Raw material supply device and methanol production device

Abstract

The present invention provides a raw material supply device and a methanol production device that can improve methanol production by utilizing formic acid produced during methanol generation, while also reducing the burden of formic acid treatment. [Solution] A raw material supply device 2 for supplying methane, which is a raw material for methanol, to a reaction device 1 that produces methanol, comprising: a formic acid recovery unit 110 for recovering formic acid produced in conjunction with methanol production in the reaction device 1; a biogasification facility 120 for producing biogas using biomass and the formic acid recovered by the formic acid recovery unit 110; and a methane supply unit 140 for supplying methane contained in the biogas produced by the biogasification facility 120 to the reaction device 1.

Description

[Technical Field]

[0001] The present invention relates to a raw material supply device and a methanol production device for supplying raw materials to a reaction apparatus that produces methanol by chemical reaction. [Background technology]

[0002] Conventional techniques for producing methanol through chemical reactions have been known. For example, Patent Document 1 describes a method for producing the product at room temperature and pressure through a chemical reaction using two liquid phases.

[0003] In the invention described in Patent Document 1, a reaction system containing an aqueous phase and an organic phase is irradiated with light in the presence of a raw material and a chlorine dioxide radical to produce an oxidation reaction product of the raw material. Furthermore, Patent Document 1 states that when methane is used as the raw material, methanol is produced as the oxidation reaction product.

[0004] On the other hand, in the manufacturing method described in Patent Document 1, formic acid is also produced as a by-product of methanol. Conventionally, attempts have been made to increase the proportion of methanol produced and decrease the proportion of formic acid produced, but it has not been achieved to reduce the amount of formic acid produced to zero. Therefore, it is desirable to make effective use of the formic acid produced along with methanol production and to reduce the burden of processing the formic acid. [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 has been made in view of the above circumstances, and the problem it aims to solve is to provide a raw material supply device and a methanol production device that can improve the amount of methanol produced by utilizing formic acid produced during methanol production, and reduce the burden of processing formic acid. [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 raw material supply device for supplying methane, which is a raw material for methanol, to a reaction device for producing methanol, comprising: a formic acid recovery unit for recovering formic acid produced in the reaction device during methanol production; a biogas generation unit for producing biogas using biomass and the formic acid recovered by the formic acid recovery unit; and a methane supply unit for supplying methane contained in the biogas produced by the biogas generation unit to the reaction device.

[0009] In claim 2, the formic acid recovery unit comprises a storage tank capable of storing formic acid.

[0010] Claim 3 further comprises a control unit that controls the amount of formic acid recovered by the formic acid recovery unit supplied to the biogas generation unit, the biogas generation unit comprising a fermentation tank to which biomass and formic acid recovered by the formic acid recovery unit are supplied and methane fermentation is performed using the supplied biomass and formic acid, and a concentration measuring unit that measures the organic acid concentration inside the fermentation tank, the control unit controlling the amount of formic acid supplied based on the organic acid concentration measured by the concentration measuring unit.

[0011] Claim 4 provides a methanol generating apparatus having a reaction apparatus for generating methanol and a raw material supply apparatus for supplying methane, which is a raw material for methanol, to the reaction apparatus, wherein the reaction apparatus comprises a reaction vessel in which a first liquid phase capable of dissolving methanol and a second liquid phase containing methane and an oxidizing agent are formed inside, an irradiation apparatus for irradiating the inside of the reaction vessel with light to cause an oxidation reaction of methane, and a separation and recovery apparatus for separating and recovering methanol produced by the oxidation reaction of methane from the first liquid phase, and the raw material supply apparatus comprises a formic acid recovery unit for recovering formic acid produced in the reaction apparatus in conjunction with methanol generation, a biogas generating unit for generating biogas using biomass and the formic acid recovered by the formic acid recovery unit, and a methane supply unit for supplying methane contained in the biogas generated by the biogas generating unit to the reaction apparatus.

[0012] In claim 5, the separation and recovery device separates and recovers formic acid produced in conjunction with methanol generation from at least one of the first liquid phase or the second liquid phase, and the formic acid recovery unit recovers formic acid from the separation and recovery device.

