JP5544808B2 - Reactor and method for producing powder for magnetic material - Google Patents

Description

  The present invention relates to a reaction furnace used when producing a magnetic material powder by HDDR (Hydrogenation Decomposition Desorption Recombination) method and a method for producing the magnetic material powder.

  A vacuum heating furnace is used for processing the hydrogen storage powder and the powder such as nitriding. For example, Patent Document 1 discloses a vacuum container, a rotary container for placing an object to be processed whose rotation axis is horizontal in the vacuum container, driving means for rotating the rotary container, and air in the vacuum container. And a substitution means for substituting the reaction gas for reacting the object to be processed, and the rotary vessel is installed in the vacuum vessel with a structure that is not fixed to the vacuum vessel by the shaft portion, and the cylindrical curved surface of the rotary vessel There is disclosed a vacuum furnace in which a drive unit for transmitting a rotational force to the unit is provided only at a lower part than the rotation axis of the rotary container.

Japanese Patent Laid-Open No. 2001-255070

  Incidentally, the HDDR method (hydrocracking / dehydrogenation recombination method) is known as a method for producing a powder for a magnetic material. With the HDDR method, the raw material (starting alloy) is heated in hydrogen to hydrogenate and decompose the raw material (HD), and then dehydrogenate and recombine (DR). This is a process for making crystals finer. The HDDR reaction is required to maintain a high temperature while confining hydrogen in the reaction furnace. In the HDDR reaction, the raw material occludes hydrogen in hydrogenation / decomposition, and hydrogen is released from the raw material in dehydrogenation / recombination, but the occlusion / desorption rate of hydrogen in the HDDR reaction is high. The amount is also large. Furthermore, in the HDDR reaction, heat enters and exits greatly, and temperature control becomes difficult when a large amount of powder for magnetic material is produced.

  In the vacuum heating furnace disclosed in Patent Document 1, a rotating container disposed in a vacuum container is hermetically sealed. For this reason, when used for reactions in which the gas concentration, temperature, and pressure in a closed furnace change rapidly as in the HDDR method, the rotating container may be deformed by expansion or contraction. In addition, since the vacuum heating furnace disclosed in Patent Document 1 does not have a means for cooling the vacuum vessel, hydrogen may leak out of the furnace due to high temperature, and it is difficult to maintain high temperature while confining hydrogen in the furnace. is there.

  Further, in the vacuum heating furnace disclosed in FIG. 2B and FIG. 3 of Patent Document 1, there is a high possibility that hydrogen leaks from a bearing that rotatably supports the vacuum rotary container, and the high temperature while confining hydrogen in the furnace is high. Is difficult to keep. For this reason, it is difficult to apply the vacuum furnace disclosed in Patent Document 1 to the production of magnetic material powder by the HDDR method. This invention is made | formed in view of the above, Comprising: It aims at providing the manufacturing method of the reactor suitable for manufacture of the powder for magnetic materials using HDDR method, and the powder for magnetic materials.

  In order to solve the above-described problems and achieve the object, a reaction furnace according to the present invention is provided with an outer container, an outer container cooling means for cooling the outer container, and an inside of the outer container. A cylindrical container to be held, supported inside the outer container so as to be rotatable or swingable about an axis intersecting with both end faces of the container, and an inner container having an opening on each end face; An inner container driving means for rotating or swinging the inner container, a heater disposed on at least one of the outer side and the inner side of the inner container, a gas introduction port for introducing gas into the outer container, and A gas outlet for discharging the gas inside the outer container to the outside of the outer container; and a gas flow control means for guiding the gas supplied from the gas inlet to the inside of the inner container. And

  Since this reactor has openings at both end faces of the inner vessel holding the raw material, the raw material suddenly absorbs a large amount of hydrogen in the HDDR reaction, or a large amount of hydrogen is suddenly released from the raw material. However, hydrogen enters and exits from the opening. Thereby, deformation of the inner container can be avoided. Further, when the raw material is cooled after the HDDR reaction is completed, the raw material can be efficiently cooled by flowing an inert gas for cooling from one opening to the other opening.

  In addition, the HDDR reaction generates heat and endotherm, but in order to react the entire raw material uniformly, avoid the difference between the internal temperature of the raw material mass and the external temperature of the raw material mass due to the exothermic or endothermic reaction. There is a need. For this reason, it is necessary to uniformly control the temperature of the entire raw material during heat generation and heat absorption in the HDDR reaction. This non-uniformity of the temperature of the entire raw material is particularly noticeable when a magnetic material powder is produced from a large amount of raw material. The reactor according to the present invention can stir the raw material by rotating or swinging the inner vessel during the HDDR reaction, and can make the temperature distribution of the whole raw material uniform, or even occlude or release hydrogen. . As a result, the whole raw material can be reacted uniformly, and the quality of the produced magnetic material powder can be improved. As described above, the reactor according to the present invention makes it relatively easy to control the entire raw material at a uniform temperature by stirring the raw material, even when the magnetic material powder is produced from a large amount of the raw material. As a result, if the reactor of the present invention is used, high quality powders for magnetic materials can be stably produced in large quantities.

  In addition, when the powder raw material is subjected to the HDDR reaction, the reaction may proceed only on the surface of the raw material mass, and the reaction may not proceed inside the mass. This is particularly noticeable when a magnetic material powder is produced from a large amount of raw materials. The reactor according to the present invention stirs the raw material by rotating or swinging the inner container to uniformly react the whole raw material, and can prevent the reaction from proceeding only on the surface of the raw material mass.

  Furthermore, since the leakage of hydrogen from the metal outer container can be reduced by cooling the outer container, the HDDR reaction can proceed while maintaining the high temperature in the reaction furnace while confining hydrogen in the reaction furnace. As described above, the reactor according to the present invention is suitable for producing a powder for a magnetic material by using the HDDR method, and particularly for stably producing a large amount of high-quality powder for a magnetic material. .

  As a desirable mode of the present invention, in the reaction furnace, it is preferred that a temperature sensor is arranged inside the inner vessel. The raw material is held inside the inner container, and the temperature sensor can be arranged in the vicinity of the raw material by arranging the temperature sensor inside the inner container. Thereby, since the reaction atmosphere temperature can be measured more accurately, the HDDR reaction can be controlled with high accuracy by using the temperature measured by the temperature sensor.

  As a desirable mode of the present invention, in the reaction furnace, it is preferable that a stirring means for stirring the raw material in the inner container is disposed inside the inner container. The raw material is also stirred by rotating or swinging the inner container, but the raw material is further stirred by disposing the stirring means inside the inner container. Thereby, the whole raw material can be further reacted uniformly.

  As a desirable mode of the present invention, in the reaction furnace, the stirring means is preferably a member protruding from the inner wall of the inner vessel. Thus, by causing the member to protrude from the inner wall of the inner container, a high stirring effect can be obtained by a synergistic effect with the rotation or swinging of the inner container. Further, by projecting the member from the inner wall of the inner container, the heat transfer area between the raw material and the inner container can be increased.

  As a desirable mode of the present invention, it is preferable that the reaction furnace has a member inserted into the inner container through at least one of the openings. By inserting an instrument or device having various functions into such a member through the opening into the inner container, higher control in the HDDR reaction becomes possible.

  As a desirable aspect of the present invention, in the reaction furnace, the member preferably supports a temperature sensor inside the inner container. Accordingly, the temperature sensor can be easily arranged inside the inner container. Moreover, the temperature of the raw material can be measured more accurately by bringing the temperature sensor supported by the member into contact with the raw material in the inner container.

  As a desirable mode of the present invention, in the reaction furnace, the member is preferably a stirring means for stirring the raw material in the inner container. Thus, since a member is inserted from an opening and a raw material is stirred, a member can also be moved. Accordingly, since the raw material can be stirred at an arbitrary position in the inner container, the entire raw material can be uniformly stirred by moving the member to a portion where stirring is insufficient.

  As a desirable aspect of the present invention, in the reaction furnace, the member preferably has a movable portion that moves so as to contact the raw material. For example, when the member is used as a stirring means, the member is inserted into the inner container through the opening without being in contact with the raw material, and then the movable part is moved to contact the raw material to stir the raw material. Thus, the material can be stirred by inserting the member into the inner container without increasing the size of the opening. And it can respond also when the stirring by a member becomes unnecessary by making a movable part the state which does not contact a raw material. Further, by attaching the temperature sensor to the member, the temperature sensor can be brought into contact with the raw material, and the temperature of the raw material can be measured more accurately.

  As a desirable mode of the present invention, in the reaction furnace, it is preferable that an additive supply means for supplying an additive to the raw material is disposed inside the inner vessel. Thus, by providing the additive supply means, the additive can be supplied to the raw material without interrupting the reaction even during the HDDR reaction, so that the working efficiency is improved.

