JP2009262142A - Plate-type reactor and production method of reaction product - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a plate-type reactor that enables uniform and easy catalyst loading in gaps between adjacent heat-transfer plates. <P>SOLUTION: The plate-type reactor includes a plurality of parallel heat-transfer plates 3 in a casing 1 and a plurality of partition plates 5 which divide the gaps between adjacent heat-transfer plates 3 into a plurality of compartments along the direction of a gas flow in the casing 1, wherein each compartment is loaded with a catalyst according to the volume of the compartment. <P>COPYRIGHT: (C)2010,JPO&INPIT

Description

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

  As a reactor used in a gas phase reaction in which a granular solid catalyst is used, such as a gas phase catalytic oxidation reaction of propane, propylene, or acrolein, and in which a granular solid catalyst is used, for example, for reacting a fluid reaction raw material A reaction vessel, a plurality of heat transfer plates provided side by side in the reaction vessel, and a device for supplying a heat medium to the heat transfer tube, the reaction vessel being supplied The reaction raw material is discharged through a gap between adjacent heat transfer plates, and the heat transfer plate includes a plurality of the heat transfer tubes connected at a peripheral edge or an edge of a cross-sectional shape. There is known a plate reactor in which a catalyst is filled in a gap between matching heat transfer plates (see, for example, Patent Document 1).

  Such a plate reactor generally has a plurality of catalyst layers formed in the gaps between adjacent heat transfer plates and has excellent contact between the heat transfer plates and the catalyst. It is excellent from the viewpoint of efficiently producing a large amount of a product obtained by a reaction such as a phase reaction, which is a contact reaction between a catalyst and a reaction raw material and involves a large exotherm or endotherm.

  On the other hand, in the gas phase reaction, it is desired to make the packing state of the catalyst uniform from the viewpoint of controlling the gas phase reaction. In a plate reactor, the gap between adjacent heat transfer plates is filled with a catalyst in layers, so it is difficult to fill each gap and the catalyst uniformly, and the gap is filled uniformly with the catalyst. A technology that can do this has been desired.

JP 2004-202430 A

  The present invention provides a plate reactor in which a catalyst can be uniformly and easily filled in a gap between adjacent heat transfer plates.

  In the present invention, a plurality of compartments capable of accommodating a catalyst are formed in the gap between adjacent heat transfer plates in a plate reactor along the flow direction of the reaction raw material, and each compartment is filled with the catalyst uniformly. A plate reactor is provided.

  That is, the present invention includes a reaction vessel for reacting a fluid reaction raw material, a heat transfer tube, a plurality of heat transfer plates provided side by side in the reaction vessel, and an apparatus for supplying a heat medium to the heat transfer tube The reaction vessel is a vessel in which the supplied reaction raw material is discharged through a gap between adjacent heat transfer plates, and the heat transfer plate has a peripheral edge or an edge of a cross-sectional shape. In a plate reactor that includes a plurality of connected heat transfer tubes and that is filled with a catalyst in a gap between adjacent heat transfer plates, the gap between adjacent heat transfer plates extends along the ventilation direction in the reaction vessel. Thus, a plate reactor is further provided which further has a partition for dividing the packed catalyst into a plurality of compartments.

Moreover, this invention provides the said plate type reactor whose each volume of the said some division is 1-200L.

  The present invention also provides the above plate reactor in which the number of compartments having the same volume is 50% or more of the whole compartments.

  The present invention also uses the plate reactor of the present invention to produce a reaction product from a fluid reaction raw material in the presence of a catalyst filled in a gap between heat transfer plates of the plate reactor. In the method, the reaction raw material includes at least one selected from the group consisting of ethylene, hydrocarbons having 3 and 4 carbon atoms, and tertiary butanol, or a group consisting of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms. At least one selected from the group consisting of hydrocarbons having 4 or more carbon atoms, one or both of xylene and naphthalene, olefins, carbonyl compounds, cumene hydroperoxide, butenes, or ethylbenzene, ethylene oxide, having 3 and 4 carbon atoms At least one of an unsaturated aliphatic aldehyde and an unsaturated fatty acid having 3 and 4 carbon atoms; maleic acid; phthalic acid; paraffin; Alcohol; to provide a method for producing a a reaction product; acetone and phenol; butadiene; or styrene.

