JP5239667B2 - Plate reactor and method for producing reaction product using the same - Google Patents

Description

  The present invention relates to a plate reactor for reacting gaseous raw materials and a method for producing a reaction product using the same.

  As a reactor used for the reaction of the raw material gas in the presence of a particulate catalyst such as a gas phase catalytic oxidation reaction, there are a reaction vessel for reacting the gaseous raw material, and a plurality of reactors provided side by side in the reaction vessel. The heat transfer plate includes a plurality of heat transfer tubes connected at a peripheral edge or an edge of a cross-sectional shape, and a catalyst is filled in a gap between adjacent heat transfer plates A reactor is known (for example, refer to Patent Document 1). As such a plate reactor, for example, a plate reactor in which a plurality of heat transfer plates are accommodated side by side in a cylindrical reaction vessel is known (see, for example, Patent Documents 2 and 3). .

  In such a plate reactor, a large gap is formed between the heat transfer plates at both ends in the direction in which the heat transfer plates are aligned and the inner wall of the reaction vessel. The plate reactor described above has various problems associated with this gap.

  First, since the gap is not used for the reaction, the container is a shell (shell) having an internal volume including such a gap, which is disadvantageous in terms of size and weight and is economically disadvantageous.

  Further, when the plate reactor is used for the production of acrylic acid by the gas phase catalytic oxidation reaction of propylene and acrolein for a long time, for example, when propylene in the raw material gas stays in the gap, the raw material gas or the reaction product gas is used. The water vapor contained can condense and form a propylene squeal. In addition, when acrolein stays in the gap, it may be oxidized and burned, and may become hot due to heat generation, which may damage the plate reactor itself. Further, when acrylic acid stays in the gap, for example, it condenses and polymerizes when the plate reactor is stopped, and the produced polymer may fill the gap and expand to cause damage to the plate reactor.

Furthermore, in the production of acrylic acid described above, the plate reactor during the reaction reaches 250 to 400 ° C., and becomes normal temperature when the reaction is stopped. In the use of the plate reactor in the production of acrylic acid, since the plate reactor is exposed to a temperature from room temperature to 400 ° C., when the gap is sealed, the components constituting the plate reactor are Plate reactors can be damaged by expansion and contraction due to temperature changes. Such inconvenience can be applied to other reactions.
JP 2004-202430 A Japanese Patent Publication No. 5-51336 Japanese translation of PCT publication No. 2003-513056

  The present invention provides a plate reactor that does not cause problems due to the gap between the inner wall of the reaction vessel and the heat transfer plate.

The present invention adopts a configuration in which a plurality of heat transfer plates are sandwiched and held in the direction in which the plurality of heat transfer plates are aligned, thereby causing a problem due to a gap between the inner wall of the reaction vessel and the heat transfer plate. Provide no plate reactor.

  That is, the present invention includes a reaction vessel for reacting a gaseous raw material and a plurality of heat transfer plates provided side by side in the reaction vessel, and the heat transfer plate has a cross-sectional peripheral edge or edge. In the plate reactor in which the catalyst is filled in the gap between the adjacent heat transfer plates, the reaction vessel is arranged in the gas transfer direction in the plurality of heat transfer plates. A gas distribution section that covers both ends and distributes gas through a gap between adjacent heat transfer plates; and a heat medium supply section that contacts both ends of the heat transfer pipe in the heat transfer plate and supplies a heat medium to the heat transfer pipe. The heat transfer plates are in contact with the heat transfer plates at both ends in the direction in which the heat transfer plates are arranged so as to block the gas flow at least along the extending direction of the heat transfer tubes. A plate-type holding portion that holds the plurality of heat transfer plates in a gas-tight manner so that the gas distribution portion, the heat medium supply portion, and the plate-holding portion are accommodated. A reactor is provided.

  Further, the present invention provides a pair of sandwiching portions in which the plate sandwiching portion is in contact with at least one heat transfer tube of the heat transfer plates at both ends in the direction in which the plurality of heat transfer plates are arranged in contact with the entire heat transfer tube in the extending direction of the heat transfer tube. Provided is the plate reactor comprising a plate and a holding rod for penetrating and holding these sandwich plates.

  Further, in the present invention, the plate sandwiching portion is in contact with the heat transfer plate at both ends in the direction in which the plurality of heat transfer plates are arranged, and the peripheral edge of the heat transfer tube at the upstream end of the heat transfer plate in the gas flow direction. A plate reactor is provided.

  In addition, the present invention provides the plate reactor, further comprising a partition that partitions a gap between adjacent heat transfer plates into a plurality of compartments containing a packed catalyst along a gas flow direction.

  The present invention also provides the plate reactor in which the holding rod is disposed at a position overlapping the partition in the gas aeration direction.

  The present invention also provides the plate reactor, wherein the gas distributor further has a manhole.

The present invention also provides the plate reactor, wherein the gas distributor further includes a safety device for preventing damage to the plate reactor due to an increase in pressure in the reaction vessel.

  Moreover, this invention provides the said plate type reactor in which the said heat-medium supply part further has a heat-medium mixing apparatus which mixes a 2nd heat-medium with the 1st heat-medium in a heat-medium supply part.

  The present invention also provides the plate reactor, further comprising a gas-permeable catalyst protective cover that covers one or both ends of the plurality of heat transfer plates in the gas flow direction.

  The present invention also provides a plate reactor in which a plurality of heat transfer plates are provided side by side in a reaction vessel, and a catalyst layer is formed by filling a catalyst in a gap between the heat transfer plates. Supplying a heat medium to a plurality of heat transfer tubes constituting the plate, supplying the raw material gas to the reaction vessel, and reacting the raw material gas in the presence of the catalyst to generate a gaseous reaction product; In the method of including, the manufacturing method of the reaction product which uses the plate type reactor of this invention mentioned above for the said plate type reactor is provided.

Further, in the present invention, the step of generating the reaction product includes a step of oxidizing ethylene to generate ethylene oxide; a hydrocarbon having 3 and 4 carbon atoms, tertiary butanol, and an unsaturated fat having 3 and 4 carbon atoms. Oxidizing at least one selected from the group consisting of group aldehydes to produce one or both of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms and unsaturated fatty acids having 3 and 4 carbon atoms; Oxidation of aliphatic hydrocarbons to produce maleic acid; O-xylene to oxidize to produce phthalic acid; Olefin to hydrogenate to produce paraffin; Carbonyl compound to hydrogenate to produce alcohol Step; Acid decomposition of cumene hydroperoxide to produce acetone and phenol; Step to oxidize butene to produce butadiene Dehydrogenating ethylbenzene to produce styrene; or oxidizing one or both of propylene and acrolein, or one or both of isobutylene and methacrolein to convert one or both of (meth) acrolein and (meth) acrylic acid. Providing the method as described above.

  In the present invention, since the reaction vessel is configured by the gas distribution unit, the heat medium supply unit, and the plate clamping unit, gas stays in a gap between the inner wall of the reaction vessel and the heat transfer plate. A plate reactor can be provided in which damage to the plate reactor is substantially prevented.

  Further, in the present invention, it is preferable that the plate sandwiching portion is constituted by the pair of sandwiching plates and the holding rod so that the gas is retained in a gap between the inner wall of the reaction vessel and the heat transfer plate. This is even more effective from the viewpoint of substantially and easily preventing damage to the vessel.

  Further, according to the present invention, the plate sandwiching portion may be in contact with the heat transfer plate at the peripheral edge of the heat transfer tube at the upstream end in the gas ventilation direction of the heat transfer plate, between the inner wall of the reaction vessel and the heat transfer plate. This is even more effective from the viewpoint of substantially and easily preventing damage to the plate reactor due to gas remaining in the gap.

  Further, in the present invention, it is more effective to further include the partition from the viewpoint of easily and quickly performing use preparation work and maintenance inspection work in the plate reactor.

