JP5190194B2 - Purification equipment - Google Patents

Description

  The present invention relates to a purification apparatus such as sublimation or distillation for purifying and collecting a substance, and more particularly to an apparatus for vaporizing and purifying a substance.

  A light-emitting element that has a layer containing an organic compound material between a pair of electrodes and emits light by passing an electric current between the electrodes has features such as a thin, lightweight, and flexible structure, and is considered to be a promising next-generation display. ing. In addition, since it is a self-luminous type, it is said that it has no problem of viewing angle and the like and has excellent visibility compared with a liquid crystal display (LCD), and has been actively developed.

  The basic structure of a light-emitting element is a structure having a layer containing an organic compound material between a pair of electrodes. The organic compound material used for the light-emitting element affects the characteristics and durability of the light-emitting element, and thus a high-purity material is required, and is generally purified using sublimation purification or the like.

For example, in Patent Document 1, a storage container for storing an organic material and a collection tube for capturing the purified organic material are arranged inside a glass tube, and a sublimation purification is performed by adding a temperature gradient to the glass tube. , And its method. Patent Document 2 discloses a sublimation tube and a sublimation purification apparatus that prevent contamination of the sublimation purification apparatus, reduce a reduction in work efficiency due to cleaning of the apparatus, and control the sublimation speed.
JP 2003-95992 A JP 2005-111303 A

  However, Patent Document 1 does not particularly take into consideration the organic material storage container and the collection tube for capturing the sublimated organic material, or the relationship between the storage container and the collection tube. Therefore, measures to separate and hold the sample and target substance, or to sublimate the organic material to the glass tube outside the collection tube, and to purify the purified organic material with high purity and high yield were not sufficient. .

  Moreover, in patent document 2, the sample chamber and the sublimation purified product collection part are provided in one sublimation tube, the glass diameter is filled in the part which made the pipe diameter between both small, and a sample chamber and the sublimation purified product collection part. Are separated. However, in the configuration of Patent Document 2, it is particularly difficult to clean the sample chamber and it is difficult to handle.

  Further, Patent Document 2 shows a sublimation tube in which a plurality of sublimation tube parts are joined by sliding in FIG. When a lubricant such as grease is used for such a sliding portion, it may be mixed with the purified product at the collecting part, and the purity of the purified product may be lowered. Further, when the purified product with reduced purity was excluded and recovered, the yield was lowered. On the other hand, when a lubricant is not used for the rubbing site, the rubbing site is difficult to come off, making it difficult to collect the purified product.

  The present invention has been made in view of such problems, and an object of the present invention is to provide a purification apparatus that can purify a target substance purified with high purity in a high yield and is easy to handle. .

  Another object of the present invention is to provide a purifier capable of preventing a purification apparatus from being contaminated and purifying a target substance purified with a high purity in a high yield.

  In the present invention, a plurality of purification tubes are arranged in a purification unit, and one purification tube is loosely fitted to another adjacent purification tube, whereby a target substance purified with high purity can be purified with high yield. It is the refinement | purification apparatus characterized by these. In this specification, the loose fit is a fit in which one refinement tube is fitted into another adjacent refinement tube, and the fitted one slides freely, that is, the fitted state has play. It means that it is in a fit state. That is, the state of rubbing is not included.

  The present invention includes a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, and a temperature adjusting unit that is provided in the vicinity of the purification unit and applies a temperature gradient to the purification unit. The purification unit includes a first purification tube and a second purification tube, and the first purification tube is loosely fitted to an adjacent second purification tube.

Further, the present invention includes a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, and a temperature adjustment unit that is provided in the vicinity of the purification unit and applies a temperature gradient to the purification unit. The purification section includes a first purification tube and a second purification tube, and one end of the first purification tube is loosely fitted to one end of the adjacent second purification tube. When the tube outer diameter of one end of the first purification tube is d ₂ and the tube inner diameter of one end of the second purification tube is e ₁ , the relationship of e ₁ > d ₂ is satisfied. It is a purification device with one of its features.

In addition, the present invention has a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, and a temperature adjusting unit that is provided in the vicinity of the purification unit and applies a temperature gradient to the purification unit, The purification unit includes a first purification tube and a second purification tube, and one end portion of the first purification tube is loosely fitted to one end portion of the adjacent second purification tube, The tube outer diameter at one end of the first purification tube is d ₂ , the tube inner diameter at one end of the second purification tube is e ₁ , and the tube inner diameter of the central region of the second purification tube is c _1. The refining apparatus is characterized by having a relationship of c ₁ > e ₁ > d ₂ .

In addition, the present invention has a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, and a temperature adjusting unit that is provided in the vicinity of the purification unit and applies a temperature gradient to the purification unit, The purification unit includes a first purification tube and a second purification tube, and one end portion of the first purification tube is loosely fitted to one end portion of the adjacent second purification tube, The tube outer diameter at one end of the first purification tube is d ₂ , the tube inner diameter at one end of the second purification tube is e ₁ , and the tube inner diameter of the central region of the second purification tube is c _1. when the tube inner diameter of the other end of the second purification tube was _{b 1,} e 1> _{d 2,} and _c 1> _{e 1,} that one of said having and _c 1> _{b 1} the relationship Purification equipment.

In addition, the present invention has a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, and a temperature adjusting unit that is provided in the vicinity of the purification unit and applies a temperature gradient to the purification unit, The purification unit includes a first purification tube and a second purification tube having a convex portion on the inner wall, and one end of the first purification tube is one end of the adjacent second purification tube. The outer diameter of one end of the first purification tube is d ₂ , the inner diameter of one end of the second purification tube is e ₁ , and the center of the second purification tube is the inner tube diameter region c1, when the height of the protrusion provided on the inner wall of the second purification tube was _{f 1,} in that it has e 1> _{d 2,} and _{c 1> f 1>} 0 the relationship It is a purification device with one of its features.

In addition, the present invention has a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, and a temperature adjusting unit that is provided in the vicinity of the purification unit and applies a temperature gradient to the purification unit, The purification unit includes a first purification tube and a second purification tube having a convex portion on the inner wall, and one end of the first purification tube is connected to one end of the adjacent second purification tube. The outer diameter of one end of the first purification tube is d ₂ , the inner diameter of one end of the second purification tube is e ₁ , and the central region of the second purification tube is loosely fitted. the inner tube diameter a c _1, the height of the protrusion provided on the inner wall of the second purification tube f _1, when the tube inner diameter of the second end of the second purification tube was b _1, e ₁ It is a purification apparatus characterized by having a relationship of> d ₂ , c ₁ > e ₁ , c ₁ > b ₁ , and c ₁ > f ₁ > 0.

  Further, the present invention is characterized in that it has a gas supply means provided in the vicinity of one end of the purification section, and a vacuum exhaust means provided in the vicinity of the other end of the purification section. This is a refining device.

The present invention includes a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, a temperature adjusting unit that is provided in the vicinity of the purification unit, and that imparts a temperature gradient to the purification unit, and one of the purification units A gas supply means provided in the vicinity of the other and a vacuum exhaust means provided in the vicinity of the other of the purification section, the purification section comprising a first purification pipe and a second purification pipe. One end portion of the first purification tube is loosely fitted to one end portion of the adjacent second purification tube, and the outer diameter of one end portion of the first purification tube is d ₂ , The purification apparatus is characterized by having a relation of e ₁ > d _{2 where} the pipe inner diameter of one end of the second purification pipe is e ₁ .

The present invention also provides a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, a temperature adjusting unit that is provided in the vicinity of the purification unit, and that provides a temperature gradient to the purification unit, and one of the purification units. Gas supply means provided in the vicinity of the end of the purification section, and vacuum evacuation means provided in the vicinity of the other end of the purification section, the purification section comprising the first purification pipe and the first purification pipe. And one end of the first purification tube is loosely fitted to one end of the adjacent second purification tube, and one end of the first purification tube When the outer diameter of the tube is d ₂ , the inner diameter of one end of the second purification tube is e ₁ , and the inner diameter of the central region of the second purification tube is c ₁ , c ₁ > e ₁ > d _It is a refiner characterized by having a relationship of ₂ .

The present invention includes a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, a temperature adjusting unit that is provided in the vicinity of the purification unit and that imparts a temperature gradient to the purification unit, and one of the purification units. A gas supply means provided in the vicinity of the end, and a vacuum exhaust means provided in the vicinity of the other end of the purification section. The purification section includes the first purification pipe and the second purification section. And one end portion of the first purification tube is loosely fitted to one end portion of the adjacent second purification tube, and one end portion of the first purification tube is outside the tube. The diameter is d ₂ , the inner diameter of one end of the second purification pipe is e ₁ , the inner diameter of the central area of the second purification pipe is c ₁ , and the other end of the second purification pipe is the pipe when an inner diameter set to _{b 1, e 1> d 2} , a and _{c 1> e} 1, and _c 1> 1 bract purified apparatus characterized by having a _{b 1} the relationship.

The present invention includes a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, a temperature adjusting unit that is provided in the vicinity of the purification unit and that imparts a temperature gradient to the purification unit, and one of the purification units. A gas supply means provided in the vicinity of the end, and a vacuum exhaust means provided in the vicinity of the other end of the purification unit. The purification unit has a first purification pipe and an inner wall. A second purification pipe having a convex portion, and one end of the first purification pipe is loosely fitted to one end of the adjacent second purification pipe. The outer diameter of the end of the second purification tube is d ₂ , the inner diameter of the second purification tube is e ₁ , the inner diameter of the central region of the second purification tube is c ₁ , A refining device having a relationship of e ₁ > d ₂ and c ₁ > f ₁ > 0, where f ₁ is the height of the convex portion provided on the inner wall.

The present invention includes a purification unit that vaporizes and purifies a substance, a fixing unit that fixes the purification unit, a temperature adjusting unit that is provided in the vicinity of the purification unit and that imparts a temperature gradient to the purification unit, and one of the purification units. A gas supply means provided in the vicinity of the end, and a vacuum exhaust means provided in the vicinity of the other end of the purification unit. The purification unit has a first purification pipe and an inner wall. A second purification pipe having a convex portion, and one end of the first purification pipe is loosely fitted to one end of the adjacent second purification pipe. The outer diameter of the end of the second purification tube is d ₂ , the inner diameter of the second purification tube is e ₁ , the inner diameter of the central region of the second purification tube is c ₁ , When the height of the convex portion provided on the inner wall is f ₁ and the inner diameter of the second end of the second purification tube is b ₁ , e ₁ > d ₂ , c ₁ > e ₁ , and c _{1> b 1,} One c _1> f 1> is one purified apparatus characterized by having a ₀ becomes relationship.

  Moreover, what is necessary is just to use inert gas, such as argon and nitrogen, as gas supplied from a gas supply means by this invention. Further, a vacuum pump or the like may be used as the vacuum exhaust means.

