Substance transfer device and transfer method, and method for removing internal residue in apparatus for substance

Abstract

The present invention pertains to a substance transfer device that is for a substance containing at least one kind selected from sulfur atoms and halogen atoms, that enables safe and efficient handling of a substance containing at least one kind selected from sulfur atoms and halogen atoms, and that comprises a spare chamber for transfer, a transfer substance inlet and a transfer substance outlet, and an introduction mechanism and a discharge mechanism for an inert gas. The transfer substance inlet and the transfer substance outlet are provided to the spare chamber for transfer and are capable of being joined to a first substance inlet and a first substance outlet of a first container for a substance, and to a second substance transfer port of a second container for a substance. The introduction mechanism for an inert gas introduces the inert gas into the spare chamber for transfer. The discharge mechanism for an inert gas discharges the inert gas from the spare chamber for transfer. Also, the present invention pertains to a transfer method and a method for removing an internal residue in an apparatus for a substance.

Description

Substance transfer device and transfer method, and method for removing internal residues from substance equipment

[0001] The present invention relates to a device and method for transferring substances and a method for removing internal residues from a substance device.

[0002] With the recent rapid spread of information-related devices and communication devices such as personal computers, video cameras, and mobile phones, the development of batteries for use as their power sources has become increasingly important. Traditionally, batteries used for such applications have used electrolytes containing flammable organic solvents. However, because the electrolytes are liquid and flammable, safety concerns regarding leakage, fire, and other issues have arisen when used in batteries. In particular, for automotive applications, high capacity and high output are required, and safety concerns regarding batteries using conventional electrolytes are becoming increasingly serious. Therefore, all-solid-state batteries in which the electrolyte is replaced with a solid electrolyte layer are being developed because such batteries eliminate the use of flammable organic solvents, simplify safety devices, and offer superior manufacturing costs and productivity.

[0003] Known methods for producing a solid electrolyte used in a solid electrolyte layer include, for example, a method for producing a solid electrolyte that includes mixing a complexing agent and a solid electrolyte raw material to prepare an electrolyte precursor (see, for example, Patent Document 1), and a method for producing a solid electrolyte that includes drying a slurry containing a complexing agent and an electrolyte precursor by fluidized drying using media particles (see, for example, Patent Document 2).

[0004] In a system for handling powder, a dispersion device is disclosed that includes an agitation mixing section that mixes powder and liquid, a sealable powder supply section that supplies powder to the agitation mixing section, and a dry gas generator that supplies dry gas to the powder supply section (see, for example, Patent Document 3). Also, in a mixing system for mixing multiple materials, a mixing mechanism that mixes multiple materials, a material adjustment section that adjusts the materials, and a dry gas supply section that supplies dry gas into a hopper that has a spout that supplies the materials to the mixing mechanism are described (see, for example, Patent Document 4).

[0005] International Publication No. 2020 / 105737 Pamphlet International Publication No. 2021 / 230189 Pamphlet Japanese Patent Application Laid-Open No. 2021-126598 Japanese Patent Application Laid-Open No. 2020-182891

[0006] The present invention has been made in view of the above circumstances, and aims to provide a substance transfer device and method, as well as a method for removing internal residues from substance-handling equipment, which are capable of safely and efficiently handling substances containing at least one atom selected from sulfur atoms and halogen atoms.

[0007] The substance transfer device according to the present invention is a substance transfer device for a substance containing at least one atom selected from sulfur atoms and halogen atoms, and comprises a transfer preparation chamber, a transfer substance inlet section and a transfer substance outlet section, and an inert gas introduction mechanism and discharge mechanism, wherein the transfer substance inlet section and the transfer substance outlet section are provided in the transfer preparation chamber and are connectable to a first substance inlet section and a first substance outlet section of a first substance container and a second substance transfer port section of a second substance container, and the inert gas introduction mechanism introduces the inert gas into the transfer preparation chamber, and the inert gas discharge mechanism discharges the inert gas from the transfer preparation chamber.

[0008] A method for transferring a substance according to the present invention uses a transfer device for a substance containing at least one atom selected from a sulfur atom and a halogen atom, the transfer device comprising a transfer pre-chamber, a transfer substance inlet and outlet, and an inert gas introduction mechanism and discharge mechanism, the transfer substance inlet and outlet are provided in the transfer pre-chamber and are connectable to the first substance inlet and first substance outlet of a first substance container and the second substance transfer port of a second substance container, the inert gas introduction mechanism introduces the inert gas into the transfer pre-chamber and the inert gas discharge mechanism discharges the inert gas from the transfer pre-chamber, and the method comprises the following operations (1A) to (3A): (1A) Connecting the transfer substance inlet and valve 1a provided in the substance outlet of the first substance container, and connecting the transfer substance outlet and valve 2 provided in the second substance transfer port of the second substance container. (2A) The valves 1a and 2 are closed, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer preliminary chamber. (3A) The supply and discharge of the inert gas are stopped, and the valves 1a and 2 are opened, and the substance stored in the first substance container is transferred to the second substance container.

[0009] A method for removing internal residue from a substance container according to the present invention uses a transfer device for a substance containing at least one atom selected from sulfur atoms and halogen atoms, the transfer device comprising: a transfer pre-chamber, a transfer substance inlet and outlet ports, and an inert gas introduction mechanism and discharge mechanism, the transfer substance inlet and outlet ports being provided in the transfer pre-chamber and connectable to a first substance inlet and first substance outlet port of a first substance container and a second substance transfer port of a second substance container, the inert gas introduction mechanism introducing the inert gas into the transfer pre-chamber and the inert gas discharge mechanism discharging the inert gas from the transfer pre-chamber, and performing the following operations (1B) and (2B): (1B) connecting the transfer substance inlet port with valve 1a provided in the substance outlet port of the first substance container. (2B) The valve 1a is opened, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the preliminary substance chamber and the first substance container.

[0010] According to the present invention, it is possible to provide a substance transfer device and method, as well as a method for removing internal residues from substance-handling equipment, which are capable of safely and efficiently handling substances containing at least one atom selected from sulfur atoms and halogen atoms.

[0011] 1 is a schematic diagram showing a preferred embodiment of a substance transfer device according to the present embodiment. 2 is a schematic diagram showing a preferred embodiment of a substance transfer device according to the present embodiment.