  In the present invention, the holding rod is disposed at a position overlapping with the partition in the gas ventilation direction, from the viewpoint of easily and quickly performing use preparation work and maintenance inspection work in the plate reactor. Is.

  Further, in the present invention, it is further effective that the gas distribution part further has a manhole from the viewpoint of performing the use preparation work and the maintenance inspection work in the plate reactor easily and quickly.

  In addition, the present invention is more effective in that the gas distribution unit has a safety device from the viewpoint of preventing sudden and abnormal pressure rise and preventing damage to the plate reactor.

  In the present invention, the heating medium supply unit may further include a heating medium mixing device that mixes the second heating medium with the first heating medium in the heating medium supply unit. Is more effective from the viewpoint of

  In the present invention, it is more effective from the viewpoint of protecting the filled catalyst that it further has a breathable catalyst protection cover that covers one or both ends of the plurality of heat transfer plates in the gas ventilation direction.

Further, the present invention produces a reaction product with high efficiency by using the plate reactor of the present invention to react a raw material gas in the presence of the catalyst to produce a gaseous reaction product. be able to.

Also, production of ethylene oxide from ethylene; 3 carbon atoms from at least one selected from the group consisting of hydrocarbons having 3 and 4 carbon atoms, tertiary butanol, and unsaturated aliphatic aldehydes having 3 and 4 carbon atoms Production of one or both of unsaturated aliphatic aldehydes 1 and 4 and unsaturated fatty acids having 3 and 4 carbon atoms; production of maleic acid from aliphatic hydrocarbons having 4 or more carbon atoms; production of phthalic acid from o-xylene Production of paraffins from olefins; production of alcohols from carbonyl compounds; production of acetone and phenol from cumene hydroperoxide; production of butadiene from butenes; production of styrene from ethylbenzene; or of propylene and acrolein; From one or both or from one or both of isobutylene and methacrolein The production of one or both of (meth) acrolein and (meth) acrylic acid of the present invention is more effective from the viewpoint of producing the reaction product with high efficiency.

  In particular, using the plate reactor to produce one or both of (meth) acrolein and (meth) acrylic acid from one or both of propylene and acrolein, or one or both of isobutylene and methacrolein, It is more effective from the viewpoint of producing (meth) acrolein and / or (meth) acrylic acid with high efficiency by a reactor, and further, gas stays in the gap between the inner wall of the reaction vessel and the heat transfer plate. Production of (meth) acrolein and / or (meth) acrylic acid by reducing the time required for maintenance and operation preparation and improving workability. It is even more effective from the viewpoint of increasing productivity in the long term.

  The plate reactor according to the present invention includes a reaction vessel for reacting a gaseous raw material and a plurality of heat transfer plates provided side by side in the reaction vessel.

  The heat transfer plate includes a plurality of heat transfer tubes connected at a peripheral edge or an edge of a cross-sectional shape. Thus, the heat transfer plate is a plate-like body including a plurality of heat transfer tubes arranged in parallel. In the heat transfer plate, the heat transfer tubes may be directly connected or indirectly connected through an appropriate member such as a plate or a hinge.

  Such a heat transfer plate is a pattern having an arc or an elliptical arc as a main component as disclosed in Patent Document 1, a pattern having a plane such as a rectangle and a part of a polygon as a main component, or these It is possible to form two corrugated plates in which a pattern in which the two are combined are continuously joined together with a convex edge formed at the end of the pattern of both corrugated plates. Alternatively, the heat transfer plate can be formed by connecting a plurality of the heat transfer tubes at a peripheral edge or an edge. Alternatively, the heat transfer plate can be formed by stacking a plurality of the heat transfer tubes so as to contact each other at the peripheral edge or the edge in the reaction vessel.

  The shape of the heat transfer plate is determined according to the shape and size of the reaction vessel, but is generally rectangular. The size of the heat transfer plate is determined according to the shape and size of the reaction vessel. For example, in the case of a rectangular heat transfer plate, the length (that is, the connection height of the heat transfer tubes) is 0.5 to 0.5. 10 m, preferably 0.5 to 5 m or less, and more preferably 0.5 to 3 m. When the length of the heat transfer plate is 1.5 m or more due to the size of the normally available thin steel plate, two heat transfer plates with a length of less than 1.5 m are joined or combined to form a single heat transfer plate Can also be configured. Moreover, the width | variety (namely, the length of a heat exchanger tube) is 0.05-20 m, Preferably it is 3-15 m normally, More preferably, it is 6-10 m. The number of heat transfer plates is determined by the amount of catalyst used in the reaction, but is usually 10 to 300.

  Adjacent heat transfer plates in the reaction vessel may be arranged so that the convex edges of the surface of the heat transfer plate face each other, or the convex edges of the surface of one heat transfer plate are the surfaces of the other heat transfer plate. You may arrange so that a concave edge may be opposed. The distance between adjacent heat transfer plates is the average of the distances between the long axes of the heat transfer tubes in each heat transfer plate so that a gap of 3 to 40 mm width is formed between the heat transfer plates in the transverse direction of the heat transfer tubes. The value can be set in a range of 23 to 50 mm (1.1 to 5 times the sum of half the widths of the heat transfer tubes in adjacent heat transfer plates).

  The heat transfer tubes in the heat transfer plate are arranged in a direction transverse to the aeration direction in the reaction vessel. The angle between the extending direction of the heat transfer tube and the aeration direction in the reaction vessel is not particularly limited as long as the heat transfer tube crosses the gas aeration direction in the reaction vessel. The heat transfer tube is formed so as to extend in a direction perpendicular to the aeration direction in the reaction vessel, that is, the direction of the heat medium flowing through the heat transfer tube is perpendicular to the aeration direction in the reaction vessel. It is more preferable from the viewpoint of controlling the reaction of the raw material by adjusting the temperature of the heat medium in the heat transfer tube.

  The heat transfer tube is formed of a material having heat transfer properties in which heat is exchanged between a heat medium in the heat transfer tube and a catalyst layer circumscribing the heat transfer tube. Examples of such materials include stainless steel and carbon steel, hastelloy, titanium, aluminum, engineering plastic, and copper. Stainless steel is preferably used. For stainless steel, 304, 304L, 316, and 316L are preferred. The cross-sectional shape of the heat transfer tube may be a circle, a substantially circular shape such as an elliptical shape or a rugby ball shape, a leaf shape formed by symmetrically connecting arcs, or a polygonal shape such as a rectangle. The peripheral edge in the cross-sectional shape of the heat transfer tube means a peripheral edge in a circular shape, and the end edge in the cross-sectional shape of the heat transfer tube means an edge of a major axis end in a substantially circular shape or a single edge in a polygon.

  The cross-sectional shape and size of each of the plurality of heat transfer tubes in one heat transfer plate may be constant or different. Regarding the size of the cross-sectional shape of the heat transfer tube, for example, the width of the heat transfer tube is 3 to 50 mm, and the height of the heat transfer tube is 10 to 100 mm.

  In the plate reactor, a catalyst is filled in a gap between adjacent heat transfer plates. As the catalyst, a normal granular catalyst filled in a gap between a tube or a heat transfer plate by a gas phase reaction can be used. One or more catalysts may be used. An example of such a catalyst is a catalyst having a particle diameter (longest diameter) of 1 to 20 mm. Examples of the shape of the catalyst include a spherical shape, a cylindrical shape, and a Raschig ring shape.

  The reaction vessel covers both ends of the plurality of heat transfer plates in the gas ventilation direction, and distributes gas through a gap between adjacent heat transfer plates; and both ends of the heat transfer tubes in the heat transfer plate The heat medium supply part that contacts the heat transfer tube and a heat transfer plate that supplies heat to the heat transfer tube and the heat transfer plates at both ends in the direction in which the heat transfer plates are arranged block gas flow along at least the extending direction of the heat transfer tube. And a plate clamping portion that clamps the plurality of heat transfer plates in the direction in which the heat transfer plates are arranged.

