JP2013141659A - REACTION APPARATUS AND METHOD FOR PRODUCING ε-CAPROLACTAM - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a reaction apparatus which can inhibit rapid oxidation or combustion reaction caused by mixing a reaction gas present in a reactor with a regeneration gas present in a regenerator.SOLUTION: The reaction apparatus includes: a fluidized bed type reactor 2 which causes chemical reaction of a raw material gas in the presence of a solid catalyst; a fluidized bed type regenerator 3 which heats a part of the solid catalyst, of which the catalytic activity is decreased by being used in the reactor 2, in an oxygen-containing gas atmosphere to regenerate the solid catalyst so as to recover the catalytic activity; and a pressure controller 6 which controls at least one of the pressure in the reactor 2 and the pressure in the regenerator 3 so that the latter becomes higher than the former.

Description

  The present invention relates to a reactor and a method for producing ε-caprolactam.

  A reactor that chemically reacts a raw material gas in the presence of a solid catalyst is known. In this reactor, a so-called coke component (carbonaceous material) adheres to the solid catalyst by polymerization of the raw material gas and the reaction gas. Due to the adhesion of the coke component to the solid catalyst, the catalyst activity may deteriorate over time.

  For example, in Patent Document 1, such a reactor is combined with a regenerator that recovers the catalytic activity by heating a part of the solid catalyst that is used in the reactor and has a reduced catalytic activity in an oxygen-containing gas atmosphere. A configuration is proposed. Thereby, it is possible to regenerate the solid catalyst whose catalytic activity has been reduced and to reuse the solid catalyst whose catalytic activity has been recovered in the reactor.

JP 2000-229939 A

  The reaction apparatus of Patent Document 1 is configured to circulate a solid catalyst between a reactor and a regenerator. In such a circulation process of the solid catalyst, the reaction gas present in the reactor and the regeneration gas present in the regenerator are mixed to cause rapid oxidation and combustion reaction, and the equipment is determined by the amount of heat generated. There is a risk of damage.

  The present invention has been made in view of such circumstances, and is a reaction capable of suppressing rapid oxidation and combustion reaction due to mixing of a reaction gas present in the reactor and a regeneration gas present in the regenerator. An object is to provide an apparatus and a method for producing ε-caprolactam.

  In order to achieve the above object, the reactor of the present invention includes a fluidized bed type reactor that chemically reacts a raw material gas in the presence of a solid catalyst, and a solid catalyst that is used in the reactor and has a reduced catalytic activity. A regenerator of a fluidized bed type that regenerates so that catalytic activity is recovered by heating a part of the gas in an oxygen-containing gas atmosphere, and the pressure in the regenerator is larger than the pressure in the reactor And a pressure control unit for controlling at least one of the pressure in the reactor and the pressure in the regenerator.

  In the present invention, the pressure control unit includes at least one of a first control valve provided in the reactor, a second control valve provided in the regenerator, the first control valve, and the second control valve. And an opening degree control unit that controls the opening degree of one of the control valves.

  In the present invention, the opening degree control unit is configured to control at least one of the first control valve and the second control valve so that a difference between the pressure in the regenerator and the pressure in the reactor is constant. The opening degree is controlled.

  In the present invention, a catalyst that transfers a part of the solid catalyst used in the reactor to the regenerator by sending air to the regenerator between the reactor and the regenerator. A transfer mechanism is provided, and between the reactor and the regenerator, a regenerated catalyst transfer pipe for returning a part of the solid catalyst regenerated in the regenerator to the reactor is provided, The regenerated catalyst transfer pipe is configured such that a part of the solid catalyst regenerated in the regenerator moves to the reactor by its own weight.

  In the present invention, the regenerated catalyst transfer pipe is provided with a regenerated catalyst transfer pipe valve.

  The present invention is characterized in that a regenerative catalyst transfer pipe valve opening degree control unit for controlling an opening degree of the regenerated catalyst transfer pipe valve is provided.

  In the present invention, the regenerated catalyst transfer pipe extends obliquely downward from a side wall of the regenerator.

  In the present invention, the angle formed by the extending direction of the regenerated catalyst transfer pipe and the vertical direction is an angle range larger than 0 ° and not larger than 45 °.

  In the present invention, the catalyst transfer mechanism includes a first catalyst transfer pipe for extracting a part of the solid catalyst used in the reactor, and a catalyst storage for storing the solid catalyst extracted by the first catalyst transfer pipe. And a second catalyst transfer pipe for introducing the solid catalyst accommodated in the catalyst accommodating portion into the regenerator, and the solid catalyst accommodated in the catalyst accommodating portion by sending air to the catalyst accommodating portion. And an air delivery part that sends out toward the regenerator through a catalyst transfer pipe.

  In the present invention, the first catalyst transfer pipe is provided with a first catalyst transfer pipe valve.

  The present invention is characterized in that a first catalyst transfer piping valve opening degree control unit for controlling the opening degree of the first catalyst transfer piping valve is provided.

  In the present invention, the first catalyst transfer pipe extends obliquely downward from the side wall of the reactor.

  In the present invention, an angle formed between the extending direction of the first catalyst transfer pipe and the vertical direction is an angle range larger than 0 ° and not larger than 45 °.

  In the present invention, a differential pressure gauge for a reactor that measures a differential pressure in the reactor, a differential pressure gauge for a regenerator that measures a differential pressure in the regenerator, and a regenerated catalyst transfer that measures a differential pressure in the regenerated catalyst transfer pipe. A differential pressure gauge for piping and a differential pressure gauge for first catalyst transfer piping for measuring a differential pressure in the first catalyst transfer piping are included.

  In the present invention, the opening degree of at least one of the regeneration catalyst transfer piping valve and the first catalyst transfer piping valve is controlled so that the differential pressure measured by the reactor differential pressure gauge becomes a constant value. It is characterized by that.

  In the present invention, when at least one measured value of the differential pressure gauge for the reactor, the differential pressure gauge for the regenerator, the differential pressure gauge for the regenerated catalyst transfer pipe, and the differential pressure gauge for the first catalyst transfer pipe becomes a threshold value or less. Further, the control is performed so that the regenerated catalyst transfer piping valve and the first catalyst transfer piping valve are closed.

  In the present invention, the regenerative catalyst transfer pipe valve opening control unit is configured to regenerate the catalyst transfer pipe when the difference between the pressure in the regenerator and the pressure in the reactor becomes a threshold value or less. Control is performed to close the valve.

  In the present invention, the first catalyst transfer piping valve opening degree control unit is configured to transfer the first catalyst transfer pipe when a difference between the pressure in the regenerator and the pressure in the reactor becomes a threshold value or less. Control is performed so that the piping valve is closed.

  In the present invention, an inert gas is supplied to the regenerated catalyst transfer pipe and the first catalyst transfer pipe, and the gas accompanying the catalyst is replaced with the inert gas.

  In the present invention, the source gas contains cyclohexanone oxime.