[0012] Hereinafter, an embodiment of the present invention (hereinafter, sometimes referred to as "the present embodiment") will be described. In this specification, the upper and lower limit values ​​of a numerical range expressed as "greater than or equal to," "less than or equal to," and "to" can be arbitrarily combined, and the numerical values ​​of the examples can also be used as the upper and lower limit values. Furthermore, preferred specifications can be arbitrarily adopted. In other words, one preferred specification can be adopted in combination with one or more other preferred specifications. It can be said that a combination of preferred items is more preferable.

[0013] (Findings Obtained by the Inventors to Achieve the Present Invention) The present inventors have conducted extensive research to solve the above-mentioned problems, and as a result have found the following, which has led to the completion of the present invention.

[0014] As studies into the practical application of all-solid-state batteries progress, mass production of sulfide solid electrolytes has become an urgent issue. In recent years, as demand for sulfide solid electrolytes has increased, full-scale operations have begun, shifting from lab-scale facilities to plant-scale facilities aimed at mass production. As methods for producing sulfide solid electrolytes, for example, those described in Patent Documents 1 and 2, have been considered. In sulfide solid electrolyte production equipment, various substances containing sulfur atoms are handled, such as solid electrolyte raw materials containing sulfur atoms, such as lithium sulfide, diphosphorus pentasulfide, and elemental sulfur; electrolyte precursors composed of these solid electrolyte raw materials and complexing agents; and sulfide solid electrolyte products. These sulfur-containing substances may react with moisture in the air to generate hydrogen sulfide, so safety must always be taken into consideration.

[0015] Furthermore, in the production of sulfide solid electrolytes, substances containing halogen atoms, such as lithium halides and elemental halogens, are used as raw materials for the solid electrolyte, mainly to improve the ionic conductivity of the solid electrolyte. Among substances containing halogen atoms, elemental halogens are highly reactive with water, and therefore, safety considerations must be taken into account.

[0016] The generation of hydrogen sulfide due to contact between a substance containing sulfur atoms and moisture in the atmosphere can occur, for example, when the substance is transferred between one container and another, so caution is required. Similarly to substances containing sulfur atoms, safety precautions must also be taken when transferring halogen-containing substances.

[0017] For example, solid electrolyte raw materials containing sulfur atoms, such as lithium sulfide, diphosphorus pentasulfide, and elemental sulfur, as well as solid electrolyte raw materials containing halogen atoms, such as lithium halides and elemental halogens, are commercially available or manufactured in a separate manufacturing apparatus. When transferring these commercially available or manufactured products from one container containing the raw material to another container storing the solid electrolyte raw material provided in the sulfide solid electrolyte manufacturing apparatus, safety must be taken into consideration when attaching or detaching the first container to the other container, as the material may come into contact with the atmosphere in the transfer piping for transferring the material and with the surrounding atmosphere unless some precautions are taken. Similar examples include the case where a sulfide solid electrolyte obtained in a sulfide solid electrolyte manufacturing apparatus is transported to a destination as a product, or when the sulfide solid electrolyte is transferred from one container storing the sulfide solid electrolyte to a container for transporting the sulfide solid electrolyte. Thus, when attempting to transfer a material containing at least one atom selected from sulfur atoms and halogen atoms from one container to another, the material may come into contact with the atmosphere.

[0018] In a production apparatus through which materials are distributed, such as a sulfide solid electrolyte production apparatus capable of carrying out the sulfide solid electrolyte production methods described in Patent Documents 1 and 2, materials must be handled in all situations, such as during operation startup, normal operation, operation shutdown, and maintenance work, and care must be taken to prevent the generation of hydrogen sulfide due to reactions between the materials and moisture in the air, etc. However, no consideration is given to the handling of materials.

[0019] The dispersion device described in Patent Document 3 above is designed to suppress the reaction between the powder and moisture in the atmosphere by supplying dry gas while supplying the powder, as the reaction between the powder and moisture can cause deterioration and decomposition of the powder, resulting in performance degradation and the generation of toxic gas (Patent Document 3, paragraph

[0008] ). However, the dispersion device described in Patent Document 3 is designed for normal operation, in which the powder is supplied to the stirring and mixing section together with dry gas and mixed with the liquid, and the only areas that are subject to a dry gas atmosphere are those through which the powder passes during normal operation, i.e., the powder supply section and the stirring and mixing section. Therefore, no consideration is given to areas where substances such as powder do not flow during normal operation.

[0020] The mixing system described in Patent Document 4, in which a hopper equipped with a dry gas supply unit and a mixing mechanism are connected in a state isolated from the outside air, is intended to enable materials such as liquids and powders to be mixed without coming into contact with moisture in the outside air, and to expose these materials to a dry gas environment (paragraphs

[0038] ,

[0044] , etc.). However, the mixing system described in Patent Document 4 also assumes normal operation in which multiple materials and dry gas coexist and are mixed inside the device, and the only locations that are subject to a dry gas environment are the hopper and mixing mechanism, which are locations through which powder passes during normal operation. Therefore, like Patent Document 3, Patent Document 4 also does not take into consideration locations where materials such as powder do not flow during normal operation.

[0021] The present inventors have studied methods for handling the above-mentioned substances, particularly during transfer, to ensure safety by minimizing reactions between the substances and moisture in the atmosphere, which occur in all situations, such as during start-up, normal operation, shutdown, and maintenance of manufacturing equipment. As a result of their studies, they have focused on using a spare chamber capable of storing an inert gas, such as nitrogen, as a transfer device. They have found that by combining such a spare chamber with a mechanism for supplying and discharging the inert gas and using the spare chamber as a transfer pipe for transferring the substances from one container to another, it is possible to minimize reactions between the substances and moisture in the atmosphere during transfer.

[0022] Although the substance flows through the auxiliary chamber when it is transferred from one container to another, the auxiliary chamber, through which the substance does not flow during normal operation, is filled with an inert gas atmosphere, and the manner in which the substance is used in a situation different from normal operation, such as when transferring a substance stored in one container to another container by connecting the one container to the other container, are matters not described at all in Patent Documents 3 and 4.

