Reaction apparatus and method for producing oxidation reaction products

Abstract

The present invention provides a reaction apparatus capable of selectively producing different types of products. [Solution] A reaction apparatus 1 for producing a product by oxidizing a raw material in a solution containing a raw material and an oxidizing agent, wherein the raw material contains a hydrocarbon or a derivative thereof, and the oxidizing agent contains a chlorine dioxide radical, and comprises a reaction vessel 10 in which a first liquid phase capable of dissolving the product and a second liquid phase containing the raw material and oxidizing agent are formed inside, an irradiation device 12 for irradiating the inside of the reaction vessel 10 with light to oxidize the raw material, a first liquid phase preparation device 30 (product recovery device) for recovering the product generated by the oxidation reaction of the raw material from the first liquid phase, and a second liquid phase preparation device 40 (solvent supply device) capable of supplying fluorescein solvents of different compositions into the reaction vessel 10 as solvents constituting the second liquid phase.

Description

[Technical Field]

[0001] This invention relates to a reaction apparatus for carrying out a chemical reaction with reactants and a technology for producing oxidation reaction products. [Background technology]

[0002] Conventional techniques for inducing chemical reactions with reactants are well known. For example, Patent Document 1 describes a method for producing products at room temperature and pressure through a chemical reaction using two liquid phases.

[0003] The invention described in Patent Document 1 above describes a method for producing oxidation reaction products of a raw material by irradiating a reaction system containing an aqueous phase and an organic phase with light in the presence of a raw material and chlorine dioxide radicals. Patent Document 1 states that when methane is used as the raw material, methanol and formic acid are produced as oxidation reaction products.

[0004] However, conventional technology has not allowed for the selective production of different products using the same reaction apparatus. [Prior art documents] [Patent Documents]

[0005] [Patent Document 1] Patent No. 6080281 [Overview of the project] [Problems that the invention aims to solve]

[0006] This invention was made in view of the above circumstances, and the problem it aims to solve is to provide a reaction apparatus capable of selectively producing different products. [Means for solving the problem]

[0007] The problems that this invention aims to solve are as described above, and the means for solving these problems will now be explained.

[0008] That is, claim 1 is a reaction apparatus that produces a product by oxidizing the raw material in a solution containing the raw material and an oxidizing agent, wherein the raw material is carbonized water The basics The oxidizing agent comprises a chlorine dioxide radical, a reaction vessel having a first liquid phase capable of dissolving the product and a second liquid phase containing the raw materials and the oxidizing agent formed inside, an irradiation device that irradiates the inside of the reaction vessel with light to cause an oxidation reaction of the raw materials, a product recovery device that recovers the product generated by the oxidation reaction of the raw materials from the first liquid phase, and a solvent supply device that can supply fluorescein solvents of different compositions into the reaction vessel as solvents constituting the second liquid phase. The solvent constituting the second liquid phase is C 8 F 13 OH 3 or C 3 F 3 H 2 The fluorescein solvent having the composition of Cl. It is.

[0009] Claim 2, wherein the product includes at least one of formic acid or methanol.

[0012] Claim 3 In this case, the fluorescein solvent having the composition C3F3H2Cl has the structure CF3CH=CHCl.

[0013] Claim 4 In this case, the fluorescein solvent having the composition C3F3H2Cl has the structure CHF2CF=CHCl.

[0014] Claim 5 The process includes a reaction step of irradiating a solution containing raw materials and chlorine dioxide radicals with light, wherein the raw materials are carbonized water. The basics The solution contains an organic phase, the organic phase contains the raw materials and the chlorine dioxide radical, and in the reaction step, the raw materials are oxidized by light irradiation to produce an oxidation reaction product of the raw materials, and the organic phase is C8F 13It contains a fluorinated solvent having a composition of OH3 or C3F3H2Cl.

Advantages of the Invention

[0015] As an effect of the present invention, the following effects are achieved.

[0016] In claim 1, it is possible to produce different products according to the purpose. Furthermore, the production ratio of methanol or formic acid can be improved.

[0017] In claim 2, it is possible to separate formic acid and methanol.

[0020] Claim 3 In it, the production ratio of formic acid can be improved.

[0021] Claim 4 In it, the production ratio of formic acid can be improved.

[0022] Claim 5 In it, it is possible to separate formic acid and methanol.

Brief Description of the Drawings

[0023] [Figure 1] Schematic diagram showing a reaction device according to an embodiment of the present invention. [Figure 2] Block diagram showing the reaction device. [Figure 3] Flowchart showing the processes executed by the reaction device. [Figure 4] Flowchart showing the continuation of the process shown in FIG. 3. [Figure 5] Diagram schematically showing an example of the reaction process. [Figure 6] Table showing the production ratios of methanol and formic acid when each solvent is used as the solvent for the second liquid phase.

