JPS6144124B2 - - Google Patents

Description

DETAILED DESCRIPTION OF THE INVENTION The present invention relates to an apparatus for reducing a metal chloride to produce the metal and vacuum purifying the same.

Among metal materials, titanium and zirconium, which are high melting point and high toughness materials, can be made by reducing their chlorides with active metals such as magnesium.
Manufactured as a metal sponge. In the past, the reduction process and the process of vacuum separation and purification of the produced metal sponge (condensation of by-products) were carried out using separate equipment, but since 18717, a device that integrates both has been proposed. It has been implemented.

Since then, improvements to this integrated device have been disclosed in Japanese Patent Application Laid-Open No. 52-49922, etc., and the applicant has already filed Japanese Patent Application No. 57-8771 (Japanese Patent Application Laid-open No. 58-8771).
126936), patent application No. 1984-47227 (Japanese Patent Application No. 58-164736)
proposed an improvement plan.

All of the conventional reduction and condensation integrated devices
A condensation chamber is disposed directly above the reaction chamber (reduction chamber), and the improvements mentioned above mainly concern the structure of its intermediate connection (gas passage) and its blocking method. For example, the device disclosed in Japanese Patent Application No. 57-8771 uses a seal pot structure filled with an easily melted and evaporable substance to block the gas passage (intermediate connection) between the reaction chamber and the condensation chamber, thereby blocking, communicating, and separating the two chambers. This has the advantage that even when the reaction chamber is still at high temperature, the condensation chamber can be separated and the reaction chamber can be taken out alone from the heating furnace. Moreover, in this apparatus, the reaction chamber and the condensation chamber could be used as containers of the same shape.

However, in this device, the condensation chamber is a bell-shaped one with an open bottom, so the operation to take out the refined metal sponge is done by separating the reaction chamber from the condensation chamber and tilting or overturning it. .
Furthermore, if the condensation chamber and reaction chamber are to be used interchangeably, the condensation chamber must be turned over by 180 degrees when the condensation chamber is next used as a reaction chamber. However, as the reactor becomes larger, it becomes difficult to tilt or overturn it.

Regarding the arrangement of the reaction chamber and condensation chamber, containers of exactly the same shape are used as the reaction chamber and condensation chamber; the condensation chamber is placed directly above the upright reaction chamber; Place the condensation chamber directly below the reaction chamber; Place the condensation chamber upside down directly above the upright reaction chamber; Place the condensation chamber on its side and place it below the side of the reaction chamber so that the bottom of the reaction chamber and the top of the condensation chamber are placed on its side. Either connect the condensation chamber with a connecting part bent at 90 degrees; lay the condensation chamber sideways and place it above the side of the reaction chamber, and connect the top of the reaction chamber and the top of the condensation chamber with a joint bent at 90 degrees; or connect the reaction chamber and the condensation chamber One possible arrangement is to arrange the rooms erect and side by side.

The present invention adopts the last arrangement mentioned above and provides a device which overcomes the above-mentioned difficulties.

That is, according to the present invention, there is provided a reaction chamber that can be heated for reducing a chloride of a high-melting-point, high-toughness metal with an active metal to obtain the metal; In an apparatus consisting of a condensation chamber for condensing the produced metal chloride, and a gas passage for connecting the two; the reaction chamber and the condensation chamber are arranged in parallel with each other, and a funnel-shaped body is installed in the upper lid of each chamber. A seal pot structure is provided with a sealing pot structure made of an easily meltable and easily evaporable material, which is formed by a pot receiving the opening leg, and a neck having a heating means for melting and vaporizing the easily melted and easily evaporated material,
Further, there is provided a device characterized in that both neck portions are connected by a connecting tube having a removable heating means.

The device of the invention is currently applied to:
Production of titanium and zirconium by reduction of their chlorides with magnesium. The easily meltable and vaporizable material used in the seal pot is magnesium or magnesium chloride.