[0023] Furthermore, for example, when performing maintenance on equipment through which the above-mentioned substances pass during the operation of a manufacturing facility, the interior may be cleaned in advance with a fluid such as water. This may cause reactions between the above-mentioned substances and the water used for cleaning, as well as atmospheric moisture. The water used for cleaning may then remain inside the equipment. Therefore, to perform maintenance more safely and quickly after shutting down the manufacturing facility, it is important to more efficiently remove the water used for cleaning that remains inside the equipment. The inventors have discovered that in such cases, by providing the above-mentioned preliminary chamber and an inert gas supply and exhaust mechanism and using the preliminary chamber as a pipe for transferring the substances, the water used for cleaning that remains inside the equipment can be more efficiently removed, resulting in a secondary effect of improving the operating rate of the manufacturing equipment. Thus, the transfer device and transfer method for a substance containing at least one atom selected from sulfur atoms and halogen atoms, and the method for removing internal residues from equipment for the substance, according to the present invention, enable safe and efficient handling of the above-mentioned substances.

[0024] (Regarding various forms of this embodiment) A substance transfer device according to a first form of this embodiment is a substance transfer device for transferring a substance containing at least one atom selected from sulfur atoms and halogen atoms, and is provided with a transfer preliminary chamber, a transfer substance inlet portion and a transfer substance outlet portion, and an inert gas introduction mechanism and discharge mechanism, wherein the transfer substance inlet portion and the transfer substance outlet portion are provided in the transfer preliminary chamber and are connectable to a first substance inlet portion and a first substance outlet portion of a first substance container and a second substance transfer port portion of a second substance container, and the inert gas introduction mechanism introduces the inert gas into the transfer preliminary chamber, and the inert gas discharge mechanism discharges the inert gas from the transfer preliminary chamber.

[0025] According to the first aspect of the present embodiment, when transferring a substance containing a sulfur atom (e.g., lithium sulfide, diphosphorus pentasulfide, elemental sulfur), or a substance containing a halogen atom (e.g., lithium halide, elemental halogen), from a first container to a second container (or from the second container to the first container), the substance transfer device has a simple structure including a transfer pre-chamber, a transfer substance inlet and outlet ports, and an inert gas introduction and exhaust mechanism, thereby suppressing reactions between the substance and moisture in the atmosphere and ensuring safety. Furthermore, since safety can be ensured, work efficiency can be improved. As a result, it becomes possible to safely and efficiently handle a substance containing at least one atom selected from sulfur atoms and halogen atoms (hereinafter, sometimes simply referred to as "substance").

[0026] A substance transfer device according to a second aspect of this embodiment is the substance transfer device according to the first aspect, wherein the inert gas introduction mechanism further introduces an inert gas from an inert gas inlet provided in the first substance container.

[0027] The inert gas introduction mechanism can introduce the inert gas through the inert gas inlet provided in the first substance container, which allows for safer and more efficient substance handling. Furthermore, when removing residue from the substance container (described later), this can be done more efficiently, which can improve the operating rate of the manufacturing equipment.

[0028] A substance transfer apparatus according to a third aspect of this embodiment is the substance transfer apparatus according to the first or second aspect, wherein the preliminary transfer chamber is cylindrical.

[0029] The cylindrical transfer chamber ensures safety and allows for smoother transfer of substances, making it possible to handle substances more safely and efficiently. Furthermore, the ease of maintenance of the substance transfer device is improved.

[0030] A substance transfer device according to a fourth aspect of this embodiment is the substance transfer device according to the third aspect, in which the transfer substance inlet portion and the transfer substance outlet portion are provided at both ends of the cylindrical transfer pre-chamber.

[0031] Such a simple structure allows for smoother material transfer while ensuring safety, making it possible to handle materials more safely and efficiently. Furthermore, the maintainability of the material transfer device is improved.

[0032] A substance transfer device according to a fifth aspect of this embodiment is the substance transfer device according to the third or fourth aspect, in which the inert gas introduction mechanism and exhaust mechanism are provided on the side of the cylindrical transfer pre-chamber.

[0033] Such a structure allows for more stable introduction and discharge of inert gas, thereby ensuring safety and enabling smoother transfer of substances in particular, thereby enabling safer and more efficient handling of substances.

[0034] A sixth aspect of this embodiment provides a method for transferring a substance using a transfer device for a substance containing at least one atom selected from a sulfur atom and a halogen atom, the method comprising: a transfer preliminary chamber, a transfer substance inlet and outlet ports, and an inert gas introduction mechanism and discharge mechanism; the transfer substance inlet and outlet ports are provided in the transfer preliminary chamber and are connectable to the first substance inlet and first substance outlet ports of a first substance container and the second substance transfer port of a second substance container; the inert gas introduction mechanism introduces the inert gas into the transfer preliminary chamber, and the inert gas discharge mechanism discharges the inert gas from the transfer preliminary chamber; and the method comprises performing the following operations (1A) to (3A): (1A) connecting the transfer substance inlet port to valve 1a provided in the substance outlet port of the first substance container, and connecting the transfer substance outlet port to valve 2 provided in the second substance transfer port of the second substance container. (2A) The valves 1a and 2 are closed, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer preliminary chamber. (3A) The supply and discharge of the inert gas are stopped, and the valves 1a and 2 are opened, and the substance stored in the first substance container is transferred to the second substance container.

[0035] The substance transfer method of this embodiment employs the substance transfer device of this embodiment. By performing the procedures (1A) to (3A) above with the substance transfer device of this embodiment, it is possible to ensure safety and, in particular, to more smoothly transfer substances, thereby enabling safe and efficient substance handling.

[0036] The substance transfer method according to the seventh aspect of this embodiment is the substance transfer method according to the sixth aspect, which comprises carrying out the operations (2A) above, (4A) and (5A) below after the operation (3A) above. (4A) The second substance container and valve 2 are removed from the transferred substance outlet portion. (5A) A closing flange is attached to the transferred substance outlet portion.

[0037] By carrying out the operations (2A), (4A) and (5A) in order following the operation (3A), it is possible to ensure safety and, in particular, to more smoothly transfer substances, thereby enabling safer and more efficient handling of substances.

[0038] A method for removing internal residue from a substance container according to an eighth aspect of this embodiment uses a transfer device for a substance containing at least one atom selected from a sulfur atom and a halogen atom, the method comprising: (1B) connecting the transfer substance inlet port to a valve 1a provided in the substance outlet port of the first substance container; (2B) The valve 1a is opened, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer pre-chamber and the first substance container.

