WO2004054926A1

WO2004054926A1 - Involved fullerene manufacturing and collecting system tool

Info

Publication number: WO2004054926A1
Application number: PCT/JP2003/016111
Authority: WO
Inventors: Rikizo Hatakeyama; Takamichi Hirata; Yasuhiko Kasama; Kenji Omote
Original assignee: Ideal Star Inc.
Priority date: 2002-12-16
Filing date: 2003-12-16
Publication date: 2004-07-01
Also published as: TW200418723A; AU2003289363A1; JP3923007B2; JP2004196562A

Abstract

A fullerene manufacturing and collecting system tool capable of manufacturing a high quality involved fullerene with a high production efficiency, comprising a vacuum chamber (1), a film formation chamber (5) having a substrate inlet port (2a) for leading a substrate (3a) therein formed on the vacuum chamber (1) side and stacking the involved fullerene on the substrate (2a), a dissolving chamber (6) having a substrate inlet port (2b) for leading, therein, a substrate (3b) on which the involved fullerene was stacked in the film formation chamber (5) formed on the vacuum chamber (1) side and also having a dissolving liquid inlet port (9) for leading dissolving liquid for melting the involved fullerene stacked on the substrate (2b) and a dissolving liquid outlet port (10) for discharging the dissolving liquid (this dissolving liquid is referred to as “resolvent”) after the involved fullerene is dissolved, and susceptors (4a, 4b) allowed to be rotated and reciprocatingly moved, allowing a plurality of substrates to be placed thereon, and capable of leading the substrates into the film formation chamber (5) and the dissolving chamber (6).

Description

Description Manufacturing and recovery system tools for endohedral fullerenes Technical field

The present invention relates to a production / collection system tool for endohedral fullerenes. Background art

In 1990, Kretschima published a method for mass synthesis of so-called fullerenes, hollow carbon clusters represented by C60 (Cretschmer et al., W. Kratshmer et al. al., Nature), 347 (1990) 354). Since then, various physical properties studies of C 60 crystal as well as itself have been conducted.

In addition, K3 C60 doped with へ in C60 thin film by Hebard et al.

= 18% superconductivity (Hepard et al., Nature (A. F. Hebard et al., 350) (1991) 600). This is attracting attention as a new superconductor material.

However, at present, no method has been established for obtaining endohedral fullerenes on substrates at high yields. That is, at present, the amount of endohedral fullerene obtained on the inner wall of the apparatus or on the substrate is very small.

At the same time, a method of collecting endohedral fullerenes obtained on the inner wall of the apparatus or on the substrate has not yet been established. For example, the fact is that soot (encapsulated fullerene) attached to the inner wall of the device is collected and collected by some method. Furthermore, the method of recovering endohedral fullerenes with high productivity and high recovery at the industrial level is completely out of interest for researchers.

On the other hand, the present inventor has separately provided a technique for obtaining a large amount of endohedral fullerene in a high yield (Japanese Patent Application No. 2002-). For large quantities of endohedral fullerenes, there is a demand for the establishment of a technology that enables high recovery rates and high productivity without changing the properties of the endohedral fullerenes.

The present invention can produce high-quality endohedral fullerenes with good production and high recovery rate. The purpose is to provide tools for the production and recovery of natural endohedral fullerenes. Disclosure of the invention

The production and recovery system tool of the present invention includes a vacuum chamber,

A film formation chamber having a substrate introduction port for introducing a substrate on the vacuum chamber side, for depositing an endohedral fullerene on the substrate;

The vacuum chamber has a substrate introduction port for introducing a substrate on which the endohedral fullerene has been deposited in the film forming chamber, and introduces a solution for dissolving the endohedral fullerene deposited on the substrate. A dissolution liquid inlet for discharging a dissolution liquid after dissolving the endohedral fullerene (this dissolution liquid is referred to as a “dissolution liquid”);

A susceptor capable of rotating and reciprocating, capable of mounting a plurality of substrates, and allowing the substrates to be introduced into the deposition chamber or the dissolution chamber;

It is characterized by having.

