JPH11124183A - Material supply cartridge - Google Patents

Abstract

PROBLEM TO BE SOLVED: To quickly supply a material such as highly reactive metal by constituting a material supply cartridge for supplying a material such as granules which are likely to be degraded in contact with an atmosphere to a manufacturing process machine, including an atmosphere adjusting means holding the inside of a container at a vacuum or in an inert gas atmosphere. SOLUTION: In filling a material 4 such as granules of an alkaline earth metal to a container 2, while a rod 3 is lowered with a lower end 3a in pressure contact with a lower port 5, the inside of the container 2 is evacuated through a pipe line 9. Then after the rod 3 is raised to have the lower port 5 opened and the material 4 is filled into the container 2, the rod 3 is lowered to have the lower port 5 closed. Thereafter an inert gas is supplied into the container 2 through the pipe 9 to bring the inside of the container 2 into an inert gas atmosphere. When the material 4 preserved in the container 2 is to be supplied to a reaction container or the like, the lower port 5 is connected with a material supply port the reaction container for attaching a cartridge 1, and the rod 3 is raised to have the lower port 5 opened, thereby supplying the material 4 into the reaction container.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for producing a powdery or granular raw material, such as a highly reactive metal powder or granule (pellet) or a gas adsorbent powder, which is susceptible to deterioration when exposed to the atmosphere, for example, in a reactor. The present invention relates to a raw material supply cartridge suitably used for supplying to a process device without deterioration.

[0002]

2. Description of the Related Art The CVD method has been used as a promising method for producing oxide-based ceramic thin films or layered ceramics, and research and development thereof have been actively conducted. For example, a CVD method is used in a manufacturing process of a superconductor thin film, a high / ferroelectric thin film, and various integrated circuits. The β-diketonate metal complex has a relatively high vapor pressure and a high reactivity, and thus is useful as a gas phase source for the CVD method. For example, alkaline earth metal β-diketonate is important as a constituent element of an oxide superconductor or a high / ferroelectric substance. This β-diketonate metal complex is prepared by mixing an alkaline earth metal or an alkali metal such as metal Sr or metal Ba with dipivaloylmethane (hereinafter referred to as DP) in an organic solvent.
M) and a β-diketone.
On the other hand, the β-diketonate metal complex is easily deteriorated under the influence of moisture and carbon dioxide in the air. For this reason, a high-purity complex cannot be obtained, and a complex containing a large amount of impurities is converted to CV.
When used in Method D, the reproducibility is poor and a good thin film cannot be obtained. Therefore, it is desired to provide a complex as pure as possible, but as described above, the β-diketonate metal complex is easily deteriorated by moisture or carbon dioxide gas in the air,
It is susceptible to deterioration in the reaction step between the raw metal and β-diketone such as DPM, the subsequent purification step, or the packaging step,
There is a disadvantage that the purity varies from batch to batch.

A problem in producing a β-diketonate metal complex is handling of a raw material metal such as an alkaline earth metal. Alkaline earth metals such as barium and strontium and alkali metals such as sodium and potassium easily react with moisture and oxygen. Conventionally, these highly active metals are stored in a state where a stable oil such as liquid paraffin is put in a container such as a screw bottle made of glass and immersed therein. Therefore, in use, in order to remove paraffin adhering to the metal, it must be washed with an organic solvent such as n-hexane, further washed with a reaction solvent, for example, benzene, and then supplied into the reaction vessel. Did not.

[0004]

As described above, conventionally, a highly active metal is immersed in a stable oil and stored, and a washing step for removing the stable oil at the time of use is required. Oxide coatings tend to form on the surface of the raw metal, which has been one of the causes for reducing the reaction yield. The present invention, without deteriorating raw materials such as highly reactive metals,
An object is to provide a raw material supply cartridge that can be supplied quickly.