[0013] In claim 6, the second liquid phase is C8F 13 It contains a fluorescein solvent having an OH3 composition. [Effects of the Invention]

[0014] The present invention provides the following effects:

[0015] Claim 1 makes it possible to increase the amount of methanol produced by utilizing formic acid generated during methanol production, while also reducing the burden of processing the formic acid.

[0016] In claim 2, depending on the internal state of the biogas generation unit, formic acid can be stored instead of being supplied to the biogasification equipment.

[0017] In claim 3, it is possible to suppress the inhibition of methane generation.

[0018] In claim 4, it is possible to improve the methanol production amount by using formic acid generated along with the production of methanol, and to reduce the burden associated with the treatment of formic acid.

[0019] In claim 5, it is possible to efficiently recover formic acid from the reaction apparatus.

[0020] In claim 6, it is possible to improve the methanol production ratio, and thus further reduce the burden associated with the treatment of formic acid.

Brief Description of the Drawings

[0021] [Figure 1] Schematic diagram showing a methanol production apparatus according to an embodiment of the present invention. [Figure 2] Schematic diagram showing a reaction apparatus. [Figure 3] Block diagram showing a methanol production apparatus. [Figure 4] Diagram schematically showing an example of a reaction process. [Figure 5] Flowchart showing the processes executed by a methanol production apparatus.

Embodiments for Carrying Out the Invention

[0022] Hereinafter, a methanol production apparatus 100 according to an embodiment of the present invention will be described.

[0023] A methanol production apparatus 100 according to an embodiment of the present invention is an apparatus for producing methanol. As shown in FIGS. 1 and 3, the methanol production apparatus 100 includes a reaction apparatus 1, a raw material supply apparatus 2, and a control apparatus 3. First, hereinafter, the configuration of the reaction apparatus 1 will be described using FIG. 2.

[0024] Reactor 1 produces products through a chemical reaction of a raw material gas in a liquid contained in a reaction vessel 10. Specifically, Reactor 1 produces products (oxidation reaction products) by irradiating a liquid containing the raw material gas and chlorine dioxide radicals (an oxidizing agent) with light to oxidize the raw material gas. Methane is used as the raw material gas in Reactor 1.

[0025] 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.

[0026] 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.

[0027] 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.

[0028] The reaction apparatus 1 according to this embodiment can obtain a product by oxidizing a raw material gas (methane) in a reaction vessel 10. The reaction apparatus 1 produces methanol as a product. In addition, formic acid is produced as a by-product in the reaction apparatus 1 along with the production of methanol. 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 separation and recovery device 50.

[0029] 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, methane, 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.

[0030] 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.

[0031] 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.

[0032] 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.

[0033] In this embodiment, as shown by the dashed line in Figure 2, 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.

[0034] 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.

[0035] The gas phase preparation unit 20 prepares the raw material gas (methane) 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 the raw material gas, the gas phase preparation unit 20 can also supply other gases used in the reaction (e.g., air or oxygen).

[0036] 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.

[0037] 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.

[0038] 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.

[0039] 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.

[0040] 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).

[0041] 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.

[0042] 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.

[0043] The second liquid phase preparation device 40 prepares a 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 amount of the second solution. Further, the second liquid phase preparation device 40 can remove by-products of the second liquid phase (second solution). The second solution is supplied to the second liquid phase preparation device 40 from a predetermined source.

[0044] The second liquid phase preparation device 40 preferably supplies a fluorinated solvent having a composition of C8F 13 OH3 to the reaction vessel 10. The fluorinated solvent having a composition of C8F 13 OH3 may have a structure of C7F 13 OCH3.

[0045] As the second solution, using a fluorinated solvent having a composition of C8F 13 OH3 (C7F 13 OCH3) can improve the production ratio of methanol (the ratio of the amount of methanol produced to the total amount of products produced). Specifically, by using a solvent having a composition of C8F 13 OH3 (C7F 13 OCH3) as the second solution, for example, the production ratio of methanol can be made 77.7% and the production ratio of formic acid can be made 22.3%. Thus, by using a fluorinated solvent having a composition of C8F 13 OH3 as the second solution, the production ratio of methanol can be improved.

[0046] As shown in FIG. 1, the second liquid phase preparation device 40 includes a second liquid phase path 41 that 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 corresponding to the separated second liquid phase (a position lower than the height position of the upper end of the second liquid phase).

[0047] 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.