The apparatus of the present invention not only eliminates the need for tipping or overturning the condensing chamber as mentioned above, but also, in its preferred embodiment, allows the same vessels to be reacted alternately, as explained in detail below. Its use as a chamber and condensation chamber allows for efficient use of the device by streamlining its operation and evening out the aging of the various parts of the device.

Among the accompanying drawings, FIGS. 1A, B, C, D, and E illustrate the arrangement of the reaction chamber and condensation chamber mentioned above.

A is a state where the condensation chamber is placed upright and directly above the upright reaction chamber, B is a state where the condensation chamber is placed upright and directly below the reaction chamber that is upright, and C is a state where the condensation chamber is placed upright and placed directly below the reaction chamber that is upright. D shows the state where the condensation chamber is placed directly above the reaction chamber, D shows the state where the condensation chamber is placed sideways and placed below the side of the upright reaction chamber, and E shows the state where the condensation chamber is placed sideways and placed above the side of the upright reaction chamber. .

The basic structure and function of the apparatus of the present invention will be explained in detail below with reference to the drawings regarding the reduction of TiCl ₄ with Mg. FIG. 2 is a longitudinal sectional view showing the mechanism of a specific example of the device of the present invention.

In this embodiment, the reaction chamber 2 and the condensation chamber 2' are cylindrical bodies having exactly the same shape and are placed side by side, with the reaction chamber being housed in the heating furnace 1 and the condensation chamber 2' being housed in the cooling device 19. Both of them have upper lids 8 and 8, respectively.
8′ and the neck (gas passage) 21, 2 integrated with
1', and are connected by an oblong inverted U-shaped connecting pipe 17 that connects the respective necks.

As mentioned above, the reaction chamber has the same shape and structure as the condensation chamber, so the details of the reaction chamber will be explained below. Since the condensation chamber has the same reference numeral with a dash as the members of the reaction chamber, the description regarding the reaction chamber directly applies to the condensation chamber.

A lattice plate 3 is provided at the bottom of the reaction chamber 2, and a MgCl ₂ discharge pipe 6 opening below the lattice plate 3 is provided. This discharge pipe rises along the wall of the reaction chamber and is fixed to the collar 23 of the reaction chamber.

A cylindrical protrusion 22 with a closed bottom is provided at the center of the bottom of the reaction chamber, and a collar 25 is provided on a part of the cylinder.
is provided. After the reaction, separation and condensation are completed, the end of the cylinder is cut open to scrape out the formed metal sponge. The collar 25 is for connecting a vacuum exhaust pipe, which will be explained later. When the reaction chamber container is used as a condensation chamber, a cut end of this cylindrical portion is provided.

The upper opening of the reaction chamber is closed by an upper lid 8, and a neck 21 is provided that passes through the upper lid and is provided with a heating means (usually an electric resistance heating device) fixed thereto. Special application 1987-8711
A seal pot similar to that disclosed in Japanese Patent Application Laid-Open No. 58-126936 is provided.

The principle of the seal pot itself is known. A pot 14 is supported in the center of the gas passageway in the neck (support means not shown), and a funnel-shaped body 27 is provided within the pot with its open leg facing out. For example, molten magnesium is injected into the pot from an inlet 15 (described again later) for an easily meltable and evaporable substance provided above, solidified, and this portion is closed. When opened, the substance is evaporated by the heating means.

A baffle plate 12 extending in an umbrella shape from the lower end of the neck is provided so that its periphery is in contact with the inner wall of the reaction chamber 2.

An introduction pipe 9 for TiCl ₄ and an introduction pipe 11 for an inert gas such as Ar (in the figure, it is a double pipe),
The Mg introduction pipe 10 passes through the upper cover 8 and the baffle plate 12
It is provided so as to open on the inner surface of the neck 2.
1 is provided with an inert gas discharge pipe 16 penetrating its wall and below the seal pot.

