts to tride should be in a powdery form having an average admix one or more of additive ingredients to the com particle diameter as ?ne as possible or, desirably, not position to be subjected to sintering due to the counter exceeding 2 pm. Such a product of titanium carboni acting adverse effects on the advantageous properties tride is commercially available. inherent to the titanium carbonitride. For example, The second of the essential components, i.e. compo titanium carbonitrides are useful as a matrix material of nent (b), is a metal boride selected from the group con cermets as sintered with metallic nickel as a binder but sisting of the MB; type metal diborides including tita such a titanium carbonitride-based cermet is defective 35 nium diboride TiBz, chromium diboride CrB2, tantalum due to the decreased resistance against oxidation and diboride TaBg, manganese diboride MnBZ, molybde poor heat resistance as a result of admixture of the me num diboride MOB2, vanadium diboride VBZ, niobium tallic nickel. Therefore, it has long been desired in the technology diboride NbBZ, hafnium diboride HfBz, aluminum dibo of ceramics to develop a sintered ceramic body based ride AIBZ and zirconium diboride ZI‘B2, of which tita on or containing titanium carbonitride and having high nium diboride TiBz is preferred, and M2B5 type metal bending strength and hardness without suffering de borides including tungsten boride W1B5 and molybde crease in the resistance against oxidation and heat resis num boride M0285. The metal boride should also be in a powdery form having an average particle diameter as tance. ?ne as possible, preferably, not exceeding 2 pm or, SUMMARY OF THE INVENTION 45 more preferably, not exceeding 0.5 um. The above An object of the present invention is to provide a named metal borides may be used either alone or as a novel and improved sintered ceramic body of high combination of two kinds or more. melting point having excellent bending strength and The powdery mixture to be subjected to sintering hardness as well as high density due to the absence of should comprise from 5 to 95% by weight of the com any porosity without suffering decrease in the resistance 50 ponent (a) and from 95 to 5% by weight of the compo against oxidation and heat resistance as prepared from a nent (b). Although typically the powdery mixture is powdery mixture comprising a titanium carbonitride as composed of the components (a) and (b) alone, i.e. the an essential ingredient. total amount of the components (a) and (b) is substan Thus, the sintered ceramic body of the invention tially equal to 100% except impurities, the essential developed as a result of the extensive investigations 55 requirement is that the total amount of the components undertaken by the inventors, in which a large number of (a) and (b) should be at least 50% by weight, the bal powdery ceramic materials have been tested as an addi ance, if any, being titanium carbide TiC, titanium nitride tive to a titanium carbonitride with the above described TiN or elementary boron. When the powdery mixture object, is a sintered body of a powdery mixture com is composed of the components (a) and (b) alone, the prising (a) from 5 to 95% by weight of a titanium car 60 amount of the component (b) should preferably be in bonitride and (b) from 95 to 5% by weight of at least the range from 20 to 70% by weight so that further one metal boride selected from the group consisting of improvements are obtained in the bending strength, MBZ type metal diboride, e.g. diborides of titanium, hardness and density of the sintered body prepared chromium, tantalum, manganese, molybdenum, vana from the powdery mixture. When the amount of the dium, niobium, hafnium, aluminum and zirconium and 65 component (b) in the powdery mixture is smaller than M3B5 type metal borides, e.g. W2B5 and Mo2B5, where 5% by weight or in excess of 95% by weight, no satis the total amount of the above described components is factory results can be obtained in respect of the bending at least 50% by weight with the balance, if any, being strength of the sintered body. 4,492,764 3 4 The powdery mixture composed of the components belonging to the IVb group of the Periodic Table, the (a) and (b), optionally, with addition of a third compo metal constituent of the boride may react with the IVb nent, which may be titanium carbide, titanium nitride or element to form a layer ofa compound of the metal and elementary boron as mentioned above, is thoroughly the IVb element having good lubricity on the surface of blended in a suitable blending machine to obtain inti the machine part. mate contact between particles of the components and a Following are the examples to illustrate the present mold ofa desired form made of, for example, graphite is invention in further detail. In the examples, the chemi ?lled with the powdery mixture which is subjected to cal composition of each of the titanium carbonitrides is sintering by heating in an atmosphere of vacuum or a given by the formula Ti(CaN;;) with substitution of neutral or reducing gas such as nitrogen, argon, hydro respective numerical values giving the molar propor gen and oxides of carbon under a die pressure of 50 to tion of the carbon and nitrogen for the suffixes Cl. and B, 300 kg/cm2 at a temperature in the range from l500° to such as TI(CO_5NQ,5).
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