[0048] 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.

[0049] The separation and recovery device 50 separates and recovers methanol and formic acid produced in the reaction vessel 10. The separation and recovery device 50 can separate and recover methanol and formic acid produced by the oxidation reaction of methane from the first liquid phase. Specifically, the separation and recovery device 50 is equipped with a distillation apparatus (multistage distillation apparatus), and by distilling the first solution recovered from the first liquid phase preparation device 30 using the distillation apparatus, methanol and formic acid dissolved in the first solution can be separated. Methanol is recovered as a product. Formic acid is recovered in the formic acid recovery unit 110, which will be described later.

[0050] Furthermore, the separation and recovery device 50 can separate the formic acid dissolved in the second solution from the second solution recovered from the second liquid phase preparation device 40. Specifically, the separation and recovery device 50 can move the formic acid from the solvent phase to the aqueous phase by adding a certain amount of water to the second solution (solvent) and stirring. In this way, the formic acid can be separated into the aqueous phase.

[0051] Figure 4 schematically shows an example of the reaction steps for producing methanol. As shown in Figure 4, chlorite ions (ClO2) are present in the first liquid phase (aqueous phase). -) reacts with an acid to form a chlorine dioxide radical (ClO2 · Chlorine dioxide radicals (ClO2) are generated. · ) dissolves in the second liquid phase (organic phase). Next, chlorine dioxide radical (ClO2 · By irradiating the second liquid phase (organic phase) containing ) with light and applying light energy hν (h is Blank's constant, ν is the frequency of light), chlorine dioxide radicals (ClO2) in the second liquid phase (organic phase) are produced. · ) decomposes into chlorine radicals (Cl · ) and oxygen molecules (O2) are generated. As a result, the starting material (RH) in the second liquid phase (organic phase) is oxidized, and methanol, which is the oxidation reaction product, is produced.

[0052] The methane used as a raw material in the methanol generator 100 is supplied to the methanol generator 100 from the raw material supply device 2. In addition to methanol, formic acid is produced as a by-product in the methanol generator 100. Furthermore, formic acid is dissolved in the second solution, and it is necessary to remove the formic acid from the second solution in order to improve the methanol production efficiency. Thus, the formic acid produced as a by-product in the reaction device 1 is used in the raw material supply device 2 to produce methane.

[0053] The configuration of the raw material supply device 2 will be described below with reference to Figure 1. The raw material supply device 2 comprises a formic acid recovery unit 110, a biogasification facility 120, a formic acid supply route 130, and a methane supply unit 140.

[0054] The formic acid recovery unit 110 recovers the formic acid produced in the reaction apparatus 1 as a result of methanol production. The formic acid recovery unit 110 comprises a storage tank 111 and a formic acid recovery path 112.

[0055] The storage tank 111 is configured to store the formic acid separated by the separation and recovery device 50 of the reaction device 1.

[0056] The formic acid recovery path 112 is a path through which formic acid from the separation and recovery device 50 can be transported. The formic acid recovery path 112 is provided to connect the separation and recovery device 50 and the storage tank 111.

[0057] In the formic acid recovery unit 110 configured in this way, formic acid is supplied from the separation and recovery device 50 via the formic acid recovery path 112, and the recovered formic acid is stored in the storage tank 111.

[0058] The biogasification facility 120 generates biogas using biomass (organic matter) and formic acid recovered by the formic acid recovery unit 110. The biogasification facility 120 is equipped with a fermentation tank 121 and an organic acid concentration measuring instrument 122.

[0059] The fermentation tank 121 is a tank to which biomass and formic acid recovered by the formic acid recovery unit 110 are supplied, and methane fermentation is carried out using the supplied biomass and formic acid. The fermentation tank 121 is configured to be able to receive biomass. Furthermore, the fermentation tank 121 is configured to be able to receive formic acid from the storage tank 111 via the formic acid supply route 130, which will be described later. The fermentation tank 121 uses formic acid as a carbon source to decompose biomass through the action of various anaerobic microorganisms, producing biogas containing methane gas and carbon dioxide.

[0060] The organic acid concentration meter 122 measures the concentration of organic acids (VFAs) inside the fermentation tank 121. The organic acid concentration meter 122 is installed at an appropriate location inside the fermentation tank 121. Inside the fermentation tank 121, the organic acid concentration increases as the supply of formic acid increases. The organic acid concentration meter 122 is configured to measure the concentration of organic acids generated in the fermentation tank 121.