  Moreover, a tube may be used as the fixing means used in the purification apparatus of the present invention, and the purification unit may be fixed by inserting the purification unit into the tube as the fixing unit.

  In addition, a glass tube or a quartz tube may be used as a purification tube used in the purification apparatus of the present invention.

  In addition, the substance refine | purified by this invention shall contain not only an organic material but the substance which can be refine | purified by vaporization in a category. In the present specification, purification refers to the use of the three-state change of substances, and includes subdivision purification and distillation. In other words, in addition to purification utilizing the phenomenon that a solid becomes a gas directly without passing through a liquid at normal temperature and normal pressure, and conversely, a solid that becomes a solid at normal temperature and normal pressure. It also includes purification using the phenomenon that gas becomes a gas through a liquid, and conversely the phenomenon that a gas becomes a solid through a liquid. Therefore, the target substance includes not only a substance that sublimes or solidifies as a solid but also a substance that condenses as a liquid. In the present specification, sublimation or solidification as a solid is referred to as precipitation.

  By adopting the structure of the present invention, the target substance can be purified with high yield. Moreover, contamination of the apparatus can be prevented, and work efficiency can be improved. Furthermore, handling of the purification apparatus can be simplified.

  Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings. However, the present invention is not limited to the following description, and it is easily understood by those skilled in the art that modes and details can be variously changed without departing from the spirit and scope of the present invention. Therefore, the present invention should not be construed as being limited to the description of the embodiments below. Note that in the structures of the present invention described below, the same reference numerals are used in common in different drawings.

(Embodiment 1)
The present invention relates to an apparatus and a purification tube for purifying a target product. Hereinafter, a specific description will be given with reference to FIGS. 1, 2, and 3.

  FIG. 1 is a cross-sectional view schematically showing a purification apparatus of the present invention. 2 and 3 are a perspective view and a cross-sectional view of a purification unit which is a part of the purification apparatus of the present invention.

  The purification apparatus 100 of the present invention includes a purification unit 110 for vaporizing a sample and purifying and recovering a target substance, a temperature control means 120 for vaporizing and purifying the sample, and a fixing for fixing the purification unit. Means 130. Note that in this specification, a sample refers to a substance in which a target substance, impurities, a solvent, and the like are mixed.

  As shown in FIG. 1, the temperature adjustment means 120 is provided in the vicinity of the purification unit 110, and the purification unit 110 is given a temperature gradient by the temperature adjustment means 120. Specifically, the purification unit 110 is provided with a temperature gradient so that at least the target substance can be isolated, purified, and recovered, such as a temperature range where the sample is completely vaporized and a temperature range where the target substance is precipitated or condensed. The temperature gradient may be such that the temperature decreases in one direction, or the center of the purification unit 110 may be a high temperature region, and the temperature may decrease in both directions.

  The sample vaporized in the purification unit 110 diffuses toward the lower vapor pressure. Vapor pressure generally increases with increasing temperature. Therefore, the vaporized sample diffuses toward the lower temperature according to the temperature gradient. That is, the vaporized sample is condensed as a liquid or deposited as a solid at a temperature at which the state changes to a liquid or a solid according to the pressure and temperature gradient in the purification tube. Note that the temperature region where the sample vaporizes is the hottest region of the purification unit 110.

  As the temperature control means 120, a heater, a hot plate, or the like may be used, and it may be provided in the vicinity of the purification unit 110 (for example, in the vicinity of a purification tube for vaporizing a sample). Although FIG. 1 shows a case where only one temperature adjusting means 120 is provided in the vicinity of the purification unit 110, the present invention is not limited to this, and a plurality of temperature adjusting means 120 may be provided. The installation location and the number of the temperature adjusting means 120 can be changed as appropriate. Moreover, it is preferable to provide a heat retaining means, a protective cover surrounding the purification unit 110, and the like so that the temperature gradient applied to the purification unit 110 can be maintained.

  When the temperature of the purification unit 110 is adjusted, it is necessary to set the temperature region such as the temperature at which the sample is vaporized and the temperature at which the target substance is precipitated or condensed to an optimum temperature. This may be set by examining the decomposition point, sublimation point or boiling point of the target substance.

  Next, the refinement | purification part 110 is demonstrated in detail using FIG. 2, FIG. 2A is a perspective view of two purification pipes included in the purification unit 110, and FIG. 2B corresponds to a cross section of a portion represented by a broken line ML in FIG. 2A. 3A, the second purification tube 202 and the loose fitting portion between the second purification tube 202 and the first purification tube 201 in the purification unit 110 shown in FIG. 2A are enlarged. The figure is shown.

  The purification unit 110 is configured by connecting at least two or more purification tubes. The number of purification tubes arranged in the purification unit 110 can be changed as appropriate. Specifically, at least two or more purification tubes including a first purification tube 201 for arranging a sample and a second purification tube 202 for collecting a target substance that has been purified and deposited or condensed are provided. It only has to have. The end of the purification tube in which the sample is arranged or the end on the side close to the purification tube in which the sample is arranged is arranged so as to be loosely fitted to the end of another adjacent purification tube. That is, in this embodiment, the first purification tube 201 in which the sample is arranged is arranged so as to be loosely fitted to the second purification tube 202.

  A temperature gradient such as a solid arrow shown in FIG. The solid line shown in FIG. 2 indicates that the temperature is decreasing in one direction from right to left with respect to the paper surface. The highest temperature in the purification unit 110 is applied to the place where the first purification tube 201 for arranging the sample is arranged.

  In the present embodiment, a second purification tube 202 for recovering the target substance is disposed adjacent to the first purification tube 201. The present invention is not limited to this, and one or more purification tubes may be arranged between the first purification tube 201 and the second purification tube 202. The region where the second purification tube 202 for collecting the target substance is disposed may be at a temperature at which the target substance examined in advance is deposited or condensed. That is, a temperature at which the target substance is deposited or condensed may be applied to the center of the second purification tube 202.

  The basic structure of the first purification tube 201 and the second purification tube 202 is a hollow tube. Further, the first purification tube 201 and the second purification tube 202 are at least at the end of the loose fitting portion with the adjacent purification tube so that the vaporized sample (including the target substance and impurities) can pass through. An opening is provided. As the purification tube, it is preferable to use a hollow tube made of glass, quartz or the like. In addition, the present invention is not limited to this, and any material that does not react with the sample, the target substance, and impurities, and that can withstand the operating temperature without being mixed into the target substance when the target substance is recovered may be used. In the present embodiment, openings are provided at both ends of the first purification tube 201 and the second purification tube 202. Of course, in the 1st refinement | purification pipe | tube 201, one edge part which is not loosely fitted to another refinement | purification pipe | tube, or one edge part of the 2nd refinement | purification pipe | tube 202 may be closed. In the case of purification at normal pressure, if the purification unit 110 is sealed and heated, the pressure in the tube may increase, which is extremely dangerous. Therefore, either end must be open.

  As shown in FIG. 3A, the first purification tube 201 has a first end portion, a central portion 321, and a second end portion 331. Similarly, the second purification tube 202 has regions of a first end portion 312, a central portion 322, and a second end portion 332. At least in the first purification pipe 201 and the second purification pipe 202, the second end 331 of the first purification pipe 201 and the first end 312 of the second purification pipe 202, which are loose fitting parts, are provided. Is provided with an opening. In FIG. 3A, the first end of the first purification tube 201 is omitted.

  In addition, a cross-sectional view perpendicular to the flow path of the vaporized sample at the second end 332 of the second purification tube 202 is shown in FIG. 3B, and at the center 322 of the second purification tube 202, A cross-sectional view in the direction perpendicular to the flow path of the vaporized sample is shown in FIG. Furthermore, a cross-sectional view perpendicular to the flow path of the vaporized sample at the second end 331 of the first purification tube 201 is shown in FIG. 3D, and the first end of the second purification tube 202 is shown. FIG. 3E shows a cross-sectional view perpendicular to the flow path of the vaporized sample at 312.

At the second end 332 of the second purification tube shown in FIG. 3 (B), the diameter of the cross section that does not include the thickness of the tube and the tube inner diameter b _1, the diameter of the cross section including the thickness of the tube outside the tube and the diameter _{b 2.} Further, extravascular in the central portion 322 of the second purification tube 202 shown in FIG. 3 (C), and the diameter of the cross section that does not include the thickness of the tube and the tube inner diameter c _1, the diameter of the cross section including the thickness of the tube the diameter _{c 2.} Further, at the second end 331 of the first purification tube 201 shown in FIG. 3 (D), and the diameter of the cross section that does not include the thickness of the tube and the tube inner diameter d _1, the diameter of the cross section including the thickness of the tube the the outer diameter _{d 2.} Further, at the first end 312 of the second purification tube 202 shown in FIG. 3 (E), the diameter of the cross section that does not include the thickness of the tube and the tube inner diameter e _1, the diameter of the cross section including the thickness of the tube the the outer diameter _{e 2.} The cross section having the tube inner diameter b ₁ , the cross section having the tube inner diameter c _1, and the cross section having the tube inner diameter e ₁ are preferably concentric circles because they are easy to arrange.

  In the second purification tube 202, the thickness of the second end 332, the thickness of the central portion 322, and the thickness of the first end 312 are used to maintain the strength of the purification tube or the temperature. Are preferably the same to prevent non-uniformity. Similarly, also in the first purification pipe 201, the thickness of the second end 331, the thickness of the central part 321 and the thickness of the first end keep the strength of the purification pipe, Or in order to prevent that temperature becomes non-uniform | heterogenous, it is preferable to make it the same.

The first purification pipe 201 is loosely fitted to the adjacent second purification pipe 202 as shown in FIGS. 2 and 3A. The present invention is characterized in that one purification tube is loosely fitted into an opening of another adjacent purification tube, and the end of the other purification tube on the side where one purification tube is loosely fitted. The first inner diameter of the first purification pipe is loosely fitted to the second purification pipe by making the inner diameter of the pipe larger than the outer diameter of the pipe at the end of the one purification pipe that is loosely fitted to the other purification pipe. Can do. In the present embodiment, the first purification tube 201 and the second purification tube 202 are adjacent to each other, and the second end portion 331 of the first purification tube 201 is the first of the second purification tube 202. It is loosely fitted in the opening of the end portion 312. That is, the innermost tube inner diameter e ₁ at the first end 312 of the second purification tube 202 is set to be larger than the outermost tube outer diameter d ₂ at the second end 331 of the first purification tube 201. Also, the first purification tube can be loosely fitted to the second purification tube. As a result, a structure that prevents the sample vaporized from the loose fitting portion from flowing out can be obtained. In addition, it is preferable to satisfy | fill following Numerical formula (1).

  More preferably, the following mathematical formula (2) is satisfied.