[0039] As mentioned above, when performing maintenance on equipment, the interior may be cleaned with a fluid such as water beforehand, which can cause reactions between the above-mentioned substances and not only atmospheric moisture but also the water used for cleaning. Thus, the medium used for cleaning, such as water, and the substance itself, may remain inside the equipment. The method for removing internal residues from a substance container of this embodiment employs the substance transfer device of this embodiment. By performing the above steps (1B) to (2B) using the substance transfer device of this embodiment, safety can be ensured while, among other things, removing internal residues from the equipment (substance container) more smoothly, thereby enabling safe and efficient substance handling. Furthermore, smoother removal of internal residues from the substance container results in purging the substance container with an inert gas, which allows for more rapid start-up of the manufacturing equipment after maintenance, thereby improving the operating rate of the manufacturing equipment.

[0040] A method for removing internal residues from a substance container according to a ninth aspect of this embodiment is a method for removing internal residues from a substance container according to the eighth aspect, in which an inert gas is introduced from an inert gas inlet provided in the first substance container by the inert gas introduction mechanism.

[0041] By introducing the inert gas not only through the valve 1a and the transfer pre-chamber but also through the first substance container, it is possible to more efficiently remove the residue inside the substance container, which results in safer and more efficient substance handling and also improves the operating rate of the manufacturing equipment.

[0042] [Substance Transfer Apparatus] The substance transfer apparatus of this embodiment is an apparatus for transferring a substance containing at least one atom selected from sulfur atoms and halogen atoms, and comprises a transfer preparation chamber, a transfer substance inlet section and a transfer substance outlet section, and an inert gas introduction mechanism and discharge mechanism, wherein the transfer substance inlet section and the transfer substance outlet section are provided in the transfer preparation chamber and are connectable to a first substance inlet section and a first substance outlet section of a first substance container and a second substance transfer port section of a second substance container, and the inert gas introduction mechanism introduces an inert gas into the transfer preparation chamber, and the inert gas discharge mechanism discharges the inert gas from the transfer preparation chamber.

[0043] (Substance containing at least one atom selected from sulfur atoms and halogen atoms) The object to be transferred by the substance transfer device of this embodiment is not particularly limited as long as it contains at least one atom selected from sulfur atoms and halogen atoms. For example, in a sulfide solid electrolyte production device in which the substance transfer device of this embodiment is suitably used, examples of the substance containing sulfur atoms include a solid electrolyte raw material containing sulfur atoms; an electrolyte precursor when a complexing agent is used; an intermediate such as a heat-treated product obtained by heat treatment in a solvent using a pressure-resistant container when a pressure-resistant container is used; a sulfide solid electrolyte product; and the like.

[0044] Examples of the substance containing a halogen atom include a solid electrolyte raw material containing a halogen atom; an electrolyte precursor when a complexing agent is used; an intermediate such as a heat-treated product obtained by heat treatment using a pressure-resistant container when a pressure-resistant container is used; a sulfide solid electrolyte product; etc. Examples of the substance containing a sulfur atom and a halogen atom include an intermediate such as an electrolyte precursor and a heat-treated product obtained using the above-mentioned solid electrolyte raw material containing a sulfur atom and a solid electrolyte raw material containing a halogen atom; a sulfide solid electrolyte product; etc. Details of these solid electrolyte raw materials, intermediates, and sulfide solid electrolytes will be described later.

[0045] The substance containing at least one atom selected from a sulfur atom and a halogen atom is a solid electrolyte raw material, an intermediate, and a sulfide solid electrolyte, as described above, and is basically in the form of a powder, but may be in the form of a liquid or a slurry containing the powder.

[0046] (Solid Electrolyte Raw Material) Examples of the solid electrolyte raw material that is a substance containing at least one atom selected from the sulfur atom and the halogen atom include lithium sulfide; lithium halides such as lithium fluoride, lithium chloride, lithium bromide, and lithium iodide; diphosphorus trisulfide (P ２ S ３ ), diphosphorus pentasulfide (P ２ S ５ ) and the like; bromine (Br ２ ), iodine (I ２ Representative examples include halogen elements such as phenylalanine, ... ４ Li containing structure ３ P.S. ４ These exemplified solid electrolyte raw materials may be in a solid (powder) or liquid form.

[0047] (Intermediate) Typical examples of intermediates include an electrolyte precursor obtained using the above-mentioned solid electrolyte raw material containing sulfur atoms and solid electrolyte raw material containing halogen atoms, and when a pressure-resistant container is used, a heat-treated product obtained by heat treatment using the pressure-resistant container. The electrolyte precursor refers to a complex formed by the combination of the solid electrolyte raw material and a solvent (also referred to as a "complexing agent") containing heteroatoms such as nitrogen atoms, oxygen atoms, and chlorine atoms, and sulfur atoms. These heteroatoms have a high affinity for lithium atoms, so a complex is formed. The complex formed by the combination of the solid electrolyte raw material and the complexing agent is heated and dried to remove the solvent containing the heteroatoms that constitute the complex, thereby producing a solid electrolyte, and is therefore referred to as an electrolyte precursor.

[0048] More specifically, the heat-treated product obtained by heat treatment using a pressure-resistant vessel is preferably obtained by pulverizing the solid electrolyte raw material as needed, roughly mixing the resulting pulverized product as needed, and further mixing and pulverizing the resulting solid electrolyte mixture in a solvent, followed by heat treatment using a pressure-resistant vessel. Here, the solvent may be a non-polar solvent such as a hydrocarbon solvent, and preferably further includes at least one polar solvent selected from a nitrile compound and an ether compound.

[0049] The heat treatment is preferably carried out at a heating temperature of 150 to 300° C., more preferably 160 to 280° C. The heat-treated product thus obtained can be called an intermediate because an argyrodite-type solid electrolyte can be obtained by firing it.

[0050] (Sulfide Solid Electrolyte) The sulfide solid electrolyte can be obtained, for example, by removing the complexing agent from the electrolyte precursor or by firing the heat-treated product. Examples of the sulfide solid electrolyte include an amorphous sulfide solid electrolyte and a crystalline sulfide solid electrolyte, which will be described later.