[0061] The formic acid supply route 130 is a route for supplying formic acid from the storage tank 111 (formic acid recovery unit 110) to the fermentation tank 121 (biogasification equipment 120). The formic acid supply route 130 is provided to connect the storage tank 111 and the fermentation tank 121. A pump 131 is provided in the middle of the formic acid supply route 130. When the pump 131 operates, formic acid is supplied from the storage tank 111 to the fermentation tank 121 via the formic acid supply route 130.

[0062] The methane supply unit 140 is a route for supplying methane contained in the biogas produced by the biogasification equipment 120 to the reactor 1. The methane supply unit 140 is provided to connect the fermentation tank 121 and the raw material tank of the gas phase preparation device 20.

[0063] The raw material supply device 2, configured in this way, recovers formic acid, which is produced as a by-product in the reactor 1, into the storage tank 111 via the formic acid recovery path 112, and supplies the recovered formic acid to the fermentation tank 121. In the fermentation tank 121, biogas is produced by methane fermentation using biomass and formic acid. The biogas contains methane gas and carbon dioxide, of which methane gas can be supplied to the raw material tank of the reactor 1 via the methane supply unit 140. The reactor 1 can produce methanol using the methane supplied from the raw material supply device 2 as a raw material.

[0064] The control device 3 shown in Figure 3 is capable of processing various types of information. The control device 3 can control the operation of each component of the reaction apparatus 1 and the raw material supply apparatus 2. The control device 3 includes a CPU, memory, and other components.

[0065] The control device 3 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, the second liquid phase preparation device 40, and the separation and recovery device 50 of the reaction apparatus 1. The control device 3 can control the operation of the gas phase preparation device 20, the first liquid phase preparation device 30, the second liquid phase preparation device 40, and the separation and recovery device 50, as well as the valves and pumps equipped in each of the above devices. In addition, the control device 3 can acquire the measurement results from the sensors equipped in each of the devices of the reaction apparatus 1.

[0066] Furthermore, the control device 3 is electrically connected to the formic acid recovery unit 110, the biogasification equipment 120 (organic acid concentration meter 122), the formic acid supply route 130 (pump 131), and the methane supply unit 140 of the raw material supply device 2. The control device 3 can control the operation of the formic acid recovery unit 110, the biogasification equipment 120, the formic acid supply route 130, and the methane supply unit 140, as well as the valves and pumps provided in each of the above devices. The control device 3 can control the operation of the pump 131 based on the measurement results of the organic acid concentration meter 122.

[0067] In this embodiment, the control device 3 is provided separately from the reaction device 1 and the raw material supply device 2, and controls each of the reaction device 1 and the raw material supply device 2. However, control devices may also be provided for each of the reaction device 1 and the raw material supply device 2.

[0068] As described above, the control device 3 controls the operation of each device in the reactor 1 and the raw material supply device 2, thereby supplying methane from the raw material supply device 2 to the reactor 1, and generating methanol in the reactor 1 using methane as a raw material.

[0069] The operation of the methanol generator 100 will be described below. The control device 3 controls each process shown in the flowchart of Figure 5, thereby enabling the production of methane, the raw material for methanol production in the reaction device 1, in the raw material supply device 2.

[0070] First, the control device 3 executes the "reaction process" shown in steps S101 to S104 of Figure 5. The reaction process is a process in which a chemical reaction is carried out in the reaction vessel 10 using methane gas from the biogas, the first solution, and the second solution.

[0071] In step S101, the control device 3 operates the various devices in the reaction vessel 10 so that the methanolization reaction can take place. More specifically, the control device 3 operates the stirring device 11 of the reaction vessel 10 to start stirring the first and second solutions in the reaction vessel 10. The control device 3 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 methane gas to the reaction vessel 10. The control device 3 also operates the gas phase preparation device 20 to prepare the methane gas and to recycle the methane gas. The control device 3 also operates the irradiation device 12 of the reaction vessel 10 to start irradiating the reaction vessel 10 with light. In this way, methanol and formic acid are produced as the various devices used in the chemical reaction are operated.