  The method for producing ε-caprolactam according to the present invention is a method for producing ε-caprolactam in which ε-caprolactam is produced from cyclohexanone oxime by a gas phase reaction using a solid catalyst, wherein the gas phase reaction using the solid catalyst is performed. The reaction apparatus according to any one of claims 1 to 18 is used as the reaction apparatus to be performed.

  ADVANTAGE OF THE INVENTION According to this invention, the reaction apparatus which can suppress rapid oxidation by the mixing of the reaction gas which exists in a reactor, and the regeneration gas which exists in a regenerator, combustion reaction, and the manufacturing method of (epsilon) -caprolactam are provided. be able to.

It is a schematic diagram which shows the reaction apparatus of one Embodiment of this invention.

Hereinafter, embodiments of the present invention will be described with reference to the drawings, but the present invention is not limited to the following embodiments.
In all the drawings below, the dimensions and ratios of the constituent elements are appropriately changed in order to make the drawings easy to see. In the following description and drawings, the same or corresponding elements are denoted by the same reference numerals, and redundant description is omitted.

FIG. 1 is a schematic view showing a reaction apparatus according to an embodiment of the present invention.
The reactor 1 shown in FIG. 1 produces ε-caprolactam by subjecting cyclohexanone oxime to Beckmann rearrangement reaction in the presence of a solid catalyst and a lower alcohol.

  As shown in FIG. 1, the reaction apparatus 1 includes a reactor 2, a regenerator 3, a catalyst transfer mechanism 4, a regenerated catalyst transfer mechanism 5, and a pressure control unit 6.

  The reactor 2 includes a reaction vessel 20, a raw material gas introduction unit 21, a reaction gas discharge unit 22, a pressure control valve (first control valve) 23, a reactor differential pressure gauge 24, a reactor thermometer 25, And a pressure gauge 71. In the reactor 2, cyclohexanone oxime is subjected to Beckmann rearrangement reaction in the presence of a solid catalyst and a lower alcohol to produce ε-caprolactam.

  The reaction vessel 20 has a cylindrical straight body portion 20a, and a bottom portion 20b is connected to a lower portion of the straight body portion 20a. A dispersion plate 26 in which a large number of pores are dispersed is provided at the boundary between the straight body portion 20a and the bottom portion 20b. On the dispersion plate 26, the powder layer 10 made of solid catalyst powder is provided. Is formed.

  A source gas introduction part 21 for introducing a source gas is connected to the bottom part 20b. A source gas containing cyclohexanone oxime is introduced into the reactor 2 from the bottom portion 20 b by the source gas introduction unit 21. The source gas is injected to the bottom of the powder layer 10 through a large number of pores formed in the dispersion plate 26. The powder layer 10 is fluidized by the flow of the raw material gas blown vertically upward from the dispersion plate 26 and becomes a fluidized bed. The source gas flows through the powder bed 10 that has become a fluidized bed, contacts the solid catalyst, and undergoes Beckmann rearrangement. Thereby, the reaction gas containing (epsilon) -caprolactam is produced | generated.

  Examples of the solid catalyst include a boric acid catalyst, a silica / alumina catalyst, a phosphoric acid catalyst, a composite metal oxide catalyst, and a zeolite catalyst. Among these, a zeolite catalyst is preferable, a pentasil type zeolite is more preferable, and an MFI zeolite is particularly preferable.

  The zeolite catalyst may be crystalline silica whose skeleton is substantially composed only of silicon and oxygen, or may be a crystalline metallosilicate containing another element as an element constituting the skeleton. . In the case of a crystalline metallosilicate or the like, examples of elements that can exist other than silicon and oxygen include, for example, Be, B, Al, Ti, V, Cr, Fe, Co, Ni, Cu, Zn, Ga, Ge, and Zr. , Nb, Sb, La, Hf, Bi and the like, and two or more of these may be included. The atomic ratio of silicon to these elements is usually 5 or more, preferably 50 or more, more preferably 500 or more. This atomic ratio can be measured by an atomic absorption method or a fluorescent X-ray method.

  The zeolite catalyst is, for example, subjected to hydrothermal synthesis using a silicon compound, a quaternary ammonium compound, water, and, if necessary, a metal compound as a raw material, and the obtained crystal is dried and calcined as necessary, and then ammonia. It can be suitably prepared by treating with an aqueous solution containing at least one of ammonium salts.

  The particle size of the solid catalyst is preferably 0.001 to 5 mm, and more preferably 0.01 to 3 mm. In addition, the solid catalyst may be, for example, a molded body substantially composed of only the catalyst component, or may be one in which the catalyst component is supported on a carrier.

The Beckmann rearrangement reaction of cyclohexanone oxime using a solid catalyst can be performed under gas phase conditions. The reaction temperature is usually 250 to 500 ° C, preferably 300 to 450 ° C. The reaction pressure is usually 0.005 to 0.5 MPa, preferably 0.005 to 0.2 MPa. The supply rate of the raw material cyclohexanone oxime per catalyst 1kg (kg / h), ie the space velocity WHSV ^{(h -1)} is usually 0.1 to 20 ^-1, preferably 0.2~10h ^-1.

  Cyclohexanone oxime is introduced into the reaction vessel 20 together with the lower alcohol. Note that cyclohexanone oxime alone may be introduced into the reaction system, or may be introduced together with an inert gas such as nitrogen, argon, carbon dioxide or the like.

  The alcohol used here is preferably a lower alcohol having 1 to 6 carbon atoms. For example, use one or more of methanol, ethanol, n-propanol, isopropanol, n-butanol, sec-butanol, isobutanol, n-amyl alcohol, n-hexanol, 2,2,2-trifluoroethanol, etc. Can do. Methanol and ethanol are particularly preferred alcohols.

  In this embodiment, the Beckmann rearrangement reaction is performed in a fluidized bed format. In the fluidized bed format, the raw material gas containing cyclohexanone oxime is supplied from the raw material gas supply unit 21 to the reaction vessel 20 in which the solid catalyst has flowed, and the solid catalyst used in the reactor 2 is extracted and regenerated. In this formulation, after being introduced into the vessel 3 and heat-treated in an oxygen-containing gas atmosphere, the heat-treated solid catalyst is returned to the reactor 2.

  In addition, you may employ | adopt not only a fluid bed format but a moving bed system, for example. The moving bed method is to supply raw material gas containing cyclohexanone oxime to the reactor, and while introducing the solid catalyst and reacting, the solid catalyst used in the reactor is extracted and introduced into the regenerator to contain oxygen In this formulation, after heat treatment in a gas atmosphere, the heat-treated solid catalyst is returned to the reactor. In the fluidized bed type and moving bed type, the solid catalyst used in the reactor is extracted, introduced into the regenerator, heat-treated in an oxygen-containing gas atmosphere, and then the heat-treated solid catalyst is returned to the reactor. Is common.

  The raw material cyclohexanone oxime reacts with the catalyst layer in a gaseous state. The lower alcohol may be previously mixed with cyclohexanone oxime in a gaseous state. Alternatively, the lower alcohol and cyclohexanone oxime may be separately supplied to the reactor. In the case of fluidized bed reaction, cyclohexanone oxime and lower alcohol do not necessarily have to be mixed in advance and can be supplied separately. Further, the lower alcohol can be divided and added.

