WO2024252938A1 - Cuve de réaction de type à tubes multiples - Google Patents

Cuve de réaction de type à tubes multiples Download PDF

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Publication number
WO2024252938A1
WO2024252938A1 PCT/JP2024/018991 JP2024018991W WO2024252938A1 WO 2024252938 A1 WO2024252938 A1 WO 2024252938A1 JP 2024018991 W JP2024018991 W JP 2024018991W WO 2024252938 A1 WO2024252938 A1 WO 2024252938A1
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Prior art keywords
reaction gas
catalyst
pipe
gas flow
tube
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Ceased
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PCT/JP2024/018991
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English (en)
Japanese (ja)
Inventor
治貴 浦部
真 土居
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JFE Engineering Corp
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JFE Engineering Corp
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Publication date
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Publication of WO2024252938A1 publication Critical patent/WO2024252938A1/fr
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside

Definitions

  • This relates to a reaction vessel equipped with a catalyst-filled vessel through which a reaction gas flows and which is filled with a catalyst, and in particular to a multi-tube reaction vessel in which the reaction vessel has multiple tubes.
  • Patent Document 1 discloses a method in which a heat transfer tube through which a refrigerant flows is provided in a catalyst packed bed, and cooling is performed from the packed bed.
  • the activity of the catalyst gradually decreases due to poisoning from impurities in the raw materials and adhesion of the products to the catalyst surface. For this reason, it is common for the catalyst packed in the reactor to be replaced periodically.
  • Patent Document 2 discloses a technique in which the tip of a double pipe is cut open, a vacuum pump hose is inserted to suck out the filler, and the pipe is refilled and then welded shut.
  • Patent Document 3 discloses a method in which a fluid is fed into a tube filled with a catalyst to flush the filler.
  • JP 2003-229147 A Japanese Patent Application Publication No. 10-328555 Japanese Unexamined Patent Publication No. 60-71036
  • the method of Patent Document 1 has a problem in that the cooling efficiency is good in the areas close to the heat transfer tubes in the packed bed, but is poor in areas away from the heat transfer tubes, such as near the wall of the packed container.
  • the vacuum pump power is used to suck out the catalyst.
  • the catalyst since the catalyst is sucked up, the catalyst may fall due to the effect of gravity, and there is a problem that it is difficult to recover all of it.
  • the container in the method of Patent Document 2, the container must be cut open prior to recovery of the catalyst, and the cut portion must be welded shut after filling, which is problematic in terms of labor and cost.
  • Patent Document 3 also has the problem that it requires power to transport the fluid. Also, when pushing the filler away, depending on the shape of the container, the filler may be trapped structurally, making it impossible to recover the entire amount.
  • the present invention was made to solve these problems, and aims to provide a multi-tube reaction vessel that has excellent cooling efficiency and allows easy replacement of the catalyst that is filled inside.
  • the multi-tube reaction vessel of the present invention is characterized by comprising a catalyst-fixed inner cooling pipe through which a cooling fluid flows and which has a porous catalyst layer fixed to its outer peripheral surface, a reaction gas flow pipe into which the catalyst-fixed inner cooling pipe is removably inserted and through which a reaction gas flows, and an outer cooling vessel that is provided on the outer periphery of the reaction gas flow pipe and through which a cooling fluid flows to cool the outer peripheral surface of the reaction gas flow pipe.
  • the catalyst-attached inner cooling pipe is characterized in that the porous catalyst layer is attached to the outer surface of a metal pipe via an intermediate layer, and the intermediate layer has the function of reducing the difference in thermal expansion coefficient between the porous catalyst layer and the pipe.