The connecting tube 17 is simply a U-shaped tube with heating means (also usually an electric resistance heating device) throughout, but near its ends there are inlets for introducing the easily evaporated substance into the sealing pot. A tube 15 is provided.

The periphery of the upper opening of the reaction chamber 2 has a flange and is removably fixed to the upper lid 8 via a heat-resistant gasket with a clamp or bolt. The upper opening of the neck also has a flange and is similarly removably fixed to a corresponding flange of the coupling tube.

All of the above-mentioned conduits are provided with valves and disconnection means from the master pipe, which are obvious to those skilled in the art and are therefore omitted from the drawings and will not be specifically described.

The heating furnace containing the reaction chamber is a known one, and
It is also convenient to use an electric resistance heating method. The reaction chamber is supported by its collar 23 on the upper edge of the furnace.

The cooling device 19 is a simple container containing a condensing chamber and having a coolant inlet pipe 20 and a discharge pipe 28, and has an opening at the bottom that allows the opening at the bottom of the condensing chamber to face the outside, and has an opening around it. An elastomeric annular gasket 24 is provided on which the bottom of the condensing chamber rests in a gas-tight manner to define a jacket space between the condensing chamber and the cooling system.

The cylindrical part at the bottom of the condensation chamber (the same vessel as the reaction chamber), which faced the opening at the bottom of the cooling device, had its end cut off at this stage and was exposed outside the opening at the bottom of the cooling device. A vacuum exhaust pipe 18 is coupled to this cylindrical portion. The latter has an inner diameter larger than the outer diameter of the cylindrical part of the condensing chamber, has a flange 26 at its open end, accommodates the tip of the cylindrical part, and connects the flange 26 and the collar 25 of the cylindrical part. is fixed in the condensing chamber by inserting a suitable gasket and fixing it with bolts, clamps, etc.

Various introduction pipes provided in the reaction chamber mentioned above,
Some of the exhaust pipes are not used when used with a condensing chamber.

If the condensation chamber is then used as a reaction chamber,
A disk having the same shape and dimensions as the cross section of the open cylindrical part is quickly welded to close the opening.

At present, this method is taken because there is no suitable gasket material that can withstand high temperatures, but if a suitable material is developed in the future, this part and the vacuum exhaust pipe will be connected by connecting the flanges of both. All you have to do is insert a gasket and secure it with bolts or clamps.

The substantial part of this device is patent application No. 57-8711.
(Japanese Unexamined Patent Publication No. 1982-), and can be easily manufactured by a person skilled in the art based on the ordinary knowledge of chemical engineering by referring to various prior art documents, the above explanation, and the attached drawings. There is no need to describe the details of production here.

However, in the device prototyped by the inventors, the reaction chamber (which also serves as a condensation chamber) is bell-shaped with an outer diameter of 700 mm and a height of 1760 mm, and the length (height) of the neck (gas passage) is 380 mm.
mm, and the inner diameter was 185 mm. The condensation chamber (reaction chamber) and connecting pipe were made of chromium-containing steel with a wall thickness of 25 mm. The seal pot part is manufactured using 5mm thick material, and the outer diameter
It was 150mm and 50mm high. Also, the diameter of the connecting pipe is
It was 185mm and its center length was 2100mm.

Next, the operation of manufacturing titanium sponge using the above-mentioned apparatus will be explained as an example of operation.

First, the entire apparatus was installed in the state shown in FIG. At this time, the bottom opening of the reaction vessel 1 is closed, and the bottom opening (cylindrical part) of the condensation chamber 1' is closed.
22' has its end cut open,
It is connected to the vacuum exhaust pipe 18. Also, at this time, the seal pots 14, 14' are closed with solidified metal magnesium, but the seal pot 14 is open (or may be closed), and the cylindrical part 22' at the bottom of the condensing chamber has its tip cut off. The exhaust pipe 18 is opened and connected to the exhaust pipe 18. When using this device for the first time, the seal pot 14' is in the open state, but if the condensation chamber and reaction chamber are used interchangeably from then on, the seal pot 14' will be in the open state during condensation work.
4' is always closed.

