NL8900695A - METHOD FOR PREPARING POWDER-RESISTANT INORGANIC COMPOUNDS AND METAL COMPOSITIONS - Google Patents

Description

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N.0. 35717 J

1_4 Process for preparing powdery refractory inorganic compounds and metal compositions.

Applicants name as inventors: 1. Alexandr Grigorievich MERZHANOV, 2. Inna Petrovna BOROVINSKAYA, 3. Sos Sarkisovich MAMIAN, 4. Yitaly Mikhailovich MASLOV and 5. Vladimir Ivanovich VERSHINNIKOV.

The invention is in the field of inorganic chemistry and more particularly relates to a process for preparing powdery refractory inorganic compounds and metal compositions.

The invention is useful in powder metallurgy for the preparation of hard alloys, refractories and materials resistant to aggressive environments and in the preparation of composite ceramic materials.

Known is a method for the preparation of powdered inorganic substances such as carbides, borides, silicides and nitrides of metals of groups IV, V and VI of the Periodic System (GB-B-1,497,025).

According to this method, at least one oxide of metals of groups IV, V and VI of the Periodic System is mixed with a metal reducing agent - aluminum, magnesium or calcium - and with nitrogen, carbon, boron or silicon. The preparation is carried out by reaction of the above-mentioned constituents under direct combustion conditions which, due to the exothermic interaction of the constituents, continue spontaneously through the reaction volume under a gaseous medium pressure of from 1 to 5000 bar. In this case, the reaction temperature reaches 4000-5000 ° C, as a result of which the product is in the form of a casting.

For the production of hard alloys based on refractory inorganic compounds, nickel, cobalt, molybdenum or oxides thereof are added in amounts of 5 to 20 wt. 2 in the above mixture. In order to improve the mechanical properties (heat resistance, wear resistance, hardness) of the hard alloys, alloying aids such as manganese are also added in an amount of 1 to 5% by weight. To avoid effervescence of the volatile constituents of the mixture and dissociation of the desired product, the 8900695. * * 2 cleaning takes place in a gaseous medium under a pressure in the range from 1000 to 5000 atmospheres.

In the preparation of the desired product, a slag is also formed - the oxide of the reducing metal - which is in the liquid state at the preparation temperature and which is layered due to its different densities. With this method, refractory compounds can be prepared in the form of compact monolithic articles. The preparation of powders from compact objects involves problems such as grinding, sieving and the like and does not lead to homogeneous powders.

A process is also known for the preparation of refractories - nitrides of metals of groups III and IV of the Periodic System - (US-A-4,459,363) according to which sodium azide is mixed with metallic calcium or magnesium and an oxide of rare earth metals, groups III or IV metals or mixtures thereof in a stoichiometric amount.

The final mixture is heated to sieve combustion temperature, allowing the mixture to burn spontaneously to form a refractory nitride composite.

Because one of the components of the mixture is an azide, it is not possible with this method to obtain powdered compounds of refractory metals other than nitrides. Even in the case of the preparation of nitrides of elements of groups III-IV, however, this production also does not allow large-scale production due to its flammable and explosive character, since the preparation involves the formation of gaseous sodium in an amount of 7.5 l per mole of metal nitride. Further, in the preparation of non-metal nitrides such as silicon nitride at the high temperatures of the self-sustaining synthesis and at relatively low nitrogen pressures, the conversion may not be complete due to dissociation of silicon nitride.

It is also known a process for the preparation of refractory carbides, borides, silicides, sulfides and nitrides of metals of groups IV-VI of the Periodic System (US-A-3,726,643). According to this method, the starting components, powders of metals of groups IV-VI and non-metals such as C, B, Si, S and N are mixed. The mixture thus prepared is mixed with a heat source - a tungsten or nichrom wire - by means of of a firing mixture, after which a self-sustaining synthesis at high temperature takes place in an inert gas medium 40. The resulting product is formed by a clumping of sintered large grains with a non-uniform size distribution which hinders further use, since further grinding and sieving is required.

Moreover, it is not possible with this method to prepare refractory compounds of elements of groups I, II, III and VIII, since elements of these groups interact with B, Si, C and N at low temperature, whereby the self sustained high temperature synthesis does not proceed or is incomplete.

The currently known processes for the preparation of refractory inorganic compounds and metal compositions are therefore not suitable for the preparation of fine powders with a uniform chemical composition and phase distribution. Currently, such powders are obtained from powders of a larger particle size or from sintered refractories by grinding in ball mills. The grinding process is quite time consuming and, because many refractories have an abrasive action, the resulting powders become contaminated with the materials of the ball mills after grinding. Since the starting materials are very variable in particle size, the powder obtained after grinding is also very little uniform. The particle size after grinding the compounds obtained in the manner described above ranges from micron fractions to 5-10 µm. This hinders the physical, mechanical and economic characteristics of the articles prepared from the thus disintegrated powders.