The gas distribution unit includes, for example, a reaction container cover that forms a cover that is separated from end portions of the plurality of heat transfer plates, and that seals both ends of the side wall of the reaction vessel formed by the heat medium supply unit and the plate holding unit. In addition, it can be constituted by a gas vent through which a source gas is supplied or a reaction product gas is discharged. As the reaction vessel cover, a cover having various shapes such as a dome shape, a cone shape, a quadrangular shape, a semi-cylindrical shape, a triangular prism shape, and a housing can be used. Moreover, the said vent hole can use the normal vent hole which has the nozzle opened to a reaction container cover, and the flange formed in the edge part, for example. The reaction vessel cover is usually provided in a pair with respect to the side wall of the reaction vessel, and these may be the same or different. In addition, one vent is usually provided in the reaction vessel cover, but a plurality of vents may be provided. Further, a pair of the vents are usually provided in the plate reactor, but these may be the same or different.

  It is preferable that the gas distribution part further has a manhole because an operator puts the inside of the reaction vessel during a catalyst filling operation and a maintenance inspection operation such as an inspection during a stop period of the plate reactor. As the manhole, a normal manhole provided for such work in the reaction vessel can be used. Normally, one manhole is provided for an integral gas distributor, but a plurality of manholes may be provided.

  The gas distributor further includes a safety device for preventing damage to the plate reactor due to an increase in the pressure in the reaction vessel. For example, when the pressure of the reaction gas has increased abnormally or an abnormal reaction has occurred. It is sometimes preferable from the viewpoint of preventing the damage of the plate reactor by safely and urgently releasing the gas in the plate reactor to the outside of the plate reactor. As the safety device, a normal device provided for such use in the reaction vessel can be used. Normally, one safety device is provided for the integrated gas distribution unit, but a plurality of safety devices may be provided. Examples of the safety device include a safety valve and a rupture disc.

  As the heat medium supply unit, a normal apparatus for supplying a heat medium to the heat transfer tube in a plate reactor can be used. The heat medium supply unit may be a device that supplies the heat medium in one direction to all of the plurality of heat transfer tubes, or supplies the heat medium in one direction to a part of the plurality of heat transfer tubes, and the plurality of heat transfer tubes The other part may be a device for supplying a heat medium in the reverse direction. The heat medium supply unit is preferably a device that circulates the heat medium inside and outside the reaction vessel via the heat transfer tube.

  The heating medium supply unit preferably has a device for adjusting the temperature of the heating medium from the viewpoint of controlling the reaction in the reaction vessel. Examples of the heating medium supply unit that adjusts the temperature of the heating medium include devices that can be used in various reactors that use such a heating medium and that can mix heating media having different temperatures. For example, in the heating medium supply unit There is a heat medium mixing device that mixes the second heat medium with the first heat medium.

  The heat medium mixing device includes, for example, a distribution pipe that protrudes into the heat medium supply unit and can disperse and supply the heat medium in the heat medium supply unit, a liquid passage plate provided in the heat medium supply unit, and a so-called static mixer Can be used. Examples of the distribution pipe include a distribution pipe having a plurality of liquid passage openings such as slits and holes in the pipe wall along the longitudinal direction of the distribution pipe, and a distribution pipe further including a branch pipe having the liquid passage opening. .

  The distribution pipe is preferably provided so as to extend in a direction orthogonal to the flow direction of the heat medium in the heat medium supply unit, and the distribution pipe having a branch pipe has a main pipe and a branch pipe, Both of them are provided so as to extend in a direction orthogonal to the flow direction of the heat medium in the heat medium supply section, and provided so that the extending directions of the main pipe and the branch pipe are orthogonal to each other. It is preferable from the viewpoint of improving efficiency in dispersion and suppressing pressure loss.

  The plate clamping portion is a member that contacts the outermost heat transfer plate so that gas does not flow between the outermost heat transfer plate. It is preferable that a plate clamping part is a member which does not deform | transform toward the heat-transfer plate which touches, and the reverse direction.

Examples of the plate sandwiching portion that does not allow gas to flow through the gap between the sandwiching heat transfer plates include, for example, a gas ventilation direction of the heat transfer plate on the heat transfer plates at both ends in the direction in which the plurality of heat transfer plates are arranged. The plate clamping part which contact | abuts to the periphery of the heat exchanger tube of the upstream end in is mentioned. Such a plate clamping part is preferable from the viewpoint of preventing the formation of a gas retention part in the gap between the heat transfer plate and the plate clamping part.

  In addition, as a plate sandwiching portion that does not cause deformation in the sandwiching direction, a plate sandwiching portion that sandwiches a plurality of heat transfer plates by a pair of sandwiching plates having sufficient heat resistance and mechanical strength against reaction in a plate reactor. Can be mentioned. Examples of the sandwiching plate include a steel plate such as stainless steel and a plate made of an inorganic material such as ceramics. The plate thickness of the sandwich plate varies depending on the pressure of the reaction gas and the area of the heat transfer plate, but is preferably 10 to 300 mm. Such a plate clamping portion is preferable from the viewpoint of suppressing deformation due to a pressure difference between the inside and outside and deformation due to thermal stress, and from the viewpoint of ease of manufacturing. The clamping plate may have openings such as a lattice and a plurality of holes as long as sufficient mechanical strength and sealing property of the reaction container are obtained. Such a clamping plate is preferable from the viewpoint of reducing the weight of the clamping plate.

  Moreover, the said plate clamping part may be fixed to the position which clamps several heat-transfer plates, and may be relatively movable with respect to several heat-transfer plates toward the clamping direction.

  Examples of the plate sandwiching portion that is relatively movable with respect to the plurality of heat transfer plates include, for example, an extension of the heat transfer tube to at least one heat transfer tube of the heat transfer plates at both ends in the direction in which the plurality of heat transfer plates are arranged. There is a plate clamping portion composed of a pair of clamping plates that are in contact with the entire heat transfer tube in the outgoing direction and a holding rod that penetrates and holds these clamping plates. The holding rod is a member that can connect the clamping plates in the opposing direction at a predetermined interval. As such a holding rod, for example, a rod made of a steel material such as stainless steel having a screw to which a nut can be screwed at least at a tip end portion can be cited. The material of the holding rod is preferably the same material as the heat transfer plate and the partition. The diameter of the holding rod varies depending on the pressure of the reaction gas and the number of holding rods, but is preferably 20 to 100 mm. The number of holding bars is preferably 10 to 50, and the installation interval is preferably 20 to 100 cm. Such a plate clamping part has a viewpoint of finely adjusting the gap with the heat transfer plate to be sandwiched, a viewpoint of easily installing a scaffold during filling of the catalyst and the inside of the plate reactor, and a plate type of other conditions It is preferable from the viewpoint that diversion to a reactor is possible.

  The reaction vessel is configured such that the gas distribution unit, the heat medium supply unit, and the plate clamping unit are hermetically joined so as to accommodate the plurality of heat transfer plates. These airtight joints can be performed by using an ordinary technique for airtightly joining adjacent members. For example, each adjacent member may be welded, or each adjacent member may be a gasket or the like. It may be energized toward the seal through the seal.

  The plate reactor of the present invention may further have other components other than the components described above. Examples of such other components include a partition that partitions a gap between adjacent heat transfer plates into a plurality of compartments, and a catalyst protection cover provided at one or both ends of the plurality of heat transfer plates.