Modes for Carrying Out the Invention

[0024] The configuration of the reactor 1 according to one embodiment of the present invention will be described below with reference to Figures 1 and 2.

[0025] Reaction apparatus 1 produces products through a chemical reaction of the raw material gas in a liquid contained in the reaction vessel 10. Specifically, reaction apparatus 1 produces products (oxidation reaction products) by irradiating the liquid containing the raw material gas and chlorine dioxide radicals, which act as an oxidizing agent, with light to oxidize the raw material gas.

[0026] A hydrocarbon or its derivative can be used as the raw material gas. The hydrocarbon may be a saturated hydrocarbon. Saturated hydrocarbons may be, for example, methane, ethane, or cyclohexane. The hydrocarbon may also be a non-aromatic unsaturated hydrocarbon. The hydrocarbon may also be an aromatic hydrocarbon. Aromatic hydrocarbons may be, for example, benzene. In this embodiment, methane is used as the raw material gas.

[0027] The liquids (reaction system) used in the above reaction include a first solution and a second solution, which are two liquids with different specific gravities. The solvent for the first solution can be a solvent capable of dissolving the product, such as water. The solvent for the second solution can be an organic solvent capable of dissolving the source gas, such as a fluorescein solvent. The types of fluorescein solvents will be described later.

[0028] The second solution contains chlorine dioxide radicals. In the reaction system, the first solution contains a source of an oxidizing agent such as chlorine dioxide radicals, and chlorine dioxide radicals are generated in the first solution (first liquid phase). The generated chlorine dioxide radicals can then be extracted from the first solution (first liquid phase) in the second solution (second liquid phase). In this embodiment, sodium chlorite is included as the source of chlorine dioxide radicals.

[0029] Furthermore, the second solution has a higher specific gravity than the first solution. Therefore, as shown in Figure 1, the first solution (first liquid phase) and the second solution (second liquid phase) separate within the reaction vessel 10.

[0030] The reaction apparatus 1 according to this embodiment can produce products by oxidizing a raw material gas in a reaction vessel 10. The reaction apparatus 1 can produce alcohols, carboxylic acids, aldehydes, ketones, percarboxylic acids, and hydroperoxides as products. In this embodiment, the reaction apparatus 1 produces methanol and formic acid as products. A detailed explanation of the chemical reaction in the reaction vessel 10 will be given later. The reaction apparatus 1 comprises a reaction vessel 10, a gas phase preparation device 20, a first liquid phase preparation device 30, a second liquid phase preparation device 40, and a control unit 50.

[0031] The reaction vessel 10 is used to chemically react the raw material gas. The reaction vessel 10 is formed in a substantially cylindrical shape that can accommodate the raw material gas, the first solution, and the second solution inside. The reaction vessel 10 is formed with a relatively large depth (vertical dimension) to facilitate the separation of the first solution and the second solution, as will be described later. The reaction vessel 10 is made of a material that has resistance to solvents and raw material gases.

[0032] As shown in Figure 1, inside the reaction vessel 10 containing the raw material gas, the first solution, and the second solution, the following phases are formed in order from top to bottom: "gas phase," "first liquid phase," and "second liquid phase." The "gas phase" is a phase consisting of a mixture of the raw material gas and other gases (gases evaporated from the liquid phase, air inside the reaction vessel 10, etc.). The "first liquid phase" is the phase (aqueous phase) composed of the first solution. The "second liquid phase" is the phase (solvent phase) composed of the second solution. The reaction vessel 10 is equipped with a stirring device 11 and an irradiation device 12.

[0033] The stirring device 11 stirs the first solution and the second solution in the reaction vessel 10. The stirring device 11 is installed inside the reaction vessel 10. The stirring device 11 is equipped with a propeller or the like that rotates around a rotation axis with its axis oriented vertically. However, the stirring device 11 is not limited to one equipped with a propeller, and various configurations capable of stirring the first solution and the second solution can be adopted. By operating the stirring device 11 and mixing the first solution and the second solution, the contact area between the first solution and the second solution can be increased, thereby promoting the reaction. The mixed first solution and the second solution will separate again after a predetermined time has elapsed since the stirring was stopped.