  Since the plate type reactor of the present invention has the partition, it can be filled with an amount of catalyst corresponding to the capacity of each section formed by the partition, and the packing state of the catalyst is made constant in each section. Thus, the catalyst can be uniformly filled in the entire gap between adjacent heat transfer plates in the plate reactor. Thus, in the plate reactor of the present invention, the catalyst can be uniformly and easily filled in the gaps between the adjacent heat transfer plates as compared with the conventional plate reactor.

  In the present invention, the volume of each of the plurality of compartments is 1 to 200 L, which is more effective from the viewpoint of facilitating the filling operation of the catalyst in each compartment.

  Further, in the present invention, it is more effective from the viewpoint of easily making the packed state of the catalyst in each section that the volume having the same volume is 50% or more of all the sections.

  In recent years, chemical products are often mass-produced in large-scale facilities, the reactors installed in the production facilities have been enlarged, and the amount of catalyst inserted has become large. It is very important to uniformly and efficiently fill the container. In particular, in the case of a reaction in which a large reaction heat is generated or absorbed, and the temperature rise or fall due to the reaction heat affects the reaction rate, the reaction result, and the degree of catalyst deterioration, the reaction raw material and the catalyst are uniformly contacted. This is a critical issue in designing a better reactor.

  Since the plate type reactor of the present invention can uniformly fill the catalyst in each section, the catalyst can be uniformly filled in the gaps between the heat transfer plates. For this reason, the plate reactor of the present invention can perform a good reaction by uniform packing of the catalyst in a catalytic reaction that may involve a large exotherm or endotherm that affects the performance and life of the catalyst. it can. Therefore, using the plate reactor of the present invention, the reaction raw material is at least one selected from the group consisting of ethylene; hydrocarbons having 3 and 4 carbon atoms, and tertiary butanol, or a non-carbon having 3 and 4 carbon atoms. Ethylene oxide using at least one selected from the group consisting of saturated aliphatic aldehydes; hydrocarbons having 4 or more carbon atoms; one or both of xylene and naphthalene; olefins; carbonyl compounds; cumene hydroperoxides; butenes; A reaction product which is at least one of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms and unsaturated fatty acids having 3 and 4 carbon atoms; maleic acid; phthalic acid; paraffin; alcohol; acetone and phenol; butadiene; In the mass production of reaction products. It is possible to perform stable production in the period.

It is a figure which shows schematically the structure in one Embodiment of the plate-type reactor of this invention. It is a figure which shows a cross section when the plate type reactor of FIG. 1 is cut | disconnected along the A-A 'line. It is a figure which shows a cross section when the plate type reactor of FIG. 1 is cut | disconnected along a B-B 'line. It is a figure which shows the adjacent heat-transfer plate 3 and the partition 5 provided between them. It is a figure which shows an example of the partition. It is a figure which shows the other example of the partition. It is a figure which shows the other example of the partition. It is a figure which shows the other example of the partition. It is a figure which shows the other example of the partition. It is a figure which shows the other example of the partition.

  The plate reactor of the present invention has a reaction vessel for reacting a fluid reaction raw material such as a gaseous raw material, a plurality of heat transfer plates having a heat transfer tube and provided side by side in the reaction vessel, A heat medium supply device that supplies a heat medium to the heat transfer pipe, and a partition that divides a gap between adjacent heat transfer plates into a plurality of compartments containing a packed catalyst along a ventilation direction in the reaction vessel. Have.

  The reaction raw material is a fluid. The reaction product obtained by the reaction of the reaction raw material is also a fluid. The reaction raw material and the reaction product have fluidity to flow through the catalyst layer filled in the compartment. Examples of the state of such reaction raw materials and reaction products include liquid, gas, and a state containing both of them.