[0072] Next, in step S102, the control device 3 determines whether the number of times the reaction process has been executed has reached a predetermined number of reactions. The predetermined number of reactions can be any number set in advance. If the control device 3 determines that the number of times the reaction process has been executed has reached the predetermined number of reactions (YES in step S102), it proceeds to step S103. On the other hand, if the control device 3 determines that the number of times the reaction process has been executed has not reached the predetermined number of reactions (NO in step S102), it performs the process in step S102 again (i.e., it does not proceed with the process until it becomes YES in step S102).

[0073] In step S103, the control device 3 separates and recovers methanol and formic acid. Specifically, the separation and recovery device 50 separates and recovers methanol and formic acid from the first solution using a distillation apparatus (multistage distillation apparatus). In addition, the separation and recovery device 50 moves the formic acid from the solvent phase to the aqueous phase by adding a certain amount of water to the second solution (solvent) and stirring, thereby separating the formic acid into the aqueous phase.

[0074] Next, in step S104, the control device 3 starts storing formic acid in the storage tank 111. The control device 3 operates a pump (not shown) provided in the formic acid recovery path 112 to supply the formic acid separated in the separation and recovery device 50 (the aqueous phase containing formic acid recovered from the first solution and formic acid from the second solution) to the storage tank 111 via the formic acid recovery path 112. In this way, formic acid is stored in the storage tank 111.

[0075] Next, the control device 3 executes the "verification process" shown in steps S105 to S106 of Figure 5. The verification process is a process of checking the internal state of the fermentation tank 121.

[0076] In step S105, the control device 3 determines whether the current time is the plant raw material input time. Here, "plant raw material input time" refers to the scheduled time (time) for inputting raw materials necessary for methane fermentation, such as formic acid and biomass, into the fermentation tank 121 (plant). The plant raw material input time can be set in advance at any time. Furthermore, multiple times can be set for the plant raw material input time within a single day.

[0077] If the control device 3 determines that it is currently time to input raw materials into the plant (YES in step S105), it proceeds to step S106. On the other hand, if the control device 3 determines that it is not yet time to input raw materials into the plant (NO in step S105), it performs the process in step S105 again (i.e., it does not proceed with the process until it becomes YES in step S105).

[0078] In step S106, the control device 3 determines whether the organic acid concentration inside the fermenter 121 is below a specified value. Here, the organic acid concentration refers to the concentration of organic acids (VFAs) inside the fermenter 121. Inside the fermenter 121, the organic acid concentration increases as the supply of formic acid increases. If the organic acid concentration becomes too high, the progress of methane fermentation is inhibited. Therefore, in the process of step S106, it is determined whether the organic acid concentration inside the fermenter 121 is below a specified value. The specified value is set considering the impact on the progress of methane fermentation, and is set to, for example, 4000 ppm.

[0079] If the control device 3 determines that the organic acid concentration is below a specified value (YES in step S106), it proceeds to step S108. On the other hand, if the control device 3 determines that the organic acid concentration is not below a specified value (exceeds a specified value) (NO in step S105), it waits for t minutes (a predetermined time) (step S107), and when it is time to input the next plant raw material (YES in step S105), it determines again whether the organic acid concentration inside the fermentation tank 121 is below a specified value (step S106).

[0080] Next, the control device 3 executes the "addition process" shown in steps S107 to S108 of Figure 5. The addition process is the process of adding formic acid to the fermentation tank 121.

[0081] In step S108, the control device 3 starts supplying liquid from the storage tank 111 to the raw material input line. Specifically, the control device 3 operates the pump 131 to supply formic acid to the fermentation tank 121 via the formic acid supply path 130.

[0082] Next, in step S109, the control device 3 determines whether or not the input of a certain amount of raw material has been completed. If the control device 3 determines that the input of a certain amount of raw material has been completed (YES in step S109), it terminates the flow shown in Figure 5. On the other hand, if the control device 3 determines that the input of a certain amount of raw material has not been completed (NO in step S109), it continues to transfer liquid from the storage tank 111 to the fermentation tank 121 until the input of a certain amount of raw material has been completed (until it becomes YES in step S109) (step S108).