  As a desirable mode of the present invention, in the reaction furnace, the inner container has a cylindrical shaft member having both ends opened between the openings, and the shaft member has a hole on a side surface. Is preferred. By this shaft member, scattering of the raw material (particularly during cooling of the raw material) can be suppressed.

  As a desirable mode of the present invention, in the reaction furnace, it is preferable that the rotating shaft of the inner vessel penetrates at least one of the openings. Thereby, by inserting a temperature sensor, a stirring means, etc. from the opening through which the rotation shaft of the inner container passes, interference between the inner container and the temperature sensor, the stirring means, etc. can be avoided.

  In order to solve the above-mentioned problems and achieve the object, the method for producing a powder for magnetic material according to the present invention comprises the above-mentioned method for producing a magnetic material powder by hydrocracking / dehydrogenation recombination. Stirring the raw material by rotating or swinging the container while supplying the hydrogen into the reaction furnace and heating the reaction furnace while charging the raw material of the powder into the container in the reaction furnace And a step of discharging hydrogen in the reaction furnace to the outside of the reaction furnace.

  In this magnetic material powder manufacturing method, since the raw material is stirred during the HDDR reaction, the temperature distribution of the raw material can be made uniform, and hydrogen can be uniformly occluded or released. As a result, the entire raw material is made uniform. Can be reacted. For this reason, even when the magnetic material powder is produced from a large amount of raw material, the temperature control of the raw material becomes relatively easy by stirring the raw material. As described above, the reactor according to the present invention is suitable for producing a powder for a magnetic material by using the HDDR method, and particularly for stably producing a large amount of high-quality powder for a magnetic material. .

  INDUSTRIAL APPLICABILITY The present invention can provide a reactor suitable for the production of magnetic material powder using the HDDR method and a method for producing magnetic material powder.

FIG. 1 is an explanatory diagram showing the structure of a reaction furnace according to the present embodiment. FIG. 2 is an AA arrow view of FIG. FIG. 3 is a perspective view showing a shaft member included in the inner container. FIG. 4 is a perspective view showing another example of the inner container. FIG. 5A is a schematic diagram illustrating a modification of the air guide body. FIG. 5B is a schematic diagram illustrating a modified example of the air guide body. FIG. 6 is a view showing an example of an inner container provided with stirring means. FIG. 7-1 is a diagram illustrating an example of an inner container provided with stirring means. FIG. 7-2 is a diagram illustrating an example of an inner container provided with stirring means. FIG. 8 is a schematic diagram showing another example of the stirring means. FIG. 9 is an explanatory view showing a modification of the stirring rod. FIG. 10 is an explanatory diagram showing a configuration of a means for supplying an additive to the inside of the inner container with the reaction furnace lid closed. FIG. 11 is a diagram illustrating another configuration example of the shaft member included in the inner container. FIG. 12 is a perspective view showing another configuration example of the shaft member provided in the inner container. FIG. 13 is a schematic diagram of the shaft member support structure shown in FIG. FIG. 14 is an explanatory view showing an example in which a heater is arranged inside the inner container. FIG. 15 is a flowchart showing a method for manufacturing a magnetic material powder according to the present embodiment.

  Hereinafter, the present invention will be described in detail with reference to the drawings. The present invention is not limited by the following modes for carrying out the invention (hereinafter referred to as embodiments). In addition, constituent elements disclosed in the following embodiments include those that can be easily assumed by those skilled in the art, those that are substantially the same, and those in a so-called equivalent range. The reactor according to the present invention is used when producing a magnetic material powder (particularly an alloy powder for a magnet) by the HDDR reaction, and the function of heating the raw material of the magnetic material powder to be produced, It has the function of supplying gas into the furnace and the function of evacuating the furnace. Moreover, the manufacturing method of the powder for magnetic materials which concerns on this invention is suitable for manufacturing the powder for magnetic materials by HDDR reaction using the reaction furnace which concerns on this invention. In addition, it does not exclude applying the manufacturing method of the powder for magnetic materials which concerns on this invention with respect to other than the reactor which concerns on this invention.

  FIG. 1 is an explanatory diagram showing the structure of a reaction furnace according to the present embodiment. FIG. 2 is an AA arrow view of FIG. The reaction furnace 1 is for producing powder for magnetic material by HDDR reaction, and the inside of the furnace can be evacuated and heated. The reactor 1 includes an outer container 10, a main body side cooling medium passage 10Bc and a lid side cooling medium passage 10Cc as outer container cooling means, an inner container 20, an inner container driving device 18 as inner container driving means, a heating The apparatus 2 is configured to include a gas inlet 12I and a gas outlet 12E, and an air guide 15 that is a gas flow control means.

  The outer container 10 has an outer container body 10B having a double structure composed of an outer shell 10o and an inner shell 10i having the same shape and smaller than the outer shell 10o disposed inside the outer shell 10o. It is comprised with the lid | cover 10C. A plurality of legs 19 are attached to the outer container body 10 </ b> B, and the reaction furnace 1 is supported by these legs 19. The outer shell 10o constituting the outer container main body 10B is a bottomed container configured by a cylindrical (cylindrical in this embodiment) outer shell side portion 10os and an outer shell bottom portion 10ob provided at one end thereof. is there. The inner shell 10i is a bottomed container that includes a cylindrical (cylindrical in this embodiment) inner shell side portion 10is and an inner shell bottom portion 10ib provided at one end thereof. The outer shell bottom portion 10ob and the inner shell bottom portion 10ib are plate members having a circular shape in plan view because the outer shell side portion 10os and the inner shell side portion 10is are cylindrical in this embodiment. The shape is varied according to the shape of 10 os and the inner shell side portion 10 is.

  The outer container body 10B has an inner shell 10i disposed inside the outer shell 10o, and the other end (opening side) of the outer shell 10o and the other end (opening side) of the inner shell 10i are annular. And it connects and is comprised by the plate-shaped edge part sealing member 10t. With this configuration, the outer container body 10B has a space surrounded by the outer shell side portion 10os, the outer shell bottom portion 10ob, the inner shell side portion 10is, the inner shell bottom portion 10ib, and the end sealing member 10t. A container with a heavy structure. And the said space which the outer container main body 10B has becomes the main body side cooling medium passage 10Bc. The outer container body 10B is a cup-shaped container having one end closed by the bottom 10Bb and the other end opened.

  The lid 10C includes a cylindrical (cylindrical in this embodiment) lid side portion 10Cs and end plates 10Ct attached to both ends of the lid side portion 10Cs. Thus, the lid 10C becomes a hollow structure having a space surrounded by the lid side portion 10Cs and the respective end plates 10Ct. The space becomes the lid-side cooling medium passage 10Cc. The lid 10 </ b> C is attached to the opening of the outer container main body 10 </ b> B so as to be freely opened and closed, for example, with a hinge. For example, a heat-resistant seal member is disposed between the lid 10C and the end sealing member 10t of the outer container body 10B. When the lid 10C is closed, the outer container body 10B and the lid 10C are surrounded. The space is configured to be sealed.

  The outer shell 10o constituting the outer container main body 10B includes a main body side cooling medium supply port 13IB that communicates the outer side of the outer shell 10o and the main body side cooling medium passage 10Bc, and the outer side of the main body side cooling medium passage 10Bc and the outer shell 10o. Is provided with a main body side cooling medium discharge port 13EB. The main body side cooling medium supply port 13IB is connected to a discharge port of a cooling pump 5 which is a cooling medium supply means, and is supplied with a cooling medium (water in this embodiment) W discharged from the cooling pump 5. The The cooling medium W supplied to the main body side cooling medium supply port 13IB cools the outer container main body 10B in the process of flowing through the entire main body side cooling medium passage 10Bc, and is discharged from the main body side cooling medium discharge port 13EB.

  The lid 10C has a lid-side cooling medium supply port 13IC that communicates the outside of the lid 10C and the lid-side cooling medium passage 10Cc, and a lid-side cooling medium discharge port 13EC that communicates the lid-side cooling medium passage 10Cc and the outside of the lid 10C. And are provided. A discharge port of the cooling pump 5 is connected to the lid-side cooling medium supply port 13IC, and the cooling medium W discharged from the cooling pump 5 is supplied thereto. The cooling medium W cools the lid 10C in the process of flowing through the entire lid-side cooling medium passage 10Cc, and is discharged from the lid-side cooling medium discharge port 13EC.

  The cooling medium W discharged from the main body side cooling medium discharge port 13EB and the lid side cooling medium discharge port 13EC is cooled by the cooling medium cooler 4 and then sucked from the suction port of the cooling pump 5. Then, it is supplied again to the main body side cooling medium passage 10Bc and the lid side cooling medium passage 10Cc by the cooling pump 5. Thus, in the present embodiment, the cooling medium W is circulated between the main body side cooling medium passage 10 </ b> Bc and the lid side cooling medium passage 10 </ b> Cc and the cooling medium cooler 4 by the cooling pump 5.