  When the reaction raw material is a gas, the reaction vessel is filled with a catalyst in a plurality of heat transfer plates arranged in parallel in the aeration direction in the reaction vessel (that is, the flow direction of the reaction raw material) and between adjacent heat transfer plates. And a plurality of catalyst layers arranged in parallel in the flow direction of the reaction raw material in the reaction vessel. For the reaction vessel, for example, a casing having a rectangular cross section with respect to the flow direction of the reaction raw material or a shell having a circular cross section is used.

  The reaction vessel is a vessel through which a fluid such as a supplied gas is discharged through a gap between adjacent heat transfer plates, and usually has a pair of flow ports. One of the pair of flow ports serves as a supply port for the reaction raw material supplied to the reaction vessel, and the other serves as a discharge port for the reaction product generated in the reaction vessel. The form of the flow port is not particularly limited as long as the supply of the fluid to the reaction vessel and the discharge of the fluid from the reaction vessel are performed. The pair of flow ports are preferably provided to face each other. Examples of such circulation ports include a pair of circulation ports provided at both ends of the casing and the shell, and are formed in a cylindrical shape in each of the central portion including the central axis of the shell and the inner peripheral portion of the shell. A pair of flow ports for allowing fluid to flow radially on the surface can be mentioned.

  The heat transfer plate is formed in a plate shape including a plurality of heat transfer tubes connected in one direction at a peripheral edge or an edge in a cross-sectional shape.

As disclosed in Patent Document 1, such a heat transfer plate is formed by forming two corrugated plates in which patterns such as arcs, elliptical arcs, and rectangles are continuously formed at the ends of the patterns of both corrugated plates. Can be formed by joining each other with convex edges. 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 1 to 3 m. Yes, the width (ie, the length of the heat transfer tube) is 0.05 to 10 m.

  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 tube in the heat transfer plate is not formed so as to extend in a direction parallel to the flow direction of the fluid in the reaction vessel, but the reaction of the reaction raw materials by adjusting the temperature of the heat medium in the heat transfer tube From the viewpoint of controlling the flow rate, and is formed so as to extend in a direction orthogonal to the flow direction of the fluid in the reaction vessel, that is, the direction of the heat medium flowing through the heat transfer tube is the flow of the fluid in the reaction vessel. The direction perpendicular to the direction is more preferable from the viewpoint of controlling the reaction of the reaction 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 a material include stainless steel and carbon steel. 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, or a rectangular shape. 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 long axis end in a substantially circular shape or a single edge in a rectangle.

  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 20 mm, and the height of the heat transfer tube is 10 to 50 mm.

  The heat medium supply device may be any device that supplies a heat medium to the heat transfer tube. Examples of such a heat medium supply device include a device that supplies a heat medium in one direction to all of the plurality of heat transfer tubes, and a heat medium that supplies a heat medium in one direction to a part of the plurality of heat transfer tubes. Another part of the heat pipe includes a device for supplying a heat medium in the reverse direction. The heat medium supply device is preferably a device that circulates the heat medium inside and outside the reaction tube via the heat transfer tube. The heating medium supply device preferably has a device for adjusting the temperature of the heating medium from the viewpoint of controlling the reaction in the reaction vessel.

  The said partition is provided in the clearance gap between adjacent heat-transfer plates along the flow direction of the fluid in a 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. The partition preferably has rigidity from the viewpoint of holding the catalyst filled in each compartment. Examples of such partitions include stainless 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 200 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. The volume of the one section is more preferably 1.2 to 100 L, further preferably 1.5 to 30 L, and further preferably 2 to 15 L.

  The volume of the compartment is determined during the design of the plate reactor and is generally known. However, the volume of the compartment is the distance between the heat transfer plates measured along the flow direction of the fluid, the length of the gap along the flow direction, and the distance between the partitions or between the partition and the wall of the reaction vessel. , Can be obtained by calculation. In addition, the volume of the compartment is, for example, forming a watertight compartment by inserting a sufficiently large plastic bag into the compartment, supplying water to the formed watertight compartment, and measuring the amount of water supplied. Can be obtained.

  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. 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.

  As the catalyst filled in the compartment, 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, a Raschig ring shape, and a pellet shape. In the case where the shape of the catalyst is formed so that the partition is not in close contact with the surface of the heat transfer plate, the catalyst has a shape in which the shortest diameter of the catalyst is larger than the gap between the heat transfer plate and the partition. From the viewpoint of preventing leakage of the catalyst.