  The amount of the lower alcohol coexisting in the reaction system is usually 0.1 to 20 times by weight with respect to cyclohexanone oxime. Preferably 10 times or less is good, More preferably, the range of 0.3-8 times is good.

In the reaction system, a vapor of a compound inert to the reaction such as benzene, cyclohexane, toluene or the like, or an inert gas such as nitrogen or carbon dioxide can coexist as a diluent gas. The reaction temperature of the present invention is usually in the range of 250 ° C to 500 ° C. If the temperature is less than 250 ° C., the reaction rate is not sufficient, and the selectivity for ε-caprolactam tends to decrease. On the other hand, if the temperature exceeds 500 ° C., the thermal decomposition of cyclohexanone oxime cannot be ignored, and the selectivity of ε-caprolactam tends to decrease. A particularly preferable temperature range is 300 ° C to 450 ° C, and a most preferable temperature range is 300 ° C to 400 ° C. The space velocity of the raw material cyclohexanone oxime is WHSV = 0.1 to 40 hr ⁻¹ (that is, cyclohexanone oxime supply rate per kg of catalyst is 0.1 to 40 kg / hr). Preferably it is 0.2-20 hr < ^-1 >, More preferably, it is chosen from the range of 0.5-10 hr < ^-1 >. Separation of ε-caprolactam from the reaction mixture can be carried out by a usual method. For example, the reaction product gas can be cooled and condensed, and then ε-caprolactam purified by extraction, distillation or crystallization can be obtained.

  The reaction gas discharge part 22 is connected to the upper part of the reaction vessel 20. A reaction gas containing ε-caprolactam generated in the reactor 2 is discharged by the reaction gas discharge unit 22. The reaction gas containing ε-caprolactam discharged from the reaction gas discharge unit 22 is then introduced into an apparatus (not shown) in the next process.

  A multistage cyclone may be provided inside the reaction vessel 20. Thereby, it is possible to prevent a part of the solid catalyst forming the powder layer 10 from being transported to the reaction gas during the production of ε-caprolactam and discharged to the outside of the reaction vessel 20 together with the reaction gas. .

  The pressure control valve 23 is provided in a part of the reaction gas discharge unit 22. The pressure control valve 23 is connected to the opening degree control unit 61. The opening degree of the pressure control valve 23 is adjusted by the control signal of the opening degree control unit 61. Thereby, the pressure inside the reaction vessel 20 is adjusted. For example, the opening degree control unit 61 controls the opening degree of the pressure control valve 23 so that the difference between the pressure in the regenerator 3 and the pressure in the reactor 2 is constant.

  The arrangement position of the pressure regulating valve 23 is not limited to this. For example, the pressure regulating valve 23 may be provided after passing through a plurality of devices and pipes. Various arrangement positions can be adopted as the arrangement position of the pressure adjusting valve 23 as long as the pressure inside the reaction apparatus 20 can be adjusted.

  The reactor differential pressure gauge 24 is provided in the straight body portion 20 a at the top of the dispersion plate 26. The reactor differential pressure gauge 24 measures the pressure difference between the pressure at the upper portion of the straight barrel portion 20a and the pressure at the lower portion of the straight barrel portion 20a in the reactor 2.

  The reactor thermometer 25 is provided in the straight body 20a. The reactor thermometer 25 measures the temperature in the reactor 2.

  Between the reactor 2 and the regenerator 3, a catalyst transfer mechanism 4 is provided. The catalyst transfer mechanism 4 transfers part of the solid catalyst used in the reactor 2 to the regenerator by sending out air toward the regenerator 3.

  The catalyst transfer mechanism 4 includes a first catalyst transfer pipe 41, a first catalyst transfer pipe valve 43, a first catalyst transfer pipe differential pressure gauge 45, a catalyst storage unit 40, a second catalyst transfer pipe 42, and air. A delivery unit 44.

  One end of the first catalyst transfer pipe 41 is connected to the straight body portion 20 a on the upper side of the dispersion plate 26 of the reaction vessel 20, and the other end is connected to the catalyst housing portion 40. The first catalyst transfer pipe 41 extends obliquely downward from the side wall of the reaction vessel 20.

  In FIG. 1, symbol θ <b> 1 is an angle formed by the extending direction of the first catalyst transfer pipe 41 and the height direction (vertical direction) of the reactor 2. In the present embodiment, the angle θ1 is an angle range that is larger than 0 ° and not larger than 45 °.

  The first catalyst transfer pipe 41 is provided with a first catalyst transfer pipe valve 43. The first catalyst transfer piping valve 43 is connected to a first catalyst transfer piping valve opening degree control unit 63 that controls the opening degree of the first catalyst transfer piping valve 43.

  For example, the first catalyst transfer piping valve opening degree control unit 63 is configured so that the measured value of the reactor differential pressure gauge 24 becomes a constant value in order to keep the height of the powder layer 10 of the reactor 2 at a constant value. The opening degree of the first catalyst transfer piping valve 43 is controlled.

  Here, the “constant value of the measured value of the differential pressure gauge 24 for the reactor” will be described. The differential pressure measured by the reactor differential pressure gauge 24 of the present invention is usually set in the range of 0.3 kPa to 10 kPa, preferably in the range of 1 kPa to 5 kPa.

  As a result, part or all of the first catalyst transfer pipe 41 can always be filled with the solid catalyst, so that the reaction gas existing in the reactor 2 can be contained in the catalyst housing part 40 or in the catalyst housing part 40. It is possible to suppress the air present in the reactor 2 from being mixed into the reactor 2.

  The first catalyst transfer piping valve opening control unit 63 includes at least one of the reactor differential pressure gauge 24, the regenerator differential pressure gauge 34, the regenerated catalyst transfer piping differential pressure gauge 53, and the first catalyst transfer piping differential pressure gauge 45. Control is performed so that the first catalyst transfer piping valve 43 is closed when the measured value is equal to or less than the threshold value.

Here, the “threshold value of the measurement value” will be described.
The threshold value of the measured value of the differential pressure gauge 24 for the reactor of the present invention is usually set in the range of 0.2 kPa to 9 kPa, preferably in the range of 0.5 kPa to 4 kPa.
The threshold value of the measured value of the regenerator differential pressure gauge 34 of the present invention is usually set in the range of 0.2 kPa to 9 kPa, preferably in the range of 0.5 kPa to 5 kPa.
The threshold value of the measured value of the differential pressure gauge 53 for the regenerated catalyst transfer pipe of the present invention is usually set in the range of 0.2 kPa to 20 kPa, preferably in the range of 0.5 kPa to 10 kPa.
The threshold value of the measured value of the differential pressure gauge 45 for the first catalyst transfer pipe of the present invention is usually set in the range of 2 kPa to 30 kPa, preferably in the range of 5 kPa to 20 kPa.