  In the present embodiment, the outer container body 10B and the lid 10C are made of metal, for example, stainless steel. During the HDDR reaction, hydrogen is supplied to the internal space 10I of the outer container 10 of the reaction furnace 1, that is, the space surrounded by the outer container main body 10B and the lid 10C, and the heating disposed in the outer container main body 10B. The chamber 2 raises the ambient temperature of the internal space 10I to about 600 ° C to 1000 ° C. For this reason, the outer container 10 becomes high temperature during the HDDR reaction. As described above, since the outer container 10 is made of a metal such as stainless steel, when the outer container 10 is heated, hydrogen existing in the inner space 10I passes through the outer container 10 and leaks outside.

  For this reason, in this embodiment, the main body side cooling medium passage 10Bc and the lid side cooling medium passage 10Cc are respectively provided in the outer container main body 10B and the lid 10C of the outer container 10, and the cooling medium W is supplied to the main body side cooling medium passage during the HDDR reaction. The outer container main body 10B and the lid 10C are cooled by flowing to 10Bc and the lid-side cooling medium passage 10Cc. Thereby, the temperature rise of the outer container 10 during the HDDR reaction is suppressed, and the amount of hydrogen that permeates the outer container 10 from the internal space 10I and leaks to the outside is reduced. Further, by providing the main body side cooling medium passage 10Bc and the lid side cooling medium passage 10Cc, the amount of the cooling medium W that is not used for cooling is reduced as compared with the case where the cooling medium W is directly injected to the outer container main body 10B or the like. Therefore, the cooling medium W can be used effectively.

  In addition, you may coat | cover the surface of the outer container main body 10B and the lid | cover 10C in the main body side cooling medium channel | path 10Bc and the lid side cooling medium channel | path 10Cc side with material (for example, glass) with low hydrogen permeability. In this way, the material having a low hydrogen permeability suppresses the permeation of hydrogen, so that the amount of hydrogen that passes through the outer container 10 from the internal space 10I and leaks to the outside can be further reduced. When the coefficient of linear expansion is different between the material with low hydrogen permeability and stainless steel, if the outer container 10 is heated during the HDDR reaction, the material with low hydrogen permeability may be cracked due to the difference in coefficient of linear expansion. There is a risk of peeling from the outer container 10. However, in this embodiment, since the outer container 10 is cooled by the cooling medium W, the temperature rise of the outer container 10 made of stainless steel can be suppressed. As a result, since the expansion of the outer container 10 can be suppressed even when the material having low hydrogen permeability and the stainless steel have different linear expansion coefficients, cracking and peeling of the material having low hydrogen permeability can be suppressed.

  Moreover, you may provide the member which improves heat-transfer performance, for example, a fin, in the surface of the outer container main body 10B and the lid | cover 10C in the main body side cooling-medium channel | path 10Bc and the lid | cover side cooling-medium channel | path 10Cc side. As a result, the heat transfer area in the main body side cooling medium passage 10Bc and the lid side cooling medium passage 10Cc can be increased, so that the outer container main body 10B and the lid 10C can be cooled more efficiently. The outer container cooling means is not limited to the main body side cooling medium passage 10Bc and the lid side cooling medium passage 10Cc. For example, the cooling medium may be directly injected into the outer container without providing the main body side cooling medium passage 10Bc and the lid side cooling medium passage 10Cc. In this way, the structure of the outer container can be simplified. Further, the cooling medium W may be other than water.

  The inner container 20 is disposed inside the outer container 10, that is, in the inner space 10I. The inner container 20 includes a cylindrical (cylindrical in this embodiment) inner container side portion 21, an inner container lid member 22T provided at one end portion thereof, and an inner container bottom member 22B provided at the other end portion thereof. It is a cylindrical container that holds a magnetic material powder raw material (magnetic powder raw material) S inside during the HDDR reaction. The inner container side portion 21, the inner container bottom member 22B, and the inner container lid member 22T are made of a metal material (stainless steel in this embodiment).

  The inner container lid member 22T and the inner container bottom member 22B have a first opening 23T and a second opening 23B, respectively, as openings. By providing the first opening 23T and the second opening 23B, in the HDDR reaction, hydrogen is held in the inner container 20 through the first opening 23T or the second opening 23B in the HD (hydrogenation / decomposition) reaction. The raw material S is reliably supplied. Further, the hydrogen released from the raw material S in the DR (dehydrogenation / recombination) reaction is reliably released from the first opening 23T or the second opening 23B to the outside of the inner container 20. As a result, the HDDR reaction can be realized with certainty, and the inner container 20 is not expanded and deformed.

  Furthermore, by providing the first opening 23T and the second opening 23B, a measuring instrument and instruments having various functions are inserted and arranged in the inner container 20, or the heater 2 is arranged in the inner container 20. You can also do it. In the present embodiment, the shape of the first opening 23T and the second opening 23B is circular in plan view, but the shape of the first opening 23T and the second opening 23B is not limited to this. A plurality of first openings 23T and second openings 23B may be provided.

  In the present embodiment, since the first opening 23T and the second opening 23B are circular and the inner container side portion 21 is cylindrical, the shapes of the inner container bottom member 22B and the inner container lid member 22T are respectively annular. . The inner container bottom member 22B and the inner container lid member 22T are plate-shaped members. The inner container bottom member 22B and the inner container lid member 22T serve as both end surfaces of the inner container 20, respectively. The inner container bottom member 22B and the inner container lid member 22T are disposed to face each other, and are disposed so that their plate surfaces are parallel to each other. The inner container bottom member 22B and the inner container lid member 22T have different shapes according to the shape of the inner container side portion 21.

  In the present embodiment, the inner container lid member 22T is preferably configured to be removable from the inner container side portion 21. As a result, the raw material S can be easily put into the inner container 20, and workability is improved. Even when the inner container lid member 22T is fixed to the inner container side portion 21, the raw material S can be charged from the first opening 23T or the second opening 23B. The temperature sensor support 3 is inserted from the second opening 23 </ b> B of the inner container 20 into the inner container 20. The temperature sensor support 3 is provided with a temperature sensor 8 serving as a temperature detection means at a tip end inserted into the inner container 20. For the temperature sensor 8, for example, a thermocouple or the like is used. The temperature sensor 8 measures the reaction atmosphere temperature of the raw material S held in the inner container 20. Thus, since the temperature sensor 8 is inserted into the inner container 20 and disposed in the vicinity of the raw material S, the reaction atmosphere temperature can be measured more accurately. Thereby, the HDDR reaction can be controlled with high accuracy.

  FIG. 3 is a perspective view showing a shaft member included in the inner container. In the present embodiment, the inner container 20 includes a cylindrical (cylindrical in this embodiment) shaft member 24 having both ends opened. The shaft member 24 is made of a metal material (stainless steel in the present embodiment). As shown in FIG. 1, the inner container lid member 22T and the inner container bottom member 22B are respectively connected to the first opening 23T portion. The second opening 23B is connected. As a result, the shaft member 24 rotates or swings together with the inner container 20.

  The shaft member 24 has a plurality of holes 25 on the side surface. From this hole 25, hydrogen or argon flows into the inner container 20 and is supplied to the raw material S held inside the inner container 20. By providing the shaft member 24, scattering of the raw material S (especially when the raw material S is cooled after the HDDR reaction is completed) can be suppressed. Further, since hydrogen and argon supplied to the inside of the inner container 20 are rectified when passing through the plurality of holes 25 of the shaft member 24, the turbulent flow of the raw material is compared with the case where the turbulent flow flows to the raw material. Scattering can be suppressed. In the present embodiment, the inner container 20 only needs to include the first opening 23T and the second opening 23B, and the shaft member 24 is not necessarily provided.

  The inner container 20 rotates or swings about an axis (inner container rotation axis) Zr that intersects (in the present embodiment, orthogonal) with both end surfaces of the inner container 20, that is, the inner container bottom member 22B and the inner container lid member 22T. It arrange | positions inside the outer container main body 10B so that it can do. Next, this structure will be described. A plurality (four in this embodiment) of inner container support members 16 are provided on the inner shell 10i of the outer container body 10B constituting the outer container 10. The inner container support member 16 is a columnar member, and one end thereof is attached to the inner shell 10i. Two inner container support members 16 are arranged outside the respective end surfaces of the inner container 20 in a direction parallel to the inner container rotation axis Zr. That is, the inner container 20 is sandwiched between the two inner container support members 16 in a direction parallel to the inner container rotation axis Zr.