The object of the invention is to provide, by modifying the starting components of the preparation, a process for the preparation of finely divided powdery refractory inorganic compounds and metal compositions of elements of groups I-VIII of the Periodic Table with a uniform particle size distribution and phase composition during the preparation of these compounds and compositions.

This object is achieved with a method of preparing powdery refractory inorganic compounds and metal compositions comprising a charge containing an element of the Periodic System and another element selected from nitrogen, carbon, boron, silicon, sulfur and phosphorus, into a reaction zone, in which a self-sustaining synthesis of the desired product is carried out at high temperature, and then separating the desired product from the reaction zone, characterized in that use is made of a batch which also contains recorded: 8900695.

* 4 - at least one element of groups I-III and VII-VIII, - and / or at least one hydride of elements of groups I-III, - and / or at least one oxide, and / or a halide of elements of groups I-VIII, 5 - at least one oxide and / or at least one halide and / or at least one organic compound of nitrogen and / or carbon and / or boron and / or silicon and / or sulfur and / or phosphorus, - and halides of alkali metals and / or ammonium halides and / or polystyrene and / or polyethylene and / or urea, and the desired product is separated off by treatment of the synthesis product with a solution of a mineral acid.

The invention has made it possible to obtain fine powders (with a particle size of 0.1 to 10.0 µm) with an even phase composition and particle size distribution. Furthermore, it has become possible to obtain powdery refractory inorganic compounds and metal compositions of elements of groups I-VIII of the Periodic System and not only of groups IV-VI.

Thus, in the process of the invention, the following are reacted: a) at least one element from groups I-VIII and / or oxides or halides thereof; b) at least one element from groups I-III and / or hydrides thereof; c) N, C, B, Si, P and / or S and / or oxides, halides or organic compounds thereof; and d) one or more alkali metal halides, ammonium halide, polystyrene, polyethylene and / or urea, and / or e) an oxide of at least one Group II metal.

According to the invention, it is preferable to use a charge consisting of a mixture of from 12.00 to 80.95% by weight of at least one element of groups I-VIII and / or at least one oxide and / or at least a halide of elements of groups I-VIII; 0.05-31.50% by weight of nitrogen and / or carbon and / or boron and / or silicon and / or sulfur and / or phosphorus and / or oxides, halides and / or organic compounds of one or more of the above elements ; 19.0-56.5 wt.% Of at least one Group I-III metal and / or at least one hydride of these metals, and additives in an amount of 1 to 25 wt.% Of the mixture, the additives consist of Group II metal oxides and / or halides of alkali metals and / or ammonium halides and / or polystyrene, polyethylene and / or urea.

In order to obtain the desired product with a small and 40 uniform particle size, it is preferred that the batch as 89 00695 · 5 additives contain 5 to 25% by weight of the above mixture of Group II and / or 1-5 metal oxides. % by weight of the mixture of alkali metal halides and / or ammonium halide and / or polystyrene and / or polyethylene and / or urea.

For example, to obtain a refractory inorganic compound with uniform particles of 2-5 µm size, use is made of a batch consisting of a mixture of 56.0 wt% titanium dioxide, 8.3 wt% carbon, 35.7 magnesium by weight and additionally as additives: 10.0% by weight of the mixture of magnesium oxide and 3.0% by weight of the mixture of polystyrene; the desired product is separated by treating the reaction mixture with a hydrochloric acid solution.

For example, to obtain a metal composition of titanium and nickel with a particle size of 2.0 to 5.0 .mu.m, use is made of a batch consisting of a mixture of 26.50 wt.% Titanium dioxide, 25.50 wt. % nickel oxide, 26.50 wt% calcium, 21.45 wt% zinc, 0.05 wt% carbon and additionally as an additive: 24.0 wt% of the mixture of calcium oxide; the desired product is separated by treatment of the reaction mixture with a sulfuric acid solution.

Other applications and advantages of the invention will be apparent from the detailed description of the method according to the invention and the examples below.

As starting materials for the preparation of powdery refractory inorganic compounds and metal compositions according to the invention, the following ingredients are used: a) Elements of groups I-VIII of the Periodic System, individually or in combination, oxides thereof, halides thereof. Preferably these elements are metals or semimetals, in particular from groups IIIA-VIIIA, such as Ti, Cr, Mn, Fe, Co, Ni, Zr, Nb, Mo, La, Ta, 30, but also, for example, Li, Ca, B , Al, Si and Cu. Examples are: a powder of elemental titanium with a powder of elemental tungsten; a powder of elemental tungsten with tungsten oxide and tungsten chloride; a powder of elemental titanium with a powder of elemental tungsten and tungsten chloride; or titanium oxide with tungsten oxide. The ratio of the components in these combinations depends on the requirements (in terms of chemical composition and phase composition) imposed on the desired product.

b) Elements of groups I-III, individually or in combination, and the hydrides thereof, for example a powder of metallic magnesium; 40 a mixture of a powder of metallic calcium with calcium hydride in 8900695 «6 any conceivable ratio; a mixture of metal powders of lithium, calcium and aluminum in any ratio; a mixture of metal powders of lithium, aluminum and magnesium hydride in any ratio depending on the desired product.