  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.

The plate reactor of the present invention may further have other components other than the components described above. As such other components, for example, a reaction vessel for a catalyst having fluidity and provided at the end of a downstream heat transfer plate in the flow direction of flow in the reaction vessel Examples include a leakage preventing member such as a ventilation plate for preventing leakage from the air and a locking member such as a hook provided at one end of the partition and hooked to the leakage preventing member or the heat transfer plate.
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 includes, for example, a rectangular casing 1 and a heat transfer tube 2 as shown in FIGS. 1 to 3, and a plurality of heat transfer plates 3 provided side by side in the casing 1. A plurality of compartments in which the catalyst is filled and held along the ventilation direction in the casing 1 through the gap between the heat transfer plate 3 and the heat transfer plate 3 that stores the heat transfer medium supplied to the heat transfer tube 2 and the adjacent heat transfer plates 3. A plurality of partitions 5, perforated plates 6, 7 provided at the upper and lower portions of the heat transfer plate 3, a pump 8 for circulating the heat medium in the heat medium accommodating portion 4, and the temperature of the circulating heat medium And a temperature adjusting device 9 for adjusting.

  The casing 1 forms an air passage having a rectangular cross-sectional shape and corresponds to the reaction vessel. The casing 1 has a pair of opposed vent holes 10 and 10 ′ at the upper end and the lower end of the casing 1. The heat transfer tube 2 is, for example, a tube having a major axis of 30 to 50 mm and a minor axis of 10 to 20 mm and an elliptical cross section.

  The heat transfer plate 3 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 3 is formed by joining two corrugated plates each having an elliptical arc formed continuously at a convex edge formed at the ends of the arcs of both corrugated plates. Adjacent heat transfer plates 3 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 3 and the other The heat transfer plates 3 are arranged in parallel so as to face the concave edges on the surface.

  For example, as shown in FIG. 4, the heat transfer plate 3 includes three types of heat transfer tubes 2 a to 2 c having different cross-sectional sizes in the upper part, the middle part, and the lower part. The heat transfer plate 3 is formed such that the long axes of the heat transfer tubes 2a to 2c are arranged in a straight line. Further, for example, the heat transfer tube 2 a forms the heat transfer plate 3 for 20% of the height of the heat transfer plate 3, and the heat transfer tube 2 b forms the heat transfer plate 3 for 30% of the height of the heat transfer plate 3. The heat transfer tube 2 c forms the heat transfer plate 3 for 40% of the height of the heat transfer plate 3. 10% of the height of the heat transfer plate 3 is formed by the upper and lower joint plate portions of the heat transfer plate 3.

  The cross-sectional shape of the heat transfer tube 2a formed on the upper part of the heat transfer plate 3 is an ellipse having a major axis of 50 mm and a minor axis of 20 mm. The cross-sectional shape is an ellipse having a major axis of 40 mm and a minor axis of 16 mm, and the sectional shape of the heat transfer tube 2 c formed at the lower part of the heat transfer plate 3 is a major axis of 30 mm and a minor axis of 10 mm. It is oval.

  The heat transfer plates 3 may be arranged in parallel at different intervals in the entire reaction vessel, but in the plate reactor of FIG. 1, the same interval (for example, the shortest distance between the outer walls of the heat transfer tube 2a is 14 mm (each The distance between the major axes of the heat transfer tubes of the heat plate 3 is 30 mm)).

  The heat medium accommodating portion 4 is a container provided on a pair of opposing walls of the casing 1, and a supply port for supplying a heat medium to each heat transfer tube 2 is formed in the wall. The heat medium is divided into a plurality at a predetermined height so that the heat medium meanders between the heat medium accommodating portions 4 via the heat transfer tubes 2.

  The partition 5 is provided between the adjacent heat transfer plates 3 along the ventilation direction in the casing 1. The partitions 5 may be provided at different intervals in the entire reaction vessel. However, in the plate type reactor of FIG. 1, a partition having a volume of 22 L is formed in parallel with the same interval (for example, 1,000 mm). .