  Two inner container support members 16 disposed outside the inner container lid member 22T and two inner container support members disposed outside the inner container bottom member 22B in the direction parallel to the inner container rotation axis Zr. 16 are arranged to face each other. And the space | interval of the inner container support members 16 arrange | positioned facing each outer side rather than each end surface of the inner container 20 is smaller than the outer diameter of the inner container 20. In the direction parallel to the inner container rotation axis Zr, the two inner container support members 16 are arranged on a straight line parallel to the inner container rotation axis Zr with the inner container rotation axis Zr interposed therebetween.

  The two inner container support members 16 arranged on a straight line parallel to the inner container rotation axis Zr are the other end portions, that is, the end portions on the opposite side to the end portions on the attachment side to the inner shell 10i, The support roller 17 is supported by both ends so that the support roller 17 can rotate about an axis parallel to the inner container rotation axis Zr. The support roller 17 has a side portion 17 </ b> S that is in contact with the inner container side portion 21. Thereby, the inner container 20 is supported by the outer container body 10B of the outer container 10 via the two support rollers 17 and the inner container support member 16, and the inner container support member 16 and the support roller 17 support the inner container. Functions as a means.

  The inner container 20 is rotated or rocked around the inner container rotation axis Zr by an inner container driving device 18 which is an inner container driving means. The inner container drive device 18 includes a support 18S, a rotating body 18R that is a power transmission member, and an electric motor 18M that is a power generation means. The electric motor 18M is controlled by the control device 50. The rotator 18R receives power from the electric motor 18M via a power transmission mechanism such as a gear or a chain, and rotates about an axis parallel to the inner container rotation axis Zr. Since the outer peripheral portion of the rotating body 18R is in contact with the outer peripheral portion of the inner container side portion 21 of the inner container 20, when the rotating body 18R rotates, the inner container 20 rotates in a direction opposite to the direction in which the rotating body 18R rotates. . In addition to rotation, the inner container 20 may be swung by the control device 50 by controlling the electric motor 18M so that the rotation direction of the inner container 20 is switched within 360 degrees. .

  FIG. 4 is a perspective view showing another example of the inner container. The inner container 20a shown in FIG. 4 is similar to the inner container 20 described above, and includes an inner container side portion 21a, an inner container lid member 22Ta provided at one end of the inner container side portion 21a, and the inner container side portion 21a. It is comprised by inner container bottom member 22Ba provided in an edge part. The inner container side portion 21a has a shape obtained by cutting a part of a cylindrical structure, and has a side portion opening 21Ha. The inner container 20a can supply and take out the raw material from the side opening 21Ha into the inner container 20a. Further, hydrogen and argon flow into the inner container 20a from the side opening 21Ha, and hydrogen released from the raw material flows out from the side opening 21Ha. In addition, in order to suppress scattering of the raw material, a lid having a plurality of holes may be provided in the side opening 21Ha so as to be attachable and detachable.

  Since the inner container 20a has the side opening 21Ha, it cannot be rotated. For this reason, the inner container 20a can only swing. Since the inner container 20a has the side opening 21Ha, the first opening 23T and the second opening 23B described above may not be provided in the inner container lid member 22Ta and the inner container bottom member 22Ba, respectively (may be provided). . This facilitates the processing of the inner container lid member 22Ta and the inner container bottom member 22Ba, and increases the volume for holding the raw material S in the inner container 20a by not providing the first opening 23T and the second opening 23B. can do. This facilitates production of a large amount of powder for magnetic material. Furthermore, since the temperature sensor support 3 having the temperature sensor 8 at the distal end portion may be inserted into the inner container 20a from the side opening 21Ha, the temperature sensor support 3 need not necessarily be provided on the inner container rotation axis Zr. Thereby, the freedom degree of design of the reactor 1 improves.

  The reaction furnace 1 can stir or pulverize the raw material S by rotating or swinging the inner container 20 in which the raw material S is held by the inner container driving means during the HDDR reaction. The inner container driving means is not limited to such a structure. For example, a gear is provided on the outer peripheral portion of the rotating body 18R, and a gear that meshes with the gear is provided on the outer peripheral portion of the inner container side portion 21. Thus, the rotational force of the rotating body 18R may be transmitted to the inner container side portion 21 by engaging both gears. Moreover, the inner container drive means may rotate the inner container 20 by rotating the support roller 17 by the power generation means.

  Thus, the inner container 20 rotates or swings inside the outer container 10. Therefore, the temperature sensor support 3 inserted into the inner container 20 from the second opening 23B needs to be configured so as not to interfere with the inner container bottom member 22B due to the rotation and swinging. Therefore, the second opening 23B into which the temperature sensor support 3 is inserted is preferably formed so as to include at least the inner container rotation axis Zr. In this way, it is possible to form a portion where the second opening 23B and the inner container rotation axis Zr do not contact when the inner container 20 makes one rotation. For this reason, if the temperature sensor support 3 is disposed in the region of the inner container rotation axis Zr (for example, on the rotation axis) rather than the portion where the second opening 23B and the inner container rotation axis Zr are closest, the inner container 20 It is possible to prevent the temperature sensor support 3 and the inner container bottom member 22B from interfering with each other even if is rotated or oscillated. In the present embodiment, the center of the second opening 23B is disposed on the inner container rotation axis Zr, and the temperature sensor support 3 is disposed on the inner container rotation axis Zr. This prevents the temperature sensor support 3 and the inner container bottom member 22B from interfering when the inner container 20 rotates or swings.

  In the reactor 1, the cylindrical inner container 20 is placed horizontally, that is, the inner container rotation axis Zr is arranged so as to be orthogonal to the vertical direction (direction of action of gravity), and the raw material S is held inside the inner container 20. Let Therefore, the raw material S is held inside the inner container 20 in a region (vertical direction side) below the first opening 23T and the second opening 23B. For this reason, the first opening 23T and the second opening 23B are disposed at positions away from the inner container rotation axis Zr, or the first opening 23T and the second opening 23B include the inner container rotation axis Zr. If it is arranged eccentrically, the volume for holding the raw material S in the inner container 20 becomes small. Therefore, the first opening 23T and the second opening 23B have a circular shape, the first opening 23T and the second opening 23B include the inner container rotation axis Zr, and the first opening 23T and the second opening 23 on the inner container rotation axis Zr. It is preferable to arrange the center of the opening 23B. By doing so, it becomes easy to secure a volume for holding the raw material S in the inner container 20, so that a structure suitable for manufacturing a large amount of powder for magnetic material can be easily formed.

  The reaction furnace 1 is located outside the inner container 20 and inside the outer container 10, that is, between the inner container side 21 constituting the inner container 20 and the inner shell 10i of the outer container body 10B constituting the outer container 10. A heater 2 is arranged. By arranging the heater 2 outside the inner container 20, there is an advantage that the degree of freedom of arrangement of the heater 2 is improved. The heater 2 is an electric heater, for example, and is controlled by the control device 50. In the HDDR reaction, the raw material S held in the inner container 20 is heated by the heater 2 through the inner container 20. As will be described later, the heater 2 may be disposed inside the inner container 20. Moreover, it is preferable to arrange a heat insulating material between the heater 2 and the inner shell 10 i of the outer container body 10 </ b> B constituting the outer container 10. By doing in this way, since it can suppress with a heat insulating material that the heat | fever discharge | released from the heater 2 and the heat | fever generate | occur | produced at the time of HDDR reaction are transmitted to the outer container main body 10B, temperature rising of the outer container main body 10B can be done more effectively. Can be suppressed.

  The reaction furnace 1 has a gas inlet 12I for introducing gas into the outer container 10 and a gas outlet 12E for discharging the gas inside the outer container 10 to the outside of the outer container 10. The gas inlet 12I and the gas outlet 12E penetrate the outer shell 10o and the inner shell 10i of the outer container main body 10B constituting the outer container 10, and communicate the outer side and the inner side of the outer container main body 10B. A pressure sensor 9 is provided at the gas inlet 12I as pressure detection means for detecting the pressure in the internal space 10I of the outer container 10. Thereby, for example, when the powder for magnetic material is manufactured, the pressure in the internal space 10I is detected and controlled to a necessary pressure. In addition, since the pressure sensor 9 should just detect the pressure of internal space 10I, the attachment location is not limited to gas inlet 12I.

  A gas supply passage 30 is connected to the gas inlet 12I. The gas supply passage 30 is provided with a gas supply pump 6 which is a gas supply means. The discharge port of the gas supply pump 6 is connected to the gas inlet 12 </ b> I through the gas supply passage 30, and the suction port is connected to the on-off valves 32 and 33 through the gas supply passage 30. An on-off valve 36 is provided between the discharge port of the gas supply pump 6 and the gas introduction port 12I. A hydrogen tank 34 for storing hydrogen is connected to the side of the on / off valve 32 opposite to the gas supply pump 6, and an argon tank for storing argon as an inert gas is connected to the side of the on / off valve 33 opposite to the gas supply pump 6. 35 is connected. With such a configuration, the gas supply pump 6 supplies gas (hydrogen or argon in the present embodiment) to the internal space 10I via the gas supply passage 30 and the gas inlet 12I. Hydrogen is used for the HDDR reaction, and argon is used for cooling the raw material S after the HDDR reaction. Hydrogen and argon are both supplied to the internal space 10I in a gaseous state.