The said partition is provided in the clearance gap between adjacent heat-transfer plates along the ventilation direction in reaction container, and forms several divisions in the said clearance gap. The partition may be a member that can hold a catalyst in each compartment when the catalyst is filled in each compartment. The partition is preferably formed of the same material as the heat transfer plate, preferably has heat transfer properties, preferably not reactive to the reaction in the reaction vessel, and the reaction in the reaction vessel is an exothermic reaction. In some cases, it is preferable to have heat resistance. Moreover, it is preferable that the partition has rigidity from the viewpoint of holding the catalyst filled in each compartment and functioning as a spacer for maintaining the distance between the heat transfer plates. The partition having rigidity is more preferable as a spacer that protects the catalyst against the clamping force of the holding rod, particularly when the heat transfer plate is connected by the holding plate and the holding rod. Examples of such partitions include stainless steel or carbon steel plates, square bars, round bars, nets, glass wool, and ceramic plates.

  The shape of the partition may be a shape in which the catalyst is held in a partition formed by each partition, and may be a shape in contact with the heat transfer tube or a shape in close contact with the partition. Further, the partition preferably has a shape in contact with the surface of the outer wall of each heat transfer tube, from the viewpoint of holding the catalyst filled in each section, and has a shape that closely contacts the surface of the outer wall of the heat transfer tube. More preferred. Moreover, it is preferable that the said partition is a shape which becomes a square which has the width | variety of the shortest distance between the heat exchanger plates which a front view adjoins from a viewpoint which installs a partition easily.

  The partition is preferably provided at an interval of 1 to 500 L from the viewpoint that the volume of the partition formed by the partition can be accurately and easily filled with the catalyst in one partition. The volumes of the compartments formed by the partitions may be the same or different, but are preferably the same from the viewpoint of accurate and easy filling of the catalyst into all the compartments. 1-100L is preferable, as for the volume of the said one division, it is more preferable that it is 1.5-30L, and it is especially preferable that it is 2-15L. The installation interval of the partitions is preferably 5 cm to 2 m, more preferably 10 cm to 1 m, and further preferably 20 to 50 cm.

  The said partition can be suitably provided in the clearance gap between heat-transfer plates according to the property of a partition. For example, a flexible partition or a partition having the shortest distance between the heat transfer plates is inserted into a gap between adjacent heat transfer plates in a plurality of heat transfer plates installed in the reaction vessel in advance. Therefore, it can be provided in the gap between the heat transfer plates. When using a flexible partition or a partition having a portion that does not contact the outer edge of the heat transfer tube of the heat transfer plate, additionally use a spacer that holds the space between the heat transfer plates or a partition that serves as a spacer. Is preferred. In addition, when the heat transfer plate is installed in the reaction vessel, the partition having a shape closely contacting the surface of the heat transfer plate can be provided in the gap between the heat transfer plates by alternately installing the heat transfer plate and the partition. it can.

  In the case where the partition is formed in a shape that does not adhere to the surface of the heat transfer plate, the shape of the catalyst is such that the shortest diameter of the catalyst is larger than the gap between the heat transfer plate and the partition, This is preferable from the viewpoint of preventing leakage of the catalyst from the compartment.

  The catalyst is filled in the gap between the adjacent heat transfer plates by filling the compartments with the catalyst. Each compartment can be filled with a catalyst by filling the same volume of catalyst in a compartment continuously or intermittently. The appropriate filling state of the catalyst is, for example, the comparison of the position of the top surface of the packed catalyst (catalyst layer) between the compartments, the measured value of the top surface in each compartment, and the calculated value of the top surface of each compartment. This can be determined by comparison.

  In the case where the plate clamping unit has the holding rod, the plurality of heat transfer clamped by the plate clamping unit may be that the holding rod is arranged at a position overlapping the partition in the gas ventilation direction. This is preferable from the viewpoint of quickly filling the gap between the heat transfer plates of the plate with the catalyst.

The catalyst protective cover is a member that has air permeability, can hold the catalyst in the gap as needed, and covers one end or both ends of the plurality of heat transfer plates in the gas aeration direction. The catalyst protective cover is preferable from the viewpoint of preventing leakage of the catalyst from the heat transfer plate and mixing of foreign matters into the catalyst between the heat transfer plates. The catalyst protective cover may be a flexible member or a rigid member that does not deform. The catalyst protective cover may be a member that covers the entire ends of the plurality of heat transfer plates, or may be a plurality of members that partially cover the ends of the plurality of heat transfer plates (for example, for each section). May be. Examples of such a catalyst protective cover include a heat-resistant net, a perforated plate used for a working scaffold, and a breathable plug that is detachably provided at one or both ends of the section in the gas ventilation direction. Is mentioned.

  The plate type reactor of the present invention can be used for a reaction in which a gas phase raw material is reacted in the presence of a solid phase catalyst. In particular, the temperature in the reactor at the time of use and the work for preparation and inspection can be performed. When used under conditions where the difference from room temperature is large, or when the source gas or product gas is exposed to the conditions at the time of use for a long time, the deterioration of these gases may cause damage to the reactor. This is more effective when the heat of reaction accompanying the reaction of the gas component is remarkably large and the catalyst is likely to be deteriorated by the heat, and the temperature control of the catalyst layer is important.

  From this point of view, the plate reactor according to the present invention is a fixed bed catalytic reactor in the method for producing a reaction product, and improves the reaction performance by carrying out the reaction while controlling the heat of reaction with a heat medium. It is suitably used for the type of reaction that can achieve the effect of That is, gas phase catalytic oxidation reaction, at least one of methacrolein and methacrylic acid, at least one of acrolein and acrylic acid, a method of producing maleic acid, phthalic acid, ethylene oxide, a method of producing butadiene by oxidative dehydrogenation reaction, And it can use suitably as a reactor in the manufacturing method of styrene which can improve reaction conversion rate by supplementing the reaction heat of endothermic reaction.

In particular, it can be particularly suitably used for the production of acrylic acid or methacrylic acid ((meth) acrylic acid) by a gas phase catalytic oxidation reaction. That is, one or both of propylene and acrolein, or one or both of isobutylene and methacrolein are oxidized in the presence of a catalyst using a molecular oxygen-containing gas to (meth) acrolein (acrolein or methacrolein) and (meta ) In the method for producing one or both of acrylic acids, the plate reactor of the present invention can be suitably used.

  Further, even in a liquid phase reaction, there may be cases where a fixed bed catalyst reactor is used and the temperature rise due to reaction heat promotes the deterioration of the catalyst or promotes the generation of by-products.

In essence, the production method of the present invention can be applied to a plate type reactor having a catalyst layer formed between two adjacent heat transfer plates, and the plate type reactor is heated. It has exchange ability and can be used for exothermic or endothermic reactions that require a heat exchange function in the reactor. Examples of reactions in which a reaction product is produced using a plate reactor include an exothermic reaction and an endothermic reaction. The reaction applicable to the production method of the present invention is not particularly limited as long as it is an exothermic or endothermic reaction, and the following can be suitably exemplified.

Among the reactions applicable to the production method of the present invention, a fixed bed catalytic reactor is adopted, and the reaction accompanied by heat generation includes (1) a reaction for producing ethylene oxide from ethylene and oxygen, (2) a carbon number of 3 and At least one reaction raw material gas selected from the group consisting of 4 hydrocarbons and tertiary butanol, or at least one reaction raw material gas selected from the group consisting of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms, A reaction that produces at least one reaction product selected from the group consisting of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms and unsaturated fatty acids having 3 and 4 carbon atoms from oxygen, (3) having 4 or more carbon atoms (4) Reaction to produce maleic acid from oxygen, (4) Reaction to produce phthalic acid from o-xylene and oxygen, (5) Paraffin by hydrogenation of olefin (6) Reaction to produce alcohol by hydrogenation of carbonyl compound, (7) Reaction to produce acetone and phenol by acid decomposition of cumene hydroperoxide, (8) Butadiene by oxidative dehydrogenation of butene The manufacture of is mentioned.

