Apparatus for producing inorganic material and method for producing inorganic material

Abstract

To provide an apparatus for manufacturing an inorganic material and a method for manufacturing an inorganic material which can improve recovery yield during manufacturing and uniformize physical property values of product materials.SOLUTION: An apparatus 10 comprises: a blowing part 100 that blows inert gas; a pulverizing part 200 that repeatedly performs vitrification of a plurality of kinds of inorganic compounds as inorganic materials, by mechanical energy and blowing-up of the plurality of kinds of vitrified inorganic compounds by the inert gas blown from the blowing part 100; a first collecting part 300 into which at least portions of the plurality of kinds of inorganic compounds blown up by the inert gas intrude and which returns the at least portions of the plurality of kinds of inorganic compounds toward the pulverizing part 200; and a system S that circulates the inert gas, from the blowing part 100 through the pulverizing part 200 and the first collecting part 300 to the blowing part 100. Arithmetic average roughness measured according to JIS B 0601(2013) of a wall surface in the apparatus of the pulverizing part 200 is 0 μm or more and 0.020 μm or less.SELECTED DRAWING: Figure 1

Description

[Technical Field]

[0001] The present invention relates to an apparatus and a method for producing an inorganic material, and more particularly to an apparatus and a method for producing an inorganic material that can improve recovery yield during production and make the physical properties of the product uniform. [Background technology]

[0002] Lithium-ion batteries are commonly used as power sources for small portable devices such as mobile phones and laptops, and recently have begun to be used as power sources for electric vehicles and power storage devices in addition to small portable devices.

[0003] Currently available lithium-ion batteries use electrolytes containing flammable organic solvents. On the other hand, lithium-ion batteries that use a solid electrolyte to create an all-solid-state battery (hereinafter referred to as all-solid-state lithium-ion batteries) do not use flammable organic solvents within the battery, which allows for simplified safety devices and is thought to be superior in terms of manufacturing cost and productivity.

[0004] In recent years, sulfide solid electrolyte materials have been used as the solid electrolyte material for such lithium-ion batteries. Sulfide-based inorganic solid electrolyte materials are made primarily from lithium sulfide (Li2S) and phosphorus pentasulfide (P2S5).

[0005] P2S5 is a highly reactive, unstable ionic crystal powder that transitions to a stable state as the chemical reaction with Li2S progresses during mechanical milling, but in the process of reaching a stable state, it adheres and accumulates on the inner walls of the equipment. Various efforts have been made to prevent this adhesion and accumulation during the powder manufacturing process, including blasting, which creates fine irregularities on the surface, as described in the following patent document.

[0006] Patent Document 1 (JP 2017-119902 A) describes a titanium component that inhibits powder adhesion, characterized in that the arithmetic mean roughness (Ra) of the surface layer having an uneven surface that comes into contact with the powder is 0.4 μm or more and 2.0 μm or less, and the Vickers hardness of the surface layer is 400 or more. In addition, examples of the powders that are handled include silver particles with a median diameter of 1.5 μm, nickel particles with a median diameter of 2.5 μm, powder paint with a median diameter of 23 μm, and alumina with a median diameter of 8 μm.

[0007] Patent Document 2 (JP 2017-128101 A) describes a powder adhesion suppression member having a coating with an uneven surface that comes into contact with powder, the uneven surface having an arithmetic mean roughness (Ra) of 0.2 μm or more and 1.6 μm or less, and the coating having a Vickers hardness of 400 or more. In addition, examples of the powders that are handled include silver particles with a median diameter of 1.5 μm, copper particles with a median diameter of 22.3 μm, PTFE particles with a median diameter of 0.3 μm, and alumina particles with a median diameter of 8 μm. [Prior art documents] [Patent documents]

[0008] [Patent Document 1] Japanese Patent Application Laid-Open No. 2017-119902 [Patent Document 2] Japanese Patent Application Laid-Open No. 2017-128101 Summary of the Invention [Problem to be solved by the invention]

[0009] However, in the production of sulfide-based inorganic solid electrolyte materials, it was found that blasting, which creates fine irregularities on the inner surface of the equipment, is ineffective and results in powder adhering and accumulating on the inner wall surface of the equipment.

[0010] The present invention has been made in consideration of the above circumstances, and aims to provide an apparatus for producing inorganic materials and a method for producing inorganic materials that can prevent adhesion and accumulation of powder on the inner wall surfaces of the apparatus, improve recovery yield during production, and uniformize the physical properties of the product. [Means for solving the problem]

[0011] The present inventors have conducted extensive research to solve this problem, and as a result have found that by making the inner wall surface of the device smooth and flat with a small arithmetic mean roughness, it is possible to prevent adhesion and accumulation of powder on the inner wall surface of the device, which led to the present invention.

[0012] That is, according to the present invention, An apparatus for producing an inorganic material, comprising: a blower for sending an inert gas; a crushing section that repeats the steps of vitrifying a plurality of inorganic compounds that will become the inorganic material by mechanical energy and blowing up the vitrified plurality of inorganic compounds by the inert gas sent from the blower section; a first recovery section into which at least a portion of the inorganic compounds blown up by the inert gas enters and which returns the at least a portion of the inorganic compounds toward the pulverization section; a system for circulating the inert gas from the blower section to the blower section via the pulverizer section and the first recovery section; An apparatus comprising: The arithmetic mean roughness Ra of the inner wall surface of the grinding section measured in accordance with JIS B 0601 (2013) is 0 μm or more and 0.020 μm or less. is provided.

[0013] Further, according to the present invention, 1. A method for producing an inorganic material, comprising: Sending the inert gas by a blower; a grinding unit repeating the steps of: vitrifying a plurality of inorganic compounds to be the inorganic material by mechanical energy; and blowing up the vitrified plurality of inorganic compounds by the inert gas sent from the blower unit; Returning at least a portion of the plurality of inorganic compounds blown up by the inert gas and entering the first recovery section from the first recovery section toward the pulverization section; circulating the inert gas from the blower section to the blower section via the pulverizer section and the first recovery section; A method including is provided. [Effects of the Invention]

[0014] According to the present invention, it is possible to provide an apparatus for producing an inorganic material and a method for producing an inorganic material that can improve the recovery yield during production and make the physical properties of the product uniform. [Brief explanation of the drawings]

[0015] [Figure 1] 1 illustrates an apparatus according to an embodiment. [Figure 2] 2 is a top view of a rotary table and a plurality of balls in the grinding section shown in FIG. 1. FIG. [Figure 3] 3 is a cross-sectional view taken along the line AA′ of FIG. 2. [Figure 4] FIG. 4 is a diagram showing a modification of FIG. 3. [Figure 5] FIG. 1 is a schematic diagram showing a sieving test according to the present embodiment. [Figure 6] 1A and 1B are schematic diagrams showing a sieving test and a pressing test according to the present embodiment. [Figure 7] FIG. 1 is a schematic diagram showing a pressing test according to the present embodiment. [Figure 8] FIG. 1 is a schematic diagram showing a pressing test according to the present embodiment. DETAILED DESCRIPTION OF THE INVENTION

[0016] Hereinafter, embodiments of the present invention will be described with reference to the drawings. In all the drawings, like components are designated by like reference numerals, and the description thereof will be omitted as appropriate.