  Thereby, even if the amount of the solid catalyst that fills the first catalyst transfer pipe 41 is insufficient, the reaction gas existing in the reactor 2 exists in the catalyst storage unit 40 or in the catalyst storage unit 40. It is possible to block the air to be mixed into the reactor 2.

  Note that the first catalyst transfer piping valve opening control unit 63 is configured such that when the pressure difference between the pressure in the reactor 2 and the pressure in the regenerator 3 becomes equal to or less than a threshold value, the first catalyst transfer piping valve 43 The control may be performed so that is closed.

  Here, “the threshold value of the differential pressure between the pressure in the reactor 2 and the pressure in the regenerator 3” will be described. The threshold value of the differential pressure between the pressure in the reactor 2 and the pressure in the regenerator 3 of the present invention is usually set in the range of 2 kPa to 20 kPa, preferably in the range of 4 kPa to 10 kPa.

  For example, the first catalyst transfer piping valve opening degree control unit 63 performs control so that the first catalyst transfer piping valve 43 is closed when the pressure in the reactor 2 becomes larger than the pressure in the regenerator 3. . As a result, the introduction of the reaction gas existing in the reactor 2 into the regenerator 3 can be blocked.

  Further, the first catalyst transfer pipe valve opening degree control unit 63 closes the first catalyst transfer pipe valve 43 when the temperature in the reactor 2 and the temperature in the regenerator 3 become equal to or higher than the threshold value. You may control. When the temperature in the reactor 2 and the temperature rise in the regenerator 3 are derived from the oxidation and combustion reaction due to the mixing of the reaction gas and the regeneration gas, such control prevents further expansion of the oxidation and combustion reaction. Can do.

  In addition, in order to improve the fluidity of the solid catalyst in the first catalyst transfer pipe 41 and to replace the reaction gas contained in the gap portion of the transferred catalyst, the first catalyst transfer pipe 41 has an inert gas such as nitrogen gas. An inert gas supply pipe 41a for supplying gas is provided. The supply of the inert gas to the first catalyst transfer pipe 41 may be performed by providing a separate inert gas container.

  When the Beckmann rearrangement reaction of cyclohexanone oxime is performed in the presence of a solid catalyst, polymerization of cyclohexanone oxime and ε-caprolactam, etc. as the reaction time elapses (as the total amount of sililohexanone oxime per catalyst unit weight increases) As a result, a so-called coke component (carbonaceous material) gradually adheres to the solid catalyst. Thereby, the catalyst activity of a solid catalyst falls with time. That is, the conversion rate of cyclohexanone oxime gradually decreases.

  A part of the solid catalyst that has been used in the reactor 2 and has reduced catalytic activity is accommodated in the catalyst accommodating portion 40 via the first catalyst transfer pipe 41. Part of the solid catalyst used in the reactor 2 is added to its own weight due to the inclination of the first catalyst transfer pipe 41, and the catalyst storage unit 40 is caused by the suction effect of air supplied from the air delivery unit 44 to the catalyst storage unit 40. To be introduced.

  The air delivery part 44 is disposed below the catalyst housing part 40. The air delivery unit 44 delivers air to the catalyst storage unit 40 and sends out the solid catalyst stored in the catalyst storage unit 40 toward the regenerator 3 via the second catalyst transfer pipe 42.

  The second catalyst transfer pipe 42 has a lower end connected to the upper part of the catalyst housing 40 and an upper end connected to the regenerator 3.

  The solid catalyst sent out by the pressure-feed air from the air delivery unit 44 is introduced into the regenerator 3.

  A plurality of regenerators are provided between the reactor 2 and the regenerator 3 in order to regenerate part of the solid catalyst used in the reactor 2 so that the catalytic activity is reduced. It may be. In the plurality of regenerators, rough regeneration that recovers a certain amount of catalyst activity is performed in stages.

  The regenerator 3 includes a regenerator 30, an air introduction part 31, an exhaust gas discharge part 32, a pressure control valve (second control valve) 33, a regenerator differential pressure gauge 34, and a regenerator thermometer 35. I have. The regenerator 3 heats a part of the solid catalyst used in the reactor 2 and whose catalytic activity has been lowered in an atmosphere of an oxygen-containing gas so as to regenerate the catalyst activity sufficiently. In the regenerator 3, regeneration is performed so that the catalyst activity is sufficiently recovered to be usable as a catalyst in the reactor 2. In the regenerator 3, the coke component adhering to the surface of the solid catalyst is burned, and water and carbon dioxide are discharged as a reaction gas (exhaust gas).

  The regeneration container 30 has a cylindrical straight body portion 30a. The other end of the second catalyst transfer pipe 42 is connected to the straight body portion 30 a, and a part of the solid catalyst used in the reactor 2 is introduced into the regeneration container 30.

  A bottom portion 30b is connected to the lower portion of the straight body portion 30a of the regenerator 3. A dispersion plate 36 in which a large number of pores are dispersed is provided at the boundary between the straight body portion 30a and the bottom portion 30b. On the dispersion plate 36, a powder layer 11 made of solid catalyst powder is provided. Is formed. The powder layer 11 includes a part of the solid catalyst that has been used in the reactor 2 and has reduced catalytic activity and the solid catalyst that has been regenerated by the regenerator 3 and has sufficiently recovered catalytic activity.

  An air introduction part 31 for introducing air is connected to the bottom part 30b. Air is introduced into the regenerator 3 from the bottom 30 b by the air introduction part 31. Air is sprayed to the bottom of the powder layer 11 through a large number of pores formed in the dispersion plate 36. The powder layer 11 is fluidized by a flow of air blown vertically upward from the dispersion plate 36 to become a fluidized bed. The air flows through the inside of the powder layer 11 which has become a fluidized bed, and efficiently burns the coke component on the surface of the solid catalyst.

  The exhaust gas discharge part 32 is connected to the upper part of the regeneration container 30. The exhaust gas generated by the regenerator 3 is exhausted by the exhaust gas discharge unit 32.

  In order to prevent a part of the solid catalyst forming the powder layer 11 from being transported to the exhaust gas and discharged to the outside of the regeneration container 30 together with the exhaust gas, a multistage type is provided inside the regeneration container 30. A cyclone may be provided.

  The pressure control valve 33 is provided in a part of the exhaust gas discharge unit 32. The pressure control valve 33 is connected to the opening degree control unit 62. The opening degree of the pressure control valve 33 is adjusted by a control signal from the opening degree control unit 62. Thereby, the pressure inside the regeneration container 30 is adjusted. For example, the opening degree control unit 62 controls the opening degree of the pressure control valve 33 so that the difference between the pressure in the regenerator 3 and the pressure in the reactor 2 is constant.

  The arrangement position of the pressure adjustment valve 33 is not limited to this. For example, the pressure regulating valve 33 may be provided after passing through a plurality of devices and pipes. Various arrangement positions can be adopted as the arrangement position of the pressure adjusting valve 33 as long as the pressure inside the regeneration container 30 can be adjusted.