Before assembling the apparatus as described above, approximately
Charge 415Kg of Mg. After the reaction chamber was made into a closed system, it was vacuum degassed using the inert gas inlet 11, and then Ar was introduced to completely create an Ar atmosphere inside the reaction chamber. After that, the reaction chamber is heated by heating furnace 1.
Mg was brought into a molten state, and TiCl ₄ was introduced through conduit 9 at 750°C to start the reaction. The reaction continued for about 28 hours and was terminated when about 1170 Kg of TiCl ₄ was consumed.
Thereafter, the furnace temperature was maintained at 900° C. for about 60 minutes, and then as much of the remaining MgCl ₂ as possible was extracted from the MgCl ₂ discharge pipe 16. Then immediately open the gas passage 1 in the upper part of the reaction chamber.
3. Exhaust passage 13' and connecting pipe 17 at the top of the condensing chamber
The temperature was raised to 750 to 800°C, and exhausting from the vacuum exhaust pipe 18 was gradually started. At this time, of course, all openings communicating with the atmosphere other than the vacuum exhaust system are completely sealed. Seal pot 1 installed in the upper gas passage of the reaction chamber shortly after the start of evacuation
4 opens when Mg evaporates. As the degree of vacuum increases, the residual Mg and MgCl ₂ evaporated from the titanium sponge produced in the reaction chamber condense and adhere to the inner wall of the condensation chamber, which is cooled by passing water through the jacket through the connection path. . As the degree of vacuum increased, the furnace temperature was raised from 900°C to 1000°C, and vacuum separation was continued for an additional 25 hours. Immediately after vacuum separation is completed, Ar is introduced into the system to bring both the reaction chamber and the condensation chamber to normal pressure, and then the Mg introduction tubes 15, 1 are
1.3 kg of molten Mg at about 750°C was injected into each tube from 5', solidified, and the exhaust passage was shut off. When the temperature of the reaction chamber dropped to 800° C. or lower, the connecting path 17 was disconnected. A sealing lid was attached to the flange of each separation surface, so that the reaction chamber and condensation chamber were kept in a sealed state to avoid contact of the contents with the atmosphere. Thereafter, the reaction chamber was lifted out of the heating furnace while keeping the inside of the reaction chamber in a slightly pressurized state with Ar, and was forced to cool down on a cooling stand (not shown). After cooling, the tip of the cylindrical part at the bottom of the reaction chamber was cut to create an opening, and approximately 280 kg of high-quality spongy titanium was scraped out. On the other hand, after draining the cooling water from the jacket, the condensing chamber was separated from the vacuum exhaust pipe 18, and its bottom opening was closed by welding a sealing lid (during this time, the condensing chamber was in communication with the atmosphere, so it was quickly operated while filling it with Ar). It was lifted up and moved into the heating furnace 1, the connecting pipe 17 was connected, and the assembly of the next run began. In this state, both seal pots are closed, so the next work can proceed efficiently.

As described above, in the production of titanium metal, the apparatus of the present invention is an integrated reduction and condensation apparatus in which the reaction chamber and the condensation chamber are placed side by side, and the upper parts of each are connected by a connecting passage, thereby eliminating the conventional complexities. It was possible to simplify the neck area, which had a tendency to
- All the advantages of the device proposed in 8771 can be inherited as is, and there is no need to tilt the condensation chamber, and moreover, it can be used as a reaction chamber for the next batch without exposing the contents to the atmosphere. can do.

With repeated use, the bottom cylindrical part of the reaction vessel (referring to the reaction chamber and condensation chamber) becomes shorter and shorter. Therefore, the length of the cylindrical portion is determined by taking into account the service life (number of uses) of the container.

FIG. 3 shows a modification of the device shown in FIG.
In this embodiment, only one seal pot is present in the gas passage between the reaction chamber and the condensation chamber, thereby reducing ventilation resistance.