[0017] FIG. 1 is a diagram showing an apparatus 10 according to an embodiment. FIG. 2 is a top view of a rotary table 212 and a plurality of balls 214 of the grinding section 200 shown in FIG. 1. FIG. 3 is a cross-sectional view taken along line AA' in FIG. 2. The apparatus 10 produces an inorganic material (A) from a plurality of inorganic compounds (A1). In FIG. 1, the upward direction in FIG. 1 is the upward direction in the vertical direction, and the downward direction in FIG. 1 is the downward direction in the vertical direction. For the sake of explanation, the pressing section 216 is not shown in FIG. 2. The black arrows in FIG. 3 indicate the flow of the plurality of inorganic compounds (A1). The white arrows in FIG. 3 indicate the flow of an inert gas.

[0018] An overview of the apparatus 10 will be described using FIG. 1. The apparatus 10 includes a blower 100, a pulverizer 200, a first recovery unit 300, and a system S. The blower 100 sends an inert gas. The pulverizer 200 repeatedly vitrifies a plurality of inorganic compounds (A1) using mechanical energy and blows the vitrified inorganic compounds (A1) upward with the inert gas sent from the blower 100. At least a portion of the inorganic compounds (A1) blown upward by the inert gas enters the first recovery unit 300. The first recovery unit 300 returns the at least a portion of the inorganic compounds (A1) toward the pulverizer 200. The system S (e.g., a pipe Pa, a buffer tank 110, a pipe Pb, a pipe Pc, and a pipe Pi, which will be described later) circulates the inert gas from the blower 100 to the blower 100 via the pulverizer 200 and the first recovery unit 300.

[0019] In this case, by reducing the arithmetic mean roughness Ra of the inner wall surface of the grinding section 200, it is possible to prevent adhesion and deposition of powder on the inner wall surface of the apparatus, thereby making it possible to produce an inorganic material that can improve recovery yield during production and uniform the physical properties of the product. Specifically, the upper limit of the arithmetic mean roughness Ra of the inner wall surface of the crushing section 200 measured in accordance with JIS B 0601 (2013) is 0.02 μm, more preferably 0.015 μm, even more preferably 0.01 μm, and particularly preferably 0.005 μm. The lower limit of the arithmetic mean roughness Ra of the inner wall surface of the pulverizing section 200 is not particularly limited, but is, for example, 0 μm or more, 0.001 μm or more, or 0.003 μm or more.

[0020] Conventional anti-adhesion techniques, such as blasting, create fine irregularities on the surface, but this has been shown to be ineffective when it comes to the raw material powder mixture of sulfide-based inorganic solid electrolyte materials. While the reason for this is unclear, one possible explanation is that P2S5, the raw material for sulfide-based inorganic solid electrolyte materials, is a highly reactive and unstable ionic crystal powder that has a high chemical affinity with the metal plates used on the inner walls of the equipment. The fine irregularities on the surface of the metal plates used on the inner walls of the equipment increase the surface area of ​​the inner walls, which is thought to result in the raw material powder mixture of sulfide-based inorganic solid electrolyte materials strongly adhering and accumulating on the inner walls of the equipment.

[0021] On the other hand, in the device according to the present embodiment, the surface area of ​​the inner wall surface of the device is reduced by making the surface of the metal plate used for the inner wall surface of the device smooth by minimizing the fine irregularities, and it is possible to make it difficult for the chemical reaction between the raw material mixed powder of the sulfide-based inorganic solid electrolyte material and the metal plate to proceed. As a result, it is thought that adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the device can be prevented. Such a smooth surface can be obtained by subjecting the surface of the metal plate to a known polishing treatment, such as buffing.

[0022] Furthermore, in the apparatus according to this embodiment, the upper limit of the maximum height Rz of the inner wall surface of the pulverization section 200 measured in accordance with JIS B 0601 (2013) is preferably 0.16 μm, more preferably 0.13 μm, even more preferably 0.10 μm, and particularly preferably 0.05 μm. By setting the maximum height Rz of the inner wall surface of the pulverization section 200 to the above upper limit or less, adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the apparatus can be more suitably prevented, improving the recovery yield during production and making it possible to uniformize the physical properties of the product. The lower limit of the maximum height Rz of the inner wall surface of the pulverizing section 200 is not particularly limited, but is, for example, 0 μm or more, 0.01 μm or more, or 0.03 μm or more.

[0023] In the apparatus according to this embodiment, the upper limit of the ten-point mean roughness Rzjis of the inner wall surface of the pulverizing section 200 measured in accordance with JIS B 0601 (2013) is preferably 0.14 μm, more preferably 0.10 μm, even more preferably 0.07 μm, and particularly preferably 0.04 μm. By setting the ten-point mean roughness Rzjis of the inner wall surface of the pulverizing section 200 to the above upper limit or less, adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the apparatus can be more suitably prevented, improving the recovery yield during production and making it possible to uniformize the physical properties of the product. The lower limit of the ten-point average roughness Rzjis of the inner wall surface of the pulverizing section 200 is not particularly limited, but is, for example, 0 μm or more, 0.01 μm or more, or 0.03 μm or more.

[0024] The structure of the device 10 will be described with reference to FIG.

[0025] The apparatus 10 includes a blower section 100, a buffer tank 110, a pulverizer section 200, a first recovery section 300, a first storage section 310, a second recovery section 400, a second storage section 410, a pressure reducing section 500, a pipe Pa, a plurality of pipes Pb (fifth pipe), a pipe Pc (second pipe), a pipe Pd (sixth pipe), a pipe Pe (first pipe), a pipe Pf (third pipe), a pipe Pg, a pipe Ph (fourth pipe), a pipe Pi, a pipe Pj, a pipe Pk, a pipe Pl, a pipe Pm, a pipe Pn, a pipe Po, a valve Va1, and a plurality of valves Vb 1 (fifth valve), valve Vc1, valve Vc2 (second valve), valve Vc3, valve Vd1 (sixth valve), valve Ve1 (first valve), valve Ve2, valve Vf1 (third valve), valve Vg1, valve Vh1, valve Vh2, valve Vi1, valve Vi2, valve Vj1, valve Vk1, valve Vl1, valve Vm1, valve Vn1, valve Vo1, line Le (first line), line Lh (second line), and exhaust duct D.

[0026] The pipe Pa is connected to the gas outlet 104 of the blower 100 and the gas inlet 112 of the buffer tank 110. The valve Va1 is provided on the pipe Pa.

[0027] Each of the multiple pipes Pb is connected to each of the multiple gas outlets 114 of the buffer tank 110 and each of the multiple gas inlets 202 of the pulverization section 200. Each of the multiple valves Vb1 is provided on each of the multiple pipes Pb. In one example, when viewed from above the turntable 212 (described in detail below) of the pulverization section 200, the multiple pipes Pb are arranged around the turntable 212, and more specifically, are arranged rotationally symmetrically with respect to the center of the turntable 212 (the rotation axis R described below).

[0028] The pipe Pc communicates with the material discharge pipe 206 of the pulverization section 200 and the suction port 302 of the first recovery section 300. Valves Vc1, Vc2, and Vc3 are provided on the pipe Pc, and are arranged in this order from the material discharge pipe 206 of the pulverization section 200 to the suction port 302 of the first recovery section 300.

[0029] The pipe Pd communicates with the material supply pipe 204 of the pulverizing section 200 and the material discharge port 304 of the first recovery section 300. A valve Vd1 is provided on the pipe Pd.