最も好ましくは、下記数式（３）を満たすと良い。

Most preferably, the following mathematical formula (3) is satisfied.

  As in the present invention, the first refining tube 201 is loosely fitted to the second refining tube 202, so that the handling becomes simpler than the structure in which the sliding portions are provided. This is because the refined tubes are easily fixed to each other when the substance is deposited on the sliding portion, whereas the loose fitting state has play so that it is difficult to be fixed.

In addition, the present invention is also characterized in that one purification tube has a structure that prevents leakage of a sample and a target substance from the purification tube in a portion loosely fitted into an opening of another adjacent purification tube. Therefore, in another refinement | purification pipe | tube, the pipe internal diameter of the center vicinity is larger than the pipe internal diameter in the edge part by the side which loosely fits one refinement | purification pipe | tube. In this embodiment, the loose fitting portion between the first purification pipe 201 and the second purification pipe 202 has a structure that prevents leakage of the sample and the target substance. In particular, the structure has a remarkable effect when the target substance is condensed as a liquid. Specifically, in the second purification pipe 202, the pipe inner diameter c ₁ of the central portion 322 is larger than the pipe inner diameter e ₁ of the first end 312, and the first end 312 of the second purification pipe 202 is used. The tube inner diameter e ₁ is larger than the tube outer diameter d ₂ of the second end 331 of the first purification tube 201.

  Therefore, in the present invention, the first purification tube is loosely fitted to the second purification tube to prevent leakage of a sample or a target substance from the loose fitting portion. There is a need.

  In addition, in order to make it a structure which prevents the leakage of a sample or a target substance from a loose fitting part, it is preferable to satisfy | fill following numerical formula (5).

More preferably, the following mathematical formula (6) is satisfied.

  Most preferably, the following formula (7) and the following formula (8) are satisfied.

  In the loose fitting portion, the first purification pipe 201 and the second purification pipe 202 may be in contact with each other or there may be a gap. Further, the first purification tube 201 only needs to enter the first end 312 of the second purification tube 202 even slightly. It is preferable that the first purification tube 201 and the second purification tube 202 are inserted until they come into contact with each other.

Furthermore, according to the present invention, one purification tube is loosely fitted into an opening of another adjacent purification tube, and the one purification tube or the other purification tube itself has a structure in which a sample or a target substance is difficult to leak. Features. Therefore, one refinement tube or another refinement tube is characterized in that the inner diameter of the tube near the center is the largest. In this embodiment, in the second purification tube 202, tube inner diameter _{c 1} of the central portion 322 is larger than the tube inner diameter _{b 1} of the first tube inner diameter _{e 1} of the end portion 312 and a second end 332 It is characterized by that. The present invention is characterized by satisfying the above-described mathematical formula (1) and satisfying the following mathematical formula (9) and the following mathematical formula (10).

  In addition, in order to make the sample and the target substance not leak from one purification tube, it is preferable to satisfy the following formula (11) and the following formula (12) as well as the above formula (2) or formula (3). .

  More preferably, it satisfies the above-described mathematical formula (2) or (3) and preferably satisfies the following mathematical formula (13) and the following mathematical formula (14).

  This structure is particularly effective when the target substance is condensed as a liquid.

  The present invention is also characterized in that no sliding portion is provided in the loose fitting portion. By not providing the sliding portion in the loose fitting portion between the purified tubes, it is not necessary to use a lubricant or the like, and the possibility of lowering the purity of the target substance by the lubricant or the like is reduced. Moreover, when removing a refinement | purification pipe | tube, the sample and a target substance adhere to a rubbing part, the problem that it becomes impossible to remove because it hardens | cures can be prevented, and handling of a refiner | purifier can be simplified.

  As in the present invention, by making a structure in which the adjacent purification tubes, for example, the first purification tube 201 are loosely fitted to the second purification tube 202, the vaporized sample or the like flows out from the joint between the purification tubes. Can be prevented. Therefore, the target substance can be obtained with a high yield.

  Furthermore, with the configuration of the present invention, particularly when the target substance condenses as a liquid, the sample is mixed into adjacent purification tubes, for example, the first purification tube 201 to the second purification tube 202, or the second It is possible to prevent the target substance from being mixed into the first purification tube from the first purification tube 202, which is very effective. Therefore, a target substance with high purity can be obtained.

  Further, with the configuration of the present invention, one purification tube, for example, the first purification tube 201 or the second purification tube 202 itself can be configured to prevent leakage of the sample or the target substance. Therefore, the target substance can be obtained with a high yield.

  The central portion 321 of the first purification tube 201 and the central portion 322 of the second purification tube 202 may be a cylindrical hollow tube having a uniform tube inner diameter and a tube outer diameter. Note that the present invention is not limited to this, and the central portion may have regions with various tube inner diameters. However, it is better to have a region with a certain tube inner diameter and tube outer diameter to some extent. 110 is easy to fix.

The shape of the second end 331 of the first purification tube 201 may be a shape that continuously decreases from the center 321 to the outermost end of the second end 331. Alternatively, the shape may be such that the outer diameter of the tube is continuously reduced up to a certain point, and the outer shape of the tube may be increased from a certain point, or vice versa. Moreover, it is good also as a shape which has an area | region where a fixed pipe outer diameter continues. At least, in the loosely fitted portion of the first purification tube 201 and the second purification tube 202, tube outer diameter d ₂ of the top end portion of the second end 331 of the first purification tube 201, a second purification What is necessary is just to be smaller than the inner diameter e ₁ of the outermost end of the first end 312 of the tube 202. In the first purification tube 201, the shape of the cross section in the direction perpendicular to the flow path of the vaporized sample is not particularly limited.

  In order to prevent the sample from leaking from the opening of the second end 331 of the first purification tube 201, it is preferable to satisfy the above-described formula (4).

  The second end 331 of the first purification pipe 201 is preferably given a curvature. By adopting such a shape, it is possible to prevent the vaporized sample from flowing out from the joint or the sample from being mixed into the adjacent purification tube. In particular, contamination when the sample or the target substance is a liquid can be prevented. In addition, the target substance precipitated as a solid can be easily recovered with a spoon. Furthermore, the strength of the refinement tube is increased by having a curvature, and the refinement tube itself can be made difficult to break.

  The second end 332 of the second purification tube 202 is not particularly limited, but it is preferable to satisfy the above formulas (9) and (10) in order to prevent the sample from leaking. . Moreover, it is preferable to satisfy the above formula (9) and formula (10) and to have the same shape as the second end 331 of the first purification pipe 201. In addition, the shape may be the same as that of the central portion 322 except when used in a purification apparatus for condensing the target substance as a liquid. If the second end 332 of the second purification tube 202 is not loosely fitted to any other purification tube, the opening at the end may not be provided.

The shape of the first end 312 of the second purification tube 202 may be such that the inner diameter of the tube continuously decreases from the central portion 322 to the outermost end of the first end 312. Alternatively, the shape may be such that the inner diameter of the tube continuously decreases up to a certain point, and the shape of the inner diameter of the tube may be increased from a certain point, or vice versa. Moreover, it is good also as a shape with the area | region where a fixed pipe | tube internal diameter continues. At least in the loose fitting portion between the first purification tube 201 and the second purification tube 202, the inner diameter e ₁ of the outermost end of the first end 312 of the second purification tube 202 has the first purification tube. It suffices if it is larger than the tube outer diameter d ₂ at the end of the second end 331 of 201. In the second purification tube 202, the shape of the cross section in the direction perpendicular to the flow path of the vaporized sample is not particularly limited.

  Further, in order to obtain a structure that prevents leakage of the target substance from the opening of the first end 312 of the second purification pipe 202, it is preferable to satisfy the above-described formula (4).

  It is preferable that the first end 312 of the second purification pipe 202 has a curvature. By adopting such a shape, it is possible to prevent the vaporized sample from flowing out from the joint or the sample from being mixed into the adjacent purification tube. In particular, contamination when the sample is liquid can be prevented. Moreover, the strength of the refinement tube can be increased by providing the curvature, and the refinement tube itself can be made difficult to break.

  In addition, the first end of the first purification tube 201 may have the same shape as the first end 312 of the second purification tube 202. Moreover, as long as no other purification pipes are loosely fitted, the same shape as the central portion 321 may be used. In the first purification tube 201, the sample is less likely to leak from the first purification tube 201 when the tube inner diameter of the central portion 321 is larger than the tube inner diameter of the first end. That is, in the first purification tube, when the tube inner diameter of the central portion 321 is maximized, it is possible to make the sample difficult to leak from the first purification tube 201. Note that the opening at the extreme end may not be provided.

  As described above, in the present invention, it is not always necessary to arrange a purification tube for arranging a sample and a purification tube for recovering the purified target substance adjacent to each other. Therefore, the purification tube for arranging the sample is the first purification tube 201 of the present embodiment, the second purification tube 202 is disposed adjacent to the first purification tube 201, and the second purification tube 201 is disposed. A purification tube for recovering the target substance may be disposed adjacent to the tube 202. Further, two or more purification tubes may be arranged between a purification tube for arranging the sample and a purification tube for collecting the target substance. Further, a purification tube may be arranged adjacent to the purification tube for collecting the target substance. Note that adjacent purification tubes are loosely fitted as described in the first purification tube 201 and the second purification tube 202 of this embodiment. At this time, it arrange | positions so that the edge part of the refinement | purification pipe | tube which has arrange | positioned the sample, or the edge part near the refinement | purification pipe | tube which has arrange | positioned the sample may be loosely fitted to the edge part of another adjacent refinement | purification tube.

  In the present invention, one purification tube may be loosely fitted to another adjacent purification tube, and the adjacent purification tubes do not have to have the same shape. In the present invention, one purification tube may be loosely fitted to another adjacent purification tube, and the first end portion, the central portion, and the second end portion are perpendicular to the flow path of the vaporized sample. The cross section may not be concentric. It should be noted that it is easier to place the first end portion, the central portion, and the second end portion having concentric cross sections perpendicular to the flow path of the vaporized sample.

  In the refining device 100 of the present invention, if both ends of the purifying unit 110 are closed and sealed, it is very dangerous when heated at normal pressure. Therefore, when using this refinement | purification apparatus at a normal pressure, you have to provide the opening which leads to the external world at least in the refinement | purification part 110 at one place.

  Next, the fixing means 130 shown in FIG. 1 may be any means that can hold and fix at least a state in which one purification pipe is loosely fitted in an adjacent purification pipe. Preferably, the purification unit 110 may be a means that can be held and fixed so as to be horizontal in the long axis direction. As the fixing means 130, each purification tube constituting the purification unit 110 may be fixed with a clamp or the like, or the purification tube may be arranged on a horizontal base. Moreover, you may arrange | position in pipes, such as glass which has a pipe inner diameter larger than the pipe outer diameter of the refinement | purification pipe | tube which comprises the refinement | purification part 110. FIG.