C) Nitrogen, carbon, boron, silicon, sulfur, phosphorus, individually or in combination, oxides thereof, halides thereof and organic compounds thereof. For example nitrogen; nitrogen and carbon; carbon and boron; carbon and boron oxide; boron chloride and polyethylene; silicon with silicon oxide and silicon chloride. The ratio between the 10 components of these combinations depends on the requirements of the desired product.

The starting mixture for the preparation of the desired product is obtained by mixing the above three components. According to the invention, 12.0-80.95 wt% of component a), 19.0-56.5 wt% of component b) and 0.05-31.5 wt% of component c) are used .

When component a) is present in the batch in an amount of less than 12.0% by weight, there is no optimum ratio of reaction components, resulting in an increased combustion temperature (synthesis) and a non-uniform phase composition of the desired product and its particle size.

When component a) is present in the charge in an amount of more than 80.95% by weight, an excess of this component is created which enters the combustion process as ballast and hinders the progress of the combustion front throughout the reaction space. and results in a disrupted phase and particle size distribution of the desired product.

When component b) is present in an amount of less than 19.0% by weight, an unreacted excess of component a) is formed in the reaction products, resulting in uniformity of the particle size and of the phase of the desired product. be disturbed.

When component b) is present in excess of 56.5% by weight during the synthesis, extensive evaporation of the excess of this component takes place, which also has a detrimental effect on the uniformity of the particle size and the phase of the desired product.

The content of component c) in the mixture is determined by the contents of components a) and b).

According to the invention, in the mixture of the components 8900 635.

7 a), b) and c) additives are added: 5-25 wt.% Of the mixture obtained to e) oxides of metals of group II and / or 1-5 wt.% Of the obtained mixture to d) halides of alkali metals and / or ammonium halide and / or polystyrene and / or polyethylene and / or urea.

By incorporating a mixture of additives in the form of oxides of Group II metals, it is possible to lower the synthesis temperature, because these oxides do not decompose or contaminate the final product and crystallization of the desired product takes place under "mild" conditions, whereby a uniform fine powder is obtained. In order to obtain a uniform particle size and structure, the oxides are selected from the group of oxides of alkaline earth metals where they may be identical with oxides of the elements of component b). This also makes it easier to purify the end product from these oxides. When these oxides are used in an amount of less than 5% by weight, no significant temperature reduction which may be necessary for the required crystallization conditions during the synthesis is obtained. The use of the oxides of component e) in an amount of more than 25% by weight causes the combustion temperature to drop too much, thereby decreasing the uniformity of the powdery product obtained.

When component d) of alkali metal halides and / or ammonium halide and / or polystyrene and / or polyethylene and / or urea is added to the above mixture of components a), b) and c), a decrease in the synthesis temperature occurs as a result of the decomposition of this substance; this gives a similar result to the inclusion in the above-mentioned Group II (e) metal oxide mixture. The amount of additional added alkali metal halides, ammonium halide, polystyrene, polyethylene and / or urea depends on the amount of the added oxides of Group II metals.

The formation of a large amount of gaseous products in the decomposition of the above-mentioned substances leads to a gas-stabilized disintegration of the end product directly in the front of combustion. In addition, the decomposing additive contains the elements necessary for complete conversion of the final product; these are carbon in the polymer composition to obtain carbides, and nitrogen in urea for nitrides. The addition of alkali metal halides or ammonium halide makes it possible to lower the synthesis temperature without contaminating the final product because the gaseous products formed are volatile. The use of the decomposing additive d) in an amount of less than 1% by weight is 89 00695.

8 in the absence of additive e) insufficient because then the required amount of gases is not formed. The use of the decomposing additive in an amount of more than 5% by weight results in a reduced synthesis temperature and in a non-uniform end product.

The batch prepared in the manner described above is placed in a reactor in which the self-sustaining synthesis takes place at high temperature. A conventional reactor can be used for this.

For example, by using a tungsten winding connected to a power source with a voltage of 50-60 V and a current strength of 5-20 A, ignition of the top layer of the charge is initiated. Subsequently, the preparation of the desired product proceeds under conditions of self-sustaining synthesis at high temperature.