[0051] Representative examples of amorphous sulfide solid electrolytes include Li ２ S-P ２ S ５ , Li ２ S-P ２ S ５ - LiI, Li ２ S-P ２ S ５ -LiCl, Li ２ S-P ２ S ５ - LiBr, Li ２ S-P ２ S ５ -LiI-LiBr and other sulfide solid electrolytes composed of lithium sulfide, phosphorus sulfide, and lithium halide; and further containing other atoms such as oxygen atoms and silicon atoms, for example, Li ２ S-P ２ S ５ -Li ２ O-LiI, Li ２ S-P ２ S ５ -Li２ O-LiI-LiBr, Li ２ S-SiS ２ -P ２ S ５ Preferred examples include sulfide solid electrolytes such as —LiI, etc. The types of atoms constituting the amorphous sulfide solid electrolyte can be confirmed, for example, by an ICP emission spectrometer.

[0052] The crystalline sulfide solid electrolyte may be a so-called glass ceramic obtained by heating an amorphous sulfide solid electrolyte to a crystallization temperature or higher, and its crystalline structure may be Li ３ P.S. ４ Crystal structure, Li ４ P ２ S ６ Crystal structure, Li ７ P.S. ６ Crystal structure, Li ７ P ３ S １１ Examples of such structures include a crystal structure having peaks at 2θ=approximately 20.2° and 23.6° (for example, JP 2013-16423 A).

[0053] Also, Li ４－ｘ Ge １－ｘ P ｘ S ４ Thio-LISICON Region II crystal structure (Kanno et al., Journal of the Electrochemical Society, 148(7)A742-746(2001)), Li ４－ｘ Ge １－ｘ P ｘ S ４ Also included are crystal structures similar to the thio-LISICON Region II type (see Solid State Ionics, 177 (2006), 2721-2725).

[0054] Also, the above Li ７ P.S. ６A preferred example of the crystalline sulfide solid electrolyte is an argyrodite-type crystal structure having a structural skeleton in which part of P is substituted with Si. The composition formula of the argyrodite-type crystal structure is, for example, the composition formula Li ７－ｘ P １－ｙ Si ｙ S ６ and Li ７＋ｘ P １－ｙ Si ｙ S ６ (x is -0.6 to 0.6, y is 0.1 to 0.6) The composition formula of the argyrodite-type crystal structure is Li ７－ｘ－２ｙ P.S. ６－ｘ－ｙ Cl ｘ (0.8≦x≦1.7, 0<y≦−0.25x+0.5) can also be mentioned.

[0055] (Applications) The substance transfer device of this embodiment is suitably used in a sulfide solid electrolyte production apparatus, as described above. Specifically, the substance transfer device is used by being connected to a component of the sulfide solid electrolyte production apparatus, through which a substance containing at least one atom selected from sulfur atoms and halogen atoms flows during operation of the production apparatus, or to a substance container or the like that stores the substance.

[0056] When the material transfer apparatus of this embodiment is used in a connected state, the equipment constituting the sulfide solid electrolyte production apparatus to which it is connected varies depending on the method for producing a sulfide solid electrolyte, but mainly includes reaction equipment used for the reaction of solid electrolyte raw materials; when a solvent (including a complexing agent) is used, heating equipment for removing the solvent (including a complexing agent) from a slurry or solution containing an intermediate such as a solid electrolyte raw material and / or an electrolyte precursor and the solvent (including a complexing agent); heating equipment for crystallization, etc.; separation equipment for separating the sulfide solid electrolyte; particle size adjustment equipment for adjusting the particle size of the sulfide solid electrolyte; when heat treatment is performed using a pressure-resistant container, heating equipment for firing the pressure-resistant container and the heat-treated product; piping connecting these devices; and material containers for storing the above-mentioned materials. These devices will be described in detail in the description of the method and apparatus for producing a sulfide solid electrolyte.

[0057] (Configuration of the substance transfer device) The configuration of the substance transfer device of this embodiment will be described with reference to Fig. 1. Fig. 1 shows that the substance transfer device of this embodiment is equipped with a transfer preliminary chamber, a transfer substance inlet and a transfer substance outlet, and an inert gas introduction mechanism and discharge mechanism. The area enclosed by the boundary line indicated as "B / L" (an abbreviation for "battery limit") in Fig. 1 corresponds to the range of the substance transfer device of this embodiment.

[0058] The transfer substance inlet and outlet ports of the substance transfer device are provided in the transfer preparation chamber, and are preferably provided at both ends of the transfer preparation chamber as shown in Fig. 1. Furthermore, the transfer substance inlet and outlet ports of the substance transfer device can be connected to the first substance inlet and first substance outlet ports of the first substance container and the second substance transfer port of the second substance container, and in Fig. 1 they are connected to the first substance outlet port of the first substance container and the second substance transfer port of the second substance container, respectively, and the substance transfer device of this embodiment is shown to be configured to connect the first substance container and the second substance container.

[0059] The inert gas introduction mechanism and exhaust mechanism are provided in the transfer prechamber, and can introduce and exhaust the inert gas into and from the transfer prechamber, as shown in Fig. 1. Fig. 1 also shows that, in a preferred embodiment, the inert gas introduction mechanism introduces the inert gas from an inert gas inlet provided in the first substance container.

[0060] 1 shows an embodiment in which a substance stored in a first substance container is transferred to a second substance container. As shown in FIG. 1, the transfer of the substance is preferably carried out by gravity.

[0061] 1 describes that the first substance container has a "first substance inlet portion (outlet portion)" and a "first substance outlet portion (inlet portion)." This means that the first substance inlet portion can be the first substance outlet portion depending on the mode of use of the substance transfer device of this embodiment, and the first substance outlet portion can be the first substance inlet portion. As described above, FIG. 1 shows a mode in which a substance stored in the first substance container is transferred to the second substance container. However, conversely, when a substance stored in the second substance container is transferred to the first substance container, i.e., when a substance stored in the second substance container is transferred to the first substance container by its own weight, the first substance inlet portion becomes the first substance outlet portion, and the first substance outlet portion becomes the first substance inlet portion.

[0062] 1 also shows that a valve 1a is provided between the transfer object inlet port of the material transfer apparatus of this embodiment and the first material outlet port of the first material container, and a valve 2 is provided between the transfer object outlet port of the material transfer apparatus of this embodiment and the second material transfer port of the second material container. These valves are provided to separate the material transfer apparatus of this embodiment from the first material container and the second material container, and are used when transferring a material between the first material container and the second material container. These valves may be valves provided in the first material container and the second material container as shown in FIG. 1, or may be valves provided in the material transfer apparatus of this embodiment.