The interval between the partitions 5 is preferably 5 cm to 2 m, and more preferably 10 cm to 1 m. The volume of the compartment formed by the heat transfer plate 3 and the partition 5 is preferably 1 to 200 L from the viewpoint of performing filling of the gap into the gap in a unit of unit and accurately and easily filling the catalyst. 2 to 100L is more preferable, and 1.5 to 30L is more preferable. The volume of each compartment can be measured, for example, by the method described above.

  In the plate reactor of FIG. 1, the amount of catalyst filled up to a predetermined height in the section formed by the partition 5 is constant as long as the length of the section in the length direction of the heat transfer tube 2 is the same. . Therefore, since the amount of the catalyst in each compartment can be managed according to the volume of each compartment, the volume of each compartment is not necessarily constant if the volume of each compartment is known.

  The volume of the compartments is preferably the same for 50% or more of all the compartments, more preferably the same for 80% or more, and the same for 90% or more, from the viewpoint of management of catalyst filling work and labor saving. More preferably it is.

  A member that can hold the filled catalyst in each compartment when the catalyst is filled in each compartment is used for the partition 5. As the partition 5, for example, as shown in FIGS. 5 to 7, a plate or net having a shape having a side edge that is in close contact with the unevenness on the surface of the heat transfer plate 3 can be used.

  In addition, the partition 5 is in contact with the heat transfer tube 2a of the adjacent heat transfer plate 3 if the catalyst filled in each partition does not leak into the adjacent partition from the gap between the partitions 5, and other partitions in the heat transfer plate 3 Members that do not contact the convex and concave edges of the heat transfer tubes 2b and 3c can be used. For example, as shown in FIGS. 8 and 9, a round having the shortest diameter or width between adjacent heat transfer plates 3 is used. A stick or a square stick can be used.

  Further, as shown in FIG. 6, the partition 5 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. 7, it may be a net having larger eyes than the catalyst particles (for example, 0.8 times or less the shortest diameter of the catalyst).

  In the case where two adjacent heat transfer plates 3 are arranged in parallel so that the convex edge of one heat transfer plate 3 faces the concave edge of the other heat transfer plate 3, the partition 5 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 3 at the side edge of the partition 5 and is separated from the convex edge of the heat transfer plate 3 can be used. Such a partition 5 has a distance between two heat transfer plates 3 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 2 in each heat transfer plate 3). 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 3, it can be suitably used.

  As shown in FIGS. 5 to 7 and 10, the partition 5 having a shape having a side edge in contact with the unevenness of the surface of the heat transfer plate 3 is provided with the heat transfer plate 3 and the heat transfer plate 3 when the heat transfer plate 3 is installed in the casing 1. By alternately installing the abutment partitions 5, they are provided between the two heat transfer plates 3. The partition 5 having the shortest distance diameter or width between the adjacent heat transfer plates 3 as shown in FIGS. 8 and 9 can be obtained by alternately installing the heat transfer plates 3 and the partitions 5 in contact with the partitions. You may provide between the heat-transfer plates 3, and you may provide by inserting between the heat-transfer plates 3 adjacent to the heat-transfer plate 3 already installed. The flexible partition 5 such as a net or a thin steel plate can be provided by being inserted between the adjacent heat transfer plates 3 of the heat transfer plates 3 already provided.

Moreover, the partition 5 of the shape which has a side edge which touches the unevenness | corrugation of the surface of the heat-transfer plate 3 like the partition shown in FIGS. 5-7 and 10, and the heat-transfer tube like the partition 5 shown in FIG.8 and FIG.9. The partition 5 in contact with the apex (convex portion) is preferably manufactured using a material having no flexibility and high rigidity, from the viewpoint of keeping the interval between the heat transfer plates 3 equal.

  The perforated plates 6 and 7 are plates each having a hole having a diameter of 0.20 to 0.99 times the longest diameter of the catalyst to be filled with an opening ratio of 20 to 99%. In the plate reactor of FIG. 1, the perforated plates 6, 7 are shown in FIG. 3 in order to prevent aeration to the gap between the outermost heat transfer plate 3 and the wall of the casing 1. Thus, it forms so that the clearance gap between the edge of the heat exchanger plate 3 arrange | positioned at the outermost side and the wall of the casing 1 may be plugged up.