  The regenerator differential pressure gauge 34 is provided in the straight body portion 30 a on the upper side of the dispersion plate 36. The regenerator differential pressure gauge 34 measures a differential pressure between the pressure in the upper portion of the straight body portion 30 a and the pressure in the lower portion of the straight body portion 30 a in the regenerator 3.

  The regenerator thermometer 35 is provided in the straight body portion 30a. The regenerator thermometer 35 measures the temperature in the regenerator 3.

  A regenerated catalyst transfer mechanism 5 is provided between the regenerator 3 and the reactor 2. The regenerated catalyst transfer mechanism 5 transfers part of the solid catalyst regenerated in the regenerator 3 to the reactor 2. The regenerated catalyst transfer mechanism 5 is configured such that a part of the solid catalyst regenerated in the regenerator 3 moves to the reactor 2 by its own weight.

  The regenerated catalyst transfer mechanism 5 includes a regenerated catalyst transfer pipe 51, a regenerated catalyst transfer pipe valve 52, and a regenerated catalyst transfer pipe differential pressure gauge 53.

  One end of the regenerated catalyst transfer pipe 51 is connected to the powder layer 11 of the straight body part 30 a of the regenerator 3, and the other end is connected to the powder layer 10 of the straight body part 20 a of the reactor 2. The regeneration catalyst transfer pipe 51 extends obliquely downward from the side wall of the regeneration container 30.

  In FIG. 1, symbol θ <b> 2 is an angle formed by the extending direction of the regenerated catalyst transfer pipe 51 and the height direction (vertical direction) of the regenerator 3. In the present embodiment, the angle θ2 is an angle range that is larger than 0 ° and not larger than 45 °.

  A part of the solid catalyst regenerated by the regenerator 3 is accommodated in the reactor 2 via the regenerated catalyst transfer pipe 51. Part of the solid catalyst regenerated by the regenerator 3 is introduced into the reactor 2 by its own weight due to the inclination of the regenerated catalyst transfer pipe 51.

  The regenerated catalyst transfer pipe 51 is provided with a regenerated catalyst transfer pipe valve 52. The regenerated catalyst transfer piping valve 52 is connected to a regenerated catalyst transfer piping valve opening degree control unit 64 that controls the opening degree of the regenerated catalyst transfer piping valve 52.

  The regenerative catalyst transfer pipe differential pressure gauge 53 measures the differential pressure between the pressure on the regenerator 3 side and the pressure on the reactor 2 side in the regenerated catalyst transfer pipe 51. It is determined that a powder seal is formed.

  For example, the regenerative catalyst transfer piping valve opening degree control unit 64 regenerates the measured value of the differential pressure gauge 24 for the reactor to a constant value in order to keep the height of the powder layer 10 of the reactor 2 at a constant value. The opening degree of the catalyst transfer piping valve 52 is controlled.

  Here, the “constant value of the measured value of the differential pressure gauge 24 for the reactor” will be described. The differential pressure measured by the reactor differential pressure gauge 24 of the present invention is usually set in the range of 0.3 kPa to 10 kPa, preferably in the range of 1 kPa to 5 kPa.

  Thereby, a part or all of the regenerated catalyst transfer pipe 51 can be always filled with the solid catalyst, so that the reaction gas existing in the reactor 2 exists in the regenerator 3 or in the regenerator 3. Mixing of the regeneration gas into the reactor 2 is suppressed.

  The regenerative catalyst transfer pipe valve opening degree control unit 64 measures at least one of the reactor differential pressure gauge 24, the regenerator differential pressure gauge 34, the regenerated catalyst transfer pipe differential pressure gauge 53, and the first catalyst transfer pipe differential pressure gauge 45. Control is performed so that the regenerated catalyst transfer piping valve 52 is closed when the value falls below the threshold value.

Here, the “threshold value of the measurement value” will be described.
The threshold value of the measured value of the differential pressure gauge 24 for the reactor of the present invention is usually set in the range of 0.2 kPa to 9 kPa, preferably in the range of 0.5 kPa to 4 kPa.
The threshold value of the measured value of the regenerator differential pressure gauge 34 of the present invention is usually set in the range of 0.2 kPa to 9 kPa, preferably in the range of 0.5 kPa to 5 kPa.
The threshold value of the measured value of the differential pressure gauge 53 for the regenerated catalyst transfer pipe of the present invention is usually set in the range of 0.2 kPa to 20 kPa, preferably in the range of 0.5 kPa to 10 kPa.
The threshold value of the measured value of the differential pressure gauge 45 for the first catalyst transfer pipe of the present invention is usually set in the range of 2 kPa to 30 kPa, preferably in the range of 5 kPa to 20 kPa.

  Thereby, even when the amount of the solid catalyst filling the regenerated catalyst transfer pipe 51 is insufficient, the reaction gas present in the reactor 2 is present in the regenerator 3 or the regenerated gas present in the regenerator 3. Can be prevented from being mixed into the reactor 2.

  Further, in order to improve the fluidity of the solid catalyst in the regenerated catalyst transfer pipe 51 and to replace the regenerated gas contained in the gap of the transferred catalyst, the regenerated catalyst transfer pipe 51 is filled with an inert gas such as nitrogen gas. An inert gas supply pipe 51a to be supplied is provided. The supply of the inert gas to the regenerated catalyst transfer pipe 51 may be performed by providing a separate inert gas container.

  In the reaction apparatus 1 of the present embodiment, when the positions of the upper surfaces of the powder layer 10 and the powder layer 11 are compared, the position of the upper surface of the powder layer 11 is higher than the position of the upper surface of the powder layer 10. ing. Therefore, the movement of the solid catalyst from the regenerator 3 to the reactor 2 can be performed only by the weight of the solid catalyst.

  For example, when the arrangement relationship between the reactor 2 and the regenerator 3 is reversed from that of the present embodiment, the position of the upper surface of the powder layer 10 becomes higher than the position of the upper surface of the powder layer 11. The movement of the solid catalyst to the reactor 2 cannot be performed only by its own weight. Therefore, a pressure feeding means such as the air delivery unit 44 is required. The use of air as the pressure-feeding medium is advantageous in terms of cost, but when the air as the pressure-feeding medium flows into the reactor 2, rapid oxidation and combustion reaction of the reaction gas occurs in the reactor 2, and at that time Equipment may be damaged by the amount of heat generated. Although it is conceivable to use an inert gas as a pumping medium instead of air, it is uneconomical and may impede the effectiveness of a chemical reaction. When the solid particles are transferred from the reactor 2 to the regenerator 3 by the pressurized air as in the present embodiment, since the air is originally used as a combustion gas in the regenerator 3, it is performed in the regenerator 3. There is no significant effect on the playback process.

In the present specification, the “position of the upper surface of the powder layer” is defined as follows. The powder layer refers to a dense layer containing a solid catalyst that is placed in a fluid state by a raw material gas or air. When the density distribution of the solid catalyst is measured using the solid catalyst layer density (kg / m ³ ) as the horizontal axis and the vertical height from the dispersion plate as the vertical axis, the solid catalyst density rises upward at a certain height. If the curve is drawn and becomes higher than that, an S-shaped curve that draws a convex curve downward is obtained. The position where the tangent at the inflection point of the S-shaped curve intersects the vertical axis is the position of the upper surface of the powder layer.