[0063] (Transfer Pre-chamber) The transfer pre-chamber is a flow path through which the substance passes when transferring the substance between the first substance container and the second substance container, and may also be used to temporarily store the substance depending on the situation.

[0064] The shape of the preliminary transfer chamber is not particularly limited as long as it allows the substance to pass through the preliminary transfer chamber and can be provided with an inert gas introduction mechanism and exhaust mechanism. When the preliminary transfer chamber is in the form of a pipe, its cross-sectional shape is preferably the same as the cross-sectional shapes of the first substance inlet and first substance outlet of the first substance container and the second substance transfer port of the second substance container, which will be described later. Examples of preferable shapes include a circle, an ellipse, a rectangle, and a square, more preferably a circle or an ellipse, and even more preferably a circle. That is, the shape of the preliminary transfer chamber is preferably cylindrical. More specifically, examples of cylindrical shapes include a cylinder, an elliptical cylinder, and a rectangular cylinder, more preferably a cylinder and an elliptical cylinder, and even more preferably a cylinder. By using such a shape, the substance is less likely to remain in the preliminary transfer chamber during substance transfer, allowing for smoother substance transfer.

[0065] When the preliminary transfer chamber is cylindrical, it can be configured, for example, by piping. By configuring it by piping, the material transfer device of this embodiment can be easily adjusted to a desired size and shape, and the material is less likely to remain in the preliminary transfer chamber during material transfer, allowing for smoother material transfer. The shape of the preliminary transfer chamber can be determined according to the desired shape. For example, when the preliminary transfer chamber is cylindrical (configured by piping), it can be linear (straight piping) or serpentine (serpentine piping). Considering that the material is less likely to remain in the preliminary transfer chamber during material transfer and allows for smoother material transfer, the linear shape (straight piping) is preferred.

[0066] The size of the cross-sectional shape of the transfer preparation chamber is also preferably the same as the size of the first substance inlet and first substance outlet of the first substance container and the second substance transfer port of the second substance container, as described below, in the same manner as the above cross-sectional shape. When the transfer preparation chamber is cylindrical, the diameter (inner diameter) of the cross-sectional shape is usually 5 mm or more and 310 mm or less, preferably 10 mm or more, more preferably 20 mm or more, with the upper limit being preferably 260 mm or less, more preferably 220 mm or less. When the transfer preparation chamber is constituted by piping, the size of the piping is usually 1 / 4 inch or more and 12 inches or less, preferably 1 / 2 inch or more, more preferably 1 inch or more, with the upper limit being preferably 10 inches or less, more preferably 8.5 inches or less.

[0067] Regarding the shape of the transfer pre-chamber, there are no particular restrictions on the length as long as an inert gas introduction mechanism and exhaust mechanism can be provided, and it is not possible to make a general statement since it can be determined depending on the installation location, etc., but the length of the piping portion should usually be 10 cm or more and 1 m or less.

[0068] (Transferred substance inlet and outlet) The transferred substance inlet and outlet provided in the preliminary transfer chamber are not particularly limited as long as they can be connected to the first substance inlet and first substance outlet of the first substance container and the second substance transfer port of the second substance container, and for example, when the preliminary transfer chamber is cylindrical (when configured by piping), it is preferable that they be provided at both ends of the cylinder (piping) as shown in Fig. 1. This makes it easier to connect the first substance container and the second substance container, improving the convenience of the substance transfer device of this embodiment.

[0069] To facilitate connection to the first and second substance containers and improve convenience, the transfer substance inlet and outlet ports provided in the transfer pre-chamber preferably adopt a configuration corresponding to the configuration of the first substance inlet and outlet ports of the first substance container and the second substance transfer port of the second substance container. For example, a connection configuration using a pipe joint such as a flange or threaded joint is preferred. By adopting such a configuration, the first substance inlet and outlet ports and the second substance transfer port of the substance transfer device of this embodiment can be easily attached and detached, improving convenience. Furthermore, when gate valves such as valve 1a and valve 2 (see FIG. 1) are used as needed, as shown in FIG. 1, the attachment and detachment of these valves can be easily achieved, improving convenience.

[0070] (Inert Gas Introduction Mechanism and Discharge Mechanism) The inert gas introduction mechanism is not particularly limited as long as it can introduce the inert gas into the transfer preparatory chamber, and preferably includes, for example, a connection part for receiving the inert gas from an inert gas supply source, piping from the connection part to the transfer preparatory chamber, and a gate valve in the piping, as shown in Fig. 1. By including the gate valve, the transfer method described below can be performed more easily, improving convenience.

[0071] When the transfer preparatory chamber is cylindrical, as shown in FIG. 1 , the inert gas introduction mechanism is preferably provided on the side of the transfer preparatory chamber. More specifically, the piping for supplying the inert gas from the connection part to the transfer preparatory chamber is preferably connected to the side of the transfer preparatory chamber. This connection allows for more stable introduction of the inert gas, thereby ensuring safety and particularly enabling smoother transfer of substances, thereby enabling safer and more efficient handling of substances. Furthermore, in the inert gas introduction mechanism, the piping for supplying the inert gas from the connection part to the transfer preparatory chamber may be connected to the transfer preparatory chamber using a connection method such as a flange or threaded piping joint, or may be directly connected to the transfer preparatory chamber as shown in FIG. 1 .

[0072] The inert gas exhaust mechanism is not particularly limited as long as it can exhaust the inert gas from the transfer preparatory chamber, and preferably includes, for example, a connecting part for exhausting the inert gas from the transfer preparatory chamber to an exhaust line for the inert gas, a pipe leading to the connecting part, and a gate valve in the pipe, as shown in Fig. 1. By including the gate valve, the transfer method described below can be carried out more easily, improving convenience.

[0073] When the transfer preparatory chamber is cylindrical, as shown in FIG. 1 , the inert gas exhaust mechanism is preferably provided on the side of the transfer preparatory chamber. More specifically, the piping for exhausting the inert gas from the transfer preparatory chamber is preferably connected to the side of the transfer preparatory chamber. This connection allows for more stable exhaust of the inert gas, ensuring safety and particularly enabling smoother transfer of substances, thereby enabling safer and more efficient handling of substances. Furthermore, in the inert gas introduction mechanism, the piping for exhausting the gas from the transfer preparatory chamber and the transfer preparatory chamber may be connected using a connection method such as a flange or threaded piping joint, or may be directly connected to the transfer preparatory chamber as shown in FIG. 1 .