The endohedral fullerene is a metal endohedral fullerene.

The metal is an alkali metal.

The solution for dissolution is characterized in that it is e-rin. Ayurin does not dissolve fullerene that is not included. Anilin dissolves the endohedral fullerene. Therefore, only endohedral fullerene can be recovered by using aniline as a solvent. As a result, it is possible to recover the fullerene that is not at a high recovery rate. Ayurin can be suitably used as a developing solution in high performance chromatography (HPLC).

An inlet passage having an inlet for introducing the liquid at one end and a discharge passage having an outlet for discharging the liquid out of the system are formed at one end, and the inlet passage and the discharge passage are respectively formed. And a nozzle structure having an opening that opens toward the substrate at the intersection and a liquid that contacts the substrate through the opening. A nozzle having pressure control means for controlling the difference between the pressure of the liquid in contact with the substrate and the atmospheric pressure so as not to flow outside is provided in the dissolving chamber, and the dissolving liquid inlet and the inlet are provided. Port, and the solution outlet is connected to the outlet. It is assumed that it continued ^ :.

A means for applying ultrasonic waves to the solution for dissolution is provided. By applying the ultrasonic waves, the endohedral fullerene deposited on the substrate can be easily detached from the substrate, so that the recovery rate of the endohedral fullerene can be further increased.

A switching valve is provided downstream of the dissolving liquid introduction port, and one of the switching valves is connected to the dissolving liquid, and the other is connected to the cleaning liquid. In order to wash the substrate, the washing chamber may be provided as described above. However, even if the washing chamber is not provided, a switching valve is provided downstream of the dissolving liquid introduction port, and one of the switching pulp is dissolved. The substrate can be cleaned by being connected to the cleaning solution and the other being connected to the cleaning solution. That is, after the dissolution step, the substrate can be cleaned by switching the valve and introducing the cleaning liquid. Of course, cleaning in the cleaning room may be performed together with such cleaning.

A cleaning chamber for cleaning the substrate after dissolution is provided between the film formation chamber and the dissolution chamber. For cleaning in the cleaning chamber, the above-described nozzle structure may be used. If the nozzle structure is provided in the cleaning chamber and the cleaning is performed by introducing the cleaning liquid, the cleaning can be easily performed.

A liquid chromatography column is connected to the dissolution chamber. A component analyzer is connected downstream of the column.

The force ram and the component analyzer are arranged in a vacuum chamber.

BRIEF DESCRIPTION OF THE FIGURES

FIG. 1 is a cross-sectional view and a plan view illustrating an example according to the first embodiment.

FIG. 2 is a cross-sectional view illustrating an example according to the second embodiment. BEST MODE FOR CARRYING OUT THE INVENTION

(Example 1)

Fig. 1 shows the tool for the production and recovery system of endohedral fullerenes of this example.

The production system 100 of the endohedral fullerene of this example has a vacuum chamber 1 and a substrate inlet 2a for introducing the substrate 3a on the vacuum chamber 1 side. H The vacuum chamber 1 has a film formation chamber 5 for depositing fullerene and a substrate inlet 2b for introducing the substrate 3b on which the endohedral fullerene has been deposited in the film formation chamber 5, and the substrate 2 b. Dissolving solution inlet 9 for introducing a dissolving solution for dissolving the endohedral fullerene deposited on b, and a dissolving solution after dissolving the endohedral fullerene. A dissolving chamber 6 having a dissolving solution discharge port 10 for discharging a solution, a rotatable and reciprocable, a plurality of substrates can be placed, and And susceptors 4 a and 4 b that can be introduced into the chamber 6.

This example will be described in more detail with reference to FIG.

The vacuum chamber 1 is provided with a film forming chamber 5 and a melting chamber 6. The film forming chamber 5 has an opening on the vacuum chamber 1 side. This opening serves as a substrate inlet 2a for introducing the substrate 3a.

In this example, a gate valve 11 is provided adjacent to the vacuum chamber 1. Substrate replacement is not required for fullerene deposition. That is, the substrate can be used repeatedly. However, a new substrate can be introduced into the vacuum chamber via the gate valve 11.