[0030] The pipe Pe communicates with the first storage unit 310 and the material supply port 308 of the first recovery unit 300. The valves Ve1 and Ve2 are provided on the pipe Pe, and are arranged in this order from the first storage unit 310 to the material supply port 308 of the first recovery unit 300. The valve Ve1 is detachably attached to the pipe Pe along with the first storage unit 310. In other words, when the valve Ve1 is removed from the pipe Pe, the first storage unit 310 and the valve Ve1 can be integrated. The pipe Pe is also connected to a line Le between the valves Ve1 and Ve2. The interior of the pipe Pe can be evacuated or replaced with an inert gas via the line Le. That is, the line Le can reduce the pressure inside the pipe Pe and introduce an inert gas into the pipe Pe.

[0031] The pipe Pf communicates with a portion of the pipe Pc located between the valve Vc1 and the valve Vc2 (i.e., between the crushing section 200 and the valve Vc2) and with the suction port 402 of the second recovery section 400. The valve Vf1 is provided in the pipe Pf.

[0032] The pipe Pg communicates with a portion of the pipe Pc located between the valve Vc2 and the valve Vc3, and with the gas exhaust pipe 406 of the second recovery section 400. The valve Vg1 is provided in the pipe Pg.

[0033] The pipe Ph communicates with the second storage unit 410 and the material discharge port 404 of the second recovery unit 400. The valves Vh1 and Vh2 are provided on the pipe Ph, and are arranged in this order from the second storage unit 410 to the material discharge port 404 of the second recovery unit 400. The pipe Ph is further connected to a line Lh between the valves Vh1 and Vh2. The inside of the pipe Ph can be evacuated or replaced with an inert gas via the line Lh. That is, the line Lh can reduce the pressure inside the pipe Ph and can also introduce an inert gas into the pipe Ph.

[0034] The pipe Pi communicates with the gas exhaust port 306 of the first collection unit 300 and the gas inlet 102 of the blower unit 100. The valves Vi1 and Vi2 are provided on the pipe Pi, and are arranged in this order from the gas exhaust port 306 of the first collection unit 300 to the gas inlet 102 of the blower unit 100.

[0035] The pipe Pj is connected to a portion of the pipe Pi located between the gas outlet 306 of the first recovery unit 300 and the valve Vi1, and to a portion of the pipe Pi located between the gas inlet 102 of the blower unit 100 and the valve Vi2. The valve Vj1 is provided in the pipe Pj.

[0036] The pipe Pk communicates with the adjustment port 116 of the buffer tank 110 and the exhaust duct D. A valve Vk1 is provided on the pipe Pk.

[0037] The pipe Pl is connected to the gas outlet 208 of the pulverizing section 200 and the pressure reducing section 500. A valve Vl1 is provided on the pipe Pl.

[0038] The pipe Pm communicates with the pressure reducing section 500 and the exhaust duct D. The valve Vm1 is provided in the pipe Pm.

[0039] The pipe Pn communicates with a portion of the pipe Pl located between the gas outlet 208 of the grinding section 200 and the valve Vl1, and with the exhaust duct D. The valve Vn1 is provided in the pipe Pn.

[0040] The pipe Po branches off from the pipe Pi and communicates with the exhaust duct D. Specifically, the pipe Pi has a portion that connects to an end of the pipe Pj that is located between the valve Vi2 and the gas inlet 102 of the blower 100. The pipe Po communicates with a portion of the pipe Pi that is located between the portion of the pipe Pi and the gas inlet 102 of the blower 100, and with the exhaust duct D. The valve Vo1 is provided in the pipe Po.

[0041] The blower 100 draws in gas from the pipe Pj through a gas inlet 102 of the blower 100. The blower 100 also discharges the gas drawn in through the gas inlet 102 of the blower 100 through a gas outlet 104 of the blower 100. In this way, the blower 100 sends gas to the buffer tank 110 via the pipe Pa. The rotation speed of the motor of the blower 100 can be changed by an inverter 106, and the flow rate of gas sent from the blower 100 can be changed as desired depending on the rotation speed of the motor.

[0042] Gas sent from the blower section 100 via piping Pa enters the gas inlet 112 of the buffer tank 110. The gas that has entered the buffer tank 110 passes through multiple gas outlets 114 of the buffer tank 110 and is sent to the pulverization section 200 via multiple piping Pb. The pressure of the gas inside the buffer tank 110 is adjusted by a valve Vk1.

[0043] Gas sent from the buffer tank 110 via multiple pipes Pb enters the multiple gas inlets 202 of the pulverizing section 200. Material sent from the first storage section 310 via pipe Pe, the first recovery section 300, and pipe Pd enters the material supply pipe 204 of the pulverizing section 200. At least a portion of the material and at least a portion of the gas inside the pulverizing section 200 are discharged from the material discharge pipe 206 of the pulverizing section 200. The pressure inside the pulverizing section 200 can be reduced by the pressure reduction section 500. In addition, the gas inside the pulverizing section 200 can be discharged to the exhaust duct D via pipe Pn.

[0044] The first collection unit 300 sucks the material and gas in the pipe Pc through the suction port 302 of the first collection unit 300. The first collection unit 300 also discharges the material sucked through the suction port 302 of the first collection unit 300 from the material discharge port 304 of the first collection unit 300. In this way, the first collection unit 300 sends the material to the pulverization unit 200 via the pipe Pd. The first collection unit 300 also discharges the gas sucked through the suction port 302 of the first collection unit 300 from the gas discharge port 306 of the first collection unit 300. In this way, the first collection unit 300 sends the gas to the blower unit 100 via the pipe Pi. The first collection unit 300 is, for example, a dust collector.

[0045] The second recovery unit 400 sucks the material and gas in the pipes Pc and Pf through a suction port 402 of the second recovery unit 400. The second recovery unit 400 also discharges the material sucked through the suction port 402 of the second recovery unit 400 from a material discharge port 404 of the second recovery unit 400. In this manner, the second recovery unit 400 sends the material to the second storage unit 410 via the pipe Ph. The second recovery unit 400 also discharges the gas sucked through the suction port 402 of the second recovery unit 400 from a gas discharge pipe 406 of the second recovery unit 400. The second recovery unit 400 is, for example, a cyclone dust collector.

[0046] Here, in the apparatus according to this embodiment, it is preferable that the inner wall surface of the apparatus in the portion through which the powder can pass is a smooth surface with a small arithmetic mean roughness. By adopting the above configuration, adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the apparatus can be more effectively prevented, improving the recovery yield during production and making the physical properties of the product uniform. Note that examples of portions through which the powder can pass include the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe. Specifically, the upper limit of the arithmetic mean roughness Ra of the inner wall surface of the apparatus in one or more parts selected from the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe, as measured according to JIS B 0601 (2013), is preferably 0.02 μm, more preferably 0.015 μm, even more preferably 0.01 μm, and particularly preferably 0.005 μm. By setting the arithmetic mean roughness Ra to the upper limit or less, adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the apparatus can be more suitably prevented, improving the recovery yield during production and uniforming the physical properties of the product. The lower limit of the arithmetic mean roughness Ra is not particularly limited, but is, for example, 0 μm or more, 0.001 μm or more, or 0.003 μm or more.

[0047] In the apparatus according to this embodiment, the upper limit of the maximum height Rz measured according to JIS B 0601 (2013) of the inner wall surface of the apparatus in one or more parts selected from the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe is preferably 0.16 μm, more preferably 0.13 μm, even more preferably 0.10 μm, and particularly preferably 0.05 μm. By setting the maximum height Rz to be equal to or less than the upper limit, adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the apparatus can be more suitably prevented, improving the recovery yield during production and uniforming the physical properties of the product. The lower limit of the maximum height Rz is not particularly limited, but is, for example, 0 μm or more, 0.01 μm or more, or 0.03 μm or more.