  A device that can transfer a heat medium having a desired temperature is used for the pump 8. The temperature adjusting device 9 is a device such as a heat exchanger that can control the temperature of the heat medium to a desired temperature. The heat medium storage unit 4, the pump 8, and the temperature adjustment device 9 constitute a heat medium supply device.

  The catalyst is filled between the heat transfer plates 3 by filling the respective compartments with the catalyst. Since all the compartments formed by the heat transfer plate 3 and the partition 5 have the same volume, the capacity equivalent to the capacity of one compartment (for example, a volume of 95 to 100% with respect to the capacity of one compartment). Of each catalyst is packed into each compartment.

  When the shape of the heat transfer tube of the heat transfer plate changes along the flow direction of the reaction raw material, check whether the catalyst filling is good or not in each region formed between the heat transfer plates due to the change of the shape of the heat transfer tube May be preferable from the viewpoint of obtaining better reaction results. In this case, a volume of catalyst of one compartment is divided and packed into the number of regions formed, for example 2 to 3, and the filling height of the catalyst is measured in each divided region, It is possible to check the state of catalyst filling more precisely.

  A good packing state of the catalyst is a state in which there is no cavity or high density portion in the catalyst layer, and the entire catalyst layer is in contact with the reaction fluid equally. Comparison with the value (for example, the error of the measured value with respect to the theoretical value is within 10%), comparison of the catalyst filling height between the compartments (for example, the difference in the filling height between the compartments is 2% of the filling height) Within).

  It is preferable to determine the state of catalyst filling by measuring the height of the catalyst layer in the compartment after filling the catalyst amount corresponding to the volume of the compartment. The height of the catalyst layer is preferably within ± 5% of the theoretical value, more preferably within ± 3%, and even more preferably within ± 1%. Furthermore, when exceeding the said range, it is preferable to extract and to refill.

  More practically, the criteria for determining the quality of the catalyst filling state, such as the theoretical value of the catalyst filling height, are the accuracy of manufacturing the uneven shape of the heat transfer plate, the accuracy of the installation interval when manufacturing the heat transfer plate, It varies depending on the degree of parallelism, the accuracy of the partition installation interval, the degree of parallelism, and the like. Confirmation of the production accuracy of the heat transfer plate and partition is done by measuring the shape of the heat transfer plate before assembling the plate reactor and measuring the volume of the compartment in the manner described above during or after assembly. This can be done by checking differences and variations. It is recommended that the criteria for determining whether or not the catalyst is filled be determined based on the confirmed production accuracy. The determination criterion is set larger than the accuracy of the volume and 1.1 to 2 times the accuracy of the volume. For example, the theoretical value of the filling height is preferably obtained from the volume of the compartment obtained from the production accuracy and the spatial density of the catalyst to be filled, and the allowable accuracy of the compartment is ± 3% of the production accuracy. In this case, the allowable filling height of the catalyst can be determined at an arbitrary ratio of ± 3.3 to ± 6.0% of the theoretical value of the filling height.

  The partition 5 has a hook that engages with an engagement portion such as a hole or a ring provided in the hole of the perforated plate 7 or the end of the heat transfer plate 3, and locks the hook to the engagement portion. By extending the partition 5 by this, it is also possible to provide in the gap between the adjacent heat transfer plates 3. According to such a structure, it becomes possible to use for the partition 5 the material which does not have shape retention property, such as glass wool.

  Since the plate type reactor has the partition 5, the catalyst can be uniformly filled in the entire reactor by filling the catalyst in a fixed state in units of compartments. Therefore, accurate filling of the catalyst can be performed more easily than the filling of the catalyst between the heat transfer plates 3 in which such compartments are not formed.

  The plate reactor is used for a single catalyst filling operation in the same volume section because 50% or more of all the sections formed by the heat transfer plate 3 and the partition 5 have the same capacity. The catalyst is constant. Therefore, the filling operation of the catalyst can be performed more quickly than the filling of the catalyst between the heat transfer plates 3 in which such a partition is not formed.