In the film forming chamber 5, deposition of the endohedral fullerene is performed. The configuration inside the film forming chamber 5 is not particularly limited as long as the endohedral fullerene can be deposited.

On the other hand, the dissolution chamber 6 is provided with a substrate introduction port 2b for introducing a substrate 3b opened to the vacuum chamber 1 side. In the dissolution chamber 2, a dissolution solution inlet 9 and a dissolution solution outlet 10 are formed. A solution (solvent) for dissolving the endohedral fullerene is introduced from the solution solution inlet 9. The dissolving solution after dissolution of the endohedral fullerene is discharged out of the dissolving chamber 6 from the dissolving solution outlet 9. The solution outlet 9 may be provided on the lower surface of the dissolution chamber, and the solution may be discharged by gravity. Alternatively, it may be discharged by suction.

Downstream of the solution outlet 9, for example, a column for liquid chromatography (especially high-performance liquid chromatography) is provided to separate and purify endohedral fullerenes. An analyzer for analyzing components of endohedral fullerenes may be connected downstream of the column. A signal from the analyzer may be sent to the film forming chamber 5 to control film forming conditions.

A drying chamber for drying the encapsulated fullerene or the substrate is provided in a vacuum chamber. You may.

Further, it is preferable that the column and the analysis device are arranged in the vacuum chamber 1. In that case, the solution outlet 10 of the solution chamber 6 is provided so as to be located in the vacuum chamber 1. With such a configuration, from film formation to analysis can be performed without exposure to the atmosphere, and higher-quality endohedral fullerenes can be obtained.

Next, the susceptor will be described.

The vacuum chamber 1 is capable of rotating and reciprocating, and is capable of mounting a plurality of substrates 3a and 3b, and for introducing the substrates 3a and 3b into the film forming chamber 5 to the melting chamber 6. Susceptors 4 a and 4 b arranged in vacuum chamber 1 are provided. In this example, the susceptor is divided into two susceptors 4a and 4b, but may be one. Needless to say, the susceptor is designed and arranged at a position where the substrate can be introduced into the film forming chamber 5 and the melting chamber 6.

In the example shown in FIG. 1, substrates 3a and 3b are arranged on susceptors 4a and 4b, respectively. For example, when an opening is provided on the vacuum chamber side to arrange a cleaning chamber and the substrate is cleaned in the cleaning chamber, one more substrate is placed on the susceptor. That is, the number of substrates corresponding to the number of processing chambers that perform processing on the substrates is placed on the susceptor.

Susceptors 4 a and 4 b are held by holder 8. When the holder 8 is raised with the substrates 3 a and 3 b placed on the susceptors 4 a and 4, respectively, the substrates 3 a and 3 b are formed through the inlets 2 a and 2 b, respectively. Introduced into chamber 5 and dissolution chamber 6. When the substrates 3a and 3b are respectively introduced, a sealed state is formed between the bottom surfaces of the film forming chamber 5 and the melting chamber 6 and the susceptors 4a and 4b, and the film forming chamber 5 and the melting chamber are formed. The inside of 6 becomes airtight. Of course, an O-ring or the like may be provided between the susceptors 4a and 4b and the bottom surfaces of the film forming chamber 5 and the melting chamber 6 in order to further improve the airtightness. Note that the susceptor itself may be used as the substrate. That is, the endohedral fullerene may be deposited directly on the surface of the susceptor.

It is preferable that the bottom surface of the melting chamber 6 and the surface of the susceptor that comes into contact with the bottom surface are mirror-finished in order to enhance the sealing property.