  As described above, with the configuration of the present invention, the target substance can be obtained in high yield. Further, it is possible to prevent leakage of a sample, a target substance, and the like from the loose fitting portion. As a result, contamination of the refining device can be prevented and work efficiency can be improved. In addition, a purification apparatus that is easy to handle can be provided.

(Embodiment 2)
In the present embodiment, an example of the shape of the purification tube constituting the purification unit will be described with reference to FIG. 4B corresponds to a cross-sectional view in a direction parallel to the flow path of the vaporized sample of the purification unit 110 illustrated in FIG.

  FIG. 4A shows a structure that further prevents leakage of the target substance from the purification unit shown in FIG. 4B. Specifically, in the loose fitting portion between the first purification tube 401 and the second purification tube 402 constituting the purification unit 410, an opening provided in the first end 412 of the second purification tube 402, the first A cross section in a direction perpendicular to the flow path of the vaporized sample in the opening provided in the second end 431 of the first purification tube 401 and the central portion 422 of the second purification tube 402 that are loosely fitted to the first end 412 Is not a concentric circle.

In the case of FIG. 4A as well, since the first purification tube 401 is loosely fitted to the second purification tube 402, it is necessary to satisfy Equation (1) described above. Further, in order to obtain a structure that prevents leakage of a sample or a target substance from the loose fitting portion, the above-described mathematical formula (4) may be satisfied. Furthermore, in order to obtain a structure in which the sample or the target substance does not leak from the purification tube itself, the above-described mathematical formulas (9) and (10) may be satisfied. As indicated by broken lines in FIG. 4 (A), the tube inner diameter of the second end 432 of the second purification tube 402 and _{b 1,} the inner tube diameter of the central portion 422 and _{c 1.} Further, the outer diameter of the tube 431 at the second end of the first purification tube 401 is d _2, and is provided at the outermost portion of the first end 412 of the second purification tube 402. the inner tube diameter of the opening to e _1.

The cross section having the tube inner diameter b ₁ and the cross section having the tube inner diameter e ₁ are concentric, and the center of the cross section having the tube inner diameter b ₁ and the cross section having the tube inner diameter e ₁ is the center of the cross section having the tube inner diameter c _1. It is preferable to arrange it further upward. By arranging in this way, it becomes possible to arrange many samples in the purification tube.

  4A, in the loose fitting portion, the maximum distance between the inner edge of the second purification tube 402 and the outer edge of the outermost end of the first purification tube 401 loosely fitted ( y) becomes larger and the target substance can be made difficult to leak. In particular, when the target substance condenses as a liquid, the effect is remarkable, and there is no possibility of mixing into adjacent purification tubes.

  Note that this embodiment mode can be combined with the structure of Embodiment Mode 1.

(Embodiment 3)
In the present embodiment, an example of the shape of the purification tube constituting the purification unit will be described with reference to FIG.

  FIG. 5A shows a structure in which a refining portion is provided at one place on the inner wall near the center of the refining tube in the refining portion 110 shown in FIG. It is the same structure. Therefore, similarly to FIG. 4B, the first purification tube 5001 is loosely fitted to the adjacent second purification tube 5002, and it is necessary to satisfy the above-described formula (1). Similarly to FIG. 4B, the above-described mathematical formulas (4), (9), and (10) may be satisfied as necessary.

In FIG. 5A, the first purification tube 5001 has a first end portion, a center portion 5021, and a second end portion 5031. Similarly, the second purification tube 5002 also has a first end portion 5012, a central portion 5022, and a second end portion 5032. As indicated by broken line in FIG. 5 (A), the tube inner diameter of the second end 5032 of the second purification tube 5002 and _{b 1,} the inner tube diameter of the central portion 5022 and _{c 1.} The outer diameter of the _second end 5031 of the first purification pipe 5001 is d ₂ and the outer diameter of the first end 5012 of the second purification pipe 5002 is provided at the outermost end. the inner tube diameter of the opening to e _1.

FIG. 5A has a structure that prevents leakage of the sample and the target substance from the purification tube more than that shown in FIG. Specifically, a convex portion 5040 having a height f ₁ is provided on the inner wall near the central portion 5022 of the second purification tube 5002. That is, the convex part 5040 region (the pipe inner diameter continuously from the pipe inner diameter c ₁ to the apex of the convex part 5040) having a height (f ₁ ) smaller than the diameter (pipe inner diameter c ₁ ) of the other region of the central portion 5022. 1 area). Note that FIG. 5B is a cross-sectional view of a portion indicated by a broken line oo ′ in FIG. Therefore, the structure of the present invention satisfies the above formula (1) and also satisfies the following formula (15).

  In addition, Preferably it is good to satisfy | fill following numerical formula (16).

More preferably, the following mathematical formula (17) is satisfied.

  Most preferably, the following mathematical formula (18) is satisfied.

  With the structure as shown in FIG. 5A, the target substance is blocked by the convex portion 5040 provided on the inner wall in the vicinity of the central portion 5022 of the second purification tube 5002. As a result, the target substance or the like can be prevented from leaking from the loosely fitting portions of the first purification tube 5001 and the second purification tube 5002 or the tip portion of the second purification tube 5002.

  5A, the region between the convex portion 5040 and the first end portion 5012 and the region between the convex portion 5040 and the second end portion 5032 are Contamination (contamination) of the precipitated or agglomerated substances can be prevented. As a result, a target substance with higher purity can be obtained.

  Note that the position where the convex portion 5040 is provided is not limited to the position shown in FIG. 5A, and the convex portion 5040 may be provided closer to the first end portion 5012 or closer to the second end portion 5032. I do not care. The convex portion 5040 is preferably disposed on the lower surface side of the second purification tube 5002.

  Similarly, a convex portion may be provided on the inner wall near the central portion 5021 of the first purification pipe 5001. By providing a convex portion on the inner wall of the first purification tube 5001, leakage of a sample or the like from the loose fitting portion or the first purification tube 5001 can be prevented. In addition, the other purification tube is not loosely fitted to the first end portion side of the first purification tube 5001, or the second end 5032 side of the second purification tube 5002 is not loosely fitted to the other purification tube. For example, the opening may not be provided at the extreme end.

  FIG. 5C shows a structure in which a convex portion is provided at one place on the inner wall near the central portion 5122 of the purification pipe in the purification unit 410 shown in FIG. ). Therefore, similarly to FIG. 4A, the first purification pipe 5101 is loosely fitted to the adjacent second purification pipe 5102, and it is necessary to satisfy the above-described formula (1). Similarly to FIG. 4A, the above-described mathematical formulas (4), (9), and (10) may be satisfied as necessary.

In FIG. 5C, the first purification tube 5101 has a first end portion, a center portion 5121, and a second end portion 5131. Similarly, the second purification tube 5102 also has a first end portion 5112, a central portion 5122, and a second end portion 5132. As indicated by broken line in FIG. 5 (C), the tube inner diameter of the second of the second end portion 5132 of the purified tube 5102 and _{b 1,} the inner tube diameter of the central portion 5122 and _{c 1.} In addition, the outer diameter of the outermost portion of the second end portion 5131 of the first purification tube 5101 is d _2, and the outermost portion of the first end portion 5112 of the second purification tube 5102 is provided. the inner tube diameter of the opening to e _1.

FIG. 5C has a structure that prevents leakage of the sample and the target substance from the purification tube and the loose fitting portion, as compared with the structure shown in FIG. Specifically, a convex portion 5140 having a height f ₁ is provided on the inner wall near the central portion 5122 of the second purification pipe 5102. That is, the convex part 5140 region (the pipe inner diameter continuously from the pipe inner diameter c ₁ to the apex of the convex part 5140) having a height (f ₁ ) smaller than the diameter (tube inner diameter c ₁ ) of the other region of the central part 5122. 1 area). Note that FIG. 5D is a cross-sectional view of a portion represented by a broken line pp ′ in FIG. Therefore, the structure of the present invention satisfies the above formula (1) and also the above formula (15).

  Note that it is preferable to satisfy the above-described formula (16). More preferably, the ratio of the above-described equation (17), and most preferably, the ratio of the above-described equation (18) may be satisfied.

  With the structure shown in FIG. 5C, the target substance is blocked by the convex portion 5140 provided on the inner wall near the central portion 5122 of the second purification tube 5102. As a result, leakage of the target substance or the like can be prevented from the loose fitting portions of the first purification tube 5101 and the second purification tube 5202 or the tip portion of the second purification tube 5202. Further, similarly to FIG. 5A, confusion (contamination) of precipitated or aggregated substances can be prevented. As a result, a target substance with higher purity can be obtained.

  Note that the position where the convex portion 5140 is provided is not limited to the position shown in FIG. 5C, and the convex portion 5140 may be provided closer to the first end portion 5112 or closer to the second end portion 5132. I do not care. The convex portion 5140 is preferably disposed on the lower surface side of the second purification tube 5102.

  Similarly, a convex portion may be provided on the inner wall near the central portion 5121 of the first purification pipe 5101. By providing a convex portion on the inner wall of the first purification tube 5101, leakage of a sample or the like from the loose fitting portion or the first purification tube 5101 can be prevented. In addition, the other purification tube is not loosely fitted to the first end portion side of the first purification tube 5101 or the second end portion 5132 side of the second purification tube 5102 is not loosely fitted to the other purification tube. For example, the opening may not be provided at the extreme end.

  FIG. 5E shows a structure in which the refining section 110 shown in FIG. 5A is provided with one more protrusion on the inner wall near the center of the refining tube, that is, two protrusions on the inner wall near the center. Is. The two convex portions are provided to face each other. Except for the convex portions provided facing each other, the configuration is the same as that in FIG. 5A, and it is necessary to satisfy Equation (1) described above. Similarly to FIG. 5A, the above-described mathematical formulas (4), (9), and (10) may be satisfied as necessary.

Similarly to FIG. 5A, the first purification tube 5201 has a first end portion, a center portion 5221, and a second end portion 5231. Similarly, the second purification tube 5202 also has a first end portion 5212, a central portion 5222, and a second end portion 5232. As indicated by broken line in FIG. 5 (E), the tube inner diameter of the second end 5232 of the second purification tube 5202 and _{b 1,} the inner tube diameter of the central portion 5222 and _{c 1.} Further, the outer diameter of the uppermost end of 5231 of the second end of the first purification tube 5201 and _{d 2,} provided at the top end portion of the first end portion 5212 of the second purification tube 5202 the inner tube diameter of the opening to e _1.