  Furthermore, since the said plate-type reactor has the partition 5, it can judge the packing state of a catalyst per division. Therefore, when the catalyst filling state is poor, it is possible to correct the catalyst filling state by refilling only the catalyst in the section determined to be defective. Therefore, the catalyst filling operation can be adjusted more easily than the catalyst filling between the heat transfer plates 3 in which such compartments are not formed.

  INDUSTRIAL APPLICABILITY The present invention is applied to a fixed bed contact reaction process in a plate type reactor, and among these reaction processes, a reaction process in which a catalyst may be deteriorated due to a high reaction heat or a reaction result may be lowered. Applies to In particular, the present invention can be applied to either a gas or a liquid as a reaction raw material, but can be suitably used when the gas is difficult to remove heat compared to a liquid state.

  For example, in the reaction to which the plate reactor of the present invention is effectively applied, the raw material is at least one selected from the group consisting of ethylene, hydrocarbons having 3 and 4 carbon atoms, and tertiary butanol, or the number of carbon atoms. At least one selected from the group consisting of 3 and 4 unsaturated aliphatic aldehydes; hydrocarbons having 4 or more carbon atoms such as n-butane and benzene; one or both of xylene and naphthalene; olefins; carbonyl compounds; Butene; or ethylbenzene; and the obtained reaction product is ethylene oxide; at least one of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms and unsaturated fatty acids having 3 and 4 carbon atoms; maleic acid; Paraffin; alcohol; acetone and phenol; butadiene; or styrene; Reaction is.

  It is particularly preferably applied to a gas phase catalytic oxidation reaction that is known to easily generate hot spots. The reaction raw material is selected from the group consisting of at least one reaction raw material selected from the group consisting of hydrocarbons having 3 and 4 carbon atoms and tertiary butanol, or the group consisting of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms. A reaction that is at least one of the raw materials can be mentioned.

  Specifically, the hydrocarbon having 3 carbon atoms includes propylene and propane. Examples of the hydrocarbon having 4 carbon atoms include isobutylene, butenes, and butanes. Examples of the unsaturated aliphatic aldehyde having 3 and 4 carbon atoms include acrolein and methacrolein, and examples of the unsaturated fatty acid having 3 and 4 carbon atoms include acrylic acid and methacrylic acid.

  Next, although it demonstrates concretely using an Example, this invention is not limited to an Example at all.

  As the plate reactor, a plate reactor having the configuration shown in FIG. 4 was prepared for a filling test. Six heat transfer plates with an effective length (heat transfer plate width) in the axial direction of the heat transfer tube in the heat transfer plate of 5 m are arranged in parallel, and a ventilation plate (perforated plate) and a ventilation plate are arranged below the heat transfer plate. And a locking member that detachably locks. The axial height of the heat transfer plate from the ventilation plate was 1.88 m, and the height of the straight portion without the heat transfer tube at the upper end of the heat transfer plate was 150 mm. The distance between the straight portions of the heat transfer plate when arranged in parallel was 24 mm.

  The heat transfer plate is formed of two steel plates so that a corrugated continuous section is formed so that a heat transfer tube having the specifications shown in Table 1 below is formed. Were formed by bonding. As the steel plate, a stainless steel plate (SUS304L) having a thickness of 1 mm was used.

  The major and minor diameters of the heat transfer tubes of the joined heat transfer plates were measured. A CCD laser displacement meter was used for measurement. Since part of the heat transfer plate exceeds 1% of the design value of the long and short diameters of the heat transfer tube, the accuracy of the volume of each section has been improved, so the error of the section volume is within 1.5% It was confirmed that.

  Partitions were provided in the gap at 50 cm intervals. As the partition, a partition having the shape shown in FIG. 5 was used, and the thickness of the partition was 5 mm. For the production of the partition, a laser-cut steel plate was used so as to match the shape of the heat transfer plate. Although the partition shown in FIG. 5 has a complicated shape, it can be manufactured with high accuracy by a laser cutting method or the like if there is information on the shape of the heat transfer plate and the manufacturing accuracy.