[0074] As the inert gas used in the substance transfer apparatus of this embodiment, for example, rare gases such as helium and argon; nitrogen, etc. can be used, and among them, nitrogen is preferable in view of its versatility.

[0075] [Substance Transfer Method] The substance transfer method of this embodiment is a substance transfer method using a substance transfer device containing at least one atom selected from sulfur atoms and halogen atoms, comprising: a transfer preliminary chamber, a transfer substance inlet and a transfer substance outlet, and an inert gas introduction mechanism and discharge mechanism, wherein the transfer substance inlet and transfer substance outlet are provided in the transfer preliminary chamber and are connectable to the first substance inlet and first substance outlet of a first substance container and the second substance transfer port of a second substance container, and the inert gas introduction mechanism introduces the inert gas into the transfer preliminary chamber, and the inert gas discharge mechanism discharges the inert gas from the transfer preliminary chamber, and comprises performing the following operations (1A) to (3A): (1A) Connecting the transfer substance inlet and valve 1a provided in the substance outlet of the first substance storage container, and connecting the transfer substance outlet and valve 2 provided in the second substance transfer port of the second substance container. (2A) The valves 1a and 2 are closed, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer preliminary chamber. (3A) The supply and discharge of the inert gas are stopped, and the valves 1a and 2 are opened, and the substance stored in the first substance container is transferred to the second substance container.

[0076] As described above, the substance transfer method of this embodiment employs the substance transfer apparatus of this embodiment. The structure of the substance transfer apparatus employed in the substance transfer method of this embodiment is as described above for the substance transfer apparatus of this embodiment.

[0077] In the method for transferring a substance of this embodiment, the substance transfer apparatus of this embodiment is used to carry out the operations (1A) to (3A) described above. Valve 1a and valve 2 used in operations (1A) to (3A) are shown in Figure 1 as being provided in the first substance container and second substance container, but they may also be valves provided in the substance transfer apparatus.

[0078] Operation (1A) is an operation of connecting the substance transfer device of this embodiment to the first substance container and the second substance container. The next operation (2A) is an operation of filling the preliminary transfer chamber with an inert gas before transferring the substance from the first substance container to the second substance container. This operation prevents the substance from reacting with moisture in the atmosphere when it passes through the preliminary transfer chamber, thereby allowing for safer substance transfer.

[0079] In operation (3A), the substance stored in the second substance container is transferred from the first substance container to the second substance container. By performing operations (1A) and (2A), the transfer chamber is filled with an inert gas, and the substance can be transferred in an environment where all moisture, such as atmospheric moisture, has been removed. This ensures safety and, in particular, allows the substance to be transferred more smoothly, enabling safer and more efficient handling of the substance.

[0080] Furthermore, in the method for transferring a substance according to this embodiment, it is preferable to carry out the above-mentioned operation (3A), followed by the above-mentioned operation (2A), and the following operations (4A) and (5A): (4A) Remove the second substance container and valve 2 from the transferred substance outlet port; (5A) Attach a closing flange to the transferred substance outlet port.

[0081] By performing operation (2A) following operation (3A), the second substance container, which transfers and stores the substance, can be safely removed from the first substance container. That is, operation (4A) below can be safely performed, and the removed second substance container can be transported to a desired location. Furthermore, by performing operation (5A), the first substance container can be isolated from the outside air. Even if the substance remains inside the first substance container and passes through valve 1a, it will be stored in the substance transfer device filled with inert gas, and the closing flange prevents atmospheric air containing moisture from entering the substance transfer device. Therefore, no reaction between the substance and moisture in the atmosphere will occur, and the substance can be handled safely.

[0082] The substance transfer method of this embodiment is intended to be a method of transferring a substance from a first substance container to a second substance container. The first substance container and the second substance container are containers used for various purposes, such as mixing, drying, pulverizing, storing, preserving, and transferring substances. In the substance transfer method of this embodiment, the first substance container is used for purposes such as mixing, drying, pulverizing, and storing substances, and the second substance container is a container used to transfer the substance stored in the first substance container to another location. More specifically, it is intended that, for example, a sulfide solid electrolyte produced by a sulfide solid electrolyte production apparatus and stored in the first substance container is shipped as a product in the second substance container from which the sulfide solid electrolyte was transferred.

[0083] Regarding the substance transfer method, as an embodiment different from the substance transfer method of this embodiment, it is also possible to transfer a substance from a second substance container to a first substance container. As described above, in Figure 1, "first substance inlet portion (outlet portion)" and "first substance outlet portion (inlet portion)" are described, and the first substance inlet portion can be a first substance outlet portion, and the first substance outlet portion can be a first substance inlet portion. In this case, as shown in Figure 2, by connecting the first substance container and the second substance container via the substance transfer device of this embodiment, it is possible to transfer the substance stored in the second substance container to the first substance container.

[0084] A substance transfer method according to another embodiment of the present invention uses a transfer device for a substance containing at least one atom selected from sulfur atoms and halogen atoms, the transfer device comprising a transfer pre-chamber, a transfer substance inlet and outlet ports, and an inert gas introduction mechanism and discharge mechanism, the transfer substance inlet and outlet ports being provided in the transfer pre-chamber and connectable to the first substance inlet and first substance outlet ports of a first substance container and the second substance transfer port of a second substance container, the inert gas introduction mechanism introducing the inert gas into the transfer pre-chamber and the inert gas discharge mechanism discharging the inert gas from the transfer pre-chamber, and the method comprises the following operations (1B) to (3B): (1B) connecting the transfer substance inlet port to valve 2 provided in the second substance transfer port of the second substance container, and connecting the transfer substance outlet port to valve 1b provided in the first substance inlet port of the first substance container. (2B) The valves 1b and 2 are closed, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer preliminary chamber. (3B) The supply and discharge of the inert gas are stopped, and the valves 1b and 2 are opened, and the substance stored in the second substance container is transferred to the first substance container.