[0034] In this embodiment, the stirring device 11 is positioned eccentrically with respect to the center of the reaction vessel 10 in a plan view. This makes it easier to thoroughly mix the first solution and the second solution, and also promotes the separation of each liquid phase after stirring stops. That is, when stirring is performed by the stirring device 11, vortices and bubbles are formed inside the reaction vessel 10, thereby improving the stirring effect. Also, if the stirring device 11 is positioned closer to the inner wall of the reaction vessel 10, the liquid phases will separate more easily after stirring stops. Therefore, by positioning the stirring device 11 eccentrically with respect to the center of the reaction vessel 10 in a plan view, and relatively close to the inner wall, the generation of vortices and the like is promoted, improving the stirring effect, and also promoting the separation of each liquid phase after stirring stops.

[0035] In this embodiment, as shown by the dashed line in Figure 1, baffles 11a are provided on the inner wall of the reaction vessel 10 to obstruct the flow of each stirred solution. The baffles 11a are formed in a long plate shape along the vertical direction. Multiple baffles 11a (for example, four) are provided along the circumferential direction of the reaction vessel 10. By obstructing the flow of each solution with the baffles 11a, turbulence (upstream and downstream) is generated during stirring, promoting the generation of vortices and improving the stirring effect. In addition, the baffles 11a can promote the separation of each liquid phase after stirring is stopped.

[0036] The irradiation device 12 irradiates light into the reaction vessel 10. In this embodiment, a photoreaction is carried out by irradiating the first solution and the second solution, which have been stirred in the reaction vessel 10, with light. The irradiation device 12 is equipped with a light source that emits light of the wavelength required for the reaction. LEDs, halogens, etc., can be used as the light source. Various light sources capable of irradiating light of the wavelength required for the reaction can be used as the light source. Although Figure 1 shows an example in which the irradiation device 12 irradiates light from above, the installation position of the irradiation device 12 is not limited to the above position, and various installation positions such as the side or bottom of the reaction vessel 10 can be used.

[0037] The gas phase preparation unit 20 prepares the raw material gas that constitutes the gas phase in the reaction vessel 10. The gas phase preparation unit 20 supplies the raw material gas to the reaction vessel 10 and recovers the raw material gas (gas of the gas phase) from the reaction vessel 10. The gas phase preparation unit 20 also removes impurities and by-products contained in the recovered gas. The gas phase preparation unit 20 is supplied with raw material gas from a source such as a raw material tank. In addition to raw material gas, the gas phase preparation unit 20 can also supply other gases used in the reaction (e.g., air or oxygen).

[0038] As shown in Figure 1, the gas phase preparation device 20 includes a gas phase supply path 21, which is a path for supplying raw material gas into the reaction vessel 10, and a gas phase recovery path 22, which is a path for recovering the raw material gas in the gas phase within the reaction vessel 10. The gas phase supply path 21 is connected to a position in the reaction vessel 10 corresponding to the separated second liquid phase (a position lower than the height of the upper end of the second liquid phase). The gas phase recovery path 22 is connected to a position in the reaction vessel 10 corresponding to the gas phase (a position above the first liquid phase). The gas phase preparation device 20 is equipped with a suitable pump (not shown) for circulating the raw material gas. The gas phase preparation device 20 is also equipped with valves (not shown) that can open and close the gas phase supply path 21 and the gas phase recovery path 22.

[0039] The raw material gas from the gas phase preparation device 20 is supplied to the reaction vessel 10 via the gas phase supply path 21 by the operation of a pump and blown into the second liquid phase (second solution). At this time, bubbles of the raw material gas are formed in the second solution, and the raw material gas dissolves into the second solution. The finer the bubbles, the easier it is for the raw material gas to remain and dissolve in the second solution. For this reason, a mechanism for generating fine bubbles may be provided in the reaction vessel 10 or the like.

[0040] Furthermore, the gas phase in the reaction vessel 10 contains undissolved raw material gas. The gas in the gas phase is recovered into the reaction vessel 10 via the gas phase recovery path 22 by the operation of a pump. The recovered gas is then subjected to the removal of impurities and by-products by the gas phase preparation device 20 and supplied back into the reaction vessel 10. In this embodiment, the raw material gas is recycled.

[0041] The first liquid phase preparation device 30 prepares the first solution that constitutes the first liquid phase in the reaction vessel 10. The first liquid phase preparation device 30 can adjust the volume, concentration, and pH of the first solution. The first liquid phase preparation device 30 can also separate the products contained in the first solution. The first solution is supplied to the first liquid phase preparation device 30 from a predetermined supply source.

[0042] As shown in Figure 1, the first liquid phase preparation apparatus 30 is equipped with a first liquid phase path 31, which is a path through which the first solution can flow. The first liquid phase path 31 is connected to a position in the reaction vessel 10 that corresponds to the separated first liquid phase (a position lower than the height of the upper end of the first liquid phase).