  The pressure controller 6 includes an opening controller 61, an opening controller 62, a pressure control valve 23, and a pressure control valve 33. The pressure controller 6 controls at least one of the pressure in the reactor 2 and the pressure in the regenerator 3 so that the pressure in the regenerator 3 becomes larger than the pressure in the reactor 2.

  For example, at least one opening degree control part among the opening degree control part 61 and the opening degree control part 62 is controlled by the control of the pressure control part 6. As a result, the opening degree of at least one of the pressure control valve 23 and the pressure control valve 33 is controlled. Thereby, the pressure in the regenerator 3 is adjusted to be larger than the pressure in the reactor 2.

  The pressure difference between the pressure in the regenerator 3 and the pressure in the reactor 2 is controlled to be constant.

  Here, the “constant value of the pressure difference between the pressure in the regenerator 3 and the pressure in the reactor 2” will be described. The constant value of the pressure difference between the pressure in the regenerator 3 and the pressure in the reactor 2 of the present invention is usually set in the range of 2 kPa to 20 kPa, preferably in the range of 4 kPa to 10 kPa. Moreover, the pressure difference between the pressure in the regenerator 3 and the pressure in the reactor 2 is usually set to a value higher than the threshold value.

  For example, the first pressure gauge 71 is provided in the reactor 2 and the second pressure gauge 72 is provided in the regenerator 3. Next, a differential pressure between the pressure in the reactor 2 and the pressure in the regenerator 3 is obtained by the first pressure gauge 71 and the second pressure gauge 72 by the differential pressure gauge 7. Then, the control valve is adjusted so that the differential pressure becomes constant.

  The regenerative catalyst transfer pipe valve opening degree control unit 64 closes the regenerated catalyst transfer pipe valve 52 when the differential pressure between the pressure in the reactor 2 and the pressure in the regenerator 3 becomes a threshold value or less. Take control.

  Here, “the threshold value of the differential pressure between the pressure in the reactor 2 and the pressure in the regenerator 3” will be described. The threshold value of the differential pressure between the pressure in the reactor 2 and the pressure in the regenerator 3 of the present invention is usually set in the range of 2 kPa to 20 kPa, preferably in the range of 4 kPa to 10 kPa.

  For example, the regeneration catalyst transfer piping valve opening degree control unit 64 performs control so that the regeneration catalyst transfer piping valve 52 is closed when the pressure in the reactor 2 becomes larger than the pressure in the regenerator 3. As a result, the introduction of the reaction gas existing in the reactor 2 into the regenerator 3 can be blocked.

  The regenerative catalyst transfer pipe valve opening degree control unit 64 controls the regenerated catalyst transfer pipe valve 52 to close when the temperature in the reactor 2 and the temperature in the regenerator 3 exceed a threshold value. May be performed. When the temperature in the reactor 2 and the temperature rise in the regenerator 3 are derived from the oxidation and combustion reaction due to the mixing of the reaction gas and the regeneration gas, such control prevents further expansion of the oxidation and combustion reaction. Can do.

In the reaction apparatus 1 of the present embodiment, the solid catalyst is circulated between the reactor 2 and the regenerator 3.
Hereinafter, although an example is given and demonstrated about a mode that a solid catalyst is circulated by operation | movement of the reaction apparatus 1, it is not limited to this.

  First, the opening degree of the first catalyst transfer pipe valve 43 is adjusted by the control signal of the first catalyst transfer pipe valve opening degree control unit 63, and as a result, the solid used in the reactor 2 and having reduced catalyst activity. A part of the catalyst flows toward the catalyst housing 40 via the first catalyst transfer pipe 41 due to the suction effect of the air supplied from the air delivery unit 44 to the catalyst housing 40 in addition to its own weight. Thereby, a part of the solid catalyst whose catalytic activity is lowered is accommodated in the catalyst accommodating portion 40. The solid catalyst housed in the catalyst housing section 40 is introduced into the regenerator 3 via the second catalyst transfer pipe 42 by the pressurized air supplied to the air delivery section 44.

  A part of the solid catalyst regenerated in the regenerator 3 is regenerated catalyst transfer piping valve by a control signal of the regenerative catalyst transfer piping valve opening degree control unit 64 to which the measured value of the differential pressure gauge 24 of the reactor 2 is transmitted. The opening of 52 is adjusted. Thereby, a part of the solid catalyst regenerated by the regenerator 3 flows toward the reactor 2 through the regenerated catalyst transfer pipe 51 by its own weight. As a result, a part of the solid catalyst whose catalytic activity has been sufficiently recovered is introduced into the reactor 2.

  In order to improve the fluidity of the solid catalyst in the regenerated catalyst transfer mechanism 5 and to replace the reaction gas contained in the gap portion of the transferred catalyst, preferably, the first catalyst transfer pipe 41 and the regenerated catalyst transfer pipe 51 are used. An inert gas such as nitrogen gas is supplied to the tank. Further, the catalyst transfer piping valve 43 and the regenerated catalyst transfer piping valve 52 may be opened and closed intermittently, and the flow rate of the solid catalyst to be transferred may be adjusted by the number of opening and closing of the valve within a predetermined time.

  As described above, the solid catalyst is circulated between the reactor 2 and the regenerator 3.

  According to the reaction device 1 of the present embodiment, the pressure in the regenerator 3 is controlled by the control signal of the pressure control unit 6 so as to be larger than the pressure in the reactor 2. For this reason, the introduction of the reaction gas present in the reactor 2 into the regenerator 3 is suppressed. Therefore, rapid oxidation and combustion reaction due to mixing of the reaction gas present in the reactor 2 and the regeneration gas present in the regenerator 3 can be suppressed.

  Further, since the pressure control unit 6 includes the control valves 23 and 33 and the opening control units 61 and 62, the pressure in the container 2 and the regenerator 3 are controlled by the control signals of the opening control units 61 and 62. The internal pressure is controlled respectively. For this reason, the freedom degree at the time of controlling a pressure spreads so that the pressure in the regenerator 3 may become larger than the pressure in the reactor 2.

  In addition, since the opening degree control unit 61 controls the opening degree of at least one of the control valves 23 and 33 so that the difference between the pressure in the regenerator 3 and the pressure in the reactor 2 is constant, It is stably suppressed that the reaction gas present in 2 is introduced into the regenerator 3. Therefore, rapid oxidation and combustion reaction due to mixing of the reaction gas present in the reactor 2 and the regeneration gas present in the regenerator 3 can be suppressed.