  A gas discharge passage 31 is connected to the gas discharge port 12E. The gas discharge passage 31 is provided with an exhaust pump 7 which is a gas discharge means. The exhaust pump 7 is controlled by the control device 50. An on-off valve 37 is connected between the suction port of the exhaust pump 7 and the gas discharge port 12E. With such a configuration, the exhaust pump 7 discharges the gas in the internal space 10 </ b> I to the outside of the outer container 10 through the gas discharge port 12 </ b> E and the gas discharge passage 31. In the present embodiment, the gas supply pump 6, the exhaust pump 7, and the on-off valves 32, 33, 36, and 37 are controlled by the control device 50.

  When supplying hydrogen to the internal space 10I of the outer container 10, the on-off valve 32 and the on-off valve 36 are opened, the on-off valve 33 and the on-off valve 37 are closed, and the gas supply pump 6 is driven. When supplying argon to the internal space 10I, the on-off valve 33 and the on-off valve 36 are opened, the on-off valve 32 and the on-off valve 37 are closed, and the gas supply pump 6 is driven. When exhausting the gas in the internal space 10I, the on-off valve 37 is opened, the on-off valve 36 is closed, and the exhaust pump 7 is driven.

  The reaction furnace 1 has a wind guide 15 as a gas flow control means for guiding the gas supplied from the gas inlet 12I to the inside of the inner container 20. The air guide body 15 is an annular plate-like member provided with an opening (hereinafter referred to as an introduction port) 15H at a position facing the first opening 23T of the inner container 20. In the present embodiment, the air guide body 15 is provided between the gas inlet 12I and the gas outlet 12E, and between the first opening 23T of the inner container 20 and the gas inlet 12I. Then, the gas flowing in from the gas inlet 12I is introduced into the inner container 20. In this embodiment, since the distance between the air guide body 15 and the first opening 23T is long, the introduction cylinder 15S, which is a cylindrical structure, is attached to the introduction port 15H. When the distance from the first opening 23T is short, the introduction port 15H may be a simple hole.

  The air guide body 15 partitions the gas inlet 12I and the gas outlet 12E, and suppresses a phenomenon in which hydrogen and argon flowing in from the gas inlet 12I are discharged from the gas outlet 12E through the outside of the inner container 20. . As a result, during the production of the magnetic material powder, hydrogen and argon flowing in from the gas inlet 12I are efficiently supplied to the raw material S held inside the inner container 20. Further, by providing the air guide body 15 between the first opening 23T of the inner container 20 and the gas introduction port 12I, the distance between the introduction port 15H and the first opening 23T can be reduced, and on the gas introduction port 12I side. The volume of the internal space 10I of the outer container 10 can be made smaller than the gas outlet 12E side. Thereby, hydrogen or argon can be efficiently supplied to the raw material S held inside the inner container 20.

  In the present embodiment, the shape of the inlet 15H is circular, but is not limited to this. If the introduction port 15H is larger than the first opening 23T, hydrogen and argon that do not flow from the first opening 23T and flow to the outside of the inner container 20 increase, and the introduction port 15H is smaller than the first opening 23T. As a result, the flow rate of hydrogen or argon passing through the introduction port 15H is reduced, so that the inflow efficiency of hydrogen or argon into the inner container 20 may be reduced. For this reason, by making the shape and size of the inlet 15H the same as the first opening 23T of the inner container 20, the amount of hydrogen and argon flowing to the outside of the inner container 20 is suppressed, and the inflow efficiency is reduced. Can be suppressed.

  When the inner container support member 16 or the support roller 17 interferes with the air guide 15, an opening other than the inlet 15 </ b> H may be provided in the air guide 15 so that these do not interfere with the air guide 15. In this embodiment, the air guide body 15 is attached to the lid 10C of the outer container 10, and moves together with the lid 10C when the lid 10C is opened. Thereby, the lid 10C is opened, and the reduction in work efficiency when the inner container 20 is arranged in the inner space 10I of the outer container 10 or the inner container 20 is taken out from the inner space 10I can be suppressed. Note that the air guide body 15 may be provided on the inner side of the inner shell 10i of the outer container body 10B so as to be attached and detached.

  FIGS. 5A and 5B are schematic diagrams illustrating modifications of the air guide body. The air guide body 15 should just be arrange | positioned between the gas inlet 12I and the gas exhaust port 12E, and is limited to the structure arrange | positioned between the 1st opening 23T of the inner container 20, and the gas inlet 12I. It is not a thing. For example, as shown in FIG. 5A, an air guide body 15 a may be provided around the inner container 20. In this case, the through hole 15Ha is provided in the air guide body 15a, and the inner container 20 is passed through the through hole 15Ha.

  Even in this case, since the gas inlet 12I and the gas outlet 12E are partitioned by the air guide body 15a, the amount of hydrogen and argon discharged from the gas outlet 12E through the outside of the inner container 20 can be reduced. As a result, at the time of manufacturing the magnetic material powder, hydrogen and argon flowing in from the gas inlet 12I are efficiently supplied to the raw material S held inside the inner container 20. Moreover, since the air guide body 15a shown to FIGS. 5-1 may be fixed to the inner shell 10i of the outer container main body 10B, it is not necessary to make it the structure which can be attached and detached with respect to the inner shell 10i. This eliminates the need for a structure that can be attached and detached, so that the structure of the reactor 1 can be simplified.

  Furthermore, like the air guide body 15b shown in FIG. 5-2, the introduction cylinder 15S which is a cylindrical structure is attached to the introduction port 15H, and the end opposite to the end attached to the introduction port 15H is the content. It is disposed in the first opening 23T of the vessel 20. In this way, hydrogen and argon that have passed through the inlet 15H can be efficiently supplied to the raw material S held inside the inner container 20. The gas flow control means is not limited to the air guides 15, 15a, 15b. For example, a duct that leads to the first opening 23T may be attached to the gas inlet 12I, or hydrogen or argon that has flowed out of the gas inlet 12I may be led to the first opening 23T by a blowing means (for example, a fan).

  In the present embodiment, the reaction furnace 1 may have a stirring means for stirring the raw material S of the magnetic material powder. When the raw material S is stirred by the stirring means in addition to rotation or swinging of the inner container 20 during the HDDR reaction, the raw material S becomes more uniform and the quality of the magnetic material powder is further improved. Next, the stirring means will be described.

  6, 7-1, and 7-2 are diagrams illustrating an example of an inner container provided with a stirring unit. The inner container 20b shown in FIG. 6 has a member (inner container protrusion) 26 that protrudes from the inner wall 20iwb of the inner container 20b as a stirring means. By this inner container projection 26, the raw material S held in the inner container 20b is agitated while the inner container 20b rotates or swings. As a result, the raw material S is further stirred and pulverized and refined, so that the reaction proceeds uniformly not only outside but also inside the raw material S, and the quality of the magnetic material powder is improved. Moreover, the lump of the raw material S can also be pulverized by the inner container protrusion 26. Furthermore, since the heat transfer area of the inner container 20b is increased by the inner container protrusion 26, heat can be efficiently transferred from the inner container 20b to the raw material S or from the raw material S to the inner container 20b.

  Inner containers 20c and 20d shown in FIGS. 7A and 7B have stirring means with the inner shape of the cross section orthogonal to the inner container rotation axis Zr as a polygon (in this example, a hexagon). In this way, the raw material is pulverized by the corners of the polygon and stirred, so that the raw material is more stirred than the inner container 20 having a circular inner shape in a cross section perpendicular to the inner container rotation axis Zr. In addition, since the reaction proceeds more uniformly to the inside of the raw material, the quality of the magnetic material powder is improved.

  In the inner container 20d shown in FIG. 7-2, the outer shape of the cross section orthogonal to the inner container rotation axis Zr is also a polygon having a similar shape to the inner shape. In this case, the inner container 20d is supported by the outer container body 10B of the outer container 10 via the two support rollers 17 and the inner container support member 16 as shown in FIG. Further, by providing the support portion 20dh having a circular outer shape, the inner container 20d can be smoothly rotated or swung.