[0048] In the apparatus according to this embodiment, the upper limit of the ten-point mean roughness Rzjis measured according to JIS B 0601 (2013) of the inner wall surface of the apparatus in one or more sections selected from the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe is preferably 0.14 μm, more preferably 0.10 μm, even more preferably 0.07 μm, and particularly preferably 0.04 μm. By setting the ten-point mean roughness Rzjis to be equal to or less than the upper limit, adhesion and deposition of the raw material mixed powder of the sulfide-based inorganic solid electrolyte material on the inner wall surface of the apparatus can be more suitably prevented, improving the recovery yield during production and uniforming the physical properties of the product. The lower limit of the ten-point average roughness Rzjis is not particularly limited, but is, for example, 0 μm or more, 0.01 μm or more, or 0.03 μm or more.

[0049] Next, the structure of the crushing section 200 will be described with reference to FIGS.

[0050] The crushing unit 200 has a rotary table 212, a plurality of balls 214, and a pressing unit 216. In the example shown in Fig. 2, the number of the plurality of balls 214 is seven. However, the number of the plurality of balls 214 is not limited to the example shown in Fig. 2.

[0051] The turntable 212 is rotatable around a rotation axis R. The rotation axis R of the turntable 212 passes through the center of the turntable 212 along the height direction (thickness direction) of the turntable 212. The height direction (thickness direction) of the turntable 212 is aligned with the vertical direction. The plurality of balls 214 are arranged around the rotation axis R of the turntable 212, and more specifically, are arranged rotationally symmetrically with respect to the rotation axis R. The plurality of balls 214 rotate with the rotation of the turntable 212. Each of the plurality of balls 214 is rotatable around a rotation axis R1 that rotates with the rotation of the turntable 212. The rotation axis R1 of each ball 214 passes through the center of the ball 214 along the height direction (thickness direction) of the ball 214. The height direction (thickness direction) of the ball 214 is aligned with the vertical direction. The pressing unit 216 presses the plurality of balls 214 toward the turntable 212 from the opposite side of the turntable 212.

[0052] Next, an example of a method for producing an inorganic material (A) from a plurality of inorganic compounds (A1) using the apparatus 10 will be described with reference to FIGS.

[0053] Valves Ve1 and Ve2 are closed, and the multiple inorganic compounds (A1) are placed in the first storage unit 310. Specifically, first, the first storage unit 310 and valve Ve1 are removed from the pipe Pe. Next, the multiple inorganic compounds (A1) are placed in the first storage unit 310. The multiple inorganic compounds (A1) are placed in an inert gas-controlled atmosphere (e.g., in a glove box). Next, with valve Ve1 closed, the first storage unit 310 and valve Ve1 are attached to the pipe Pe. In this case, even if the first storage unit 310 and valve Ve1 are exposed to the atmosphere, the multiple inorganic compounds (A1) in the first storage unit 310 are not exposed to the atmosphere (air) because valve Ve1 is closed. Furthermore, any atmosphere that has entered the pipe Pe during installation of the first storage unit 310 can be replaced with an inert gas through line Le connected to the pipe Pe. This prevents the inorganic compound (A1) from being exposed to the atmosphere (air) when it passes through the pipe Pe. Next, the valves Ve1, Ve2, and Vd1 are opened to send the multiple types of inorganic compounds (A1) from the first storage unit 310 to the pulverization unit 200 via the pipe Pe, the first recovery unit 300, and the pipe Pd. That is, the first storage unit 310 stores the multiple types of inorganic compounds (A1) to be supplied to the pulverization unit 200.

[0054] Furthermore, valves Ve1, Ve2, Vf1, Vg1, Vh1, Vh2, Vj1, Vl1, Vm1, Vn1, and Vo1 are closed, and valves Va1, Vb1, Vc1, Vc2, Vc3, Vd1, Vi1, and Vi2 are opened to supply inert gas to the portion of pipe Pi located between valves Vi1 and Vi2. Next, the blower 100 is operated while adjusting the pressure inside the buffer tank 110 with valve Vk1. As a result, system S, i.e., the system from blower 100 through pipe Pa, buffer tank 110, pipe Pb, pulverizer 200, pipe Pc, first recovery section 300, and pipe Pi to blower 100, circulates inert gas and is closed from the outside (i.e., system S is not exposed to the atmosphere (air)).

[0055] The supply of the inert gas to the portion of the pipe Pi located between the valves Vi1 and Vi2 may be carried out before or after the supply of the plurality of inorganic compounds (A1) from the first storage unit 310 to the pulverization unit 200, or may be carried out while the plurality of inorganic compounds (A1) are being supplied from the first storage unit 310 to the pulverization unit 200. The position to which the inert gas is supplied does not have to be the portion of the pipe Pi located between the valves Vi1 and Vi2, and may be any portion of the system S. Furthermore, the inert gas may be supplied to multiple portions of the system S (including the portion of the pipe Pi located between the valves Vi1 and Vi2).

[0056] In this embodiment, the inert gas introduced is, for example, nitrogen gas. The nitrogen gas is supplied, for example, from a nitrogen cylinder via a nitrogen purification device. In this example, the impurity concentration (e.g., moisture concentration or oxygen concentration) of the nitrogen gas can be reduced. For example, the moisture concentration of the nitrogen gas can be reduced to 400 ppm or less, preferably 40 ppm or less, and more preferably 2 ppm or less, and the oxygen concentration of the nitrogen gas can be reduced to 400 ppm or less, preferably 40 ppm or less, and more preferably 2 ppm or less. However, the inert gas may be a gas other than nitrogen gas, such as argon gas.

[0057] Furthermore, the pulverizing section 200 is operated. Specifically, the turntable 212 is rotated about the rotation axis R, the balls 214 are rotated about the rotation axis R1, and the pressing section 216 presses the plurality of balls 214 toward the turntable 212. The operation of the pulverizing section 200 may be started before or after the supply of the plurality of inorganic compounds (A1) from the first storage section 310 to the pulverizing section 200, or may be started while the plurality of inorganic compounds (A1) are being supplied from the first storage section 310 to the pulverizing section 200. The pulverizing section 200 repeatedly vitrifies the plurality of inorganic compounds (A1) by mechanical energy and blows up the vitrified plurality of inorganic compounds (A1) with the inert gas sent from the blower section 100, as follows.

[0058] First, as shown by the black arrows extending from the material supply pipe 204 toward the turntable 212 in Figure 3, multiple types of inorganic compounds (A1) supplied from the first storage section 310 pass through the material supply pipe 204 and reach the center of the turntable 212 or its periphery (rotation axis R and its periphery).

[0059] Thereafter, as indicated by the two black arrows extending from both sides around the center (rotation axis R) of the turntable 212 in FIG. 3 , the multiple inorganic compounds (A1) move from the center (rotation axis R) of the turntable 212 toward the balls 214 due to centrifugal force generated by the rotation of the turntable 212, and enter the gap between the turntable 212 and the balls 214. The multiple inorganic compounds (A1) that have entered the gap between the turntable 212 and the balls 214 are vitrified by mechanical energy. Specifically, shear stress and compressive stress are applied to the multiple inorganic compounds (A1) that have entered the gap between the turntable 212 and the balls 214 by the rotation of the balls 214 and the pressing of the balls 214 against the turntable 212 by the pressing unit 216. The multiple inorganic compounds (A1) are vitrified by the shear stress and compressive stress. In other words, the multiple inorganic compounds (A1) are subjected to mechanical milling.