Further, in the present embodiment in which a part of the solid catalyst used in the reactor 2 is transferred to the regenerator 3 by the pressurized air, the solid catalyst is regenerated in the regenerator 3 in an atmosphere containing an oxygen-containing gas. Therefore, even if a part of the solid catalyst is transferred to the regenerator 3 and the pressurized air is introduced into the regenerator 3, the compressed air is used as the oxygen-containing gas in the regenerator 3.
Here, a configuration in which a part of the solid catalyst regenerated by the regenerator 3 is transferred to the reactor 2 by pressurized air is considered. In this configuration, when a part of the solid catalyst is transferred to the reactor 2 and the pressurized air is introduced into the reactor 2, the pressurized air and the reaction gas in the reactor 2 are mixed. As a result, rapid oxidation and combustion reaction of the reaction gas occurs due to the mixing of the reaction gas and the pressurized air, and the device may be damaged by the amount of heat generated at that time.
On the other hand, in the present embodiment, a configuration is adopted in which a part of the solid catalyst used in the reactor 2 is transferred to the regenerator 3 by the pressurized air. The reaction gas is not mixed. Further, the reaction gas present in the reactor 2 and the regeneration gas present in the regenerator 3 are not mixed in the process in which the solid catalyst used in the reactor 2 is introduced into the regenerator 3. Therefore, rapid oxidation and combustion reaction due to mixing of the reaction gas and the regeneration gas can be suppressed.
In addition, since the pressurized air is used as a means for transferring the solid catalyst toward the regenerator, the transfer cost of the solid medium can be reduced as compared with the case where a medium other than air is used.
Further, the regenerated catalyst transfer mechanism 5 is configured such that a part of the solid catalyst regenerated by the regenerator 3 moves to the reactor 2 by its own weight. Therefore, it is not necessary to separately provide a means for transferring the regenerated solid catalyst to the reactor 2. Therefore, the reaction apparatus 1 can be simplified.

  Further, the first catalyst transfer pipe 41 extends obliquely downward from the side wall of the reactor 2, and supplies pressurized air from the air delivery part 44 to the catalyst housing part 40, so that it was used in the reactor 2. Part of the solid catalyst moves to the catalyst housing 40 due to the suction effect of air supplied from the air delivery unit 44 to the catalyst housing 40 in addition to its own weight. Therefore, the means for transferring the solid catalyst used in the reactor 2 to the catalyst housing 40 can be realized with a simple configuration.

Further, since the angle θ1 formed between the extending direction of the first catalyst transfer pipe 41 and the vertical direction is an angle range larger than 0 ° and not larger than 45 °, the solid catalyst used in the reactor 2 is stored in the catalyst housing portion. The flow rate when transferring to 40 can be stabilized.
On the other hand, if the angle θ1 formed is larger than 45 °, the inclination of the first catalyst transfer pipe 41 becomes gentle, and it is difficult to stably transfer the solid catalyst used in the reactor 2 to the catalyst storage unit 40. Become.

  Further, since the regenerated catalyst transfer pipe 51 is provided with the regenerated catalyst transfer pipe valve 52, the regenerated catalyst transfer pipe 51 is controlled by controlling the valve opening degree or the opening / closing operation of the regenerated catalyst transfer pipe valve 52. The flow rate of the solid catalyst in can be adjusted.

  Further, since the regenerated catalyst transfer pipe 51 extends obliquely downward from the side wall of the regenerator 3, a part of the solid catalyst regenerated by the regenerator 3 moves to the reactor 2 by its own weight. Therefore, means for transferring the solid catalyst regenerated in the regenerator 3 to the reactor 2 can be realized with a simple configuration.

Further, since the angle θ2 formed between the extending direction of the regenerated catalyst transfer pipe 51 and the vertical direction is an angle range larger than 0 ° and 45 ° or less, a part of the solid catalyst regenerated in the regenerator 3 is reacted. It is possible to stabilize the flow rate when transported to the vessel 2.
On the other hand, when the formed angle θ2 is larger than 45 °, the regeneration catalyst transfer pipe 51 is inclined gently, and it is difficult to stably transfer a part of the solid catalyst regenerated by the regenerator 3 to the reactor 2. It becomes.

  In this embodiment, a raw material gas containing cyclohexanone oxime is used as the raw material gas. However, the present invention is not limited to this, and a raw material gas containing various materials that can cause the problem of the present invention can be used. .

  In the reactor of the present embodiment, ε-caprolactam is generated by Beckmann rearrangement reaction of cyclohexanone oxime in the presence of a solid catalyst and a lower alcohol, but is not limited thereto. For example, ε-caprolactam may be produced in an environment that does not contain a lower alcohol. That is, it is sufficient that ε-caprolactam is generated at least in the presence of a solid catalyst.

  The present invention can also be applied to a method for producing ε-caprolactam in which ε-caprolactam is produced from cyclohexanone oxime by a gas phase reaction using a solid catalyst. For example, the above-described reaction apparatus 1 of the present invention can be used as a reaction apparatus that performs a gas phase reaction using a solid catalyst.

  The preferred embodiments of the present invention have been described above with reference to the accompanying drawings, but it goes without saying that the present invention is not limited to such examples. Various shapes, combinations, and the like of the constituent members shown in the above-described examples are examples, and various modifications can be made based on design requirements and the like without departing from the gist of the present invention.

  Examples of the present invention will be described below, but the present invention is not limited thereto.

Example 1
The solid catalyst powder having reduced catalytic activity was introduced into the regenerator, and heated air was supplied from the lower part of the regenerator to fluidize the powder while heating the temperature in the regenerator to about 430 ° C. In order to maintain the powder pressure in the regenerator at about 120 mmH ₂ O, the powder was continuously introduced into the regenerator.
On the other hand, the powder regenerated by the regenerator was continuously transferred toward the reactor by the powder pressure difference while adjusting the flow rate with the regenerated catalyst transfer piping valve. In order to prevent the gas supplied to the reactor from flowing into the regenerator and mixing with the gas supplied to the regenerator, the powder pressure in the regenerated catalyst transfer pipe was maintained at about 500 mmH ₂ O. In addition, in order to improve the fluidity of the powder, ₁₀ to 50 L / h of heated N ₂ was supplied to the regenerated catalyst transfer pipe.
A powder of a solid catalyst whose catalytic activity was recovered was introduced into the reactor, and a gas containing an organic solvent heated was supplied from the bottom of the reactor to fluidize the powder in the reactor. Since an exothermic reaction occurred in the reactor, heat was removed by a cooling device, and the temperature in the reactor was maintained at about 379 ° C. The gas composition at the outlet of the reactor was about 60% methanol, about 6% inert gas containing water, and about 34% ε-caprolactam containing reaction byproducts.
A pressure gauge was installed in each of the gas phase part of the regenerator and the gas phase part of the reactor. A control valve for adjusting the gas flow rate was installed in the exhaust gas piping of the regenerator. While obtaining the pressure difference between the pressure in the regenerator and the pressure in the reactor, the opening of the control valve was adjusted so that the pressure difference was constant.
As a result of estimating and evaluating the explosion range (lower limit and upper limit of the magnitude of explosion) of the reactor gas using literature values, the regeneration gas in the reactor may flow into the reactor. It has been confirmed that is relatively safe compared to the case of flowing into the regenerator. Therefore, adjustment was performed with a control valve so that the pressure of the regenerator was larger than the pressure of the reactor (approx. 250 mmH ₂ O pressure).
As a result, the gas mixture of the regeneration gas of the regenerator and the reaction gas of the reactor prevents the target chemical reaction from being hindered, and does not cause rapid oxidation or combustion reaction. The powder could be moved.