  FIG. 8 is a schematic diagram showing another example of the stirring means. The stirring means shown in FIG. 8 is a member inserted into the inner container 20 from at least one of the two openings (in this example, the second opening 23B) provided on both end surfaces of the inner container 20 ( Stirring rod) 40. The stirring rod 40 is inserted into the inner container 20 that is rotating or swinging from the second opening 23B. At this time, the stirring rod 40 is inserted into the inner container 20 so as to intersect the inner container rotation axis Zr. Then, the raw material S is agitated in contact with the raw material S held in the inner container 20. When stirring the raw material S, the stirring rod 40 may be vibrated to promote stirring. Further, the stirring rod 40 may be reciprocated in a direction parallel to the inner container rotation axis Zr. In this way, since the raw material S can be stirred over the entire direction parallel to the inner container rotation axis Zr, the raw material S can be stirred more uniformly to produce a magnetic material powder with more uniform quality.

  FIG. 9 is an explanatory view showing a modification of the stirring rod. The stirring rod 40a is constituted by a link mechanism in which the first arm 41 and the second arm 42 are connected so as to be swingable by a pin 43 serving as a swing center axis. And the part (stirring tool 47) which stirs the raw material S can move so that the raw material S may be touched. An input lever 44 is attached to the first arm 41 so as to intersect the first arm 41 and to be orthogonal to the swinging central axis. The input lever 44 is connected so that the connecting rod 45 can swing. Is done. With this structure, when the connecting rod 45 is moved in a direction parallel to the second arm 42, the first arm 41 swings about the swing center axis. That is, the 1st arm 41 becomes a movable part. A stirring tool 47 is attached to the distal end portion of the first arm 41, that is, the end portion on the opposite side to the swinging central axis.

  When the stirring rod 40a is used, the second gap between the connecting rod 45 and the raw material S is changed from at least one of the two openings (for example, the second opening 23B) provided on both end surfaces of the inner container 20 respectively. With the two arms 42 present, the stirring rod 40a is inserted. When the raw material S is stirred, the connecting rod 45 is pushed in the direction from the second arm 42 toward the first arm 41 when the inner container 20 is rotating or swinging. Then, the first arm 41 is bent at the position of the pin 43, and the stirring tool 47 moves toward the raw material S. When the stirring tool 47 comes into contact with the raw material S, the connecting rod 45 is fixed at that position, and the raw material S is stirred. When the stirring of the raw material S is finished, the connecting rod 45 is pulled out in the direction from the first arm 41 to the second arm 42. Then, the first arm 41 rotates away from the raw material S around the position of the pin 43, and as a result, the stirring tool 47 moves away from the raw material S. Thereby, stirring of the raw material S is completed.

  When the stirring bar 40a is inserted into the inner container 20, it is not necessary to cross the stirring bar 40a with the inner container rotation axis Zr. As shown in the example shown in FIG. 8, when the stirring bar 40 intersects the inner container rotation axis Zr, the stirring bar 40 is placed inside the inner container 20 unless there is a certain margin in the inner diameter of the outer container body 10 </ b> B shown in FIG. 1. Cannot insert. However, the stirring rod 40a shown in FIG. 9 does not need to intersect the stirring vessel 40a with the inner vessel rotation axis Zr. Therefore, even if the inner diameter of the outer vessel main body 10B shown in FIG. The raw material S can be stirred by inserting 40a into the inner container 20. Note that the stirring tool 47 attached to the stirring rod 40 a may be configured to be replaceable, and a jig for collecting the raw material S during reaction, various sensors, and the like may be attached instead of the stirring tool 47. In this way, the progress of the HDDR reaction can be confirmed, and various physical quantities other than the temperature in the reaction atmosphere can be measured. For example, the temperature of the raw material S can be directly measured by attaching the temperature sensor 8 described above to the stirring rod 40a instead of the stirring tool 47 and bringing the temperature sensor 8 into contact with the raw material S. Thereby, the HDDR reaction can be controlled with higher accuracy. In addition, you may attach the jig | tool for collecting the raw material S in reaction, etc. to the stirring rod 40 shown in FIG.

  FIG. 10 is an explanatory diagram showing a configuration of a means for supplying an additive to the inside of the inner container with the reaction furnace lid closed. An additive such as Dy or Tb may be supplied to the raw material S during the HDDR reaction. For this reason, the reaction furnace 1 shown in FIG. 1 may have a means (additive supply means) 60 for supplying an additive to the inside of the inner container. If the additive supply means 60 is used, the additive can be supplied to the raw material S without interrupting the HDDR reaction, so that the working efficiency in producing the magnetic material powder is improved.

  As shown in FIG. 10, the additive supply means 60 is disposed inside the inner container 20. More specifically, the additive supply means 60 is connected to the inside of the inner container 20 from at least one of the two openings (in this example, the second opening 23B) provided on both end faces of the inner container 20. Inserted and placed inside the inner container 20. The additive supply means 60 includes, for example, an additive passage 61 formed of a pipe, a first door 63 provided on the additive inlet 62 side of the additive passage 61 to open and close the additive passage 61, and an additive The second door 65 is provided on the additive inlet 64 side of the passage 61 and opens and closes the additive passage 61, and a space 66 defined by the first door 63 and the second door 65 is included. The additive passage 61 is inserted into the inner space 10I from the outer container body 10B shown in FIG. 1, the additive passage 61 is inserted into the inner container 20 through the second opening 23B, and the additive inlet 64 is inserted into the inner container 20. The first door 63 and the second door 65 are disposed outside the outer container body 10B.

  When supplying the additive to the raw material S, the additive is introduced from the additive inlet 62 with the first door 63 opened and the second door 65 closed. The added additive is fed into the space 66 through the first door 63. When the additive is fed into the space 66, the first door 63 is closed and the second door 65 is opened. Then, the additive in the space 66 is supplied from the additive inlet 64 to the raw material S in the inner container 20 through the additive passage 61. In this way, the additive can be added to the raw material S during the HDDR reaction. Further, since the additive passage 61 of the additive supply means 60 is inserted into the inner container 20 from the second opening 23B, the second opening 23B is formed in a predetermined region including the inner container rotation axis Zr. If the additive passage 61 is inserted so as not to contact the second opening 23B, the additive can be supplied to the raw material S even if the inner container 20 is rotating or swinging.

  FIG. 11 is a diagram illustrating another configuration example of the shaft member included in the inner container. The shaft member 24a shown in FIG. 11 omits a plurality of holes provided on the side surface. Since the shaft member 24 shown in FIGS. 1 and 3 connects the inner container lid member 22T and the inner container bottom member 22B, when the inner container 20 rotates or swings, the shaft member 24 also rotates with the inner container 20 or Swing. For this reason, when the reaction furnace 1 shown in FIG. 1 includes the stirring rods 40 and 40a and the additive supply means 60 described above, there is a configuration in which the shaft member 24 is not used. Further, like the shaft member 24a shown in FIG. 11, the first shaft member 24a1 and the second shaft member 24a2 constitute the shaft member 24a, and the first shaft member 24a1 and the second shaft member 24a2 are connected to the inner container rotating shaft. They are spaced apart by a predetermined distance in the direction parallel to Zr. Here, one end portions of the first shaft member 24a1 and the second shaft member 24a2 are connected to the inner container lid member 22T and the inner container bottom member 22B, respectively, and the first shaft member 24a1 and the second shaft are connected. A spacer 27 is provided at each of the other end portions of the member 24a2 so as to maintain a predetermined distance from the inner container side portion 21.

  With such a configuration, a gap 28 is formed between the first shaft member 24a1 and the second shaft member 24a2. The gap 28 is formed for one turn in the circumferential direction of the shaft member 24a. When the inner container 20 rotates or swings by inserting the stirring rods 40 and 40a and the additive supply means 60 into the gap 28, the stirring rods 40 and 40a and the additive supply means 60 and the shaft member 24a Interference can be avoided. When the movement of the inner container 20 is only swinging, the gap 28 does not need to be formed for one turn in the circumferential direction of the shaft member 24a.

  FIG. 12 is a perspective view showing another configuration example of the shaft member provided in the inner container. FIG. 13 is a schematic diagram of the shaft member support structure shown in FIG. The shaft member 24b shown in FIGS. 12 and 13 omits a plurality of holes provided on the side surface. The shaft member 24b has a cutout 28b on the side surface, and the stirring rods 40, 40a and the additive supply means 60 are inserted into the cutout 28b, and the stirring rod 40 is moved from the inside to the outside of the shaft member 24b. , 40a and additive supply means 60 penetrate.

  As shown in FIG. 13, the first opening 23Te provided in the inner container lid member 22Te of the inner container 20e and the second opening 23Be provided in the inner container bottom member 22Be respectively support both ends of the shaft member 24b. Bearings 29T and 29B are provided. The shaft member 24b is rotatably supported by the inner container cover member 22Te and the inner container bottom member 22B constituting the inner container 20e by the bearings 29T and 29B so that the shaft member 24b can rotate independently of the inner container 20e. Composed.