[0060] As shown by the two white arrows on either side of the turntable 212, the plurality of balls 214, and the pressing unit 216 in Figure 3, a flow of inert gas is generated outside the turntable 212 from below to above the pulverizing unit 200. This flow is generated by inert gas sent from the blower unit 100 via the gas inlet 202 of the pulverizing unit 200. As shown by the two black arrows on either side of the plurality of balls 214 and the pressing unit 216 in Figure 3, the vitrified inorganic compounds (A1) are blown upward by the inert gas. At this time, the rotation speed of the motor of the blower unit 100 is kept low by the inverter 106, which keeps the flow rate of the inert gas sent from the blower unit 100 to the pulverizing unit 200 low and prevents as much of the inorganic compounds (A1) from escaping through the material discharge pipe 206 as possible.

[0061] 3, as indicated by two black arrows extending from the outside of the turntable 212 toward the center of the turntable 212 above the pressing unit 216, some of the multiple inorganic compounds (A1) blown up by the inert gas move from the outside of the turntable 212 toward the center of the turntable 212 above the pressing unit 216. Similar to the multiple inorganic compounds (A1) supplied from the material supply pipe 204, these multiple inorganic compounds (A1) reach the center of the turntable 212 or its periphery (rotation axis R and its periphery). Thereafter, the multiple inorganic compounds (A1) are subjected to mechanical milling in the same manner as described above.

[0062] As shown by the two black arrows extending above the pressing unit 216 in FIG. 3 , some of the inorganic compounds (A1) blown up by the inert gas may enter the material discharge pipe 206 without returning to the turntable 212. For example, inorganic compounds (A1) with small particle sizes tend to enter the material discharge pipe 206 without returning to the turntable 212. The inorganic compounds (A1) that have entered the material discharge pipe 206 are sent to the first recovery unit 300 via the pipe Pc, and from the first recovery unit 300 are sent to the material supply pipe 204 of the pulverization unit 200 via the pipe Pd, and then returned to the turntable 212. Therefore, even the inorganic compounds (A1) that have entered the material discharge pipe 206 can be subjected to mechanical milling again by the pulverization unit 200.

[0063] During the mechanical milling in the pulverizing section 200, as described above, the system S, i.e., the system from the blower section 100 via the pipe Pa, the buffer tank 110, the pipe Pb, the pulverizing section 200, the pipe Pc, the first recovery section 300, and the pipe Pi to the blower section 100, circulates an inert gas and is closed from the outside. Therefore, it is possible to reduce contact between the plural kinds of inorganic compounds (A1) and the air.

[0064] The plurality of inorganic compounds (A1) are subjected to mechanical milling in the pulverizing section 200, whereby the plurality of inorganic compounds (A1) are vitrified, and an inorganic material (A) is produced from the plurality of inorganic compounds (A1).

[0065] Next, an example of a method for taking out the inorganic material (A) from the device 10 will be described.

[0066] Valve Vc2 is closed, valves Vf1 and Vg1 are opened, and the inverter 106 connected to the motor of the blower 100 is controlled to increase the rotation speed of the motor of the blower 100, thereby increasing the flow rate of the inert gas sent to the gas inlet 202 of the pulverizer 200 (at this stage, valves Vh1 and Vh2 are closed). By increasing the flow rate of the inert gas sent to the gas inlet 202 of the pulverizer 200, the inorganic material (A) blown up by the inert gas in the pulverizer 200 is sent into the material discharge pipe 206 with little or no material returning to the turntable 212. The inorganic material (A) sent into the material discharge pipe 206 passes through pipes Pc and Pf and enters the suction port 402 of the second recovery unit 400. As a result, the inorganic material (A) is recovered by the second recovery unit 400. Next, valves Vh1 and Vh2 are opened. As a result, the inorganic material (A) recovered by the second recovery unit 400 flows into the second storage unit 410 via the pipe Ph. Next, valves Vh1 and Vh2 are closed. Next, the second storage unit 410 is removed from the pipe Ph. In this case, since valves Vh1 and Vh2 are closed, the inside of the pipe Ph can be prevented from being exposed to the atmosphere (air). When the second storage unit 410 is reattached to the pipe Ph, the atmosphere that has entered the pipe Ph can be replaced with an inert gas in the line Lh connected to the pipe Ph. This prevents the inorganic material (A) from being exposed to the atmosphere (air) as it passes through the pipe Ph.

[0067] Next, an example of the operation of the pressure reducing unit 500 will be described.

[0068] The inside of the pulverization unit 200 may be exposed to the atmosphere (gas), for example, when cleaning the internal parts of the pulverization unit 200 (for example, the turntable 212, the ball 214, or the pressing unit 216). In this case, the air inside the pulverization unit 200 can be removed by reducing the pressure inside the pulverization unit 200 using the decompression unit 500. For example, the decompression unit 500 can be operated by closing the multiple valves Vb1, Vc1, Vd1, and Vn1 and opening the valves Vl1 and Vm1.

[0069] By heating the inorganic material (A), an inorganic material (B) with improved crystallinity can be produced. The inorganic material (B) is not particularly limited, but examples thereof include an inorganic solid electrolyte material, a positive electrode active material, and a negative electrode active material.

[0070] The inorganic solid electrolyte material is not particularly limited, but examples thereof include sulfide-based inorganic solid electrolyte materials, oxide-based inorganic solid electrolyte materials, and other lithium-based inorganic solid electrolyte materials. Among these, sulfide-based inorganic solid electrolyte materials are preferred. Furthermore, the inorganic solid electrolyte material is not particularly limited, but examples thereof include those used in solid electrolyte layers constituting all-solid-state lithium ion batteries.

[0071] Examples of sulfide-based inorganic solid electrolyte materials include Li2S-P2S5 materials, Li2S-SiS2 materials, Li2S-GeS2 materials, Li2S-Al2S3 materials, Li2S-SiS2-Li3PO4 materials, Li2S-P2S5-GeS2 materials, Li2S-Li2O-P2S5-SiS2 materials, Li2S-GeS2-P2S5-SiS2 materials, Li2S-SnS2-P2S5-SiS2 materials, Li2S-P2S5-Li3N materials, and Li2S 2+X Examples of suitable lithium sulfide materials include LiS-P4S3 materials and LiS-P2S5-P4S3 materials. Among these, LiS-P2S5 materials and LiS-P2S5-Li3N materials are preferred due to their excellent lithium ion conductivity and stability over a wide voltage range, preventing decomposition. Here, for example, the LiS-P2S5 material refers to an inorganic material obtained by chemically reacting an inorganic composition containing at least LiS (lithium sulfide) and P2S5 with mechanical energy, and the LiS-P2S5-Li3N material refers to an inorganic material obtained by chemically reacting an inorganic composition containing at least LiS (lithium sulfide), P2S5, and Li3N with mechanical energy. In this embodiment, lithium sulfide also includes lithium polysulfide.

[0072] Examples of oxide-based inorganic solid electrolyte materials include NASICON-type materials such as LiTi2(PO4)3, LiZr2(PO4)3, and LiGe2(PO4)3, perovskite-type materials such as (La 0.5+x Li 0.5-3x )TiO3, Li2O-P2O5 materials, Li2O-P2O5-Li3N materials, and the like.