Further, on the inner wall in the vicinity of the center portion 5222 of the second purification tube 5202, the convex portion of the height f ₁ are provided at two locations to face. That is, a convex region 5240 having two convex portions having a height (f ₁ ) smaller than the diameter (tube inner diameter c ₁ ) of the other region of the central portion 5222 (from the pipe inner diameter c ₁ to the apex of the convex portion). And a region in which the inner diameter of the tube continuously decreases. Incidentally, FIG. 5 (F) is a cross-sectional view of a portion represented by a broken line q-q 'in FIG. 5 (E), the the circular diameter of the cross section of the raised region 5240 and the tube inner diameter g _1. The structure of the present invention satisfies the above formula (1) and also satisfies the following formula (19).

  Note that the position where the convex region 5240 is provided is not limited to the position shown in FIG. 5E, and the convex region 5240 may be provided closer to the first end 5212 or closer to the second end 5232. It doesn't matter.

Incidentally, the inner tube diameter _{g 1} is smaller than the tube inner diameter _{c 1,} may preferably satisfy the following equation (20).

More preferably, the following mathematical formula (21) is satisfied.

  Most preferably, the following mathematical formula (22) is satisfied.

  Of course, you may provide a convex area | region similarly to the inner wall of central part 5221 vicinity of the 1st refinement | purification pipe | tube 5201. FIG. With the structure illustrated in FIG. 5E, leakage of a sample, a target substance, and the like from the loose fitting portion, the first purification tube 5201, and the second purification tube 5202 can be prevented. Further, similarly to FIG. 5A, it is possible to prevent the contamination of the precipitated or condensed material. As a result, a target substance with higher purity can be obtained. In addition, the other purification tube is not loosely fitted to the first end portion side of the first purification tube 5201, or the second end portion 5232 side of the second purification tube 5202 is not loosely fitted to the other purification tube. For example, it is not necessary to provide an opening at the end.

  FIG. 5G shows a structure in which, in the refining unit 410 shown in FIG. 5C, one more protrusion is provided on the inner wall near the center of the refining tube, that is, two protrusions are provided on the inner wall near the center. Is. Two convex portions are provided facing each other. The configuration is the same as that of FIG. 5C except for the convex portions provided to face each other. Therefore, it is necessary to satisfy the above formula (1). Moreover, what is necessary is just to satisfy | fill the above-mentioned Numerical formula (4), Numerical formula (9), and Numerical formula (10) as needed.

As in FIG. 5C, the first purification tube 5301 has a first end portion, a central portion 5321, and a second end portion 5331. Similarly, the second purification tube 5302 also has a first end portion 5312, a central portion 5322, and a second end portion 5332. As indicated by broken line in FIG. 5 (G), the tube inner diameter of the second end 5332 of the second purification tube 5302 and _{b 1,} the inner tube diameter of the central portion 5322 and _{c 1.} The outer diameter of the outermost end of the second end 5331 of the first purifying tube 5301 is d _2, and the outer end of the first end 5312 of the second purifying tube 5302 is provided at the outermost end. the inner tube diameter of the opening to e _1.

Further, on the inner wall in the vicinity of the center portion 5322 of the second purification tube 5302, the convex portion of the height f ₁ are provided at two locations to face. That is, a convex region 5340 having two convex portions having a height (f ₁ ) smaller than the diameter (tube inner diameter c ₁ ) of the other region of the central portion 5322 (from the pipe inner diameter c ₁ to the apex of the convex portion). And a region in which the inner diameter of the tube continuously decreases. Incidentally, FIG. 5 (H) is a sectional view of a portion represented by FIG dashed r-r of 5 (G) ', the circular diameter of the cross section of the raised region 5340 and the tube inner diameter g _1. The structure of the present invention satisfies the above formula (1) and also satisfies the above formula (13). Note that the position where the convex region 5340 is provided is not limited to the position shown in FIG. 5G, and the convex region 5340 may be provided closer to the first end portion 5312 or closer to the second end portion 5332. It doesn't matter.

As in the FIG. 5 (C), the tube inner diameter _{g 1} indicated by a broken line in FIG. 5 (E) is smaller than the tube inner diameter _{c 1.} It is preferable to satisfy the above formula (20), more preferably the above formula (21), and most preferably the above formula (22).

  Of course, you may provide a convex area | region similarly in the inner wall near the center part 5321 of the 1st refinement | purification pipe | tube 5301. FIG. With the structure illustrated in FIG. 5D, leakage of a sample, a target substance, and the like from the loose fitting portion, the first purification tube 5301, and the second purification tube 5302 can be prevented. Further, similarly to FIG. 5C, confusion of contaminated substances can be prevented. As a result, a target substance with higher purity can be obtained. In addition, the other purification tube is not loosely fitted to the first end portion side of the first purification tube 5301, or the second end portion 5332 side of the second purification tube 5302 is not loosely fitted to the other purification tube. For example, it is not necessary to provide an opening at the end.

  Note that this embodiment mode can be combined with the structure of Embodiment Mode 1.

(Embodiment 4)
In this embodiment, a configuration in which a gas supply unit and a vacuum exhaust unit are provided in the purification apparatus in addition to the configurations of Embodiments 1 to 3 will be described with reference to FIG. Since other configurations are the same as those in the first to third embodiments, the description thereof is omitted.

  The purification apparatus 6000 of the present embodiment includes a purification unit 6010, a temperature adjustment unit 6020, a fixing unit 6030, a gas supply unit 6040, and a vacuum exhaust unit 6050.

  The purification unit 6010 includes a first purification tube 6011 for arranging a sample and a second purification tube 6012 for recovering a target substance. In the present embodiment, a tube made of glass, quartz or the like (referred to as an outer tube in this specification) is used as the fixing means 6030, the purification tube constituting the purification unit 6010 is inserted inside the outer tube, and the purification unit 6010 is fixed. The material of the outer tube that is the fixing means 6030 is not limited to glass and quartz, and is a material that does not react with the sample, the target substance, and impurities, and is not mixed into the target substance when the target substance is recovered. Any material can be used. Further, when a vacuum pump is used as the evacuation unit 6050, any material that can maintain strength even when the pressure is reduced may be used.

  In addition to the glass tube, the fixing unit 6030 may be any unit that can maintain an airtight state such as a vacuum chamber and can hold a loose fitting portion between the purification tubes included in the purification unit 6010. Note that the fixing means 6030 only serves to hold the loose fitting part between the purification tubes, and a means for keeping the purification part 6010 in an airtight state may be provided separately.

  As described in Embodiments 1 to 3, the purification unit 6010 is loosely fitted to the second purification tube 6012 adjacent to the first purification tube 6011. Note that the first purification tube 6011 and the second purification tube 6012 may be those described in Embodiment Modes 1 to 3. Further, in the present embodiment, the purification unit 6010 is configured with two purification tubes, but the present invention is not limited thereto, and may be configured with three or more purification tubes.

  The temperature adjusting means 6020 is provided in the vicinity of the purification unit 6010. As the temperature adjusting means 6020, a heater such as a heater or a hot plate may be provided so that the sample can be heated to at least a temperature at which the sample is vaporized. Further, the highest temperature of the purification unit 6010 is applied to the first purification tube 6011 in which the sample is arranged.

  In addition, in order to maintain the temperature gradient after the temperature gradient is applied to the purification unit 6010, the purification unit 6010 as a whole may be provided with temperature adjusting means 6020 having a heat retaining function. Further, a protective cover such as a metal cover or glass wool may be provided so as to surround the purifying unit 6010 or the fixing means 6030, and the temperature gradient state may be maintained.

The gas supply means 6040 is provided at the end of the purification unit 6010. Specifically, it is provided at the end near the first purification tube 6011 in which the sample is arranged. The fixing means 6030 including the gas supply means 6040 and the purification unit 6010 may be connected using a pipe 6060 or the like. By introducing an inert gas such as argon (Ar) or nitrogen (N ₂ ) as a carrier gas from the gas supply means 6040 to the purification unit 6010, the vaporized sample can be diffused smoothly. As a result, the target substance can be efficiently precipitated or condensed in one direction.

  The carrier gas introduced into the purification unit 6010 from the gas supply means 6040 may be other than an inert gas, but an inert gas is preferable because it can suppress oxidation, decomposition, etc. of a sample or a target substance. . Of course, a gas that reacts with a sample, a target substance, or the like present in the purification unit 6010 must not be used.

  On the other hand, the evacuation unit 6050 is provided at the end of the purification unit 6010 on the opposite side where the gas supply unit 6040 is provided. The fixing means 6030 including the vacuum exhaust means 6050 and the purification unit 6010 may be connected using a pipe 6070 or the like. As the vacuum exhaust means 6050, a vacuum pump or the like can be used. Further, a cooling trap using liquid nitrogen or the like may be provided between the purification unit 6010 and the vacuum exhaust unit 6050. The inside of the refining unit 6010 can be evacuated by the evacuation means 6050 to reduce the pressure. As a result, the temperature at which the sample vaporizes can be lowered. That is, when the purification unit 6010 is depressurized using the vacuum evacuation means 6050, the sublimation or evaporation temperature of the sample is lowered, and the sample that is not vaporized under atmospheric pressure can be vaporized.

  In the present embodiment, both the gas supply means 6040 and the vacuum exhaust means 6050 are provided. However, the present invention is not limited to this, and only one of the means may be provided. However, when only the gas supply means 6040 is provided, the purification unit 6010 is not sealed. In the case where the vacuum evacuation unit 6050 is provided, it is preferable to arrange the purification unit 6010 in an outer tube such as glass or quartz, or a vacuum chamber.

  By disposing the gas supply means 6040 and the vacuum evacuation means 6050 in the purification apparatus 6000 as in the present embodiment, the target substance can be purified efficiently. In addition, the purification speed can be increased, and the working efficiency can be improved. Furthermore, it is possible to purify a sample that does not evaporate in the atmosphere, and the target substance can be easily obtained.

  Note that this embodiment mode can be combined with the structures of Embodiment Modes 1 to 3.

(Embodiment 5)
In this embodiment, a purification method using the purification device described in any of Embodiments 1 to 4 is described with reference to FIGS. In particular, a sublimation purification method in which a target substance and impurities are precipitated as a solid using a solid sample will be described.

  The purification apparatus 6000 has the same configuration as that of the fourth embodiment, and includes a purification unit 6010, a temperature adjustment unit 6020, a fixing unit 6030, a gas supply unit 6040, and a vacuum exhaust unit 6050. The purification unit 6010 includes a first purification tube 6011 for arranging a sample and a second purification tube 6012 for collecting a target substance. Of course, the present invention is not limited to this, and may have three or more purification tubes.

  First, the solid sample 7011 is placed in the first purification tube 6011 before loosely fitting in the second purification tube 6012. The solid sample may be directly arranged in the first purification tube 6011, or may be placed in a box-like or cylindrical container, and the container containing the sample may be inserted into the first purification tube 6011. The container in which the sample is placed is not particularly limited as long as it uses a material that does not chemically react with the sample, but glass, quartz, or the like is preferably used.