  • a baffle plate is provided that is disposed close to the inner surface of the reaction gas flow pipe to prevent the porous catalyst layer from contacting the inner surface of the reaction gas flow pipe and to provide resistance to the flow of the reaction gas.
  • a catalyst-fixed inner cooling pipe through which a cooling fluid flows and which has a porous catalyst layer fixed to its outer peripheral surface, a reaction gas flow pipe into which the catalyst-fixed inner cooling pipe is removably inserted and through which a reaction gas flows, and an outer cooling vessel which is provided on the outer periphery of the reaction gas flow pipe and through which a cooling fluid flows to cool the outer surface of the reaction gas flow pipe, thereby making it possible to cool the porous catalyst layer from both the inside and the outside, resulting in excellent cooling efficiency.
  • the porous catalyst layer can be removed at the same time, which provides excellent workability in catalyst replacement work.
  • FIG. 1 is an explanatory diagram of a multi-tube reaction vessel according to an embodiment of the present invention.
  • FIG. 2 is a cross-sectional view of the multi-tube reaction vessel shown in FIG. 1.
  • FIG. 2 is an explanatory diagram of a method for replacing a catalyst in the multi-tube reactor shown in FIG. 1.
  • FIG. 2 is an explanatory diagram of an embodiment in which a baffle plate is provided in the multi-tube reaction vessel shown in FIG. 1.
  • FIG. 5 is an explanatory diagram of the function when the baffle plate of FIG. 4 is provided.
  • FIG. 11 is an explanatory diagram of another embodiment of the baffle plate (part 1).
  • FIG. 2 is an explanatory diagram of another embodiment of the baffle plate (part 2).
  • FIG. 1 is an explanatory diagram of a multi-tube reaction vessel according to an embodiment of the present invention.
  • FIG. 2 is a cross-sectional view of the multi-tube reaction vessel shown in FIG. 1.
  • FIG. 2 is an explanatory diagram of
  • FIG. 4 is an explanatory diagram of another embodiment of the baffle plate (part 3).
  • FIG. 2 is an explanatory diagram (part 1) of another aspect of a multi-tube reaction vessel according to an embodiment of the present invention.
  • FIG. 10 is an explanatory diagram of the operation of the multi-tube reaction vessel shown in FIG.
  • FIG. 2 is an explanatory diagram (part 2) of another aspect of a multi-tube reaction vessel according to an embodiment of the present invention.
  • FIG. 4 is an explanatory diagram (part 3) of another aspect of a multi-tube reaction vessel according to an embodiment of the present invention.
  • the multi-tube reactor 1 includes a catalyst-fixed inner cooling tube 3, a reaction gas flow tube 5, and an outer cooling vessel 7. Each component will be described in detail below.
  • the catalyst-fixed inner cooling pipe 3 has a cooling fluid flowing through it and a porous catalyst layer 9 fixed to its outer circumferential surface.
  • the porous catalyst layer 9 is cooled from the inside by the cooling fluid flowing through it. will be done.
  • the catalyst-fixed inner cooling pipe 3 is removably inserted into the reaction gas flow pipe 5, and in the inserted state, the space between the inner surface of the reaction gas flow pipe 5 and the outer surface of the catalyst-fixed inner cooling pipe 3, i.e., the porous catalyst layer
  • the space in which the porous catalyst layer 9 is disposed is a space through which the reaction gas flows. When the reaction gas passes through the porous catalyst layer 9 disposed in this space, a catalytic reaction takes place.
  • a cover member 11 is attached to the upper part of the catalyst-fixed inner cooling pipe 3, which closes the upper end opening 5a (see Figure 3) of the reaction gas flow pipe 5 with the catalyst-fixed inner cooling pipe 3 inserted into the reaction gas flow pipe 5.
  • the lower end of the catalyst-fixed inner cooling pipe 3 is adapted to close the lower end opening 5b (see FIG. 3) of the reaction gas flow pipe 5 when the catalyst-fixed inner cooling pipe 3 is inserted into the reaction gas flow pipe 5.
  • the porous catalyst layer 9 of the catalyst-attached inner cooling pipe 3 is formed as a film and attached (integrated) to the outer circumferential surface of the pipe.
  • the catalyst is a ceramic or carbon-based material such as alumina, silica, or zeolite
  • the film is formed directly by CVD or sputtering, or a precursor gel or slurry is dip-coated or wash-coated. After the film is formed, it is heated to adhere and adhere.
  • a zeolite material it is possible to directly synthesize and form a membrane by hydrothermal synthesis.