[0073] Examples of other lithium-based inorganic solid electrolyte materials include LiPON, LiNbO3, LiTaO3, Li3PO4, LiPO 4-x N x (where x is 0 < x ≤ 1), LiN, LiI, LISICON, and the like. Furthermore, glass ceramics obtained by precipitating crystals of these inorganic solid electrolytes can also be used as inorganic solid electrolyte materials.

[0074] Sulfide-based inorganic solid electrolyte materials preferably contain Li, P, and S as constituent elements. Also, from the perspective of further improving lithium ion conductivity, electrochemical stability, stability in moisture and air, and handleability, etc., the molar ratio of the content of Li to the content of P (Li / P) in the solid electrolyte material is preferably 1.0 or more and 10.0 or less, more preferably 2.0 or more and 5.0 or less, still more preferably 2.5 or more and 4.0 or less, even more preferably 2.8 or more and 3.6 or less, even more preferably 3.0 or more and 3.5 or less, even more preferably 3.1 or more and 3.4 or less, particularly preferably 3.1 or more and 3.3 or less. Also, the molar ratio of the content of S to the content of P (S / P) is preferably 1.0 or more and 10.0 or less, more preferably 2.0 or more and 6.0 or less, still more preferably 3.0 or more and 5.0 or less, even more preferably 3.5 or more and 4.5 or less, even more preferably 3.8 or more and 4.2 or less, even more preferably 3.9 or more and 4.1 or less, particularly preferably 4.0. Here, the contents of Li, P, and S in the solid electrolyte material can be determined, for example, by ICP emission spectroscopic analysis or X-ray photoelectron spectroscopy.

[0075] The shape of the inorganic solid electrolyte material can be, for example, particulate. The particulate inorganic solid electrolyte material is not particularly limited, but preferably has an average particle diameter d 50 However, the average particle diameter d of the inorganic solid electrolyte material is preferably 1 μm or more and 100 μm or less, more preferably 3 μm or more and 80 μm or less, and further preferably 5 μm or more and 60 μm or less. 50 By setting the value of the thickness of the solid electrolyte membrane to within the above range, good handling properties can be maintained and the lithium ion conductivity of the resulting solid electrolyte membrane can be further improved.

[0076] The positive electrode active material is not particularly limited, and examples thereof include positive electrode active materials that can be used in the positive electrode layer of a lithium ion battery. For example, lithium cobalt oxide (LiCoO), lithium nickel oxide (LiNiO), lithium manganese oxide (LiMnO), solid solution oxide (LiMnO-LiMO (M=Co, Ni, etc.)), lithium manganese nickel oxide (LiNi 1 / 3 Mn 1 / 3 Co 1 / 3Examples of suitable cathode active materials include composite oxides such as olivine-type lithium phosphate oxide (LiFePO4), CuS, Li-Cu-S compounds, TiS2, FeS, MoS2, V2S5, Li-Mo-S compounds, Li-Ti-S compounds, Li-VS compounds, and Li-Fe-S compounds. Among these, sulfide-based cathode active materials are preferred, with Li-Mo-S compounds, Li-Ti-S compounds, and Li-VS compounds being more preferred, due to their higher discharge capacity density and superior cycle characteristics. Li-Mo-S compounds contain Li, Mo, and S as constituent elements and can be obtained by chemically reacting inorganic compositions containing molybdenum sulfide and lithium sulfide, which are raw materials, with each other using mechanical energy. Li-Ti-S compounds contain Li, Ti, and S as constituent elements and can be obtained by chemically reacting inorganic compositions containing titanium sulfide and lithium sulfide, which are raw materials, with each other using mechanical energy. Li-VS compounds contain Li, V, and S as constituent elements, and are usually obtained by chemically reacting inorganic compositions containing vanadium sulfide and lithium sulfide, which are raw materials, with each other using mechanical energy.

[0077] The negative electrode active material is not particularly limited, and examples thereof include negative electrode active materials that can be used in the negative electrode layer of a lithium ion battery. Examples include metal-based materials mainly composed of lithium alloys, tin alloys, silicon alloys, gallium alloys, indium alloys, aluminum alloys, etc.; lithium titanium composite oxides (e.g., Li4Ti5O 12 ); graphite-based materials, etc.

[0078] The multiple inorganic compounds (A1) include materials that can be converted into the inorganic material (B) by mechanical milling and heating. For example, the multiple inorganic compounds (A1) contain Li element.

[0079] FIG. 4 is a diagram showing a modification of FIG.

[0080] The pulverizing unit 200 further includes a cover unit 220. The cover unit 220 is located above the pressing unit 216. As shown by the white arrows extending along the cover unit 220 in FIG. 4 , the cover unit 220 directs the flow of the inert gas blowing up the multiple inorganic compounds (A1) toward the center of the pulverizing unit 200 (the rotation axis R of the turntable 212) and below the pulverizing unit 200. In this case, compared to when the cover unit 220 is not provided, the amount of the multiple inorganic compounds (A1) blown up by the inert gas and entering the material discharge pipe 206 can be reduced, and the amount of the multiple inorganic compounds (A1) blown up by the inert gas and returning to the turntable 212 can be increased. Therefore, the efficiency of mechanical milling in the pulverizing unit 200 can be improved compared to when the cover unit 220 is not provided.

[0081] Although the embodiments of the present invention have been described above with reference to the drawings, these are merely examples of the present invention, and various other configurations can also be adopted.

[0082] For example, in this embodiment, the pulverizing unit 200 presses the balls 214 against the turntable 212 by the pressing unit 216. However, the pressing unit 216 may press a roller against the turntable 212 instead of the balls 214. Even in this case, the pulverizing unit 200 can perform mechanical milling on multiple types of inorganic compounds (A1). [Example]

[0083] EXAMPLES The present invention will be described below with reference to examples and comparative examples, but the present invention is not limited to these.

[0084] [1] Raw material mixture powder of sulfide-based inorganic solid electrolyte material The raw materials used were Li2S (manufactured by Furukawa Co., Ltd., purity 99.9%), P2S5 (manufactured by Kanto Chemical Co., Ltd.), and Li3N (manufactured by Furukawa Co., Ltd.). These powders were mixed in a molar ratio of 71.0:23.7:5.3 to obtain a raw material mixed powder for a sulfide-based inorganic solid electrolyte material.

[0085] [2] Test piece If good results were obtained for the adhesion and deposition of the raw material mixed powder on a plate made of the same material as the inner wall surface of the device, it is expected that similar results would be obtained within the device of this embodiment. Therefore, a test piece representing the inner wall surface of the device was prepared using SUS304, the same material as the inner wall surface of the device. The method for preparing the test piece is described below.

[0086] Example 1 A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive to create test piece 1. After buffing, the surface of test piece 1 was measured in accordance with JIS B 0601 (2013) to find that the arithmetic mean roughness Ra was 0.005 μm, the maximum height Rz was 0.030 μm, and the ten-point mean roughness Rzjis was 0.026 μm.

[0087] <Example 2> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive to create test piece 2. After buffing, the arithmetic mean roughness Ra of the surface of test piece 2, measured in accordance with JIS B 0601 (2013), was 0.010 μm, the maximum height Rz was 0.065 μm, and the ten-point mean roughness Rzjis was 0.058 μm.

[0088] Example 3 A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive to produce test piece 3. After buffing, the arithmetic mean roughness Ra of the surface of test piece 3, measured in accordance with JIS B 0601 (2013), was 0.020 μm, the maximum height Rz was 0.160 μm, and the ten-point mean roughness Rzjis was 0.140 μm.