DESCRIPTION OF SYMBOLS 1 ... Reaction apparatus, 2 ... Reactor, 3 ... Regenerator, 4 ... Catalyst transfer mechanism, 5 ... Regenerated catalyst transfer mechanism, 6 ... Pressure control part, 23 ... Pressure control valve (1st control valve), 24 ... For reactor Differential pressure gauge, 33 ... Pressure regulating valve (second regulating valve), 34 ... Differential pressure gauge for regenerator, 40 ... Catalyst housing part, 41 ... First catalyst transfer pipe, 42 ... Second catalyst transfer pipe, 43 ... First catalyst transfer Piping valve, 44 ... Air delivery part, 45 ... First catalyst transfer piping differential pressure gauge, 51 ... Regenerated catalyst transfer piping, 52 ... Regenerated catalyst transfer piping valve, 53 ... Regenerated catalyst transfer piping differential pressure gauge, 63 ... No. 1 catalyst transfer piping valve opening degree control unit, 64... Regeneration catalyst transfer piping valve opening degree control unit, .theta.1... Angle formed by extending direction of first catalyst transfer piping and vertical direction, .theta.2. Angle between extension direction and vertical direction

Claims (21)

A fluidized bed type reactor that chemically reacts a raw material gas in the presence of a solid catalyst;
A fluidized bed type regenerator that regenerates a part of the solid catalyst used in the reactor, the catalyst activity of which has been reduced, by heating in a gas-containing gas atmosphere to recover the catalyst activity;
A pressure controller that controls at least one of the pressure in the reactor and the pressure in the regenerator so that the pressure in the regenerator is larger than the pressure in the reactor. Reactor. The pressure controller is
A first control valve provided in the reactor;
A second control valve provided in the regenerator;
The reaction apparatus according to claim 1, further comprising: an opening degree control unit that controls an opening degree of at least one of the first control valve and the second control valve.   The opening control unit controls the opening of at least one of the first control valve and the second control valve so that the difference between the pressure in the regenerator and the pressure in the reactor is constant. The reaction apparatus according to claim 2, wherein: A catalyst transfer mechanism is provided between the reactor and the regenerator to transfer a part of the solid catalyst used in the reactor to the regenerator by sending air toward the regenerator. And
Between the reactor and the regenerator, a regenerated catalyst transfer pipe for returning a part of the solid catalyst regenerated in the regenerator to the reactor is provided,
The regenerated catalyst transfer pipe is configured such that a part of the solid catalyst regenerated in the regenerator moves to the reactor by its own weight. The reactor described.   The reaction apparatus according to claim 4, wherein the regenerated catalyst transfer pipe is provided with a regenerated catalyst transfer pipe valve.   6. The reaction apparatus according to claim 5, further comprising a regenerative catalyst transfer pipe valve opening degree control unit that controls an opening degree of the regenerated catalyst transfer pipe valve.   The reaction apparatus according to any one of claims 4 to 6, wherein the regenerated catalyst transfer pipe extends obliquely downward from a side wall of the regenerator.   The reaction apparatus according to claim 7, wherein an angle formed between the extending direction of the regenerated catalyst transfer pipe and the vertical direction is in an angle range of greater than 0 ° and equal to or less than 45 °. The catalyst transfer mechanism includes:
A first catalyst transfer pipe for extracting a part of the solid catalyst used in the reactor;
A catalyst housing portion for housing the solid catalyst extracted by the first catalyst transfer pipe;
A second catalyst transfer pipe for introducing the solid catalyst accommodated in the catalyst accommodating portion into the regenerator;
An air delivery part for delivering air to the catalyst accommodation part and delivering the solid catalyst accommodated in the catalyst accommodation part toward the regenerator via the second catalyst transfer pipe. The reaction apparatus according to any one of 4 to 8.   The reactor according to claim 9, wherein the first catalyst transfer pipe is provided with a first catalyst transfer pipe valve.   11. The reaction apparatus according to claim 10, further comprising a first catalyst transfer pipe valve opening degree control unit that controls an opening degree of the first catalyst transfer pipe valve.   The reaction apparatus according to any one of claims 9 to 11, wherein the first catalyst transfer pipe extends obliquely downward from a side wall of the reactor.   The reaction apparatus according to claim 12, wherein an angle formed between the extending direction of the first catalyst transfer pipe and the vertical direction is in an angle range of greater than 0 ° and equal to or less than 45 °.   A differential pressure gauge for a reactor that measures a differential pressure in the reactor, a differential pressure gauge for a regenerator that measures a differential pressure in the regenerator, a differential pressure gauge for a regenerated catalyst transfer pipe that measures a differential pressure in the regenerated catalyst transfer pipe, The reaction apparatus according to any one of claims 9 to 13, further comprising a differential pressure gauge for a first catalyst transfer pipe for measuring a differential pressure in the first catalyst transfer pipe.   The opening degree of at least one of the regenerated catalyst transfer piping valve and the first catalyst transfer piping valve is controlled so that the differential pressure measured by the reactor differential pressure gauge becomes a constant value. The reaction apparatus according to claim 14.   Transfer of the regenerated catalyst when at least one measured value of the differential pressure gauge for the reactor, the differential pressure gauge for the regenerator, the differential pressure gauge for the regenerated catalyst transfer pipe, and the differential pressure gauge for the first catalyst transfer pipe falls below a threshold value 15. The reaction apparatus according to claim 14, wherein control is performed so that the piping valve and the first catalyst transfer piping valve are closed.   The regenerative catalyst transfer pipe valve opening control unit controls the regenerated catalyst transfer pipe valve to be closed when a difference between the pressure in the regenerator and the pressure in the reactor becomes a threshold value or less. The reaction apparatus according to claim 6, wherein:   The first catalyst transfer piping valve opening degree control unit closes the first catalyst transfer piping valve when a difference between the pressure in the regenerator and the pressure in the reactor becomes equal to or less than a threshold value. The reaction apparatus according to claim 11, wherein the control is performed.   17. The inert gas is supplied to the regenerated catalyst transfer pipe and the first catalyst transfer pipe, and the gas accompanying the catalyst is replaced with the inert gas. 17. Reactor.   The reactor according to any one of claims 1 to 19, wherein the source gas contains cyclohexanone oxime. A method for producing ε-caprolactam, wherein ε-caprolactam is produced from cyclohexanone oxime by a gas phase reaction using a solid catalyst,
21. A process for producing ε-caprolactam, wherein the reaction apparatus according to any one of claims 1 to 20 is used as a reaction apparatus for performing a gas phase reaction using the solid catalyst.

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