[0005]

According to the present invention, there is provided a material supply cartridge having an opening through which a powdery or granular material is taken in and out, a container for storing the material therein, and opening and closing of the opening of the container. It has an opening / closing means and an atmosphere adjusting means for maintaining the inside of the container in a vacuum or an inert gas atmosphere. In this raw material supply cartridge, the opening / closing means is vertically movably inserted into the container, and an opening / closing mechanism including a rod body for closing the mouth by pressing its tip against the mouth, or a shutter-type opening / closing mechanism. An opening / closing mechanism provided with a valve may be used. Further, as the atmosphere adjusting means, one having a pipe connected to the container and a valve provided in the pipe can be used. Another raw material supply cartridge of the present invention has a lower opening for taking in and out a powdery or granular raw material, an upper opening formed with a screw portion on the inner surface, and a container for storing the raw material therein, A thread portion screwed with the thread portion of the upper mouth portion is formed on the upper outer peripheral surface, a rod inserted into the container, a conduit connected to the container, and a valve provided in the conduit And an atmosphere adjusting means for maintaining the inside of the container in a vacuum or an inert gas atmosphere, wherein the rod moves up and down with respect to the container by rotating in the forward and reverse directions, At the time of the lowest descent, the lower end of the rod comes into pressure contact with the periphery of the lower opening of the container to close the lower opening. The lower mouth portion is configured to open apart from the main body. In this raw material supply cartridge, the rod is provided with an enlarged diameter portion, and when the rod is raised and the lower opening is sufficiently opened, the expanded portion comes into contact with the inner wall of the container, and the rod is excessively raised. May be prevented. Further, the container may be formed of an organic solvent-resistant material capable of storing a powdery or granular raw material and an organic solvent.

[0006]

DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS A raw material supply cartridge according to the present invention has an opening through which powdery or granular raw materials are taken in and out, a container for storing the raw material therein, and an opening / closing means for opening and closing the opening of the container. And an atmosphere adjusting means for maintaining the inside of the container in a vacuum or an inert gas atmosphere.
When the raw material is filled in the container, preferably, the inside of the container is made to be an inert gas atmosphere in advance, and the opening is opened by operating the opening / closing means, and the raw material in powder or granular form is filled in the container. After the filling of the raw material is completed, the opening and closing means is operated to close the mouth, and the atmosphere in the container is kept in a vacuum or an inert gas atmosphere by the atmosphere adjusting means, so that the raw material in the container is stored for a long time without deterioration. be able to. When the raw material is used, the mouth of the container is connected to the raw material supply port of the manufacturing apparatus, the opening / closing means is operated, and the raw material in the container is discharged from the mouth. As described above, the raw material supply cartridge of the present invention can rapidly supply a highly reactive metal raw material without deterioration.

FIG. 1 shows an embodiment of a raw material supply cartridge according to the present invention. In the figure, reference numeral 1 denotes a raw material supply cartridge (hereinafter, referred to as a cartridge). The cartridge 1 has a lower port 5 through which powdery or granular raw material 4 is put in and out, and an upper port 7 in which a screw portion 6 is formed on the inner surface, and a container 2 that stores the raw material therein, A screw portion 8 is formed on the upper outer peripheral surface to be screwed with the screw portion 6 of the upper opening 7. The rod 3 inserted into the container 2, a pipe 9 connected to the container 2, and the pipe 9 And an atmosphere adjusting means 11 for maintaining the inside of the container 2 in a vacuum or an inert gas atmosphere. The screw 8 of the rod 3 and the upper opening 7 of the container 2 having the screw 6 on the inner surface move the rod 3 up and down by rotating the rod 3 in the forward and reverse directions. This serves as opening and closing means for opening and closing the lower opening 5 of the container 2.

The container 2 has a strength enough to withstand an atmospheric pressure load when the inside is evacuated, and is made of glass or the like which has no reactivity with a raw material 4 such as a highly active metal to be filled therein. . In the cartridge 1 exemplified in this embodiment, the main body 2a of the container 2 and the upper part 2b having the upper mouth 7 are separate members, and flanges 12 and 13 are provided at the upper end of the main body 2a and the lower end of the upper part 2b, respectively. The upper and lower flanges 12, 13 are fastened and integrated by a clamp 15 with a seal ring 14 made of fluororesin or the like interposed between the respective flanges 12, 13. In addition, the container 2 may be an integral body, and furthermore, the main body 2
a may be divided into one or a plurality of pieces, and the structure may be air-tightly joined.

The rod body 3 is formed of a material having no reactivity with a raw material such as a highly active metal filled therein, and is preferably formed of a self-lubricating fluororesin or the like. In the cartridge 1 exemplified in the present embodiment, a screw portion 8 is formed at the upper portion, a central portion is bulged to provide an enlarged diameter portion 16, and a round bar-like bar having a flange-like handle 17 formed at an upper end portion. It has a configuration using the body 3. The enlarged diameter portion 16 raises the rod 3 with respect to the container, and when the lower end 3a of the rod 3 is sufficiently separated from the inner wall surface of the lower opening 5 of the container 2, the enlarged diameter portion 16 The upper end abuts directly below the upper opening 7 of the container 2,
Function as a stopper to prevent the rise of Further, the enlarged diameter portion 16 is slidably fitted in the hole of the seal ring 14 described above. Thus, the inside of the container 2 below the seal ring 14 can be maintained in a vacuum or an inert atmosphere.