  • the catalyst-attached inner cooling pipe 3 is made of metal, it is preferable to provide an intermediate layer 13 made of cermet or binder material, as shown in the enlarged view of Figure 2, in order to reduce the difference in thermal expansion coefficient between the metal and the porous catalyst layer 9 (oxide carrier) and ensure adhesion.
  • cooling fluid flows from the top to the bottom of the catalyst-fixed inner cooling pipe 3 .
  • cooling fluids include, but are not limited to, air, inert gas, water, seawater, ethylene glycol, and the like.
  • reaction gas flow tube The catalyst-fixed inner cooling pipe 3 is removably inserted into the reaction gas flow pipe 5, and the reaction gas flows inside the reaction gas flow pipe 5.
  • a gas inlet 15 through which the reaction gas enters is provided at the bottom of the reaction gas flow pipe 5, and a gas outlet 17 through which the reaction gas (which may contain liquid) is discharged is provided at the top of the reaction gas flow pipe 5. Therefore, the flow of the reaction gas in the reaction gas flow pipe 5 is from bottom to top, opposite to the flow of the cooling fluid in the catalyst-fixed inner cooling pipe 3, and is a counterflow to the cooling fluid.
  • the reaction gas and the cooling fluid may be counterflowed, and in some cases, the reaction gas and the cooling fluid may be parallel flows in order to preferentially cool the superheated part (gas inlet part).
  • the outer cooling vessel 7 is provided around the outer periphery of the reaction gas flow pipe 5 and cools the outer periphery of the reaction gas flow pipe 5 by passing a cooling fluid therethrough.
  • the outer cooling vessel 7 of this embodiment is made of a cylinder having a larger diameter than the reaction gas flow pipe 5, and is provided with a cooling fluid inlet 19 on the upper side and a cooling fluid outlet 21 on the lower side. Therefore, the flow of the cooling fluid in the outer cooling vessel 7 is from the top to the bottom, similar to the catalyst fixing inner cooling pipe 3, and is a counterflow to the reaction gas.
  • reaction heat is generated by a catalytic reaction occurring when the reaction gas passes through the porous catalyst layer 9. This reaction heat is cooled from the inside by the cooling fluid flowing through the catalyst-fixed inner cooling pipe 3 and from the outside by the cooling fluid flowing through the outer cooling vessel 7.
  • the heat of the catalytic reaction is cooled from both the inside and the outside, resulting in good cooling efficiency.
  • the catalyst-fixed inner cooling pipe 3 is disposed approximately at the center of the reaction gas flow pipe 5, so that cooling from the inside can be performed without bias.
  • the reaction gas flow pipe 5 is disposed approximately at the center of the outer cooling vessel 7, so that cooling from the outside can be performed without bias.
  • the present invention is characterized in that the porous catalyst layer 9 is cooled from the inside and the outside, it is not limited to the case where the catalyst-fixed inner cooling pipe 3 is disposed at the center of the reaction gas flow pipe 5, and it is also not limited to the case where the reaction gas flow pipe 5 is disposed at the center of the outer cooling vessel 7.
  • the catalyst when it is time to replace the porous catalyst layer 9, the catalyst can be replaced by simply pulling out the catalyst-fixed inner cooling pipe 3 from the reaction gas flow pipe 5 and inserting a new catalyst-fixed inner cooling pipe 3, making the catalyst replacement work extremely easy.
  • the porous catalyst layer 9 can be cooled from both the inside and outside, and therefore the cooling efficiency is excellent.
  • the catalyst can be replaced by replacing the inner cooling pipe 3 to which the catalyst has adhered, the catalyst replacement work efficiency is excellent.
  • the catalyst-fixed inner cooling tube 3 can be placed horizontally, and the installation position of the multi-tube reaction vessel 1 is not limited.
  • a baffle plate 23 on the outer periphery of the catalyst-fixed inner cooling pipe 3, which is disposed close to the inner surface of the reaction gas flow pipe 5 (dotted line in FIG. 4) to prevent the porous catalyst layer 9 (double-dotted line in FIG. 4) from contacting the inner surface of the reaction gas flow pipe 5 and to provide resistance to the flow of the reaction gas.
  • the porous catalyst layer 9 is not shown in FIG. 4.