[0089] <Comparative Example 1> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 2 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 4. After blasting, the surface of test piece 4 was measured according to JIS B 0601 (2013), and the arithmetic mean roughness Ra was 3.0 μm, the maximum height Rz was 18.8 μm, and the ten-point mean roughness Rzjis was 17.0 μm.

[0090] <Comparative Example 2> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 1 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 5. After blasting, the surface of test piece 5 was measured according to JIS B 0601 (2013), and the arithmetic mean roughness Ra was 1.5 μm, the maximum height Rz was 7.0 μm, and the ten-point mean roughness Rzjis was 6.1 μm.

[0091] <Comparative Example 3> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 0.8 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 6. After blasting, the surface of test piece 6 was measured according to JIS B 0601 (2013), and found to have an arithmetic mean roughness Ra of 1.0 μm, a maximum height Rz of 5.7 μm, and a ten-point mean roughness Rzjis of 4.6 μm.

[0092] <Comparative Example 4> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 0.3 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 7. After blasting, the surface of test piece 7 was measured according to JIS B 0601 (2013), and found to have an arithmetic mean roughness Ra of 0.5 μm, a maximum height Rz of 2.4 μm, and a ten-point mean roughness Rzjis of 2.1 μm.

[0093] <Comparative Example 5> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 0.2 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 8. After blasting, the surface of test piece 8 was measured according to JIS B 0601 (2013), and the arithmetic mean roughness Ra was 0.3 μm, the maximum height Rz was 1.6 μm, and the ten-point mean roughness Rzjis was 1.2 μm.

[0094] <Comparative Example 6> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 0.05 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 9. After blasting, the surface of test piece 9 was measured according to JIS B 0601 (2013), and the arithmetic mean roughness Ra was 0.1 μm, the maximum height Rz was 0.6 μm, and the ten-point mean roughness Rzjis was 0.5 μm.

[0095] <Comparative Example 7> A test piece (W: 100 mm × D: 100 mm × H: 2 mm) made of SUS304 was buffed using #800 abrasive. After buffing, a blasting treatment was performed under the following conditions: average shot particle size: 0.01 μm, blasting pressure: 0.5 MPa, blasting distance: 300 mm, blasting angle: 90°, to produce test piece 10. After the blasting treatment, the surface of test piece 10 was measured according to JIS B 0601 (2013), and the arithmetic mean roughness Ra was 0.05 μm, the maximum height Rz was 0.29 μm, and the ten-point mean roughness Rzjis was 0.24 μm.

[0096] [3] Sieving test In the apparatus of this embodiment, for example, in the piping and each storage section, it is believed that many sulfide-based inorganic solid electrolyte materials and their raw material mixtures are in continuous contact with the inner wall surfaces of the apparatus. Therefore, in each example and comparative example, a sieving test was conducted to evaluate the adhesion and deposition of the raw material mixture powder on a test piece representing the inner wall surface of the apparatus when the raw material mixture powder of the sulfide-based inorganic solid electrolyte material was sieved onto the test piece. Below, FIG. 5 shows a schematic diagram of sieving the raw material mixture powder 740 of the sulfide-based inorganic solid electrolyte material, and FIG. 6 shows a schematic diagram of impacting the test piece with a zirconia ball 780. The measurement method of the sieving test conducted on the test piece will be described with reference to FIGS. 5 and 6.

[0097] First, test piece 710 prepared in the following examples and comparative examples was placed on a jig installed on a horizontal surface 720. At this time, the angle of test piece 710 with respect to horizontal surface 720 was adjusted to be 45°. Next, 10 g of raw material mixed powder 740 of sulfide-based inorganic solid electrolyte material was sieved using a sieve 750 with a mesh size of 250 μm from a position at a height 760 of 10 cm from the horizontal surface 720 so that raw material mixed powder 740 of sulfide-based inorganic solid electrolyte material was sieved over the entire test piece 710. Furthermore, a 47 g zirconia ball 780 (manufactured by Nikkato Corporation, spherical, 2.5 cm in diameter) was dropped three times from a position where the height 770 from the top end of the test piece 710 was 5 cm, so as to hit only the top end of the test piece 710 and not the surface of the test piece 710 to which the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material was attached, thereby applying an impact to the test piece 710. Finally, the surface of the test piece 710 to which the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material was attached after the impact was photographed with a camera, and the photograph was separated into a powder-adhered portion and an unadhered portion using image processing software Paint.net (v4.2.16). The area of ​​the powder-adhered portion was measured using image analysis software ImageJ (1.52a), and the ratio (adhered area) to the area of ​​one side of the test piece 710 was calculated. The adhered area was evaluated using the following three levels. ○: The adhesion area of ​​the sulfide-based inorganic solid electrolyte material is 10% or less of the surface area of ​​the test piece to which the sulfide-based inorganic solid electrolyte material is attached. △: The adhesion area of ​​the sulfide-based inorganic solid electrolyte material is 30% or less of the surface area of ​​the test piece to which the sulfide-based inorganic solid electrolyte material is attached. ×: The area of ​​the surface of the test piece to which the sulfide-based inorganic solid electrolyte material is attached is 50% or less

[0098] [4] Pressurization test In the apparatus of this embodiment, for example, in the pulverization section, the pressing unit presses balls against the rotary table. Therefore, it is believed that the raw material mixed powder of the sulfide-based inorganic solid electrolyte material is also pressed against the inner wall surface of the apparatus in the pulverization section, or that a certain amount of force is applied when the raw material mixed powder collides with the inner wall surface of the apparatus. Therefore, in each example and comparative example, a pressing test was conducted in which the raw material mixed powder of the sulfide-based inorganic solid electrolyte material was pressed with a certain amount of force against a test piece representing the inner wall surface of the apparatus, and the adhesion and deposition of the raw material mixed powder to the test piece was evaluated. Below, FIG. 7 shows a schematic diagram of sieving the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material, FIG. 8 shows a schematic diagram of pressing the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material, and FIG. 6 shows a schematic diagram of impact by zirconia balls 780. The measurement method for the pressing test performed on the test piece will be described with reference to FIGS. 6 to 8.

[0099] First, a test piece 710 prepared in the following examples and comparative examples was placed on a jig installed on a horizontal surface 720. At this time, the angle of the test piece 710 with respect to the horizontal surface 720 was adjusted to 0° (parallel to the horizontal surface 720). Then, 10 g of raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material was sieved using a sieve 750 with a mesh size of 250 μm from a position where the height 760 from the horizontal surface 720 was 10 cm, so that the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material was sieved over the entire test piece 710. Furthermore, a backing plate 810 made by buffing a SUS304 plate with a #800 abrasive was placed on top of the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material, and a weight 820 of 1 kg was placed on top of it and left to stand for 30 seconds, thereby pressing the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material against the test piece 710. After being left to stand, the backing plate 810 and the weight 820 were removed, and the test piece 710 was tilted from 0° to 45° over 3 seconds using a jig. Next, a 47 g zirconia ball 780 (manufactured by Nikkato Corporation, spherical with a diameter of 2.5 cm) was dropped three times from a position at a height 770 of 5 cm from the top end of the test piece 710 so as to hit only the top end of the test piece 710 but not the surface of the test piece 710 to which the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material was attached, thereby applying an impact to the test piece 710. Finally, the surface of the test piece 710 to which the raw material mixed powder 740 of the sulfide-based inorganic solid electrolyte material had been attached after the impact was photographed with a camera, and the photograph was separated into a powder-attached portion and an unattached portion using image processing software Paint.net (v4.2.16). The area of ​​the powder-attached portion was measured using image analysis software ImageJ (1.52a), and the ratio (attached area) of this to the area of ​​one side of the test piece 710 was calculated. The attached area was then evaluated according to the following three levels. ○: The adhesion area of ​​the sulfide-based inorganic solid electrolyte material is 10% or less of the surface area of ​​the test piece to which the sulfide-based inorganic solid electrolyte material is attached. △: The adhesion area of ​​the sulfide-based inorganic solid electrolyte material is 30% or less of the surface area of ​​the test piece to which the sulfide-based inorganic solid electrolyte material is attached. ×: The area of ​​the surface of the test piece to which the sulfide-based inorganic solid electrolyte material is attached is 50% or less