On the other hand, the reaction accompanied by endotherm includes a reaction of generating styrene by dehydrogenation of ethylbenzene.

The reaction product produced using the production method of the present invention is preferably at least one of methacrolein and methacrylic acid, at least one of acrolein and acrylic acid, maleic acid, phthalic acid, styrene, ethylene oxide, and butadiene. Illustrated. Further, known reaction conditions can be applied as reaction conditions for obtaining these reaction products.

For example, in the production of (meth) acrylic acid, propane, propylene or isobutylene is present in the presence of a catalyst as described in JP-A-2003-252807, except that the plate reactor of the present invention is used as a reactor. It can be carried out by a known method of oxidizing using molecular oxygen or a gas containing it under. In addition, the catalyst includes a Mo—V—Te composite oxide catalyst, a Mo—V—Sb composite oxide catalyst, a Mo—Bi composite oxide catalyst, and a Mo— A well-known catalyst can be used by a well-known usage in the use in the gas phase catalytic oxidation reaction which produces | generates (meth) acrylic acid, such as a V type complex oxide catalyst.

  Hereinafter, the plate reactor of the present invention will be described more specifically with reference to the drawings.

  The plate reactor of the present invention has a heat transfer tube 1 as shown in FIGS. 1 to 4, for example, and a plurality of heat transfer plates 2 provided side by side in the reaction vessel, and the direction in which the heat transfer plates 2 are arranged. A pair of sandwiching plates 3 that are in contact with the heat transfer plates 2 at both ends in the direction of the heat transfer tube 1 and sandwich the plurality of heat transfer plates 2 in the direction in which the heat transfer plates 2 are arranged, and sandwiching these plates A plurality of holding rods 4 for connecting the plates, a heat medium supply part 5 that contacts both ends of the heat transfer tube 1 in the heat transfer plate 2 and supplies a heat medium to the heat transfer tube 1, and a plurality of heat transfer members in the gas ventilation direction. The gas distribution part 6 which covers both ends of the heat plate 2 and distributes the gas to the gap between the adjacent heat transfer plates 2 and the gap between the adjacent heat transfer plates 2 are filled along the gas ventilation direction. Partition that divides into multiple compartments containing catalyst When, and a vent plug (not shown) for closing the lower end of each partition. A pair of clamping plates 3 and holding rods 4 constitute the plate clamping portion. Each section of the gap between adjacent heat transfer plates 2 is filled with a catalyst.

  The heat transfer tube 1 is, for example, a tube whose cross-sectional shape having a major axis (L) of 30 to 50 mm and a minor axis (H) of 10 to 20 mm is a shape whose main component is a part of an arc, an elliptical arc, a rectangle, or a polygon. It is. FIG. 5 shows a heat transfer tube having a leaf shape in cross section with an arc as a component of the cross section. In FIG. 5, the major axis of the heat transfer tube is represented by L, and the minor axis is represented by H.

  The heat transfer plate 2 has a shape in which a plurality of heat transfer tubes 2 are connected by an edge having a cross-sectional shape. The heat transfer plate 2 is formed by joining two corrugated plates each having an elliptical arc formed continuously with a convex edge formed at the ends of the arcs of both corrugated plates. The adjacent heat transfer plates 2 may be arranged in parallel so that the convex edges of the surfaces face each other, but in the plate reactor of FIG. 1, the convex edges of the surface of one heat transfer plate 2 and the other The heat transfer plates 2 are arranged in parallel so as to face the concave edges on the surface.

The heat transfer plates 2 may all be constituted by the same heat transfer tube 1 or may be constituted by the heat transfer tubes 1 having different cross-sectional sizes. For example, in the heat transfer plate 2, the upper portion, the middle portion, and the lower portion of the heat transfer plate 2 may be configured by three types of heat transfer tubes having different cross-sectional sizes. More specifically, the heat transfer plate 2 is formed so that the major axes of the three types of heat transfer tubes are arranged in a straight line. For example, the upper portion of the heat transfer plate 2 is the height of the heat transfer plate 2. 20% of the heat transfer tube a has the largest cross-sectional size, and the middle part of the heat transfer plate 2 is the heat transfer tube having the second largest cross-sectional size of 30% of the height of the heat transfer plate 2 The lower part of the heat transfer plate 2 is composed of a heat transfer tube c having the smallest cross-sectional size for 40% of the height of the heat transfer plate 2, and 10% of the height of the heat transfer plate 2 The heat transfer plate 2 may be formed by a joining plate portion at the upper end portion and the lower end portion. As the cross-sectional shape of the heat transfer tube a, for example, the long diameter (L) is 50 mm, the short diameter (H) is a leaf shape of 20 mm, and the cross-sectional shape of the heat transfer tube b is, for example, the long diameter (L) is 40 mm, The short diameter (H) is a leaf shape of 16 mm, and the cross-sectional shape of the heat transfer tube c is, for example, a long diameter (L) of 30 mm and a short diameter (H) of 10 mm.

  The heat transfer plates 2 may be arranged in parallel at the same interval, or may be arranged in parallel at different intervals. For example, the heat transfer plates 2 are arranged in parallel at equal intervals such that the shortest distance between the outer walls of the heat transfer tubes a is 14 mm (the distance between the major axes of the heat transfer tubes of each heat transfer plate 2 is 30 mm).

  As shown in FIG. 6, the sandwiching plate 3 is a pair of plates, for example, a pair of stainless steel plates. The clamping plate 3 is formed larger than the heat transfer plate 2 so that it can be joined by the holding rod 4 at the edge.

  As shown in FIGS. 1 and 6, the holding rod 4 is a plurality of rods that penetrate and connect the pair of clamping plates 3, and is, for example, a stainless steel rod having screws at both ends. As shown in FIGS. 1 and 2, the holding plate 3 is fixed by nuts at both ends of the holding rod 4 at a position in contact with the outer periphery of the heat transfer tube 1 (the heat transfer tube a) above the heat transfer plate 2. The The clamping plate 3 can be fixed by changing the position in the direction of clamping the heat transfer plate 2 within the range of the installation length of the screws of the holding rod 4. Further, as shown in FIG. 6, the holding rod 4 is arranged at a position overlapping with the partition 7 arranged in the gap between the heat transfer plates 2 in the vertical direction.

  As shown in FIG. 3, the heat medium supply unit 5 is a pair of containers that are in contact with both ends of the heat transfer tube 1 of the heat transfer plate 2, and is, for example, a stainless steel jacket having an opening corresponding to the heat transfer tube 1 that is in contact. . The heat medium supply unit 5 has a nozzle 8 in one or both of the pair of jackets. The heat medium is supplied to the jacket via the nozzle 8 and discharged from the jacket. For example, as indicated by an arrow Y in FIG. 3, the heat medium supply unit 5 is provided so that the heat medium flows from one jacket to the other jacket in one direction in all the heat transfer tubes 1. The heat medium supply unit 5 can be airtightly joined to the sandwiching plate 3 at the side edge portion of the sandwiching plate 3 using a normal fixing member such as a screw and a nut and a seal such as a gasket. .

  As shown in FIGS. 1 and 2, the gas distribution unit 6 is fixed to, for example, the upper end edge of the sandwiching plate 3 and the upper end edge of the jacket, and the lower end edge of the sandwiching plate 3 and the lower end edge of the jacket. These are a pair of members that are airtightly bonded using a member and a seal and cover both ends of the plurality of heat transfer plates 2. The gas distribution unit 6 is, for example, a kamaboko type stainless steel lid. The gas distribution unit 6 includes a nozzle 9 and a manhole 10 in each of the lids. The gas is supplied to the gap between the heat transfer plates 2 through the nozzle 9 of one lid, and the gas is discharged from the gap through the nozzle 9 of the other lid. The manhole 10 is an open / close door for an operator to enter and exit the gas distribution unit 6 in a state where the gas distribution unit 6 is installed. The arrangement of the nozzle 9 and the manhole 10 is not particularly limited, but when the gas distribution unit 6 is a kamaboko type lid, for example, as shown in FIG. 2, the nozzle 9 is provided at one end of the lid, and the manhole 10 is a lid. Provided at the other end. Further, the gas distributor 6 includes a safety device (not shown) such as a safety valve or a rupture plate as a safety measure in case of an abnormal pressure sudden increase or abnormal reaction, and the main body of the gas distributor 6 at the inlet and / or outlet. Or the nozzle 9.