  • the baffle plate 23 shown in FIG. 4 is annular and has many gas passage holes 23a through which the reaction gas passes. By providing the gas passage holes 23a, the reaction gas is guided by the baffle plate 23 to the porous catalyst layer 9 side as shown in FIG. 5, and contact with the porous catalyst layer 9 is improved.
  • the baffle plate 23 is also expected to have a retention effect on the porous catalyst layer 9.
  • the outer diameter of the baffle plate 23 is approximately equal to the inner diameter of the reaction gas flow pipe 5, and the outer diameter of the porous catalyst layer 9 is slightly smaller than the outer diameter of the baffle plate 23.
  • the reason for this is as follows.
  • the catalyst-fixed inner cooling pipe 3 When it is time to replace the catalyst, the catalyst-fixed inner cooling pipe 3 is pulled out from the reaction gas flow pipe 5 and a new catalyst-fixed inner cooling pipe 3 is inserted. If the porous catalyst layer 9 hits the inner surface of the reaction gas flow pipe 5 during the pulling out or insertion, it will be damaged. However, since the outer peripheral end face of the baffle plate 23 protrudes beyond the porous catalyst layer 9, it is possible to prevent the porous catalyst layer 9 from hitting the inner surface of the reaction gas flow pipe 5. It is preferable to provide a plurality of baffle plates 23 in the axial direction of the catalyst-fixing inner cooling pipe 3 .
  • baffle plate 23 As another embodiment of the baffle plate 23, as shown in FIG. 6, it may be a semicircular ring-shaped plate divided in half in the circumferential direction and positioned axially out of alignment.
  • baffle plates 23 When multiple baffle plates 23 are provided, it is necessary to ensure that the baffle plates 23 do not interfere with the protrusions 25 when inserting and removing the catalyst-fixed inner cooling pipe 3 into and from the reaction gas flow pipe 5. For this reason, for example, as shown in FIG. 8, the inner surface of the reaction gas flow pipe 5 can be tapered downward, with the baffle plates 23 on the lower side having a smaller diameter, so that the lower baffle plates 23 do not interfere with the upper protrusions 25.
  • a cover member 11 was required to close the upper end surface of the reaction gas flow pipe 5 when the catalyst-fixed inner cooling pipe 3 was inserted into the reaction gas flow pipe 5.
  • the catalyst-fixed inner cooling pipe 3 a tapered surface that narrows downward and making the upper part of the tapered surface slightly larger than the inner diameter of the reaction gas flow pipe 5 (see Figure 10)
  • the porous catalyst layer 9 adhered to the tapered surface of the catalyst-adhered inner cooling pipe 3 is thinner at the top and thicker toward the bottom. Therefore, as shown in Figure 10, if the reactive gas is introduced from the top where the layer is thinner, the amount of catalyst in contact with the reactive gas at the top is small, so heat generation in the catalyst layer due to catalytic reaction can be suppressed, and although the catalyst layer is thicker at the bottom, less of the reactive gas is left unreacted, so heat generation is suppressed, and as a result, the temperature gradient from upstream to downstream can be equalized.
  • the upper end part of the catalyst-fixed inner cooling pipe 3 may be made into a tapered surface, and the porous catalyst layer 9 may be fixed to the straight pipe part below the tapered surface.
  • the thickness of the porous catalyst layer 9 is constant, so that the porous catalyst layer 9 can be easily controlled during its formation.
  • only the upper end of the catalyst-fixed inner cooling pipe 3 may be enlarged to have a T-shaped cross section, and the underside of the part corresponding to the horizontal side of the T may be abutted against the upper end surface of the reaction gas flow pipe 5.
  • the catalyst-fixed inner cooling pipe 3 can be easily manufactured.
  • one pair of a reaction gas flow pipe 5 and a catalyst-fixed inner cooling pipe 3 is provided for one outer cooling vessel 7, but the present invention is not limited to this, and multiple pairs of a reaction gas flow pipe 5 and a catalyst-fixed inner cooling pipe 3 may be provided for one outer cooling vessel 7.
  • the thickness of the porous catalyst layer 9 fixed to each catalyst-fixed inner cooling pipe 3 becomes thinner in this embodiment, and the cooling efficiency from the inside and outside is improved.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)