[0100] [Table 1]

[0101] In the Examples, most of the raw material mixed powder fell off the test piece after both the sieving test and the pressing test, which was effective in preventing the raw material mixed powder from adhering to the inner wall surfaces of the device. On the other hand, in each of the Comparative Examples, much of the raw material mixed powder remained on the test piece after the test, which may have caused adhesion to the inner wall surfaces of the device. [Explanation of symbols]

[0102] 10 equipment 100 Blower 102 Gas inlet 104 Gas outlet 106 Inverter 110 Buffer Tank 112 Gas inlet 114 Gas outlet 116 Adjustment port 200 Crushing section 202 Gas inlet 204 Material supply pipe 206 Material discharge pipe 208 Gas outlet 212 Rotating Table 214 balls 216 Pressing section 220 Cover 300 First Recovery Department 302 Suction port 304 Material discharge port 306 Gas outlet 308 Material supply port 310 First Storage Unit 400 Second Collection Section 402 Suction port 404 Material discharge port 406 Gas exhaust pipe 410 Second storage section 500 Pressure reduction section 710 Test Piece 720 horizontal plane 730 Installation angle 740 Raw material mixed powder of sulfide-based inorganic solid electrolyte material 750 Sieve 760 Height from horizontal plane 720 770 Height from the top of the test piece 710 780 Zirconia Ball 810 Backing plate 820 weight D Exhaust duct Le 1st Line Lh 2nd Line Pa piping Pb 5th pipe Pc 2nd piping Pd No. 6 Pipe Pe No. 1 Piping Pf Third piping Pg piping Ph 4th Pipe Pi piping Pj Plumbing Pk Piping Pl Piping Pm piping Pn piping Po piping S series Va1 valve Vb1 valve Vc1 valve Vc2 valve Vc3 valve Vd1 valve Ve1 Valve Ve2 valve Vf1 valve Vg1 valve Vh1 valve Vh2 valve Vi1 Valve Vi2 Valve Vj1 valve Vk1 Valve Vl1 valve Vm1 valve Vn1 valve Vo1 valve

Claims

1. An apparatus for producing an inorganic material, comprising: a blower for sending an inert gas; a crushing section that repeats the steps of vitrifying a plurality of inorganic compounds that become the inorganic material by mechanical energy and blowing up the vitrified plurality of inorganic compounds by the inert gas sent from the blower section; a first recovery section into which at least a portion of the inorganic compounds blown up by the inert gas enters and which returns the at least a portion of the inorganic compounds toward the pulverization section; a system for circulating the inert gas from the blower section to the blower section via the pulverizer section and the first recovery section; An apparatus comprising: The apparatus, wherein the arithmetic mean roughness Ra of the inner wall surface of the grinding section measured in accordance with JIS B 0601 (2013) is 0.02 μm or less.

2. 10. The apparatus of claim 1, The apparatus wherein the maximum height Rz of the inner wall surface of the crushing section measured in accordance with JIS B 0601 (2013) is 0.16 μm or less.

3. 3. The device according to claim 1 or 2, The apparatus wherein the ten-point average roughness Rzjis of the inner wall surface of the grinding section measured according to JIS B 0601 (2013) is 0.14 μm or less.

4. The device according to any one of claims 1 to 3, a first storage section that stores the plurality of inorganic compounds to be supplied to the grinding section; a first pipe communicating with the first recovery unit and the first storage unit; a first valve detachably attached to the first pipe together with the first housing portion; The apparatus further comprises:

5. 5. The apparatus of claim 4, The apparatus further comprises a first line for introducing an inert gas into the first pipe.

6. The device according to any one of claims 1 to 5, a second recovery section into which the inorganic material blown up by the inert gas enters; a second pipe communicating with the pulverizing section and the first recovery section; a second valve provided in the second pipe; a third pipe communicating with a portion of the second pipe located between the crushing unit and the second valve and the second recovery unit; a third valve provided in the third pipe; The apparatus further comprises:

7. 7. The apparatus of claim 6, a second storage section that stores the inorganic material recovered by the second recovery section; a fourth pipe communicating with the second recovery section and the second storage section; a second line for introducing an inert gas into the fourth pipe; The apparatus further comprises:

8. The device according to any one of claims 1 to 7, a fifth pipe connecting the blower unit and the pulverizer unit; a fifth valve provided in the fifth pipe; a sixth pipe that returns the at least a portion of the plurality of inorganic compounds from the first recovery section toward the crushing section; a sixth valve provided in the sixth pipe; The apparatus further comprises:

9. 9. The apparatus of claim 8, The apparatus has an inner wall surface in one or more parts selected from the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe, the inner wall surface of the apparatus having an arithmetic mean roughness Ra of 0.02 μm or less as measured in accordance with JIS B 0601 (2013).

10. 10. The device according to claim 8 or 9, An apparatus in which the maximum height Rz of the inner wall surface of the apparatus in one or more parts selected from the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe is 0.16 μm or less, as measured in accordance with JIS B 0601 (2013).

11. The device according to any one of claims 8 to 10, An apparatus in which the ten-point average roughness Rzjis of the inner wall surface of the apparatus in one or more parts selected from the first recovery section, the second recovery section, the first storage section, the second storage section, the first pipe, the second pipe, the third pipe, the fourth pipe, the fifth pipe, and the sixth pipe is 0.14 μm or less, as measured in accordance with JIS B 0601 (2013).

12. The device according to any one of claims 1 to 11, The apparatus further comprises a pressure reducing section for reducing the pressure inside the grinding section.

13. The device according to any one of claims 1 to 12, The crushing unit includes a rotary table, a plurality of balls arranged around a rotation axis of the rotary table and each of the balls is rotatable about the rotation axis that rotates together with the rotation of the rotary table, and a pressing unit that presses the plurality of balls toward the rotary table from the opposite side of the rotary table.

14. The device according to any one of claims 1 to 13, The crushing unit has a cover unit that directs the flow of the inert gas that blows up the multiple types of inorganic compounds toward the center of the crushing unit and below the crushing unit.

15. The device according to any one of claims 1 to 14, The device, wherein the plurality of inorganic compounds includes a Li element.

16. A method for producing an inorganic material by the apparatus according to any one of claims 1 to 15, comprising: Sending the inert gas by a blower; a grinding unit that repeatedly vitrifies the inorganic compounds by mechanical energy and blows the vitrified inorganic compounds upward with the inert gas sent from the blower unit; returning at least a portion of the plurality of inorganic compounds blown up by the inert gas and entering the first recovery section from the first recovery section toward the crushing section; circulating the inert gas from the blower section to the blower section via the pulverizer section and the first recovery section; A method comprising:

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