[0083] As described above, in the raw material supply device 2 and methanol production device 100 according to this embodiment, formic acid produced as a by-product from the reactor 1 is stored in the storage tank 111, and formic acid is supplied from the storage tank 111 to the fermentation tank 121. This allows formic acid to be used as a carbon source for methane fermentation in the fermentation tank 121, thereby promoting the production of biogas. By supplying the methane contained in the biogas to the reactor 1, methane can be used as a raw material in the reactor 1. In this way, formic acid produced as a by-product from the reactor 1 can be effectively utilized as a raw material for methanol production in the reactor 1, thereby improving the amount of methanol produced. Furthermore, by effectively utilizing formic acid in methane production, the burden of processing formic acid can be reduced.

[0084] Furthermore, as mentioned above, it is necessary to keep the organic acid concentration below a specified value inside the fermenter 121 so as not to hinder the progress of methane fermentation. If too much formic acid is supplied to the fermenter 121, there is a high possibility that the organic acid concentration inside the fermenter 121 will exceed the specified value. Therefore, in order to make all of the formic acid produced in the reactor 1 available for methane fermentation in the biogasification facility 120, it is necessary to make the methanol production ratio (the ratio of methanol production to the total amount of products produced) in the reactor 1 as high as possible (the formic acid production ratio as low as possible).

[0085] In this embodiment, C8F is used as the second solution. 13OH3(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 products produced) can be improved. Therefore, the entire amount of formic acid produced in reactor 1 can be used (recycled) for methane fermentation in biogasification facility 120. This suppresses the generation of formic acid that cannot be used for methane fermentation, and consequently reduces the burden of formic acid treatment.

[0086] As described above, the raw material supply device 2 according to this embodiment is A raw material supply device 2 for supplying methane, which is a raw material for methanol, to a reaction device 1 that produces methanol, The reaction apparatus 1 includes a formic acid recovery unit 110 for recovering formic acid produced in conjunction with methanol generation, A biogasification facility 120 (biogas generation unit) that generates biogas using biomass and formic acid recovered by the formic acid recovery unit 110, A methane supply unit 140 supplies methane contained in the biogas produced by the biogasification equipment 120 to the reaction unit 1, It is equipped with the following features.

[0087] By configuring the system in this way, it is possible to increase the amount of methanol produced by utilizing the formic acid generated during methanol production, while also reducing the burden of processing the formic acid.

[0088] Furthermore, the formic acid recovery unit 110 is It is equipped with a storage tank 111 capable of storing formic acid.

[0089] By configuring it in this way, formic acid can be stored instead of being supplied to the biogasification facility 120, depending on the internal conditions of the biogasification facility 120.

[0090] Furthermore, the raw material supply device 2 according to this embodiment is The system includes a control device 3 (control unit) that controls the amount of formic acid recovered by the formic acid recovery unit 110 supplied to the biogasification equipment 120, The biogasification equipment 120 is, A fermentation tank 121 is supplied with biomass and formic acid recovered by the formic acid recovery unit 110, and methane fermentation is carried out using the supplied biomass and formic acid. The organic acid concentration measuring instrument 122 (concentration measuring unit) measures the organic acid concentration inside the fermentation tank 121, It is equipped with, The control device 3 is The amount of formic acid supplied is controlled based on the organic acid concentration measured by the organic acid concentration measuring instrument 122.

[0091] By configuring it in this way, the inhibition of methane production can be suppressed.

[0092] Furthermore, the methanol generator 100 includes a reaction apparatus 1 for producing methanol, and a raw material supply apparatus 2 for supplying methane, which is a raw material for methanol, to the reaction apparatus 1, The reaction apparatus 1 is A reaction vessel 10 in which a first liquid phase capable of dissolving methanol and a second liquid phase containing methane and an oxidizing agent are formed inside, An irradiation device 12 that irradiates light into the inside of the reaction vessel 10 to cause the methane oxidation reaction, A separation and recovery apparatus 50 for separating and recovering methanol produced by the oxidation reaction of methane from the first liquid phase, It is equipped with, The raw material supply device 2 is The reaction apparatus 1 includes a formic acid recovery unit 110 for recovering formic acid produced in conjunction with methanol generation, A biogasification facility 120 (biogas generation unit) that generates biogas using biomass and formic acid recovered by the formic acid recovery unit 110, A methane supply unit 140 supplies methane contained in the biogas produced by the biogasification equipment 120 to the reaction unit 1, It is equipped with the following features.