Abstract

La présente invention concerne une cuve de réaction de type à tubes multiples qui présente une efficacité de refroidissement exceptionnelle et facilite le remplacement d'un catalyseur à remplir.　Une cuve de réaction de type à tubes multiples 1 selon la présente invention est caractérisée en ce qu'elle comprend : un tuyau de refroidissement côté interne fixe de catalyseur 3 à travers lequel un fluide de refroidissement s'écoule dans l'intérieur, et dans lequel une couche de catalyseur poreux 9 est fixée à une surface périphérique externe ; un tuyau de passage de gaz de réaction 5 dans lequel le tuyau de refroidissement côté interne fixe de catalyseur 3 est inséré de manière amovible, et à travers lequel un gaz de réaction s'écoule dans l'intérieur ; et un récipient de refroidissement côté externe 7 qui est disposé sur la périphérie externe du tuyau de passage de gaz de réaction 5 et refroidit la surface périphérique externe du tuyau de passage de gaz de réaction 5 en permettant au fluide de refroidissement de s'écouler à travers celui-ci.
PCT/JP2024/018991 2023-06-09 2024-05-23 Cuve de réaction de type à tubes multiples Ceased WO2024252938A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2023095237A JP2024176571A (ja) 2023-06-09 2023-06-09 多重管式反応容器
JP2023-095237 2023-06-09

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WO2024252938A1 true WO2024252938A1 (fr) 2024-12-12

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS49125282A (fr) * 1973-04-06 1974-11-30
JPS6071036A (ja) * 1983-09-29 1985-04-22 ケルンフオルシユングスアンラ−ゲ・ユ−リツヒ・ゲゼルシヤフト・ミト・ベシユレンクテル・ハフツング 細い管型反応容器において触媒を交換するための方法および装置
JPS6320029A (ja) * 1986-07-15 1988-01-27 Mitsubishi Heavy Ind Ltd 反応器
JPH05213603A (ja) * 1992-01-31 1993-08-24 Japan Atom Energy Res Inst 水蒸気改質器
JP2005298413A (ja) * 2004-04-13 2005-10-27 Kitakyushu Foundation For The Advancement Of Industry Science & Technology メタノールの高効率合成法及びそのための装置

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS49125282A (fr) * 1973-04-06 1974-11-30
JPS6071036A (ja) * 1983-09-29 1985-04-22 ケルンフオルシユングスアンラ−ゲ・ユ−リツヒ・ゲゼルシヤフト・ミト・ベシユレンクテル・ハフツング 細い管型反応容器において触媒を交換するための方法および装置
JPS6320029A (ja) * 1986-07-15 1988-01-27 Mitsubishi Heavy Ind Ltd 反応器
JPH05213603A (ja) * 1992-01-31 1993-08-24 Japan Atom Energy Res Inst 水蒸気改質器
JP2005298413A (ja) * 2004-04-13 2005-10-27 Kitakyushu Foundation For The Advancement Of Industry Science & Technology メタノールの高効率合成法及びそのための装置

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