  Therefore, even if the shaft member 24b is stationary, the inner container 20e can rotate or swing. For this reason, in a state where the stirring rods 40, 40a and the additive supply means 60 are inserted into the notch 28b, the shaft member 24b remains stationary together with the stirring rods 40, 40a and the additive supply means 60, and the inner container 20e rotates. Or it can swing. As a result, the inner container 20e can be rotated or swung while the stirring rods 40, 40a and the additive supply means 60 are inserted into the notch 28b.

  FIG. 14 is an explanatory view showing an example in which a heater is arranged inside the inner container. In the above description, the heater 2 is arranged outside the inner container 20 as shown in FIG. 1, but the heater 2 may be arranged inside the inner container 20 as shown in FIG. 14. In this case, the heater 2 is supported by a heater support 2H provided on the inner shell 10i of the outer container body 10B shown in FIG. Then, it is inserted into the inner container 20 from the opening of the inner container 20 (in this example, the second opening 23B). When the heater 2 is arranged inside the inner container 20, the space is small compared to the outside of the inner container 20, so it is necessary to secure a space for arranging the heater 2. There is an advantage that it can be heated. Next, the manufacturing method of the powder for magnetic materials is demonstrated.

FIG. 15 is a flowchart showing a method for manufacturing a magnetic material powder according to the present embodiment. The manufacturing method of the powder for magnetic materials according to the present embodiment can be realized by the reaction furnace 1 described above. In the following description, an example in which the method for manufacturing a magnetic material powder according to the present embodiment is realized using the reaction furnace 1 shown in FIGS. 1 and 2 will be described. Next, an example in which a powder of Nd ₂ Fe ₁₄ B, which is a rare earth alloy powder, is manufactured as the magnetic material powder will be described. In step S <b> 101, the operator starts the circulation of the cooling medium W by turning on the power of the reactor 1 and operating the control device 50 to drive the cooling pump 5.

Next, it progresses to step S102 and an operator opens the cover 10C of the outer container 10, and takes out the inner container 20 from the outer container main body 10B. Then, the process proceeds to step S103, and the operator opens the inner container lid member 22T of the inner container 20, and a predetermined amount of the raw material S for magnetic material powder (prepared object, In the embodiment, the Nd ₂ Fe ₁₄ B alloy) is charged and then the inner container lid member 22T is closed, and the inner container lid member 22T is attached to the inner container side portion 21. Here, the crystal size of the Nd ₂ Fe ₁₄ B alloy as the raw material S is 10 μm to 100 μm.

  Then, it progresses to step S104 and an operator mounts the inner container 20 between the two support rollers 17 provided in the outer container main body 10B, and closes the lid | cover 10C of the outer container 10. FIG. And it progresses to step S105 and an operator operates the control apparatus 50, closes the on-off valve 36, opens the on-off valve 37, and then drives the exhaust pump 7, whereby the gas in the internal space 10I of the outer container 10 is driven. Evacuate and vacuum. When the pressure in the internal space 10I reaches a predetermined pressure set in advance, the operator operates the control device 50, closes the on-off valve 37, and then stops the exhaust pump 7, thereby terminating the exhaust.

  Next, proceeding to step S106, the operator operates the control device 50 to open the on-off valve 32 and the on-off valve 36, close the on-off valve 33 and the on-off valve 37, and drive the gas supply pump 6. Hydrogen is supplied from the hydrogen tank 34 to the internal space 10I. In step S107, the pressure in the internal space 10I is maintained at a predetermined pressure P1 (for example, 100 kPa). In this case, for example, the control device 50 operates the gas supply pump 6 so that the deviation between the actual pressure P in the internal space 10I detected by the pressure sensor 9 and the target value P1p of the predetermined pressure P1 becomes zero. Feedback control.

  Next, the process proceeds to step S108, and the operator operates the control device 50 to drive the electric motor 18M, thereby rotating or swinging the inner container 20. And it progresses to step S109 and an operator operates the control apparatus 50 and starts the heating by the heater 2. FIG. In step S109, the control device 50 continues heating until the temperature detected by the temperature sensor 8 (that is, the temperature of the internal space 10I) T reaches a predetermined temperature T1 (for example, 100 ° C.).

  Thereafter, the process proceeds to step S110, and the control device 50 holds the internal space 10I at a predetermined temperature T1 and a predetermined pressure P1 for a predetermined time τ1 (for example, 120 minutes). In this case, for example, the control device 50 supplies the electric power supplied to the heater 2 so that the deviation between the temperature T of the internal space 10I detected by the temperature sensor 8 and the target value T1p of the predetermined temperature T1 becomes zero. Feedback control. In addition, the control apparatus 50 also continues the control which hold | maintains the pressure of the internal space 10I mentioned above to the predetermined pressure P1. In step S <b> 110, the raw material S held in the inner container 20 occludes hydrogen inside the inner container 20. At this time, since the inner container 20 rotates or swings and the raw material S is agitated, the entire raw material S occludes hydrogen evenly, and the non-uniform hydrogen occlusion state is reduced.

  When the predetermined time τ1 has elapsed, the process proceeds to step S111. In step S111, the operator operates the control device 50 to maintain the pressure in the internal space 10I at a predetermined pressure P2 (for example, 40 kPa). In this case, for example, the control device 50 opens the on-off valve 37 to reduce the pressure in the internal space 10I. Thereafter, the control device 50 feedback-controls the operation of the gas supply pump 6 so that the deviation between the actual pressure P in the internal space 10I detected by the pressure sensor 9 and the target value P2p of the predetermined pressure P2 becomes zero. The operation of the on-off valve 37 is also feedback-controlled as necessary.

  Next, it progresses to step S112 and an operator operates the control apparatus 50, and continues heating until the temperature T which the temperature sensor 8 detected reaches predetermined | prescribed predetermined temperature T2 (for example, 800 degreeC). Thereafter, the process proceeds to step S113, and the control device 50 holds the internal space 10I at a predetermined temperature T2 and a predetermined pressure P2 for a predetermined time τ2 (eg, 360 minutes). In this case, for example, the control device 50 supplies the electric power supplied to the heater 2 so that the deviation between the temperature T of the internal space 10I detected by the temperature sensor 8 and the target value T2p of the predetermined temperature T2 becomes zero. Feedback control. In addition, the control apparatus 50 also continues the control which hold | maintains the pressure of the internal space 10I mentioned above to the predetermined pressure P2.

In step S113, the raw material S held in the inner container 20 is hydrogenated and decomposed to generate a fine matrix (NdHx, α-Fe, Fe ₂ B matrix) on the order of 100 nm, that is, HD reaction is occurring. At this time, the raw material S generates heat, but this heat is absorbed by the inner container 20. Further, since the raw material S is stirred by rotating or swinging the inner container 20, the temperature distribution of the raw material S is reduced.

  When the predetermined time τ2 has elapsed, the process proceeds to step S114. In step S114, the operator operates the control device 50 to heat the temperature T detected by the temperature sensor 8 until the temperature reaches a predetermined temperature T3 (for example, 850 ° C.). And it progresses to step S115 and an operator operates the control apparatus 50 and stops supply of hydrogen to the internal space 10I. In this case, the control device 50 closes the on-off valve 36 and the on-off valve 32 and stops the operation of the gas supply pump 6. Next, the process proceeds to step S116, and the operator exhausts the gas in the internal space 10I to reduce the internal space 10I to a predetermined exhaust end pressure Pf. In this case, the control device 50 opens the on-off valve 37 and drives the exhaust pump 7.

  In depressurizing the internal space 10I, the control device 50 first depressurizes to a predetermined pressure P3 (for example, 6 kPa) at a predetermined speed V1 (for example, 4 kPa / min). Thereafter, the control device 50 reduces the pressure to a predetermined exhaust end pressure Pf (for example, 1 kPa) at a predetermined speed V2 (for example, 0.1 kPa / min). When the pressure in the internal space 10I reaches a predetermined exhaust end pressure Pf, the controller 50 is operated to end the exhaust of the gas in the internal space 10I. In this case, the control device 50 closes the on-off valve 37 and stops the exhaust pump 7.

In step S116, the raw material S held in the inner vessel 20 undergoes a reaction in which an Nd ₂ Fe ₁₄ B phase is generated by dehydrogenation and recombination, that is, a DR reaction. At this time, the raw material S absorbs heat. Nd ₂ Fe ₁₄ B produced in the DR reaction has a crystal size of 100 nm to 500 nm. Hydrogen released from the raw material S in the DR reaction, that is, hydrogen existing in the internal space 10I of the outer container 10 of the reaction furnace 1 is discharged to the outside from the gas outlet 12E provided in the outer container body 10B. While the DR reaction proceeds, the inner container 20 rotates or swings and the raw material S is agitated, so that the HD reaction can be uniformly advanced throughout the raw material S. Further, the hydrogen released from the raw material S in the DR reaction is surely discharged from the inside of the inner container 20 through the second opening 23B of the inner container 20 shown in FIG.