In the film formation chamber 5 with the substrates 3a and 3b introduced, the endohedral fullerene is deposited. After the deposition is completed, the holder 8 is lowered. At that time, the vacuum chamber 1 It is kept under reduced pressure. It may be filled with an inert gas. By lowering the holder 8, the substrates 3a and 3b are taken out of the film forming chamber 5 and the melting chamber 6, respectively, into the vacuum chamber 1. Next, the holder 8 is rotated, and the substrate 3 a on which the endohedral fullerene is deposited is brought below the melting chamber 6. At that time, the substrate 3 b is located below the film forming chamber 5. Next, the holder 8 is raised, and the substrate 3 b is introduced into the film forming chamber 5, and the substrate 3 a on which the encapsulated fullerene is deposited is introduced into the melting chamber 6. In this state,

In step 5, the endohedral fullerene is deposited. At the same time, in the melting chamber 6, the endohedral fullerene deposited on the substrate 3a is melted. Repeat the above operation

Five.

As described above, since the endohedral fullerenes are not exposed to the atmosphere, high-quality endohedral fullerenes can be obtained, and it is possible to produce endohedral fullerenes with high production efficiency by performing film formation and dissolution simultaneously. It becomes.

(Example 2)

FIG. 2 shows a second embodiment.

This example is an example in which dissolution in a dissolution chamber is performed using a wet processing liquid supply nozzle.

Forming an inlet passage 210 having an inlet 207 for introducing the liquid at one end, and a discharge passage 221 having an outlet 215 for discharging the liquid out of the system at one end; The introduction passage 210 and the discharge passage 212 cross each other at their other ends to form an intersection 214, and open at the intersection 214 toward the substrate 201. A nozzle assembly having an opening 206, and a substrate 201 connected to the substrate 201 so that liquid contacting the substrate 201 through the opening 206 does not flow out of the discharge passage 212. A nozzle 202 having pressure control means 2 13 for controlling the difference between the pressure of the liquid in contact and the atmospheric pressure is provided in the dissolution chamber 6, and the dissolution liquid inlet 9 and the The inlet port 207 is connected, and the lysis solution outlet port 10 is connected to the outlet port 215. The pressure control means may be interposed between the solution outlet 10 and the outlet 215.

In the above embodiment, even after the solution is recovered from the inside of the dissolution chamber 6, the solution remains in the dissolution chamber 6. Therefore, when the substrate is taken out of the melting chamber, contamination by the solution in the vacuum chamber or a decrease in the degree of vacuum is caused. In this example, the solution for dissolution is not made into the atmosphere in the dissolution chamber 6. Therefore, recovery of the lysate is very simple. In addition, even when the substrate is taken out of the melting chamber, contamination by the solution in the vacuum chamber or a decrease in the degree of vacuum does not occur.

After dissolving the endohedral fullerene on the substrate, the substrate surface may need to be cleaned. In that case, it is necessary to provide a cleaning chamber for cleaning the substrate between the film formation chamber and the dissolution chamber, with the substrate inlet opening to the vacuum chamber side.

However, if the solution is switched between the solution for dissolution and the washing solution by switching the solution, it is sufficient to simply switch the introduced solution from the solution to pure water or ultrapure water after dissolution. That is, since the substrate can be cleaned without providing a cleaning chamber, the configuration of the tool can be simplified.

In FIG. 2, reference numeral 202 denotes a wet processing liquid supply nozzle. The wet processing liquid supply nozzle 202 mainly includes a nozzle structure 250 and a pressure control unit 21.

In the figure, the pressure control unit 2 13 is constituted by a pressure reducing pump provided on the discharge port 2 15 side. That is, by controlling the suction pressure of the decompression pump, the difference between the pressure of the processing liquid to be processed and, consequently, the atmospheric pressure and the pressure of the processing liquid in contact with the processing object 1 is controlled.

That is, a pressure reducing pump 2 17 is used for the pressure control section 2 13 on the side of the discharge passage 212. The pressure of the liquid to be processed is controlled by the pressure-reducing pump 217, which controls the suction force of the jet processing liquid at the intersection 2 14 (including the surface tension of the wet processing liquid and the surface tension of the processed surface of the workpiece to be wet). And the pressure in the melting chamber 6. In other words, (including the surface tension of the treated surface of Uetsuto processing solution surface tension and the Uetsuto processed material) pressure P _w of Uetsuto treatment liquid in contact with the atmosphere of the dissolution chamber 6 at the opening 2 0 6 and the dissolution chamber by the relationship between the pressure P _a and P _w P _a, it is supplied to the substrate 2 0 1 via the opening 2 0 6, lysis solution in contact with the substrate 2 0 1 Uetsuto processing liquid outside of the supply nozzle The liquid is discharged to the discharge passage 212 without leaking to the discharge passage.