  Next, the purification unit 6010 is fixed by the fixing means 6030. As the fixing means 6030, a pipe (hereinafter referred to as an outer pipe) having a pipe inner diameter larger than the maximum pipe outer diameter of the first purification pipe 6011 and the second purification pipe 6012 is used. The outer tube preferably has a uniform tube inner diameter.

  The first purification tube 6011 and the second purification tube 6012 are inserted into the outer tube, which is the fixing means 6030, and the first purification tube 6011 is loosely fitted into the second purification tube 6012. In addition, after inserting the 1st refinement | purification pipe | tube 6011 and the 2nd refinement | purification pipe | tube 6012 in the outer pipe | tube which is the fixing means 6030, you may insert the container which put the solid sample.

  Moreover, it is preferable to hold | maintain the outer tube which is the fixing means 6030 horizontally in a major axis direction. In the present embodiment, the fixing means 6030 is a tube. However, the present invention is not limited to this, and any means can be used as long as it can be fixed so that at least the loose fitting portion of the purification tube constituting the purification unit 6010 can be held. However, if the purification unit 6010 is in a vacuum state, a tube or a vacuum chamber made of glass, quartz, or the like that can make the purification unit 6010 airtight is preferably used as the fixing means 6030.

  By using the purification unit 6010 of the present invention, it is possible to prevent the sample in the first purification tube 6011 from leaking into the outer tube as the fixing means 6030 or mixing into the adjacent second purification tube 6012.

  Next, the gas supply means 6040 and the vacuum exhaust means 6050 are connected to the fixing means 6030 including the purification unit 6010 using the pipe 6060, the pipe 6070, and the like. Note that the gas supply means 6040 is disposed on the end side near the first purification pipe 6011 of the purification unit 6010. Further, the vacuum evacuation means 6050 is disposed at the other end of the purification unit 6010. And the refinement | purification part 6010 containing the outer tube | pipe of the fixing means 6030 is made into an airtight state.

  Next, a temperature gradient is applied to the purification unit 6010 using the temperature adjusting means 6020. As the temperature adjusting means 6020, a heater such as a heater or a hot plate may be used. Further, after applying the temperature gradient, a heat retaining means may be provided so as to maintain the temperature gradient state. These temperature adjusting means 6020 may be provided in the vicinity of the purification unit 6010, or may be provided outside the outer tube that is the fixing means 6030. Furthermore, a protective cover made of metal, glass wool, or the like may be provided so as to surround the refining unit 6010 or the outer tube that is the fixing means 6030 so as to maintain the temperature gradient state.

  The solid sample 7011 disposed in the first purification tube 6011 is vaporized by the temperature adjusting means 6020. At this time, a carrier gas is introduced from the gas supply means 6040 into the purification section 6010, and the inside of the purification section 6010 is brought into a vacuum state by the vacuum exhaust means 6050.

  The vaporized sample diffuses toward the lower temperature according to the temperature gradient of the purification unit 6010. In the present embodiment, in the purification unit 6010, the temperature decreases in one direction from the side where the gas supply unit 6040 is disposed to the side where the vacuum exhaust unit 6050 is disposed. Note that the vaporized sample can be smoothly diffused by introducing the carrier gas from the gas supply means 6040.

  The second purification tube 6012 for recovering the target substance is set to a temperature region in which the target substance is precipitated by the temperature adjusting means 6020. Of the vaporized sample, only the purified target substance 7012 is deposited in the second purification tube 6012.

  In the present embodiment, the purification unit 6010 has two purification tubes, but the present invention is not limited to this, and may have three or more purification tubes. For example, a purification tube for collecting impurities having a deposition temperature higher than that of the target substance, a purification tube for collecting impurities having a deposition temperature lower than that of the target substance, and the like may be arranged. In addition, also when arrange | positioning three or more refinement pipes, suppose that the loose fitting part of adjacent refinement pipes uses the structure of this invention. That is, one purification tube is loosely fitted to an adjacent purification tube.

  Further, although the gas supply means 6040 and the vacuum evacuation means 6050 are provided in the purification apparatus 6000 of the present embodiment, the present invention is not limited to this, and only one means or both means may be provided. It does not have to be provided.

  By performing sublimation purification using the purification apparatus of the present invention, the target substance can be efficiently purified, and a high yield can be achieved.

  Note that this embodiment mode can be combined with any of Embodiment Modes 1 to 4.

(Embodiment 6)
In this embodiment, a purification method using the purification device described in any of Embodiments 1 to 4 is described with reference to FIGS. In particular, a distillation method for condensing a target substance and impurities as a liquid using a liquid sample will be described.

  The purification apparatus 6000 has the same configuration as that of the fourth embodiment, and includes a purification unit 6010, a temperature adjustment unit 6020, a fixing unit 6030, a gas supply unit 6040, and a vacuum exhaust unit 6050. The purification unit 6010 includes a first purification tube 6011 for arranging a sample and a second purification tube 6012 for collecting a target substance. Of course, the present invention is not limited to this, and may have three or more purification tubes.

  First, the liquid sample 8011 is put into the first purification tube 6011 before loosely fitting into the second purification tube 6012. The liquid sample may be put directly into the first purification tube 6011, or may be put into a box-like or cylindrical container, and the container containing the sample may be inserted into the first purification tube 6011. The container in which the sample is placed is not particularly limited as long as it uses a material that does not chemically react with the sample, but glass, quartz, or the like is preferably used.

  Next, the purification unit 6010 is fixed by the fixing means 6030. As the fixing means 6030, a pipe (outer pipe) having a pipe inner diameter larger than the maximum pipe outer diameter of the first purification pipe 6011 and the second purification pipe 6012 is used. The outer tube preferably has a uniform tube inner diameter.

  The first purification tube 6011 and the second purification tube 6012 are inserted into the outer tube, which is the fixing means 6030, and the first purification tube 6011 is loosely fitted into the second purification tube 6012. In addition, after inserting the 1st refinement | purification pipe | tube 6011 and the 2nd refinement | purification pipe | tube 6012 in the outer tube | pipe which is the fixing means 6030, you may insert the container which put the liquid sample.

  In addition, it is preferable to fix the outer tube which is the fixing means 6030 horizontally in the major axis direction and fix the purification unit 6010 to be inserted. In the present embodiment, the fixing means 6030 is a tube. However, the present invention is not limited to this, and any means can be used as long as it can be fixed so that at least the loose fitting portion of the purification tube constituting the purification unit 6010 can be held. However, if the purification unit 6010 is in a vacuum state, a tube or a vacuum chamber made of glass, quartz, or the like that can make the purification unit 6010 airtight is preferably used as the fixing means 6030.

  By using the purification unit 6010 of the present invention, there is little risk that the liquid sample in the first purification tube 6011 leaks into the outer tube as the fixing means 6030 or enters the adjacent second purification tube 6012. In particular, this effect is remarkable in the case of a liquid sample.

  Next, the gas supply means 6040 and the vacuum exhaust means 6050 are connected to the fixing means 6030 including the purification unit 6010 using the pipe 6060, the pipe 6070, and the like. Note that the gas supply means 6040 is disposed at the end of the purification unit 6010 near the first purification tube 6011. Further, the vacuum evacuation means 6050 is disposed at the other end of the purification unit 6010. And the refinement | purification part 6010 containing the outer tube | pipe of the fixing means 6030 is made into an airtight state.

  Next, a temperature gradient is applied to the purification unit 6010 using the temperature adjusting means 6020. As the temperature adjusting means 6020, a heater such as a heater or a hot plate may be used. Further, after applying the temperature gradient, a heat retaining means may be provided so as to maintain the temperature gradient state. These temperature adjusting means 6020 may be provided in the vicinity of the purification unit 6010, or may be provided outside the outer tube that is the fixing means 6030. Furthermore, a protective cover made of metal or the like may be provided so as to surround the purification unit 6010 or the outer tube as the fixing means 6030 so as to maintain the temperature gradient state.

  The liquid sample 8011 disposed in the first purification tube 6011 is vaporized by the temperature adjusting means 6020. At this time, a carrier gas is introduced from the gas supply means 6040 into the purification section 6010, and the inside of the purification section 6010 is brought into a vacuum state by the vacuum exhaust means 6050.

  Note that when the liquid sample 8011 that is liquid at normal temperature is vaporized, a stirrer for a magnetic stirrer or the like is placed in the first purification tube 6011 or a container containing the liquid sample 8011 and stirred to prevent bumping and the like. Is preferred. When the purification unit 6010 is not in a vacuum state (when the evacuation unit 6050 is not provided), a boiling stone may be added.

  The vaporized sample diffuses toward the lower temperature according to the temperature gradient of the purification unit 6010. In the present embodiment, in the purification unit 6010, the temperature decreases in one direction from the side where the gas supply unit 6040 is disposed to the side where the vacuum exhaust unit 6050 is disposed. Note that the vaporized sample can be smoothly diffused by introducing the carrier gas from the gas supply means 6040.

  The second purification tube 6012 for recovering the target substance has a temperature region in which the target substance is condensed by the temperature adjusting means 6020. Of the vaporized sample, only the purified target substance 8012 is condensed in the second purification tube 6012.

  In the present embodiment, the purification unit 6010 has two purification tubes, but the present invention is not limited to this, and may have three or more purification tubes. For example, a purification tube for collecting impurities having a higher condensation temperature than the target substance, a purification tube for collecting impurities having a lower condensation temperature than the target substance, and the like may be arranged. In addition, also when arrange | positioning three or more refinement pipes, suppose that the loose fitting part of adjacent refinement pipes uses the structure of this invention. That is, one purification tube is loosely fitted to an adjacent purification tube.

  Further, although the gas supply means 6040 and the vacuum evacuation means 6050 are provided in the purification apparatus 6000 of the present embodiment, the present invention is not limited to this, and only one means or both means may be provided. It does not have to be provided.

  By performing purification (distillation) using the purification apparatus of the present invention, the target substance can be efficiently purified, and a high yield can be achieved. Further, it is possible to prevent liquid from being mixed into the adjacent purification tubes.

  In addition, when the target substance is condensed as a liquid as in the present embodiment, the target substance may be solidified if the temperature is lowered to recover the purified target substance from the purification unit 6010. At this time, if the target substance leaks from the purification pipe to the outer pipe, it will solidify to the target substance that has entered the gap between the purification pipe and the outer pipe, making it difficult to remove the purification pipe from the outer pipe. End up. In addition, it becomes difficult to separate the loose fitting portion of the purification tube. According to the present invention, it is possible to prevent a sample, a target substance, and the like from leaking from the purification unit, so that the purification device can be handled easily and damage to the purification device can be suppressed.

  In addition, it is difficult to recover the target substance leaking from the purification pipe, and the yield decreases. Furthermore, since the target substance melts and spreads to the portion where the impurities are condensed, the purity is lowered. According to the present invention, it is possible to prevent a sample, a target substance, and the like from leaking from the purification unit, and thus a high-purity target substance can be purified with a high yield.