That is, the upper lid 8, 8' of the reaction chamber (condensation chamber) is provided with two openings 21, 21', 25, 25', each of which is provided with a neck (gas passage), but the seal pot has a corresponding one. They are provided only on the opposing sides (25, 25' in FIG. 3). (21,2
It may be provided on the 1' side. ) The neck portion of one chamber without a seal pot and the neck portion of the other chamber without a seal pot are connected by a connecting pipe 17.
Neck without seal pot (2 in case of Figure 2)
1, 21'), the introduction pipe provided in this part is covered with a lid 26 when the connecting pipe is not connected.
The discharge pipe can be simply attached to this lid. Note that this lid can be used alternately for the reaction chamber and the condensation chamber, so only one lid is required (ie, 26' is not provided).

The rest of the structure is substantially the same as the device shown in FIG. 2, and like parts have been given the same reference numerals and will be understood from the foregoing description.

It is self-evident that the apparatus of the invention can also be used for the production of metallic zirconium. As described in detail above, the present invention streamlines the production of high-melting-point, high-toughness metals such as titanium and zirconium, equalizes wear and tear on equipment, and streamlines the service life of the equipment.

[Brief explanation of the drawing]

FIG. 1 shows the arrangement of a reaction chamber and a condensation chamber in an integrated high-melting-point, high-toughness metal device. FIG. 2 is a schematic diagram showing one embodiment of the apparatus of the present invention, and FIG. 3 is a schematic diagram showing another embodiment thereof. 1... Heating furnace, 2... Reaction chamber, 2'... Condensation chamber, 3... Grid plate, 6... Discharge pipe, 8... Upper cover, 9... TiCl ₄ introduction pipe, 10... Mg introduction pipe ,1
DESCRIPTION OF SYMBOLS 1... Inert gas introduction pipe, 12... Buff full baffle plate, 13... Exhaust passage, 14... Shutoff means (seal pot), 15... Easily meltable substance inlet,
16...Inert gas outlet, 17... Connection path, 1
8... Vacuum exhaust pipe, 19... Jacket, 20...
...Cooling water inlet, 21...Neck, 28...Cooling water outlet.

Claims (1)

[Claims] 1. A reaction chamber that can be heated for reducing a chloride of a high-melting-point, high-toughness metal with an active metal to obtain the metal, and an unreacted active metal separated from the produced metal; In a device consisting of a condensation chamber for condensing the metal chloride produced and a gas passage for communicating the two: The reaction chamber and the condensation chamber are arranged in parallel with each other, and a funnel-shaped body and a funnel-shaped body are placed on the upper lid of each chamber. A sealing pot structure made of an easily meltable evaporable material consisting of a pot receiving an opening leg is provided with a neck having a cutting hand and a heating means for melting and evaporating the easily meltable evaporable material, and both necks are removable. A device characterized in that it is connected by a connecting pipe having heating means. 2. The apparatus according to claim 1, wherein the reaction chamber and the condensation chamber are containers of the same shape and are used interchangeably. 3. The apparatus according to claim 2, wherein both the reaction chamber and the condensation chamber have a closable opening at the bottom. 4. The device according to claim 3, which is a container capable of accommodating a condensation chamber, and has an opening at the bottom that allows the bottom opening of the condensation chamber to be exposed, and a container surrounding the opening. , an annular gasket made of an elastomer that can be tightly attached to the bottom of the condensing chamber, and having a liquid inlet pipe and a liquid discharge pipe, so as to form a jacket space when the condensing chamber is housed with its bottom placed on the annular gasket. characterized in that it is equipped with a cooler configured. 5. The apparatus according to any one of claims 1 to 4, wherein the reaction chamber and the condensation chamber upper lid each have two necks, and only one of the necks is provided with passage blocking means. 1. A device characterized in that the chambers having passage blocking means and the chambers not having passage blocking means are connected by a connecting pipe.