The conduit 9 of the atmosphere adjusting means 11 is connected to a vent (not shown) formed on the side surface of the container 2 so as to project therefrom. The conduit 9 can be appropriately selected according to the production scale, such as a rubber tube or a metal pipe. In addition, the valve 10 provided in the pipe 9 may be any valve that can switch the evacuation and the filling of the inert gas through the pipe 9 and maintain the atmosphere in the container 2 after the atmosphere adjustment for a long time. .
Further, it is desirable that the valve 10 be a three-way switching valve, and that a configuration be provided in which a vacuum evacuation line and an inert gas filling line are connected.
Further, the tip of the pipe 9 may have a fixed type structure which is always connected to a vacuum pump for evacuation and a pipe from an inert gas cylinder such as nitrogen gas or argon gas. A configuration is also possible in which the pipe is connected detachably so that only the cartridge 1 can be used or stored. In the case of this detachable structure, it is preferable to attach a coupler which can be easily connected to another pipeline at the end of the pipeline 9.

Next, a procedure for using the cartridge 1 will be described. The raw material 4 to be filled in the container 2 may be in the form of powder (the particle size is not limited and may be ultrafine particles, granules, or flakes) or granular (the shape is not limited and may be elliptical or amorphous). . The material is not limited, for example, alkaline earth metals such as metal barium and metal strontium, alkali metals such as metal sodium and metal potassium, high-purity metals or high-purity nonmetallic elements for semiconductor production such as gallium and arsenic, and getters. Materials that need to be handled in a vacuum or inert gas, such as materials, gas adsorbents such as zeolites, ignitable elements or compounds. As an example, a case where particles (pellets) of an alkaline earth metal for producing a β-diketonate metal complex will be described.

When the raw material 4 is filled, the cartridge 1
Inside is as clean as possible, in FIG. 1, the rod 3 is turned down as shown by the dashed line, and the lower end 3a is brought into pressure contact with the inner wall surface of the periphery of the lower opening 5, that is, in a closed state,
Further, the inside is evacuated through a pipe 9. Next, the granular raw material 4 is filled in the container 2. At this time, the inside of the storage tank or the transport container for the raw material 4 is set to a vacuum atmosphere,
Further, it is more preferable that the supply port of the raw material 4 and the lower port 5 of the container 2 have a joint structure capable of airtight connection. Further, when the raw material 4 is filled, it may be performed in an atmosphere of an inert gas such as nitrogen gas or argon gas. The lower mouth 5 is opened by raising the rod 3 and the raw material 4 is filled in the container 2, and then the rod 3 is turned to lower the rod 3, and the lower end 3 a is pressed against the periphery of the mouth 5 to press the mouth 3. Close the part 5.

After the filling of the raw material 4 is completed, an inert gas such as nitrogen or argon gas is supplied into the container 2 through the pipe 9 to make the inside of the container 2 an inert gas atmosphere. At this time, an organic solvent (for example, n-hexane) used together with the raw material 4 at the time of synthesis may be put in the container 2, and the raw material 4 may be immersed in the organic solvent. Further, in order to complete the inert gas atmosphere in the container 2, the evacuation of the container 2 and the supply of the inert gas may be repeatedly performed through the pipe 9. By filling the raw material 4, closing the lower opening 5 of the container 2 with the lower end 3 a of the rod 3, and completely closing the valve 10 of the pipe 9, the raw material 4 in the container 2 is kept under an inert gas atmosphere. Since the raw material 4 can be stored in a vacuum atmosphere, the raw material 4 in the container does not come into contact with the atmosphere even when stored for a long time, and there is no risk of deterioration such as formation of an oxide film.