  Note that this embodiment mode can be combined with the structures of Embodiment Modes 1 to 4.

  A purification method and a purified product using the purification apparatus of the present invention will be described with reference to FIG. 9, FIG. 10, FIG.

  As shown in FIG. 9A, the purification apparatus 9000 of the present invention includes a purification unit 9010, a temperature adjustment unit 9020a, a temperature adjustment unit 9020b, an outer tube 9030, a gas supply unit 9040, and a vacuum exhaust unit 9050. The gas supply means 9040 and the vacuum evacuation means 9050 are connected to an outer pipe 9030 including a purification unit 9010 via a pipe 9060 and a pipe 9070. The temperature adjusting unit 9020a and the temperature adjusting unit 9020b may have the same set temperature or different set temperatures. Further, the outer tube 9030 serves as a fixing means for the purification unit 9010.

  The purification unit 9010 includes a first purification tube 9011, a second purification tube 9012, and a third purification tube 9013. The vacuum exhaust means 9050 includes a vacuum gauge 9051, a cold trap 9052, and a vacuum pump (rotary pump) 9053.

  First, the sample 9800 (3.0 g) was inserted into the first purification tube 9011. Sample 9800 includes 3- [N- (1-naphthyl) -N- (9-phenylcarbazol-3-yl) amino] -9-phenylcarbazole represented by Structural Formula (1), an impurity, a solvent, It was a mixture of

  Next, a purification unit 9010 including a first purification tube 9011, a second purification tube 9012, and a third purification tube 9013 containing the sample 9800 was inserted into the outer tube 9030. At this time, as described in Embodiments 1 to 6, the first purification tube 9011, the second purification tube 9012, and the third purification tube 9013 are the ends of the purification tubes in which the samples are arranged, or the samples. It arrange | positioned so that the edge part near the refinement | purification pipe | tube which has arrange | positioned may be loosely fitted to the edge part of the adjacent other refinement | purification pipe | tube. (FIG. 9A).

  FIG. 10 shows a cross-sectional view of the first purification tube 9011 in the direction parallel to the vaporized sample flow path. In FIG. 10, the sample 9800 inserted into the first purification tube 9011 is omitted.

As shown in FIG. 10, as the first purification tube 9011, a quartz tube having a wall thickness (t) of 2 mm and a total length (w) of 120 mm was used. The first purifying tube 9011 has a first end portion 9111 whose inner diameter is continuously increased from 20 mm to 24 mm, a central portion 9211 having a uniform inner diameter of 24 mm, and an inner diameter of 24 mm to 14 mm. A structure having a second end portion 9311 including a continuously decreasing region and a region (s) where the inner diameter of the tube is 14 mm and 10 mm is uniform. Further, the first end portion 9111, the central portion 9211, and the second end portion 9311 have a structure in which a cross section in a direction perpendicular to the flow path of the vaporized sample is concentric. The tube inner diameter (e ₁ ) of the first end portion 9111 is 20 mm, the tube inner diameter (c ₁ ) of the central portion 9211 is 24 mm, and the tube inner diameter (c ₁ ) of the second end portion 9311 is 24 mm. The tube inner diameter (b ₁ ) was 14 mm. That is, the vertical distance (v) between the innermost edge of the first end portion 9111 and the extension line of the outer edge of the center portion 9211 is 4 mm, and the extension line of the outer edge of the center portion 9211 and the second end portion 9311 are. The vertical distance (u) from the outer edge of the outermost part was 5 mm.

  The second purification tube 9012 and the third purification tube 9013 were also used in the same shape as the first purification tube 9011. The second end portion 9311 of the first purification tube 9011 was loosely fitted to the first end portion of the second purification tube 9012. Similarly, the second end of the second purification tube 9012 was loosely fitted to the first end of the third purification tube 9013. The region (s) in which the inner diameter of the second end portion 9311 of the first purification tube 9011 is 14 mm and is uniform by 10 mm is arranged so as to be loosely fitted to the adjacent second purification tube 9012. Similarly, the second end of the second purification tube 9012 was arranged so as to be loosely fitted to the adjacent third purification tube 9013.

  Next, the outer tube 9030 including the purification unit 9010 was evacuated with a vacuum pump 9053.

  Subsequently, vacuum is applied from the side where the first purification tube 9011 containing the sample 9800 is placed in the outer tube 9030 including the purification unit 9010 via the pipe 9060 at a rate of 5 cc / min from the gas supply means 9040. It flowed toward the pump 9053 side. And it was confirmed with the vacuum gauge 9051 that the vacuum degree of the refinement | purification part 9010 became about 10 Pa.

  Subsequently, the temperature adjusting means 9020a and 9020b were heated from room temperature to 110 ° C., then heated from 110 ° C. to 310 ° C. over 5 hours, and then heated at 310 ° C. for about 15 hours. At this time, the liquid was condensed inside the second purification tube 9012 of the purification unit 9010.

  After the purification, heating was stopped and the outer tube 9030 was cooled to room temperature, and then the purification unit 9010 was slowly exposed to the atmosphere. At this time, a substance that was liquid at the time of heating was deposited as solid 9900 in the second purification tube 9012 (FIG. 9B).

  Subsequently, the first purification tube 9011, the second purification tube 9012, and the third purification tube 9013 were taken out from the outer tube 9030. At this time, by tilting the outer tube 9030, the first purification tube 9011, the second purification tube 9012, and the third purification tube 9013 could be easily taken out.

  Subsequently, 2.1 g of solid 9900 was recovered from the second purification tube 9012 at a recovery rate of 85% using a medicine spoon. Note that a mixture (hereinafter, referred to as a residue) containing 0.2 g of the target substance and impurities remained in the first purification tube 9011. The recovery rate is obtained from the following mathematical formula (23).

  The yield of solid 9900 was 79%. The yield is obtained from the following formula (24).

In addition, the sample before purification (corresponding to the sample 9800 put in the first purification tube 9011) and the recovered product (corresponding to the solid 9900 deposited inside the second purification tube 9012) of this example Measurement was performed by a magnetic resonance method ( ¹ H-NMR (300 MHz, DMSO-d ₆ )).

A ¹ H-NMR chart of Sample 9800 is shown in FIG. FIG. 11B shows an enlarged view of the range of 6.5 ppm to 8.5 ppm in the chart of FIG.

A ¹ H-NMR chart of solid 9900 is shown in FIG. Further, FIG. 12B shows an enlarged view of the range of 6.5 ppm to 8.5 ppm in the chart of FIG. From FIG. 12, the solid 9900, which is a purified substance, is purified 3- [N- (1-naphthyl) -N- (9-phenylcarbazol-3-yl) amino] -9-phenylcarbazole. I understood.

  11A and 11B in which the sample 9800 before purification is measured and FIGS. 12A and 12B in which the solid 9900 which is a recovered product after purification is compared. The peak derived from impurities that appeared in the vicinity of 0.5 ppm to 2.5 ppm decreased in FIG. In addition, the impurity-derived peak observed in the vicinity of 7.1 ppm to 7.2 ppm in FIG. 11B is not observed in FIG.

Incidentally, it is seen in both FIGS. 11 and 12, the peak of 3.33ppm and 2.54ppm is the peak derived from each and water _{DMSO-d 6,} which is derived from the solvent during the sample preparation for ¹ H-NMR belongs to.

  From the above results, it was confirmed that the target substance with high purity can be obtained by performing purification using the purification apparatus of the present invention.

  Further, when the operation from the insertion of the sample 9800 shown in this example to the recovery of the solid 9900 deposited in the second purification tube 9012 was performed twice under the same conditions, the following table (1) was obtained. Results were obtained.

  Therefore, it was confirmed that the target substance with high purity can be obtained in high yield by performing purification using the purification apparatus of the present invention.

  In this example, Experiment A in which the target substance was purified using the purification apparatus of the present invention and Experiment B purified using the purification apparatus in the comparative example will be described. As a sample before purification, a mixture of 9-phenylcarbazole represented by the following structural formula (2) and the target substance after purification and impurities was used.

  First, Experiment A using the purification apparatus of the present invention will be described. Since the same purification apparatus as that described in Embodiment 1 is used, detailed description thereof is omitted. Hereinafter, a description will be given with reference to FIG. In FIG. 13, the purification unit 9010 and the outer tube 9030 are shown, but in addition to these, a vacuum evacuation unit, a gas supply unit, a temperature control unit, and the like including a vacuum gauge, a trap unit, and a vacuum pump may be provided. it can.

  13A and 13B are diagrams illustrating Experiment A. FIG. 13A shows before purification of the target substance, and FIG. 13B shows after purification of the target substance. The purification unit 9010 has a first purification tube 9011, a second purification tube 9012, and a third purification tube 9013, as in the first embodiment, and is fixed by an outer tube 9030.

  Sample 1480 (5.0 g) was inserted into the first purification tube 9011. Sample 1480 is a mixture of 9-phenylcarbazole represented by the structural formula (2) and impurities.

  Next, a purification unit 9010 composed of a first purification tube 9011 into which the sample 1480 was inserted, a second purification tube 9012, and a third purification tube 9013 was inserted into the outer tube 9030. At this time, as described in Example 1, the first purification tube 9011, the second purification tube 9012, and the third purification tube 9013 are the end of the purification tube in which the sample before purification is arranged, or before purification. The end portion on the side close to the purification tube on which the sample was placed was placed so as to be loosely fitted to the end portion of the adjacent purification tube (see FIG. 13A).

  Next, after the outer tube 9030 including the purification unit 9010 was evacuated, argon gas was flowed into the outer tube 9030 including the purification unit 9010 so that the degree of vacuum of the purification unit 9010 was 100 Pa. Argon gas was flowed from the first purification tube 9011 side to the third purification tube 9013 side. Then, after heating for 1 hour so that the high temperature part in the temperature gradient attached to the refinement | purification part 9010 might be 150 degreeC and a low temperature part was 110 degreeC, it heated for 4 hours in the state as it was. At this time, the liquid condensed inside the second purification tube 9012 of the purification unit 9010.

  After completion of purification, heating was stopped and the outer tube 9030 including the purification unit 9010 was cooled to room temperature, and then the purification unit 9010 was slowly exposed to the atmosphere. At this time, a substance condensed as a liquid at the time of heating in the second purification tube 9012 was deposited as a solid 1490 (see FIG. 13B).

  Subsequently, the purification unit 9010 including the first purification tube 9011, the second purification tube 9012, and the third purification tube 9013 was taken out from the outer tube 9030. At this time, the purifying unit 9010 could be easily taken out by tilting the outer tube 9030.