The product obtained contains impurities from combustion by-products (compounds of component b)). To purify the desired product from these impurities, the product is treated with a solution of an inorganic acid, for example hydrochloric or sulfuric acid. After treatment with the acid, the product is dried, for example at a temperature of 100 to 150 ° C for 4 to 5 hours.

The product thus obtained is a powdery substance with a uniform composition in phase and particle size; the particle size ranges from 0.1 to 10.0 µm. The product obtained is clearly distinguishable in terms of morphology from similar products obtained by other methods.

The control of the product obtained can be carried out by chemical analysis, X-ray analysis and diffraction analysis.

With the method of the invention, it is possible to obtain a powdered product having the above properties from starting materials that are more readily available and less expensive such as oxides and halides instead of the expensive and poorly available metal powders used hitherto.

Furthermore, it is possible with the method according to the invention to obtain compounds of groups I-VIII of the Periodic System, for example boron caride, tungsten carbide, which because of the low exothermic content. the interaction between the elemental metal compounds and non-metal compounds as starting materials previously could not be obtained under conditions of self-sustaining synthesis at high temperature.

8900635.

«9

Example I

56 parts of titanium dioxide powder, 35.7 parts of magnesium powder and 8.3 parts of carbon carbon black are stirred in a stainless steel drum for 5 hours. Then 10 parts by weight of magnesium oxide powder and 3 5 parts by weight of polystyrene powder are added and stirred. The mixed powders are then placed in a reactor and tamped. The reactor is closed, rinsed two to three times with an inert gas, filled with argon and closed. The contents are then locally lit using a tungsten winding which is connected to a power source with a voltage of 50-60 V and a current of 5-20 A. The temperature at the combustion of the charge reaches 2300 ° C.

After complete combustion of the batch, the reactor with contents is cooled to 18 ° C. The product is taken out of the reactor and treated with a solution of hydrochloric acid. The separated powder is titanium carbide-15 (TiC) with uniform particles of dark gray color and sizes from 2 to 5 µm. The product is in a phase with a cubic lattice of the NaCl type.

The resulting titanium carbide can be used as a starting powder for the preparation of hard alloy materials and scouring pastes without any preparatory operation (such as grinding or sieving).

According to the procedure of Example I, 145 more experiments were carried out with different physico-chemical conditions of the synthesis, i.e. other temperatures, pressures, compositions, etc. The results are shown in the table below.

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Claims (8)

1. A process for the preparation of powdery refractory inorganic compounds and metal compositions in which at least one element of the Periodic System and another element selected from nitrogen, carbon, boron, silicon, sulfur and phosphorus or compounds thereof are formed into a self in maintaining a high temperature reaction and separating the desired product from the reaction mixture, characterized in that it is reacted: a) at least one element of groups I-VIII of the Periodic Table and / or oxides or halides thereof , b) at least one element of groups I-III of the Periodic System and / or hydrides thereof, c) nitrogen, carbon, boron, silicon, sulfur and / or phosphorus and / or oxides, halides or organic compounds of these elements ; and d) one or more alkali metal halides, ammonium halide, polystyrene, polyethylene and / or urea, and / or e) an oxide of at least one Group II metal of the Periodic System, and isolates the desired product by treating the reaction mixture -20 sel with a solution of an inorganic acid. Process according to claim 1, characterized in that both component d) and component e) are used. 3. Process according to claim 1 or 2, characterized in that from component a) 12.0-80.95 wt.% With respect to the total of a), b) and c) is used, of component b) 19.0-56.5 wt% relative to the total of a), b) and c) of component c) 0.05-31.5 wt% relative to the total of a), b ) and c), and 30 of components d) and / or e) are used together from 1 to 25% by weight, based on the total of a), b) and c). 4. Process according to claim 2 or 3, characterized in that from component d) 1-5 wt.% Of the total of a), b) and e) is used, and from component e) 5-25 wt. % relative to the total of a), b) and c) used. Process according to any one of claims 1 to 4, characterized in that an oxide or a halide is used for at least one element of component a) or c). 6. Process according to any one of claims 1-5, characterized in that the components a), b) and c) are used in approximately stoichiometric amounts. Process according to claim 6, characterized in that about 56.0 wt% titanium dioxide, about 8.3 wt% carbon, about 5 35.7 wt% magnesium and in addition 5-25 wt% magnesium oxide and 2-4% by weight of polystyrene and separating the desired product by treatment with a solution of hydrochloric acid. 8. Process according to claim 6, characterized in that about 26.5% by weight of titanium dioxide, about 25.5% by weight of nickel oxide, about 26.5% by weight of calcium, about 21.45% by weight zinc, about 0.05 wt% carbon and additionally about 24.0% calcium oxide are used and the desired product is separated off by treating the reaction mixture with a solution of sulfuric acid. +++++++ 8900695.