[0043] The first liquid phase preparation device 30 is equipped with a suitable pump (not shown) for circulating the first solution. The first liquid phase preparation device 30 is also equipped with a valve (not shown) that can open and close the first liquid phase path 31, and a sensor (not shown) that can measure the amount of the first solution supplied to the reaction vessel 10.

[0044] By operating the pump of the first liquid phase preparation device 30, the first solution, whose concentration and other properties have been adjusted, can be supplied from the first liquid phase preparation device 30 into the reaction vessel 10. Furthermore, by operating the pump, the first solution from the first liquid phase can be discharged from the reaction vessel 10 to the first liquid phase preparation device 30. The first liquid phase preparation device 30 separates the products contained in the discharged first solution and can discharge these products to a predetermined destination. In the illustrated example, a single first liquid phase path 31 is shown for supplying and discharging the first solution; however, separate paths may be provided for supplying and discharging the first solution.

[0045] The second liquid phase preparation device 40 prepares the second solution that constitutes the second liquid phase in the reaction vessel 10. The second liquid phase preparation device 40 can adjust and regenerate the solvent volume of the second solution. In addition, the second liquid phase preparation device 40 can remove by-products from the second liquid phase (second solution). The second solution is supplied to the second liquid phase preparation device 40 from a predetermined supply source.

[0046] The second liquid phase preparation device 40 can supply fluorescein solvents of different compositions to the reaction vessel 10 as a second solution. For example, the second liquid phase preparation device 40 may be connected to multiple supply sources, each capable of supplying fluorescein solvents of different compositions, and by switching between the supply sources, fluorescein solvents of different compositions can be supplied to the reaction vessel 10. Alternatively, the second liquid phase preparation device 40 may be configured such that the user prepares the fluorescein solvents to be supplied to the second liquid phase preparation device 40, thereby enabling the supply of fluorescein solvents of different compositions to the reaction vessel 10.

[0047] The second liquid phase preparation device 40 can supply a fluorescein solvent having the composition C3F3H2Cl to the reaction vessel 10 as the second solution. The fluorescein solvent having the composition C3F3H2Cl may also have the structure CF3CH=CHCl. ​​Alternatively, the fluorescein solvent having the composition C3F3H2Cl may also have the structure CHF2CF=CHCl. ​​Furthermore, the second liquid phase preparation device 40 can supply C8F as the second solution. 13A fluorescein solvent having an OH3 composition can be supplied to the reaction vessel 10. C8F 13 A fluorescein solvent having an OH3 composition is C7F 13 It may also have the structure of OCH3.

[0048] As shown in Figure 1, the second liquid phase preparation apparatus 40 is equipped with a second liquid phase path 41, which is a path through which the second solution can flow. The second liquid phase path 41 is connected to a position in the reaction vessel 10 that corresponds to the separated second liquid phase (a position lower than the height of the upper end of the second liquid phase).

[0049] The second liquid phase preparation device 40 or the second liquid phase passage 41 is equipped with a suitable pump (not shown) for circulating the second solution. The second liquid phase preparation device 40 is also equipped with a valve (not shown) that can open and close the second liquid phase passage 41, and a sensor (not shown) that can measure the amount of the second solution supplied to the reaction vessel 10.

[0050] By operating the pump of the second liquid phase preparation device 40, the second solution, with the solvent volume and other parameters adjusted, can be supplied from the second liquid phase preparation device 40 into the reaction vessel 10. Furthermore, by operating the pump, the second solution from the second liquid phase can be discharged from the reaction vessel 10 to the second liquid phase preparation device 40. In the illustrated example, a single second liquid phase path 41 is used for supplying and discharging the second solution; however, separate paths may be provided for supplying and discharging the second solution.

[0051] The control unit 50 shown in Figure 2 is capable of processing various types of information. The control unit 50 includes a CPU, memory, and other components. As shown in Figure 2, the control unit 50 is electrically connected to the reaction vessel 10 (stirring device 11 and irradiation device 12), the gas phase preparation device 20, the first liquid phase preparation device 30, and the second liquid phase preparation device 40 of the reaction apparatus 1. The control unit 50 can control the operation of the gas phase preparation device 20, the first liquid phase preparation device 30, and the second liquid phase preparation device 40, as well as the valves and pumps equipped in each of these devices. The control unit 50 can also acquire the measurement results from the sensors equipped in each of the devices of the reaction apparatus 1.

[0052] The operation of Reactor 1 will be described below. Reactor 1 (control unit 50) generates the product by controlling each process shown in the flowcharts in Figures 3 and 4. Reactor 1 can generate the above product at room temperature and atmospheric pressure. At the start of the following control, the inside of the reaction vessel 10 is assumed to be empty and all valves of Reactor 1 are closed.