  At this time, when the outer tube 9030 after the purification unit 9010 was taken out was observed, the vicinity where the loose fitting part between the adjacent purification tubes was located was not very dirty, and the sample, purified product, impurities, etc. leaked too much. I knew it was n’t there. Moreover, when the taken out 2nd refinement | purification pipe | tube 9012 was observed, it turned out that the solid of the target substance has precipitated and collected in the refinement | purification pipe | tube.

  Subsequently, when a solid 1490, which is 9-phenylcarbazole as a target substance, was recovered from the second purification tube 9012 using a medicine spoon or the like, the recovery amount was 3.6 g. The recovery rate was 89% when determined from the above formula (23). Note that 0.9 g of a residue (a mixture including the target substance and impurities) remained in the first purification tube 9011. Further, the yield of the solid 1490 was determined from the above mathematical formula (24) and found to be 73%.

  Next, Experiment B, which is a comparative example, will be described. In Experiment B, a purification tube having a shape different from that in Experiment A was used for the purification unit 9010. Since other configurations and experimental conditions are the same as those in Experiment A, detailed description thereof is omitted.

  13C and 13D are diagrams illustrating Experiment B. FIG. FIG. 13C shows the target substance before purification, and FIG. 13D shows the target substance after purification. The purification unit 9010 has a first purification tube 1511, a second purification tube 1512, and a third purification tube 1513, and is fixed by an outer tube 9030. In Experiment B, the first purification tube 1511, the second purification tube 1512, and the third purification tube 1513 were cylindrical hollow tubes having uniform tube inner diameters. Further, the maximum pipe inner diameter, the total length of the pipe, and the material of the pipe were the same as those in Experiment A.

  Sample 1580 (5.0 g) was inserted into the first purification tube 1511. Sample 1580 is a mixture of 9-phenylcarbazole represented by the structural formula (2) and an impurity.

  Next, a purification unit 9010 including a first purification tube 1511 into which the sample 1580 was inserted, a second purification tube 1512, and a third purification tube 1513 was inserted into the outer tube 9030. At this time, the first purification tube 9011, the second purification tube 9012, and the third purification tube 9013 were arranged in a line without being fitted to each other (see FIG. 13C).

  Next, after the outer tube 9030 including the purification unit 9010 was evacuated, argon gas was flowed into the outer tube 9030 including the purification unit 9010 so that the degree of vacuum of the purification unit 9010 was 100 Pa. Argon gas was flowed from the first purification tube 1511 side to the third purification tube 1513 side. Then, after heating for 1 hour so that the high temperature part in the temperature gradient attached to the refinement | purification part 9010 might be 150 degreeC and a low temperature part was 110 degreeC, it heated for 4 hours in the state as it was. At this time, the liquid condensed inside the second purification tube 9012 of the purification unit 9010.

  After completion of purification, heating was stopped and the outer tube 9030 including the purification unit 9010 was cooled to room temperature, and then the purification unit 9010 was slowly exposed to the atmosphere. At this time, a substance condensed as a liquid at the time of heating in the second purification tube 9012 was deposited as a solid 1590 (see FIG. 13D).

  Subsequently, the purification unit 9010 including the first purification tube 1511, the second purification tube 1512, and the third purification tube 1513 was taken out from the outer tube 9030. At this time, the purification unit 9010 is fixed to the outer tube 9030, and it is difficult to remove it even if the outer tube 9030 is inclined.

  After the purification unit 9010 was removed from the outer tube 9030, the outer tube 9030 was observed, and the vicinity where the seam (adjacent part) between adjacent purification tubes was located was very dirty, and samples, purified products, impurities, etc. I found out that it was leaking. Moreover, when the taken out refinement | purification tube was observed, solid had adhered to the outer side of the refinement | purification tube. Therefore, it was found that the solid adhering to the outside of the purification tube also adhered to the outer tube, and the purification tube was fixed to the outer tube, making it difficult to remove the purification unit.

  Subsequently, when a solid 1590 which is 9-phenylcarbazole as a target substance was recovered from the second purification tube 1512 using a medicine spoon or the like, the recovered amount was 3.5 g. The recovery rate was 89% when determined from the above formula (23). Note that 1.1 g of a residue (a mixture including the target substance and impurities) remained in the first purification tube 1511. The yield of solid 1590 was determined from the above mathematical formula (24) and found to be 69%.

  The results of comparing Experiment A and Experiment B are shown in Table 2 below.

  From the above results, it was found that the purification apparatus of the present invention can prevent leakage of the sample and the target substance from the purification tube and can be purified with a high yield. Therefore, it has been found that application of the present invention can prevent contamination of the apparatus and simplify the handling of the apparatus.

The figure which shows an example of the refinement | purification apparatus of this invention. The figure which shows an example of the refinement | purification apparatus of this invention. The figure which shows an example of the refinement | purification apparatus of this invention. The figure which shows an example of the refinement | purification pipe | tube of this invention. The figure which shows an example of the refinement | purification pipe | tube of this invention. The figure which shows an example of the refinement | purification apparatus of this invention. The figure which shows an example of the sublimation purification method using the refinement | purification apparatus of this invention. The figure which shows an example of the distillation method using the refiner | purifier of this invention. The figure which shows an example of the purification method using the refinement | purification apparatus of this invention. The figure which shows an example of the refinement | purification apparatus of this invention. ^{The 1 H-NMR} chart of the previous material to be purified using the purification apparatus of the present invention. ^{The 1 H-NMR} chart of the purified product using purification apparatus of the present invention. The figure which shows an example of the purification method using the refinement | purification apparatus of this invention.

Explanation of symbols

100 refining apparatus 110 refining unit 120 temperature adjusting means 130 fixing means 201 first purifying pipe 202 second purifying pipe

Claims (10)

A purification unit for vaporizing and purifying the substance;
Fixing means for fixing the purification section;
A temperature adjusting means which is provided in the vicinity of the purifying unit and applies a temperature gradient to the purifying unit;
Gas supply means provided in the vicinity of one end of the purification unit;
Vacuum evacuation means provided close to the other end of the purification unit;
Have
The purification unit includes a first purification tube and a second purification tube provided in a horizontally long manner,
The first purification pipe has a first end portion, a second end portion, and a first central portion sandwiched between the first end portion and the second end portion,
An opening is provided in each of the first end and the second end,
The inner diameter of the first end portion and the inner diameter of the second end portion are smaller than the inner diameter of the first central portion,
The second purification tube has a third end portion, a fourth end portion, and a second central portion sandwiched between the third end portion and the fourth end portion,
An opening is provided in each of the third end and the fourth end,
The inner diameter of the third end portion and the inner diameter of the fourth end portion are smaller than the inner diameter of the second central portion,
The second end of the first purification tube is loosely fitted to the third end of the second purification tube;
The cross section of the second end of the first purification tube and the cross section of the fourth end of the second purification tube are concentric circles;
The center of the cross section of the second end portion and the cross section of the fourth end portion is provided above the center of the cross section of the second central portion of the second purification tube. apparatus. A purification unit for vaporizing and purifying the substance;
Fixing means for fixing the purification section;
A temperature adjusting means which is provided in the vicinity of the purifying unit and applies a temperature gradient to the purifying unit;
Gas supply means provided in the vicinity of one end of the purification unit;
Vacuum evacuation means provided close to the other end of the purification unit;
Have
The purification unit includes a first purification tube and a second purification tube provided in a horizontally long manner,
The first purification pipe has a first end portion, a second end portion, and a first central portion sandwiched between the first end portion and the second end portion,
An opening is provided in each of the first end and the second end,
The inner diameter of the first end portion and the inner diameter of the second end portion are smaller than the inner diameter of the first central portion,
The second purification tube has a third end portion, a fourth end portion, and a second central portion sandwiched between the third end portion and the fourth end portion,
An opening is provided in each of the third end and the fourth end,
The inner diameter of the third end portion and the inner diameter of the fourth end portion are smaller than the inner diameter of the second central portion,
A convex portion smaller than the inner diameter of the second central portion is provided on a part of the inner wall of the second central portion of the second purification pipe,
The second end of the first purification tube is loosely fitted to the third end of the second purification tube;
A cross section of the second end of the first purification pipe, a cross section of the second central portion of the second purification pipe where the convex portion is not provided , and the second purification pipe The refinement | purification apparatus characterized by the cross section of the said 4th edge part being a concentric circle. A purification unit for vaporizing and purifying the substance;
Fixing means for fixing the purification section;
A temperature adjusting means which is provided in the vicinity of the purifying unit and applies a temperature gradient to the purifying unit;
Gas supply means provided in the vicinity of one end of the purification unit;
Vacuum evacuation means provided close to the other end of the purification unit;
Have
The purification unit includes a first purification tube and a second purification tube provided in a horizontally long manner,
The first purification pipe has a first end portion, a second end portion, and a first central portion sandwiched between the first end portion and the second end portion,
An opening is provided in each of the first end and the second end,
The inner diameter of the first end portion and the inner diameter of the second end portion are smaller than the inner diameter of the first central portion,
The second purification tube has a third end portion, a fourth end portion, and a second central portion sandwiched between the third end portion and the fourth end portion,
An opening is provided in each of the third end and the fourth end,
The inner diameter of the third end portion and the inner diameter of the fourth end portion are smaller than the inner diameter of the second central portion,
A convex portion smaller than the inner diameter of the second central portion is provided on a part of the inner wall of the second central portion of the second purification pipe,
The second end of the first purification tube is loosely fitted to the third end of the second purification tube;
The cross section of the second end of the first purification tube and the cross section of the fourth end of the second purification tube are concentric circles;
The center of the cross section of the second end portion and the cross section of the fourth end portion is more than the center of the cross section of the second central portion of the portion of the second purification tube where the convex portion is not provided. A purification apparatus characterized by being provided above. In claim 2 or claim 3,
The refining apparatus is characterized in that a cross-sectional shape of the second central portion provided with the convex portion is a kamaboko shape. In any one of claims 2 to 4,
The said convex part is provided in the lower surface side of a said 2nd refinement | purification pipe | tube, The refinement | purification apparatus characterized by the above-mentioned. In any one of Claims 1 thru | or 5,
The refining apparatus, wherein the second end portion has a curvature, and the third end portion also has a curvature. In any one of Claims 1 thru | or 6,
The purification apparatus according to claim 1, wherein the gas supply means is means for supplying an inert gas to the purification section. In any one of Claims 1 thru | or 7,
The purification device according to claim 1, wherein the fixing means is a tube, and the purification unit is inserted and fixed in a tube as the fixing means. In any one of Claims 1 thru | or 8,
The purification apparatus characterized in that the first purification pipe and the second purification pipe are glass tubes or quartz tubes. In any one of Claims 1 thru | or 9,
The purification apparatus, wherein the first purification pipe is provided on the gas supply means side, and the second purification pipe is provided on the vacuum exhaust means side.

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