In addition, it is more preferable that the shape of the ceiling at the intersection is such that the Coanda effect is generated because the pressure can be easily balanced.

In addition, an ultrasonic wave applying means 220 is provided on the ceiling part 218 of the nozzle. When dissolving By applying the ultrasonic wave, the endohedral fullerene can be more easily detached from the substrate.

It goes without saying that the present invention is not limited to the embodiments described above.

For example, in FIG. 1, the apparatus has been described as a vertical type in which the holder 8 moves up and down, but the apparatus in FIG. 1 may be a horizontal type in which the apparatus is inclined 90 degrees. Further, the susceptor may be configured to be able to variably apply a bias voltage. Industrial applicability

High-quality endohedral fullerenes can be produced with high production efficiency.

Claims

1. The vacuum chamber and

A film formation chamber having a substrate introduction port for introducing a substrate on the vacuum chamber side, and for depositing an included fullerene on the substrate;

The vacuum chamber has a substrate inlet for introducing a substrate on which the endohedral fullerene has been deposited in the film forming chamber, and a dissolving solution for dissolving the endohedral fullerene deposited on the substrate is introduced. A dissolution solution inlet for dissolving the endohedral fullerene and a dissolution solution outlet for discharging the dissolution solution after dissolution of the endohedral fullerene (this solution is referred to as “dissolution solution”). When,

A susceptor capable of rotating and reciprocating, capable of mounting and surrounding a plurality of substrates, and capable of introducing the substrates into the film formation chamber or the dissolution chamber;

A production and recovery system tool for endohedral fullerenes, comprising:

2. The production / recovery system tool for an internal fullerene according to claim 1, wherein the internal fullerene is a metal internal fullerene.

3. The production / recovery system for internal fullerenes according to claim 2, wherein the metal is aluminum metal.

4. The production / recovery system tool for endohedral fullerene according to any one of claims 1 to 3, wherein the solution for dissolution is ananiline.

5-An inlet passage having an inlet for introducing the liquid at one end and a discharge passage having an outlet for discharging the liquid out of the system are formed at one end, and the inlet passage and the discharge passage are connected to each other. At the other end of each nozzle, an intersection is formed by forming an intersection at the intersection, and an opening that opens toward the substrate is provided at the intersection, and a liquid that has come into contact with the substrate via the opening is formed. A nozzle having pressure control means for controlling a difference between the pressure of the liquid in contact with the substrate and the atmospheric pressure so as not to flow out of the discharge passage; 5. The production / recovery system tool for an endohedral fullerene according to any one of claims 1 to 4, wherein the dissolving liquid outlet and the outlet are connected together with the inlet and the inlet.

6. A means for applying ultrasonic waves to the solution is provided. Manufacturing and recovery system rules for the included fullerenes listed above.

7. The encapsulation according to claim 5 or 6, wherein a switching valve is provided downstream of the dissolving liquid inlet, one of the switching valves is connected to the dissolving liquid, and the other is connected to the washing liquid. Fullerene manufacturing · Collection system tool.

8. The encapsulation according to any one of claims 1 to 7, wherein a cleaning chamber for cleaning the substrate after dissolution is provided between the film formation chamber and the dissolution chamber. Fullerene manufacturing and collection system tools.

9. The production / recovery system tool for endohedral fullerenes according to any one of claims 1 to 8, wherein a column for liquid chromatography is connected to the dissolution chamber.

10. The tool for producing and recovering endohedral fullerene according to claim 9, wherein a component analyzer is connected downstream of the column.

11. The tool for producing and recovering endohedral fullerenes according to claim 10, wherein the power ram and the component analyzer are arranged in the vacuum chamber.