The partition 7 is provided between the adjacent heat transfer plates 2 along the gas aeration direction X in the plate reactor. The partitions 7 may be provided at the same interval in the whole plate reactor or may be provided at different intervals. The partitions 7 are provided in parallel at the same interval of 400 mm, for example, and form a plurality of compartments having a volume of 12 L in the gaps between the heat transfer plates 2.

  A member that can hold the filled catalyst in each compartment when the catalyst is filled in each compartment is used for the partition 7. As the partition 7, for example, as illustrated in FIGS. 7 to 9, a plate or a net having a shape having a side edge that is in close contact with the unevenness on the surface of the heat transfer plate 2 can be used.

  Further, the partition 7 is in contact with the heat transfer tube (the heat transfer tube a) above the adjacent heat transfer plate 2 if the catalyst filled in each partition does not leak from the gap between the partitions 7 to the adjacent partition. The member which does not contact | abut to the convex edge and concave edge of the other heat exchanger tube in the heat-transfer plate 2 can be used. For example, as the partition 7, as shown in FIGS. 10 and 11, a round bar or a square bar having the shortest diameter or width between adjacent heat transfer plates 2 can be used.

  Further, as shown in FIG. 8, the partition 7 may be a net having an eye smaller than the size of the catalyst particles to be filled, or if the catalyst filled in each compartment does not leak into the adjacent compartment, As shown in FIG. 9, it may be a net having larger eyes (for example, 0.8 times or less the shortest diameter of the catalyst).

  When two adjacent heat transfer plates 2 are arranged in parallel so that the convex edge of one heat transfer plate 2 faces the concave edge of the other heat transfer plate 2, the partition 7 has a shape as shown in FIG. In addition, a zigzag plate or net that protrudes toward the concave edge of the heat transfer plate 2 at the side edge of the partition 7 and is separated from the convex edge of the heat transfer plate 2 can be used. Such a partition 7 has a distance between two heat transfer plates 2 arranged in parallel so that one convex edge faces the other concave edge (an average of distances between major axes of the heat transfer tubes 1 in each heat transfer plate 2). When the value is 0.9 to 1.5 times the sum of the half-values of the maximum short diameters of the heat transfer tubes in each heat transfer plate 2, it can be suitably used.

  7 to 9 and 12, the partition 7 having a side edge in contact with the unevenness of the surface of the heat transfer plate 2 is a partition that contacts the heat transfer plate 2 when the heat transfer plate 2 is aligned. 7 are provided alternately between the two heat transfer plates 2. The partition 7 having the shortest distance diameter or width between adjacent heat transfer plates 2 as shown in FIGS. 10 and 11 can be obtained by alternately installing the heat transfer plates 2 and the partitions 7 that abut on the partitions 7. You may provide between the heat-transfer plates 2, and you may provide by inserting between the heat-transfer plates 2 adjacent to the heat-transfer plate 2 already installed. The flexible partition 7 such as a net or a thin steel plate can also be provided by inserting it between the adjacent heat transfer plates 2 of the heat transfer plates 2 already provided.

  In the plate reactor of FIG. 1, for example, a plurality of heat transfer plates 2 are alternately arranged with partitions 7 as necessary, and are arranged with a gap of a predetermined interval. , The plurality of heat transfer plates 2 are sandwiched by the sandwiching plate 3 so that the sandwiching plate 3 is in contact with all the peripheral edges in the longitudinal direction of the heat transfer tube 1 above the heat transfer plate 2, and the plurality of heat transfer plates 2 are sandwiched. The holding plate 3 is fixed by the holding rod 4 at the position where the heat transfer tube 1 is located, the heat medium supply unit 5 is disposed so as to be in contact with the heat transfer tube 1 in the extending direction of the heat transfer tube 1, and the holding plate 3 is airtightly fixed to the holding plate 3. The heat medium supply unit 5 is fixed at a position in contact with the heat pipe 1, and the openings formed by the upper and lower edges of the sandwich plate 3 and the heat medium supply unit 5 are sealed with the gas distribution unit 6, In front of the lower end of each section formed in the gap It can be constructed by plugging in vent plug. The vent plug may be installed before sealing by the gas distributor 6.

The catalyst is filled between the heat transfer plates 2 by loading the equipment into the upper part of the plate reactor via the manhole 10, and assembling a working scaffold on the holding rod 4 as necessary, It is done by filling. Since all the sections formed by the heat transfer plate 2 and the partition 7 have the same volume, the capacity equivalent to the capacity of one section (for example, a volume of 95 to 100% with respect to the capacity of one section). Of each catalyst is packed into each compartment.

  The good packing state of the catalyst means comparison between the theoretical value of the catalyst filling height and the actual measurement value (for example, the error of the actual measurement value with respect to the theoretical value is within 10%), and comparison of the catalyst filling height between the sections. (For example, the difference in filling height between the sections is within 2% of the filling height).

  The packed catalyst can be extracted, for example, by an operator entering the inside of the plate reactor through the manhole 10 in the lower lid and removing the vent plug from the lower end of the compartment.

  When the acrolein is produced from propane or propylene by a gas phase catalytic oxidation reaction, and acrylic acid is further produced from the obtained acrolein by a gas phase catalytic oxidation reaction, the plate type reactor is used for the former gas phase catalytic oxidation reaction. In some cases, for example, as described in JP-A No. 2003-151807, the atomic ratio is Mo: Bi: Co: Fe: Na: B: K: Si: O = 12: 1: 0.6: 7: Mo: Bi composite oxide catalyst of 0.1: 0.2: 0.1: 18: X (where X is a value determined by the oxidation state of each metal element) is packed between the heat transfer plates 2. The A raw material gas composed of propylene, air, and water vapor is supplied from a nozzle 9 above the heat transfer plate 2, and a heat medium of 300 to 350 ° C. is supplied from the heat medium supply unit 5 to each heat transfer tube 1. The internal pressure of the plate reactor during the reaction is, for example, 150 to 200 kPa (kilopascal).

  Propylene in the raw material gas is oxidized into acrolein and acrylic acid when passing through the catalyst layer between the heat transfer plates 2 in the X direction. The heat generated by the oxidation is absorbed by the heat medium flowing in the heat transfer tube 1, and the generated acrolein and acrylic acid are discharged from the nozzle 9 below the heat transfer plate 2.

  In the plate reactor, the surface of the sandwich plate 3 and the surface of the heat transfer tube 1 (the heat transfer tube a) above the heat transfer plate 2 are in contact with each other. The gas flow in the gap is blocked, but a gap is formed from the upper end of the heat transfer plate 2 in contact with the sandwiching plate 3 to the heat transfer tube 1 at the most upstream position in the heat transfer plate 2, and the raw material is formed in the upper gap. Gas can stay. In the plate reactor, a gap is generated from the lower end of the heat transfer plate 2 in contact with the sandwiching plate 3 to the middle heat transfer tube 1 in the heat transfer plate 2, and the generated gas can stay in the lower gap.