[0053] First, the control unit 50 executes the "reaction preparation process" shown in steps S101 to S106 of Figure 3. The reaction preparation process is the process of preparing the reaction in the reaction vessel 10 before starting the reaction.

[0054] In the process from step S101 to step S103, the control unit 50 fills the reaction vessel 10 with a preset amount (specified amount) of the first solution. More specifically, the control unit 50 opens the valve of the first liquid phase path 31 and operates the pump of the first liquid phase preparation device 30 to start filling the reaction vessel 10 with the first solution (aqueous solution containing sodium chlorite) (step S101). The control unit 50 also determines whether the specified amount of the first solution has been filled into the reaction vessel 10 based on the measurement results from the sensor of the first liquid phase preparation device 30 (step S102).

[0055] If the control unit 50 determines that the reaction vessel 10 has been filled with a specified amount of the first solution (step S102: YES), it stops the pump of the first liquid phase preparation device 30 and closes the valve of the first liquid phase path 31, thereby stopping the filling of the reaction vessel 10 with the first solution (step S103). After executing the process in step S103, the control unit 50 proceeds to the process in step S104. If the control unit 50 determines that the reaction vessel 10 has not been filled with a specified amount of the first solution (step S102: NO), it proceeds to the process in step S101 (continues filling with the first solution).

[0056] In the process from step S104 to step S106, the control unit 50 fills the reaction vessel 10 with a preset amount (specified amount) of the second solution. More specifically, the control unit 50 opens the valve of the second liquid phase path 41 and operates the pump of the second liquid phase preparation device 40 to start filling the reaction vessel 10 with the second solution (fluorescein solvent) (step S104). The control unit 50 also determines whether the specified amount of the second solution has been filled into the reaction vessel 10 based on the measurement results from the sensor of the second liquid phase preparation device 40 (step S105).

[0057] If the control unit 50 determines that the reaction vessel 10 has been filled with a specified amount of the second solution (step S105: YES), it stops the pump of the second liquid phase preparation device 40 and closes the valve of the second liquid phase path 41, thereby stopping the filling of the reaction vessel 10 with the second solution (step S106). After executing the process in step S106, the control unit 50 proceeds to the process in step S107. If the control unit 50 determines that the reaction vessel 10 has not been filled with a specified amount of the second solution (step S105: NO), it proceeds to the process in step S104 (continues filling with the second solution).

[0058] As a result of performing the above reaction preparation steps, a first liquid phase and a second liquid phase are formed in the reaction vessel 10.

[0059] Next, the control unit 50 executes the "reaction process" shown in steps S107 to S110 of Figure 3. The reaction process is a process in which a chemical reaction is carried out in the reaction vessel 10 using the raw material gas, the first solution, and the second solution.

[0060] In the process from step S107 to step S109, the control unit 50 operates each device used in the chemical reaction. More specifically, the control unit 50 operates the stirring device 11 of the reaction vessel 10 to start stirring the first solution and the second solution in the reaction vessel 10 (step S107). The control unit 50 also opens the valves of the gas phase preparation device 20 (gas phase supply path 21 and gas phase recovery path 22) and operates the pump of the gas phase preparation device 20 to start supplying the raw material gas (methane gas) into the reaction vessel 10 (step S108). The control unit 50 also operates the gas phase preparation device 20 to prepare the raw material gas and to recycle the raw material gas. The control unit 50 also operates the irradiation device 12 of the reaction vessel 10 to start irradiating the reaction vessel 10 with light (step S109). After executing the process in step S109, the control unit 50 proceeds to the process in step S110.

[0061] In step S110, the control unit 50 determines whether a specified time has elapsed. The specified time can be the time (period) in which the chemical reaction in the reaction vessel 10 is estimated to have progressed sufficiently. The specified time can be set based on the amounts of the first solution and the second solution filled in the reaction preparation step. If the control unit 50 determines that the specified time has elapsed (step S110: YES), it proceeds to step S111. On the other hand, if the control unit 50 determines that the specified time has not elapsed (step S110: NO), it proceeds to step S119 (continues light irradiation, etc.).

[0062] By executing the above reaction process, a chemical reaction using a raw material gas, a first solution, and a second solution is carried out in the reaction vessel 10. More specifically, in the reaction process, the raw material gas is blown into the first solution and the second solution stirred in the reaction vessel 10. As a result, chlorine dioxide (chlorine dioxide gas) generated from the raw material gas (methane gas) and the first solution, and oxygen in the reaction vessel 10 are dissolved in the second solution (fluorinated solvent), which is the solvent. In this state, by irradiating light from the irradiation device 12, a reaction that converts methane, which is the raw material gas, into methanol and formic acid occurs in the reaction vessel 10. The product generated in the reaction vessel 10 does not dissolve in the second solution and moves to the first liquid phase after liquid phase separation.