[0085] In a method for transferring a substance according to another embodiment different from the method for transferring a substance according to this embodiment, the first substance container is used for mixing, drying, grinding, storing, and the like of the substance, and the second substance container is a container used to transfer an object received at a location separate from the first substance container to the first substance container. More specifically, for example, a solid electrolyte raw material that is commercially available or produced by another manufacturing device is transferred to the second substance container, the second substance container storing the solid electrolyte raw material is connected to the first substance container via a material transfer device, and the solid electrolyte raw material is transferred from the second substance container to the first substance container and used to produce a sulfide solid electrolyte. Here, when a solid electrolyte raw material that is commercially available or produced by another manufacturing device is transferred to the second substance container, the substance may be transferred to the second substance container in accordance with the method for transferring a substance according to this embodiment.

[0086] [Method for Removing Internal Residue from a Substance Container] The method for removing internal residue from a substance container of this embodiment uses a transfer device for a substance containing at least one atom selected from sulfur atoms and halogen atoms, the transfer device comprising: a transfer preliminary chamber, a transfer substance inlet and outlet ports, and an inert gas introduction mechanism and discharge mechanism, the transfer substance inlet and outlet ports being provided in the transfer preliminary chamber and connectable to the first substance inlet and first substance outlet ports of a first substance container and the second substance transfer port of a second substance container, the inert gas introduction mechanism introducing the inert gas into the transfer preliminary chamber and the inert gas discharge mechanism discharging the inert gas from the transfer preliminary chamber, and performing the following operations (1B) and (2B): (1B) connecting the transfer substance inlet port to valve 1a provided in the substance outlet port of the first substance container. (2B) The valve 1a is opened, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer pre-chamber and the first substance container.

[0087] As described above, the method for removing internal residue from a substance container of this embodiment employs the substance transfer device of this embodiment. The configuration of the substance transfer device employed in the method for removing internal residue from a substance container of this embodiment is as described above for the substance transfer device of this embodiment.

[0088] In the method for removing internal residues from a substance container of this embodiment, the substance transfer device of this embodiment is used to carry out the above-mentioned steps (1B) and (2B). The valve 1a used in steps (1B) and (2B) is shown in Figure 1 as being provided in the first substance container and the second substance container, but it may also be a valve provided in the substance transfer device.

[0089] In addition, in the method for removing internal residues from a substance container according to this embodiment, it is preferable to introduce an inert gas through an inert gas inlet provided in the first substance container using an inert gas introduction mechanism. This makes it possible to more efficiently remove internal residues from the substance container. As a result, the substance can be handled more safely and efficiently, and the operating rate of the manufacturing equipment can be improved.

[0090] The substance transfer device, substance transfer method, and method for removing internal residue from a substance container according to the present embodiment are suitable for use in a sulfide solid electrolyte production apparatus. The sulfide solid electrolyte obtained by the sulfide solid electrolyte production apparatus has high ionic conductivity and is therefore suitable for use as a solid electrolyte or electrode composite in lithium ion batteries, particularly lithium ion batteries used in information-related devices and communication devices such as personal computers, video cameras, and mobile phones, as well as in vehicles such as automobiles, and particularly all-solid-state batteries.

Claims

1. A substance transfer device for transferring a substance containing at least one atom selected from sulfur atoms and halogen atoms, comprising: a transfer preliminary chamber; a transfer substance inlet section and a transfer substance outlet section; and an inert gas introduction mechanism and discharge mechanism, wherein the transfer substance inlet section and the transfer substance outlet section are provided in the transfer preliminary chamber and are connectable to a first substance inlet section and a first substance outlet section of a first substance container and a second substance transfer port section of a second substance container, and the inert gas introduction mechanism introduces the inert gas into the transfer preliminary chamber, and the inert gas discharge mechanism discharges the inert gas from the transfer preliminary chamber.

2. The substance transfer device according to claim 1, wherein the inert gas introduction mechanism further introduces the inert gas from an inert gas introduction port provided in the first substance container.

3. A substance transfer device according to claim 1 or 2, wherein the transfer preliminary chamber is cylindrical.

4. A substance transfer device according to claim 3, wherein the transfer substance inlet and transfer substance outlet are provided at both ends of the cylindrical transfer pre-chamber.

5. A substance transfer device according to claim 3 or 4, wherein the inert gas introduction mechanism and exhaust mechanism are provided on the side of the cylindrical transfer pre-chamber.

6. A method for transferring a substance containing at least one atom selected from sulfur atoms and halogen atoms, the method comprising: (1) connecting the transfer substance inlet port to valve 1a provided in the substance outlet port of the first substance container; and (2) connecting the transfer substance outlet port to valve 2 provided in the second substance container. (2A) The valves 1a and 2 are closed, and the inert gas is supplied and discharged by the inert gas introduction mechanism and discharge mechanism, filling the inert gas into the transfer preliminary chamber. (3A) The supply and discharge of the inert gas are stopped, and the valves 1a and 2 are opened, and the substance stored in the first substance container is transferred to the second substance container.

7. The method for transferring a substance according to claim 6, wherein the steps (3A) and (2A) are carried out, followed by the steps (4A) and (5A) below: (4A) Remove the second substance container and valve 2 from the transferred substance outlet. (5A) Attach a closing flange to the transferred substance outlet.

8. A method for removing internal residues from a substance container using a transfer device for a substance containing at least one atom selected from sulfur atoms and halogen atoms, the method comprising: a transfer prechamber; a transfer substance inlet port and a transfer substance outlet port; and an inert gas introduction mechanism and discharge mechanism; the transfer substance inlet port and transfer substance outlet port are provided in the transfer prechamber and are connectable to the first substance inlet port and first substance outlet port of a first substance container and the second substance transfer port of a second substance container; the inert gas introduction mechanism introduces inert gas into the transfer prechamber; and the inert gas discharge mechanism discharges inert gas from the transfer prechamber; and the method comprises the following operations (1B) and (2B): (1B) connecting the transfer substance inlet port to valve 1a provided in the substance outlet port of the first substance container; (2B) opening valve 1a, supplying and discharging inert gas using the inert gas introduction mechanism and discharge mechanism, and filling the inert gas into the transfer prechamber and the first substance container.

9. A method for removing internal residues from a substance container according to claim 8, wherein the inert gas introduction mechanism introduces an inert gas from an inert gas introduction port provided in the first substance container.

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