  However, although these gaps have the same length as the width of the heat transfer plate 2, the width of the upper gap is about half the width of the heat transfer tube a, and the width of the lower gap is the width of the heat transfer tube a. And half the width of the heat transfer tubes b and c. That is, in the plate type reactor, only a very small (thin) gap is formed between the sandwiching plate 3 and the heat transfer plate 2 in contact with the holding plate 3 with respect to the internal volume of the reaction vessel. Therefore, even if the raw material gas or the product gas is altered, the influence thereof is extremely small, so that damage to the plate reactor due to the retention of the gas in the reaction vessel can be prevented. In order to fill the gap, the gap can be filled with an inorganic substance such as clay or cement, or an unevenness corresponding to the unevenness of the heat transfer plate is provided on one surface of the holding plate facing the heat transfer plate. It is possible.

The supplied raw material gas is usually at a pressure higher than atmospheric pressure, and the internal pressure of the plate reactor may become very high due to a cause such as deterioration of the raw material gas or product gas. In this case, the gas in the plate reactor is quickly released from the safety device to the outside, and damage to the plate reactor due to a sudden rise in pressure is prevented.

In addition, it is necessary for the clamping plate to hold the heat transfer plate 2 even when a pressure is applied during the reaction. When the heat transfer plate 2 becomes large, a strong force is applied to the sandwiching plate as a whole. In this case, it is conceivable that the thickness of the sandwiching plate increases and the weight of the sandwiching plate increases. In this case, the heat transfer plate 2 can be supported even during the reaction with the pressure by using a sufficiently reinforced plate such as a grid-like plate except for the portion that supports the holding rod 4. Is possible.

  Therefore, in the plate type reactor, instead of the sandwiching plate 3, as shown in FIG. 13, a frame having a rectangular opening at the center of a rectangular plate and the entire opening of the frame are provided. It is possible to use a sandwiching plate 13 having an opening at the center or a thin plate thickness, which is composed of a lattice extending obliquely with respect to the side and intersecting. The sandwiching plate 13 sandwiches the heat transfer plate 2 by being fixed by a nut so that the frame and the peripheral edges of the heat transfer tubes a and c are in contact with each other in the longitudinal direction of the heat transfer tubes. According to such a sandwiching plate 13, the gas flow between the heat transfer plate 2 and the sandwiching plate 13 can be blocked, sufficient mechanical strength can be ensured, and the steel material required for the sandwiching plate can be secured. The amount can be reduced, and the gas retention portion can be further reduced as compared with the use of the clamping plate 3.

  Further, in the plate type reactor, instead of the heat medium supply unit 5, a heat medium as shown in FIG. 14 is supplied and discharged, and the heat discharged from the heat transfer tube 1 is discharged. A heat medium supply unit including a second jacket 22 that forms a flow path for supplying a medium to another heat transfer tube 1 can be used. The first jacket 21 has a flow path separation plate 23 that divides the inside so as to form two chambers in the height direction when installed, and nozzles 24 and 25 provided in the respective formed chambers. . The second jacket 22 does not have a nozzle and a flow path separation plate, and forms a single chamber as a whole.

  According to such a heat medium supply unit, the heat medium supplied to the first chamber of the first jacket 21 via the nozzle 24 is, for example, the heat transfer pipe 1 (the heat transfer pipe a) on the upper part of the heat transfer plate 2. Is supplied to the second jacket 22, and is reversed in the second jacket 22 to pass through the middle and lower heat transfer tubes 1 (the heat transfer tubes b and c) of the heat transfer plate and the first jacket 21. It is supplied to the two chambers and discharged to the outside through the nozzle 25. In the case of using the plate reactor for the gas phase catalytic oxidation reaction in the production of (meth) acrylic acid, since this reaction is an exothermic reaction, the heat medium passing through the heat transfer tube a absorbs the initial large reaction heat. Then, it becomes a heat medium having a temperature higher than the initial temperature and flows through the heat transfer tubes b and c. As described above, the heating medium supply unit can form two reaction zones having different temperatures in the catalyst layer by supplying one kind of heating medium. The heat medium discharged to the outside is circulated to the nozzle 24 of the jacket 21 of the plate reactor again after the temperature is adjusted by a temperature control device (not shown in the figure) comprising a heat exchanger. Is done.

  The flow path separation plate 23 is used as a first flow path separation plate, and a second flow path separation plate is disposed between the first flow path separation plate and the nozzle 25 in the first jacket 21, In the jacket 22, the third flow forming two chambers in the second jacket 22 between the first and second flow path separation plates and the second flow path separation plate in the height direction. By providing the path separation plate, it is possible to form a heat medium flow path in which the heat medium reciprocates between the first and second jackets 21 and 22. Similarly, a plurality of reaction zones having different temperatures in the catalyst layer can be formed by supplying a single type of heat medium by further disposing the flow path separation plates in the first and second jackets.

Further, in the plate reactor, a heat medium supply unit further having a heat medium mixing device as shown in FIG. 14 can be used instead of the heat medium supply unit 5. The heating medium mixing device includes a further nozzle 31 that communicates between the inside and outside of the jacket, and a distribution pipe 32 that is connected to the nozzle 31 inside the jacket and extends in a direction orthogonal to the flow direction of the heating medium in the jacket. The distribution pipe 32 is, for example, a pipe having a closed end and provided with a plurality of holes over the entire length of the distribution pipe.

  According to such a heat medium supply unit, by supplying a heat medium having a temperature different from that of the heat medium in the jacket from the distribution pipe 32, the heat medium from the distribution pipe 32 is quickly mixed with the heat medium in the jacket. In addition, the temperature of the heat medium in the jacket can be adjusted. In the plate reactor, the above-described flow path separation plate such as a heat medium supply unit having the distribution pipe in one or both of the second chamber and the second jacket 22 of the first jacket 21 and the distribution chamber are provided. It is also possible to use a heat medium supply unit that has both piping.

  The partition 7 has a hook that engages with an engaging portion such as a hole or a ring provided at the end of the heat transfer plate 2, and the partition 7 is stretched by locking the hook to the engaging portion. By providing, it is also possible to provide in the gap between the adjacent heat transfer plates 2. According to such a structure, the material which does not have shape retention property, such as glass wool, can be used for the partition 7.

  Further, a perforated plate may be disposed on the holding rod 4 above the plurality of heat transfer plates 2 for the purpose of protecting the working scaffold, protecting the filled catalyst, and distributing the supplied gas. The perforated plate has 20 to 50% of holes having a mechanical strength sufficient as a working scaffold and, for example, 0.20 to 0.99 times the longest diameter of the catalyst to be filled. One or more plates provided with an aperture ratio can be used.

  The plate reactor holds a plurality of heat transfer plates 2 by being sandwiched by a pair of sandwiching plates 3. Since the clamping plate 3 is in contact with the heat transfer plate 2 on the outer surface of the heat transfer tube above the heat transfer plate 2, a gap in which the gas stays is substantially formed between the heat transfer plate 2 and the reaction vessel. Not. Therefore, the plate reactor can prevent the heat transfer plate 2 from being damaged due to combustion or alteration of the staying gas.

  In addition, the plate reactor has a partition 7 for dividing the filled catalyst into a plurality of compartments along the gas flow direction, so that the catalyst between the heat transfer plates 2 can be easily and uniformly filled. can do.

  Moreover, since the said plate type reactor has a vent plug which plugs up the lower end of each division, the catalyst with which the said clearance gap was filled can be extracted for every division. Therefore, since only a part of the catalyst layer that needs to be replaced or refilled can be extracted for each section, uniform filling of the catalyst and replacement of the catalyst can be performed more quickly.

  In the plate reactor, the upper part of the heat transfer plate 2 is constituted by a heat transfer tube having the largest cross section, the middle part of the heat transfer plate 2 is constituted by a heat transfer tube having the second largest cross section, and the lower part of the heat transfer plate 2 Is composed of heat transfer tubes having the smallest cross section, and the heat transfer plates 2 are arranged at equal intervals, so that the gap whose width gradually increases from the upstream side to the downstream side in the gas ventilation direction X is formed. Can be formed. Accordingly, when the plate reactor is used for heat removal in an exothermic reaction such as a gas phase catalytic oxidation reaction, the heat removal efficiency on the upstream side in the gas aeration direction X is compared with the downstream side depending on the width of the gas flow path. Can be increased.