[0063] FIG. 5 schematically shows an example of the reaction process for generating alcohol. As shown in FIG. 5, chlorite ions (ClO2 - ) in the first liquid phase (aqueous phase) react with an acid to generate chlorine dioxide radicals (ClO2 · ). ClO2 · dissolves in the second liquid phase (organic phase). Next, the second liquid phase (organic phase) containing chlorine dioxide radicals (ClO2 · ) is irradiated with light to give light energy hν (h is Planck's constant, ν is the frequency of light), so that the chlorine dioxide radicals (ClO2 · ) in the second liquid phase (organic phase) decompose to generate chlorine radicals (Cl · ) and oxygen molecules (O2). As a result, the raw material (RH) in the second liquid phase (organic phase) is oxidized, and an alcohol (R-OH), which is an oxidation reaction product, is generated.

[0064] Next, the control unit 50 executes the "reaction field regeneration process" shown from step S111 to step S117 in FIG. 4. The reaction field regeneration process is a process of recovering the product generated in the reaction vessel 10 and preparing each liquid phase.

[0065] In the processes from step S111 to step S114, the control unit 50 stops each device that was operating in the reaction process and waits for a predetermined time. More specifically, the control unit 50 stops the irradiation of light by the irradiation device 12 (step S111). The control unit 50 also closes the valve of the gas phase preparation device 20 and stops the pump to stop the supply of raw material gas into the reaction vessel 10 (step S112). The control unit 50 also stops the stirring by the stirring device 11 (step S113) and waits in this state for a predetermined time (step S114). The predetermined time can be the time it is estimated that the first liquid phase and the second liquid phase mixed by stirring will separate. After executing the process in step S114, the control unit 50 proceeds to the process in step S115.

[0066] In step S115, the control unit 50 determines whether the first liquid phase and the second liquid phase have separated. The control unit 50 makes this determination based on the measurement results of a sensor (not shown), such as an optical sensor, which is provided in the reaction vessel 10 and capable of measuring the separation state of the liquid phases. If the control unit 50 determines that each liquid phase has separated (step S115: YES), it proceeds to step S116. On the other hand, if the control unit 50 determines that each liquid phase has not separated (step S115: NO), it proceeds to step S114 (and waits for a predetermined time).

[0067] In the example described above, both the process of waiting for a predetermined time to separate each liquid phase (step S114) and the process of determining whether or not each liquid phase has separated (step S115) were performed, but the system is not limited to the above configuration. For example, only one of the above processes may be performed.

[0068] In steps S116 and S117, the control unit 50 operates the first liquid phase preparation device 30 and the second liquid phase preparation device 40 to recover the product and prepare each liquid phase. More specifically, the control unit 50 operates the first liquid phase preparation device 30 to extract a portion of the first solution of the first liquid phase, and then prepares the extracted first solution (adjusting the concentration of chlorine dioxide, pH, etc.) and supplies it into the reaction vessel 10 (step S116). In this way, when the first liquid phase preparation device 30 is operated, the first solution is circulated between the first liquid phase preparation device 30 and the reaction vessel 10. The first liquid phase preparation device 30 also extracts the product (methanol) from the extracted first solution. The extracted product is discharged to an appropriate destination (not shown).

[0069] Furthermore, the control unit 50 operates the second liquid phase preparation device 40 to extract a portion of the second solution from the second liquid phase, and prepares the extracted second solution (adjusting the amount of solvent, etc.) before supplying it to the reaction vessel 10 (step S117). In this way, when the second liquid phase preparation device 40 is operated, the second solution is circulated between the second liquid phase preparation device 40 and the reaction vessel 10. The second liquid phase preparation device 40 also recovers by-products (e.g., fixed matter, etc.) contained in the extracted second solution. The recovered by-products are discharged to an appropriate destination (not shown). After executing the process in step S117, the control unit 50 proceeds to the process in step S118.

[0070] By performing the reaction field regeneration process described above, the first and second liquid phases inside the reaction vessel 10 are regenerated to a state where the reaction process can be carried out again. The control unit 50 also counts the number of times the reaction field regeneration process and the reaction process have been executed since the start of the control.