[0093] By configuring the system in this way, it is possible to increase the amount of methanol produced by utilizing the formic acid generated during methanol production, while also reducing the burden of processing the formic acid.

[0094] Furthermore, the separation and recovery device 50 is The formic acid produced in conjunction with methanol generation is separated and recovered from at least one of the first liquid phase or the second liquid phase. The formic acid recovery unit 110 is Formic acid is recovered from the separation and recovery device 50.

[0095] By configuring it in this way, formic acid can be efficiently recovered from the reaction apparatus 1.

[0096] Furthermore, the second liquid phase is C8F 13 It contains a fluorescein solvent having an OH3 composition.

[0097] By configuring the system in this way, the methanol production ratio can be improved, and consequently, the burden of processing formic acid can be further reduced.

[0098] Although one embodiment of the present invention has been described above, the present invention is not limited to the above embodiment. For example, the configuration of each part constituting the reaction apparatus 1 and the raw material supply apparatus 2 is not limited to those described above and can be changed as appropriate.

[0099] Furthermore, in this embodiment, the separation and recovery device 50 separates and recovers formic acid from either the first or second liquid phase, but it may also separate and recover formic acid from either the first or second liquid phase.

[0100] Furthermore, in this embodiment, the organic acid concentration inside the fermentation tank 121 is measured by the organic acid concentration meter 122, but it may also be measured simply based on the pH inside the fermentation tank 121. [Explanation of Symbols]

[0101] 1. Reactor 2 Raw material supply device 3. Control device 50 Separation and recovery device 110 Formic Acid Recovery Section 111 Storage Tank 120 Biogasification facilities 121 Fermentation tank 122 Organic Acid Concentration Meter 140 Methane supply unit

Claims

1. A raw material supply device for supplying methane, which is a raw material for methanol, to a reaction apparatus that produces methanol, The reaction apparatus includes a formic acid recovery unit for recovering formic acid produced in conjunction with methanol generation, A biogas generation unit that generates biogas using biomass and formic acid recovered by the formic acid recovery unit, A methane supply unit that supplies methane contained in the biogas produced by the biogas generation unit to the reaction apparatus, Equipped with, Raw material supply equipment.

2. The formic acid recovery unit is, It is equipped with a storage tank capable of storing formic acid. The raw material supply apparatus according to claim 1.

3. The system includes a control unit that controls the amount of formic acid recovered by the formic acid recovery unit supplied to the biogas generation unit, The biogas generation unit is A fermentation tank is supplied with biomass and formic acid recovered by the formic acid recovery unit, and methane fermentation is carried out using the supplied biomass and formic acid. A concentration measuring unit for measuring the organic acid concentration inside the fermentation tank, It is equipped with, The control unit, The amount of formic acid supplied is controlled based on the concentration of the organic acid measured by the concentration measuring unit. A raw material supply device according to claim 1 or claim 2.

4. A methanol production apparatus having a reaction apparatus for producing methanol, and a raw material supply apparatus for supplying methane, which is a raw material for methanol, to the reaction apparatus, The reaction apparatus is A reaction vessel in which a first liquid phase capable of dissolving methanol and a second liquid phase containing methane and an oxidizing agent are formed inside, An irradiation device that irradiates light into the inside of the reaction vessel to oxidize methane, A separation and recovery apparatus for separating and recovering methanol produced by the oxidation reaction of methane from the first liquid phase, It is equipped with, The raw material supply device is The reaction apparatus includes a formic acid recovery unit for recovering formic acid produced in conjunction with methanol generation, A biogas generation unit that generates biogas using biomass and formic acid recovered by the formic acid recovery unit, A methane supply unit that supplies methane contained in the biogas produced by the biogas generation unit to the reaction apparatus, Equipped with, Methanol generator.

5. The separation and recovery device is The formic acid produced in conjunction with methanol generation is separated and recovered from at least one of the first liquid phase or the second liquid phase. The formic acid recovery unit is, Formic acid is recovered from the aforementioned separation and recovery apparatus. The methanol generating apparatus according to claim 4.

6. The second liquid phase is C ８ F １３ OH ３ A fluorescein solvent having the following composition: A methanol generating apparatus according to claim 4 or claim 5.

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