When the raw material 4 stored in the container 2 is supplied to the reaction container or the like, the mouth 5 is airtightly connected to the raw material supply port of the reaction container, the cartridge 1 is mounted, and the rod 3 is turned up. Then, by opening the opening 5, the internal raw material 4 can be supplied into the reaction vessel. To describe in detail a reaction vessel for producing a β-diketonate metal complex as an example, the mouth 5 of the cartridge 1 containing the raw material 4 is connected to a joint-type supply port of the reaction vessel. After the evacuation of the reaction vessel and the filling of the inert gas are repeated, the pressure inside the reaction vessel is reduced. Then, the rod 5 of the cartridge 1 is turned in the ascending direction to open the mouth 5, and a raw material such as granular metal barium or the raw material and an organic solvent such as n-hexane are charged into the reaction vessel. Next, after argon gas is sealed in the container 2 through the pipe 9, the valve 10 of the pipe 9 is closed. Thereafter, the cartridge 1 is kept set in the reaction container until the reaction is completed.

As described above, by applying the cartridge 1 to supply of a highly active metal raw material in the production of a β-diketonate metal complex, a highly active metal such as barium metal or strontium can be reacted without contacting the atmosphere. Since the metal complex can be stored up to a maximum, a metal complex with higher purity can be produced. In addition, if the raw material 4 is stored by the cartridge 1, it is not necessary to immerse and store the raw material 4 in a stable oil such as liquid paraffin, and a step of washing and removing paraffin when used is not required. Conventionally, highly active metals have been supplied in the form of ribbons (strips) which can be easily immersed and stored in stable oil. However, if this cartridge 1 is used, the raw materials are stably maintained until the reaction without exposing them to the atmosphere. Since it can be stored, it is possible to use the granular or powdered raw material 4 which is easy to handle and has good reaction efficiency.

The above-described embodiment is merely an example of the present invention, and the present invention is not limited to the above-described embodiment, and various modifications are possible. For example, in the above example, the opening and closing means for opening and closing the mouth portion 5 by moving the rod body 3 up and down is used. However, an appropriate opening and closing mechanism such as a shutter valve may be attached to the lower mouth portion 5.

[0017]

As described above, according to the present invention,
It is possible to provide a raw material supply cartridge capable of rapidly supplying a raw material such as a highly reactive metal without deteriorating the raw material.

[Brief description of the drawings]

FIG. 1 is a sectional view showing one embodiment of a raw material supply cartridge of the present invention.

[Explanation of symbols]

DESCRIPTION OF SYMBOLS 1 ... Cartridge, 2 ... Container, 3 ... Bar (opening / closing means), 4 ... Material, 5 ... Lower mouth, 6 ... Screw, 7
... Upper mouth portion, 8 screw portion, 11 atmosphere control means.

Claims (6)

[Claims] 1. A container having an opening through which powdery or granular raw materials are taken in and out, a container for storing the raw materials therein, an opening / closing means for opening and closing the opening of the container, and a vacuum or inert gas inside the container. A raw material supply cartridge provided with an atmosphere adjusting means for maintaining a gas atmosphere. 2. The opening / closing mechanism, wherein the opening / closing means is inserted into the container so as to be vertically movable, and has an end provided with a rod body for closing the opening by pressing the opening against the opening, or a shutter-type opening / closing valve. The raw material supply cartridge according to claim 1, wherein the raw material supply cartridge is an opening / closing mechanism provided with: 3. A raw material supply cartridge, wherein the atmosphere adjusting means includes a pipe connected to the container, and a valve provided in the pipe. 4. A container having a lower opening through which a powdery or granular raw material is taken in and out, an upper opening having a screw portion formed on an inner surface thereof, and a container for storing the raw material therein, and an upper outer peripheral surface formed by a container. A screw portion screwed with the screw portion of the upper mouth is formed, a rod inserted into the container, a pipe connected to the container,
An atmosphere adjusting means for maintaining the inside of the container in a vacuum or an inert gas atmosphere, wherein the rod is rotated in the forward and reverse directions to the container. When the rod moves down, the lower end of the rod is brought into a closed state in which the lower end of the rod is pressed against the periphery of the lower opening of the container to close the lower opening, and the rod is raised from the closed state. A raw material supply cartridge wherein the lower end of the rod is separated from the periphery of the lower opening and the lower opening is opened. 5. An enlarged diameter portion is provided on the rod, and when the rod is lifted and the lower opening is sufficiently opened, the extended portion comes into contact with the inner wall of the container to prevent excessive rise of the rod. 5. The raw material supply cartridge according to claim 4, wherein the raw material supply cartridge is configured to be blocked. 6. The raw material supply cartridge according to claim 4, wherein the container is formed of an organic solvent-resistant material capable of storing a powdery or granular raw material and an organic solvent in the container.