  Further, in the plate reactor, the holding plate 3 is fixed by nuts at both ends of the holding rod 4, so that the holding plate 3 is attached to the heat transfer plate 2 within the range of the installation length of the screws of the holding rod 4. In the clamping direction, the position can be changed and fixed. Therefore, the distance between the pair of sandwiching plates 3 can be finely adjusted according to the alignment length of the plurality of heat transfer plates 2 due to the alignment of the heat transfer plates 2.

  Further, in the plate reactor, the holding rod 4 is arranged at a position overlapping the partition 7 in the vertical direction (gas aeration direction X). It is possible to charge the catalyst and extract the catalyst from each compartment. Therefore, the catalyst can be charged and extracted quickly, and the time required for such maintenance work is shortened. The productivity of the reaction products such as ethylene oxide, butadiene, etc. in the medium or long term (for example, in the year or in the total operating time of the plate reactor) can be increased.

  Moreover, since the gas distribution part 6 has the manhole 10, the said plate type reactor can perform the filling of a catalyst and the maintenance inspection work inside a plate type reactor, without disassembling the edge part of a plate type reactor. . Therefore, the time required for such maintenance work is shortened, and as a result, in the production by the plate reactor, productivity in the long term among the reaction products can be further enhanced.

  Reactors such as plate reactors generally require periodic inspections for security and maintenance. The plate type reactor of the present invention is excellent from the viewpoint of safety because it does not substantially have a gap in which gas stays inside the reaction vessel. Can be done quickly. Thus, the plate reactor of the present invention is excellent in safety, stability, convenience, and productivity in long-term use including maintenance and inspection, and has a great effect from the viewpoint of industrial use. .

It is a figure which shows roughly the principal part of the structure of one Embodiment of the plate type reactor of this invention. It is a figure which shows the principal part of the external appearance containing the clamping board 3 in the plate type reactor of FIG. It is a figure which shows roughly the principal part of a structure containing the heat-medium supply part 5 in the plate type reactor of FIG. It is a figure which shows the some heat-transfer plate 2 which aligns in the plate type reactor of FIG. It is a figure which shows an example of the heat exchanger plate in the plate type reactor of FIG. 1 in detail. FIG. 2 is a diagram partially showing a plurality of heat transfer plates 2 and a sandwiching plate 3 that sandwiches them in the plate reactor of FIG. 1. It is a figure which shows an example of the partition 7 used for the plate type reactor of FIG. It is a figure which shows another example of the partition 7 used for the plate type reactor of FIG. It is a figure which shows another example of the partition 7 used for the plate type reactor of FIG. It is a figure which shows another example of the partition 7 used for the plate type reactor of FIG. It is a figure which shows another example of the partition 7 used for the plate type reactor of FIG. It is a figure which shows another example of the partition 7 used for the plate type reactor of FIG. It is a figure which shows the other form of the clamping board used for the plate type reactor of FIG. It is a figure which shows the other form of the heat-medium supply part used for the plate type reactor of FIG. It is a figure which shows the further another form of the heat-medium supply part used for the plate type reactor of FIG.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Heat transfer tube 2 Heat transfer plate 3, 13 Holding plate 4 Holding rod 5 Heat-medium supply part 6 Gas distribution part 7 Partition 8, 9, 24, 25, 31 Nozzle 10 Manhole 21 First jacket 22 Second jacket 23 Flow Road separation plate 32 distribution pipe X Arrow indicating the gas ventilation direction Y Arrow indicating the direction in which the heat medium flows

Claims (11)

A reaction vessel for reacting gaseous raw materials, and a plurality of heat transfer plates provided side by side in the reaction vessel,
The heat transfer plate includes a plurality of heat transfer tubes connected at a peripheral edge or an edge of a cross-sectional shape,
In a plate reactor in which a catalyst is filled in a gap between adjacent heat transfer plates,
The reaction container covers both ends of the plurality of heat transfer plates in the gas ventilation direction, and a gas distribution unit that distributes gas through a gap between adjacent heat transfer plates;
A heat-medium supply section that contacts both ends of the heat-transfer tube in the heat-transfer plate and supplies a heat medium to the heat-transfer tube;
A direction in which the plurality of heat transfer plates are arranged in contact with the heat transfer plates at both ends in the direction in which the heat transfer plates are arranged so as to cut off the gas flow at least along the extending direction of the heat transfer tubes And the gas distribution unit, the heat medium supply unit, and the plate clamping unit are hermetically joined so as to accommodate the plurality of heat transfer plates. A plate reactor.   The plate clamping portion includes a pair of clamping plates that contact the entire heat transfer tube in the extending direction of the heat transfer tubes, at least one of the heat transfer plates at both ends in the direction in which the plurality of heat transfer plates are arranged, and The plate-type reactor according to claim 1, comprising a holding rod that penetrates and holds the sandwiching plate.   The plate clamping portion is in contact with a heat transfer plate at both ends in a direction in which the plurality of heat transfer plates are arranged in contact with a peripheral edge of a heat transfer tube at an upstream end of the heat transfer plate in a gas ventilation direction. Item 3. The plate reactor according to Item 1 or 2.   4. The apparatus according to claim 1, further comprising a partition that divides a gap between adjacent heat transfer plates into a plurality of compartments containing the filled catalyst along a gas ventilation direction. The plate reactor as described.   The plate reactor according to claim 4, wherein the holding rod is disposed at a position overlapping the partition in a gas aeration direction.   The plate reactor according to claim 1, wherein the gas distribution unit further includes a manhole. The plate type according to any one of claims 1 to 6, wherein the gas distributor further includes a safety device for preventing damage to the plate type reactor due to an increase in pressure in the reaction vessel. Reactor.   The heat medium supply unit further includes a heat medium mixing device that mixes the second heat medium with the first heat medium in the heat medium supply unit. The plate reactor as described.   The plate reactor according to any one of claims 1 to 8, further comprising a gas-permeable catalyst protective cover that covers one end or both ends of the plurality of heat transfer plates in a gas flow direction. A plurality of heat transfer plates are arranged using a plate reactor in which a plurality of heat transfer plates are provided side by side in a reaction vessel, and a catalyst layer is formed by filling a catalyst between gaps between the heat transfer plates. A reaction medium including a step of supplying a heat medium to the heat transfer tube, supplying the raw material gas to the reaction vessel, and reacting the raw material gas in the presence of the catalyst to generate a gaseous reaction product. In the manufacturing method,
A method for producing a reaction product, wherein the plate reactor according to any one of claims 1 to 9 is used for the plate reactor. Producing the reaction product comprises:
Oxidizing ethylene to produce ethylene oxide;
An unsaturated aliphatic aldehyde having 3 and 4 carbons by oxidizing at least one selected from the group consisting of hydrocarbons having 3 and 4 carbons, tertiary butanol, and unsaturated aliphatic aldehydes having 3 and 4 carbons; Producing one or both of unsaturated fatty acids having 3 and 4 carbon atoms;
Oxidation of aliphatic hydrocarbons having 4 or more carbon atoms to produce maleic acid;
oxidizing o-xylene to produce phthalic acid;
Hydrogenating olefins to produce paraffin;
Hydrogenating a carbonyl compound to produce an alcohol;
Acid decomposition of cumene hydroperoxide to produce acetone and phenol;
Oxidative dehydrogenation of butene to produce butadiene;
Dehydrogenating ethylbenzene to produce styrene; or
11. A step of oxidizing one or both of propylene and acrolein, or one or both of isobutylene and methacrolein to produce one or both of (meth) acrolein and (meth) acrylic acid. A process for producing the reaction product described in 1.

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