  The catalyst used was Mo (12) Bi (5) Co (3) Ni (2) Fe (0.4) Na (0.4) B (0.2) K (0.08) Si (24) O. A composite metal oxide powder having the composition (x) is prepared, molded, formed into a cylindrical shape having an outer diameter of 4 mmφ and a height of 3 mm, and fired. Here, Mo, Bi, Co, Ni, Fe, Na, B, K, Si, and O are atomic symbols, and (x) of O (x) is a value determined by the oxidation state of each metal oxide.

  The catalyst filling method was performed using a vibration feeder having the same width as the partition plate interval of 50 cm. 11.6 liters of the catalyst was weighed and 55 bags each divided into plastic bags were prepared, and each compartment was filled with a feeder. The catalyst was supplied at a filling rate of 1 L (liter) or less (about 0.8 to 0.9 L / min) per minute. The filling height value calculated from the average compartment volume is 182.5 cm.

Thereafter, the upper surface of the formed catalyst layer was leveled in order to measure the filling height. The distance between the upper surface of the averaged catalyst layer and the upper end of the heat transfer plate was measured, and the filling height was determined from the difference between the height of the heat transfer plate and the measured distance.

  There was a variation in the catalyst supply speed by the vibration feeder, and the supply speed sometimes increased temporarily. When the supply speed fluctuates extremely, the catalyst layer height increases, sometimes bridging occurs, and sometimes overflows from the compartment, but at that time, the locking member attached to the lower part of the compartment is removed. The vent plate was removed and the catalyst was extracted from the compartment and filled again. Refilling should be carried out three times in total in a total of 150 fillings.

  From the measurement result of the filling height, the variation in the layer height of the catalyst layer was within ± 5 cm. This was a variation of ± 2.7% with respect to the total filling height of the catalyst. From this measurement result, it was found that the catalyst was filled into the gaps of the plate reactor very uniformly by filling the compartments formed by the partitions with the catalyst.

  In a plate reactor, the reaction may be controlled by adjusting the thickness of the catalyst layer. In such a plate reactor, it is more difficult to uniformly fill the catalyst in the entire reactor. However, the plate reactor of the present invention allows the catalyst to be charged quickly, accurately, and easily. It is expected that the workability in the installation, maintenance and management of plate reactors will be greatly improved.

DESCRIPTION OF SYMBOLS 1 Casing 2, 2a-2c Heat-transfer tube 3 Heat-transfer plate 4 Heat-medium accommodating part 5 Partition 6, 7 Perforated board 8 Pump 9 Temperature control apparatus 10, 10 'Vent

Claims (4)

A reaction vessel for reacting a fluid reaction raw material, a heat transfer tube, a plurality of heat transfer plates provided side by side in the reaction vessel, and a device for supplying a heat medium to the heat transfer tube ,
The reaction vessel is a vessel in which the supplied reaction raw material is discharged through a gap between adjacent heat transfer plates,
The heat transfer plate includes a plurality of the 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,
A 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 ventilation direction in the reaction vessel.   The plate reactor according to claim 1, wherein each of the plurality of compartments has a volume of 1 to 200L.   The plate reactor according to claim 1 or 2, wherein there are 50% or more of the compartments having the same volume. Using the plate reactor according to any one of claims 1 to 3, a reaction product from a reaction raw material in fluid in the presence of a catalyst filled in a gap between heat transfer plates of the plate reactor. A method for manufacturing
The reaction raw material is at least one selected from the group consisting of ethylene, hydrocarbons having 3 and 4 carbon atoms, and tertiary butanol, or at least 1 selected from the group consisting of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms. Using one or both of xylene and naphthalene; olefin; carbonyl compound; cumene hydroperoxide; butene; or ethylbenzene;
A reaction that is ethylene oxide; at least one of unsaturated aliphatic aldehydes having 3 and 4 carbon atoms and unsaturated fatty acids having 3 and 4 carbon atoms; maleic acid; phthalic acid; paraffin; alcohol; acetone and phenol; butadiene; A method for producing a reaction product, characterized by producing a product.

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