[0071] In step S118, the control unit 50 determines whether the number of times the reaction field regeneration process (reaction process) has been executed is the specified number of cycles. The specified number of cycles is set in advance. If the control unit 50 determines that the number of times the reaction field regeneration process has been executed is the specified number of cycles, it terminates the process of the reactor 1. On the other hand, if the control unit 50 determines that the number of times the reaction field regeneration process has been executed is not the specified number of cycles, it proceeds to step S107 and executes the reaction process again.

[0072] By implementing the control described above, the reaction apparatus 1 can continuously produce products through a chemical reaction using two liquid phases. Specifically, by circulating the raw material gas, first solution, and second solution using the gas phase preparation device 20, the first liquid phase preparation device 30, and the second liquid phase preparation device 40, products can be continuously produced without having to discharge all of the solutions in the reaction vessel 10. This allows for more efficient product production compared to, for example, a batch-type system.

[0073] The control configuration described above is merely an example, and the content of each process can be modified as appropriate. For example, the above example shows a configuration in which the reaction process and the regeneration process of the reaction field are repeated until a predetermined number of cycles are reached (step S118), but the system is not limited to this configuration. For example, a sensor capable of measuring the concentration of the product generated in the reaction process is provided in the reaction vessel 10, and when the measurement value of the sensor exceeds a predetermined threshold, the reaction process is terminated and the first liquid phase preparation device 30 is activated to recover the product.

[0074] Here, in step S104, the second liquid phase preparation device 40 can supply fluorescein solvents of different compositions to the reaction vessel 10 as the second solution, as described above. The second liquid phase preparation device 40 can supply fluorescein solvents having the composition C3F3H2Cl to the reaction vessel 10 as the second solution (solvent). Alternatively, the second liquid phase preparation device 40 can supply C8F 13 A fluorescein solvent having an OH3 composition can be supplied to the reaction vessel 10.

[0075] By supplying a fluorescein solvent having the composition C3F3H2Cl (CF3CH=CHCl, or CHF2CF=CHCl) as a second solution to the reaction vessel 10, the formic acid production ratio (the ratio of formic acid production to the total amount of product produced) can be improved. Specifically, as shown in Figure 6, as the second solution, C6F 14 When using a solvent with the composition (current solvent), the methanol production ratio is 24.7% and the formic acid production ratio is 75.3%. However, when solvent A, which has the composition C3F3H2Cl(CF3CH=CHCl), is used as the second solution, the methanol production ratio can be reduced to 0% and the formic acid production ratio to 100%. Furthermore, by supplying solvent B, which has the composition C3F3H2Cl(CHF2CF=CHCl), to the reaction vessel 10 as the second solution, the methanol production ratio can be reduced to 1.8% and the formic acid production ratio to 98.2%.

[0076] On the other hand, as the second solution, C8F 13 OH3(C7F 13 By using a fluorescein solvent having the composition OCH3, the methanol production ratio (the ratio of methanol production to the total amount of product produced) can be improved. Specifically, as shown in Figure 6, C8F is used as the second solution. 13 OH3(C7F 13 By using solvent C having the composition OCH3, the methanol production ratio can be increased to 77.7% and the formic acid production ratio to 22.3%.

[0077] In this way, by changing the fluorescein solvent of the second solution, the product can be selectively prepared according to the purpose. For example, if you want to improve the production ratio of formic acid, you can use a fluorescein solvent with the composition C3F3H2Cl as the second solution. On the other hand, if you want to improve the production ratio of methanol, you can use C8F 13 A fluorescein solvent having an OH3 composition can be used.

[0078] As described above, the reaction apparatus 1 according to this embodiment is A reaction apparatus 1 that produces a product by oxidizing the raw materials in a solution containing raw materials and an oxidizing agent, The raw material comprises a hydrocarbon or a derivative of the hydrocarbon. The oxidizing agent contains chlorine dioxide radicals, A reaction vessel 10 having a first liquid phase in which the product can be dissolved and a second liquid phase containing the raw materials and the oxidizing agent formed inside, An irradiation device 12 irradiates the inside of the reaction vessel 10 with light to cause the raw materials to undergo an oxidation reaction, A first liquid phase preparation device 30 (product recovery device) recovers the product generated by the oxidation reaction of the raw materials from the first liquid phase, The second liquid phase preparation device 40 (solvent supply device) is capable of supplying fluorescein solvents of different compositions into the reaction vessel 10 as the solvent constituting the second liquid phase, It is equipped with the following features.

[0079] By configuring it in this way, it is possible to selectively produce different products depending on the purpose.

[0080] Furthermore, the product contains at least one of formic acid or methanol.

[0081] By configuring it in this way, it is possible to selectively produce formic acid and methanol.