  When the pressure reduction in step S116 ends, the process proceeds to step S117, and the operator operates the control device 50 to end the power supply to the heater 2. Next, it progresses to step S118, an operator operates the control apparatus 50, supplies argon as a cooling inert gas which cools a raw material to the internal space 10I, and cools the raw material S after a HDDR reaction. . When supplying argon, the control device 50 opens the on-off valve 33 and the on-off valve 36, closes the on-off valve 32 and the on-off valve 37, and drives the gas supply pump 6 to drive argon from the argon tank 35 to the internal space 10I. Is supplied. Next, the process proceeds to step S119, and cooling is continued until the temperature of the internal space 10I reaches a predetermined temperature T4 (for example, 30 ° C.).

  When the temperature T detected by the temperature sensor 8 reaches the predetermined temperature T4, the process proceeds to step S120, and the operator operates the control device 50 to finish the rotation or swing of the inner container 20, and then the argon gas Stop supplying. In this case, the control device 50 stops driving the electric motor 18M, closes the on-off valve 33 and the on-off valve 36, and stops the gas supply pump 6. And it progresses to step S121 and an operator opens the cover 10C of the outer container 10, and takes out the inner container 20 from the internal space 10I. And it progresses to step S122 and an operator opens the inner container cover member 22T of the inner container 20, and takes out the raw material S after HDDR reaction is complete | finished, ie, the powder for magnetic materials completed. The completed powder for magnetic material becomes a magnet by being magnetized.

  When the process is subsequently executed (step S123, Yes), the process returns to step S103, and the subsequent steps are executed. Subsequently, when the process is not executed (step S123, No), the process proceeds to step S124. In step S124, the worker executes an end work. That is, the operator attaches the inner container lid member 22T to the inner container 20 and then returns to the inner space 10I to close the lid 10C. And after operating the control apparatus 50 and stopping the drive of the cooling pump 5, the power supply of the reactor 1 is turned off.

  As described above, in the present embodiment, the reactor 1 is provided with the first opening 23T and the second opening 23B in the inner vessel 20, so that in the HDDR reaction, hydrogen is reliably supplied to the raw material S, and from the raw material S The released hydrogen can be reliably released to the outside of the inner container 20. As a result, the storage and release speed of hydrogen is large and the amount is large. As a result, in the HDDR reaction in which the pressure change in the inner container 20 is large, the deformation of the inner container 20 is avoided and the magnetic material powder is reliably manufactured. it can. Moreover, since the cooling inert gas (for example, argon) supplied after completion | finish of HDDR reaction is also reliably supplied to the raw material S, the raw material S can be cooled reliably. Moreover, since the reactor 1 cools the outer container 10, leakage of hydrogen from the outer container 10 can be suppressed in the HDDR reaction in which a large amount of heat enters and exits during the reaction process.

  Here, in the method in which the raw materials are placed directly and the HDDR reaction is performed, the reaction proceeds only on the surface of the raw material aggregate, and the reaction inside the raw material aggregate ends in the middle. However, since the reaction furnace 1 rotates or swings the inner container 20 and stirs the raw material S, the HDDR reaction of the entire raw material S can surely proceed. In addition, the reaction furnace 1 can make the temperature distribution of the raw material S uniform and the absorption and release of hydrogen by the stirring of the raw material S by the rotation or swinging of the inner container 20, thereby uniformly reacting the entire raw material S. it can. As a result, the quality of the produced magnetic material powder is improved.

  In addition, since the reactor 1 can quickly and uniformly make the temperature of the raw material S by stirring the raw material S, it is easy to control the temperature of the raw material S in the HDDR reaction in which a large amount of heat enters and exits during the reaction process. There are advantages. When a large amount of the raw material S is subjected to the HDDR reaction, the heat input and output in the reaction process becomes larger and the temperature control of the raw material S becomes more difficult. The temperature can be controlled. Thus, the reactor 1 is particularly suitable for producing a large amount of powder for magnetic material by the HDDR method.

  Further, even if the raw material S is a large lump, it can be pulverized and refined by rotating or swinging the inner container 20, so that a situation where the HDDR reaction proceeds only on the surface of the lump can be avoided. Further, since the large lump raw material S can be pulverized by rotating or swinging the inner container 20, it is not necessary to pulverize the raw material in advance. This improves the workability when manufacturing the magnetic material powder.

  Further, the inner vessel 20 provided in the reaction furnace 1 measures the temperature near the raw material S in the inner vessel 20 by inserting the temperature sensor 8 from the openings provided on both end faces, so that the atmosphere closer to the HDDR reaction field Temperature can be measured. As a result, the accuracy of temperature control in the HDDR reaction is improved, and the quality of the produced magnetic material powder is improved. Furthermore, since an instrument having various functions can be arranged from the opening of the inner container 20 to the inside of the inner container 20, in actual operation, the reactor 1 can be adapted flexibly without major modification. . Moreover, since the reactor 1 can also arrange | position the heater 2 in the inner container 20 from the opening of the inner container 20, it can respond flexibly also to a future design change.

  As described above, the reactor according to the present invention is useful for producing a magnetic material powder using the HDDR reaction.

DESCRIPTION OF SYMBOLS 1 Reactor 2 Heater 3 Temperature sensor support body 4 Cooling medium cooler 5 Cooling pump 6 Gas supply pump 7 Exhaust pump 8 Temperature sensor 9 Pressure sensor 10 Outer container 10B Outer container main body 10Bc Main body side cooling medium passage 10C Cover 10Cc Cover Side cooling medium passage 10I Inner space 10i Inner shell 10o Outer shell 12I Gas inlet 12E Gas outlet 13IB Main body side cooling medium supply port 13IC Lid side cooling medium supply port 13EB Main body side cooling medium outlet 13EC Lid side cooling medium outlet 15 , 15a, 15b Air guide body 16 Inner container support member 17 Support roller 18 Inner container drive device 20, 20a, 20b, 20c, 20d, 20e Inner container 22T, 22Ta, 22Te Inner container cover member 22B, 22Ba, 22Be Inner container bottom member 23T, 23Te 1st opening 23B, 23Be 2nd opening 24, 24a, 24b shaft member 25 bore 26 inner container projections 40,40a stirrer 47 stirring device 50 controller 60 additive supply means

Claims (12)

A reactor used for hydrocracking and dehydrogenation recombination,
An outer container,
An outer container cooling means for cooling the outer container;
A cylindrical container that is disposed inside the outer container and holds the raw material, and is supported inside the outer container so that it can rotate or swing around an axis that intersects both end faces of the container. An inner container having an opening on each of both end faces;
An inner container driving means for rotating or swinging the inner container;
A heater disposed on at least one of the outer side and the inner side of the inner container;
And the outer hydrogen inlet for introducing hydrogen into the container, and the hydrogen discharge port for discharging hydrogen in the interior of the outer vessel to the outside of the outer container,
The hydrogen supplied from the hydrogen inlet, and a hydrogen flow control means leading from the opening into the interior of the inner container,
A reactor characterized by comprising:   The reaction furnace according to claim 1, wherein a temperature sensor is disposed inside the inner container.   The reactor according to claim 1, wherein a stirring means for stirring the raw material in the inner container is disposed inside the inner container.   The reactor according to claim 3, wherein the stirring means is a member protruding from an inner wall of the inner container.   The reactor according to claim 1, further comprising a member that is inserted into the inner vessel through at least one of the openings.   The reactor according to claim 5, wherein the member supports a temperature sensor inside the inner container.   The reactor according to claim 5, wherein the member is a stirring unit that stirs the raw material in the inner container. The stirring means is composed of a link mechanism coupled to the movable to so that around the movable shaft reactor of claim 7 having a movable portion which moves in contact with the material. The reaction furnace according to claim 1, wherein an additive supply means for supplying an additive to the raw material is disposed.
An additive charging port disposed outside the outer container and capable of charging an additive;
The additive inserted into the inner container from at least one of the two openings of the inner container in communication with the additive inlet, and the additive introduced from the additive inlet into the raw material inside the inner container A reactor including an additive outlet capable of being supplied.   The reaction according to any one of claims 1 to 9, wherein the inner container has a cylindrical shaft member having both ends opened between the openings, and the shaft member has a hole on a side surface. Furnace.   The reaction furnace according to any one of claims 1 to 10, wherein a rotation shaft of the inner container passes through at least one of the openings. In producing powder for magnetic materials by hydrocracking / dehydrogenation recombination method,
Introducing the raw material for the magnetic material powder into a container in a reactor;
While cooling the reactor, hydrogen is supplied into the reactor, the hydrogen is introduced into the vessel, the hydrogen in the vessel is released to the outside, and the reactor is heated while the vessel is heated. Agitating the raw material by rotating or swinging;
Discharging hydrogen in the reactor out of the reactor;
A method for producing a powder for a magnetic material, comprising:

Images