[0082] Furthermore, the solvent constituting the second liquid phase is C8F 13 This is the fluorescein solvent having an OH3 composition.

[0083] By configuring it in this way, the methanol production ratio can be improved.

[0084] Furthermore, the solvent constituting the second liquid phase is The fluorescein solvent has the composition C3F3H2Cl.

[0085] By configuring it in this way, the formic acid production ratio can be improved.

[0086] Furthermore, the fluorescein solvent having the composition C3F3H2Cl has the structure CF3CH=CHCl.

[0087] By configuring it in this way, the formic acid production ratio can be improved.

[0088] Furthermore, the fluorescein solvent having the composition C3F3H2Cl has the structure CHF2CF=CHCl.

[0089] By configuring it in this way, the formic acid production ratio can be improved.

[0090] Furthermore, the method for producing the oxidation reaction product is: The reaction step includes irradiating a solution containing raw materials and chlorine dioxide radicals with light, The raw material comprises a hydrocarbon or a derivative of the hydrocarbon. The aforementioned solution contains an organic phase, The organic phase comprises the raw material and the chlorine dioxide radical, In the reaction step, the raw material is oxidized by light irradiation to produce an oxidation reaction product of the raw material. The aforementioned organic phase is C8F 13 It contains a fluorescein solvent having the composition OH3 or C3F3H2Cl.

[0091] By configuring it in this way, it is possible to selectively produce formic acid and methanol.

[0092] Although one embodiment of the present invention has been described above, the present invention is not limited to the above embodiments. For example, the configuration of each part constituting the reaction apparatus 1 is not limited to those described above and can be changed as appropriate.

[0093] Furthermore, although the above embodiment shows an example in which the stirring device 11 is provided at an eccentric position with respect to the center of the reaction vessel 10 in a plan view, the embodiment is not limited to this, and the stirring device 11 may be provided at the center of the reaction vessel 10 in a plan view.

[0094] Furthermore, although the above embodiment shows an example in which a baffle plate 11a is provided inside the reaction vessel 10, the embodiment is not limited to this configuration, and the baffle plate 11a may be omitted.

[0095] Furthermore, although the above embodiment shows an example in which the first liquid phase is formed on the upper side and the second liquid phase on the lower side within the reaction vessel 10, the embodiment is not limited to this configuration, and the first liquid phase may be formed on the lower side and the second liquid phase on the upper side.

[0096] Furthermore, although the above embodiment shows an example in which the reaction process is carried out at room temperature and atmospheric pressure, the embodiment is not limited to this configuration. For example, the reaction process may be carried out by pressurizing the reaction vessel 10 with a raw material gas. Alternatively, the reaction process may be carried out while the reaction vessel 10 is heated or cooled. [Explanation of symbols]

[0097] 1. Reactor 10 Reaction vessel 20. Gas phase adjustment device 30 First liquid phase preparation device 40 Second liquid phase preparation device 50 Control Unit

Claims

1. A reaction apparatus for producing a product by oxidizing the raw materials in a solution containing the raw materials and an oxidizing agent, The aforementioned raw material contains hydrocarbons, The oxidizing agent contains chlorine dioxide radicals, A reaction vessel having a first liquid phase in which the product can be dissolved and a second liquid phase containing the raw materials and the oxidizing agent formed inside, An irradiation device that irradiates light into the inside of the reaction vessel to cause the raw materials to undergo an oxidation reaction, A product recovery apparatus for recovering the product generated by the oxidation reaction of the raw materials from the first liquid phase, A solvent supply device capable of supplying fluorescein solvents of different compositions into the reaction vessel as solvents constituting the second liquid phase, It is equipped with, The solvent constituting the second liquid phase is The fluorescein solvent having the composition C8F13OH3 or C3F3H2Cl, Reaction apparatus.

2. The product includes at least one of formic acid or methanol. The reaction apparatus according to claim 1.

3. The fluorescein solvent having the composition C3F3H2Cl has the structure CF3CH=HCl The reaction apparatus according to claim 1.

4. The fluorescein solvent having the composition C3F3H2Cl has the structure CHF2CF=HCl The reaction apparatus according to claim 1.

5. A reaction step comprising irradiating a solution containing raw materials and chlorine dioxide radicals with light, The aforementioned raw material contains hydrocarbons, The aforementioned solution contains an organic phase, The organic phase comprises the raw material and the chlorine dioxide radical, In the reaction step, the raw material is oxidized by light irradiation to produce an oxidation reaction product of the raw material. The organic phase comprises a fluorescein solvent having the composition C8F13OH3 or C3F3H2Cl. A method for producing oxidation reaction products.

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