CN113514490A - Reaction analysis device, reaction analysis system, and reaction analysis method - Google Patents

Abstract

The present invention relates to a reaction analysis device, a reaction analysis system, and a reaction analysis method. The reaction analysis device is a reaction analysis device that specifies a reaction state of a reaction fluid flowing through a flow reactor, and includes a processing unit that specifies the reaction state of the reaction fluid based on a reaction parameter indicating the reaction state of the reaction fluid obtained from a temperature distribution of the reaction fluid immediately after the start of a reaction along a flow direction of the reaction fluid.

Description

Reaction analysis device, reaction analysis system, and reaction analysis method

Technical Field

The present invention relates to a reaction analysis device, a reaction analysis system, and a reaction analysis method.

The present application claims priority from Japanese patent application No. 2020-.

Background

In the production of pharmaceuticals and fine chemicals using organic chemical reactions, optimization of reaction conditions is important for high efficiency of production. The reaction conditions include, for example, the selection of the solvent type and the reagent, concentration, temperature, reaction time, and the like. In the optimization step, conditions for obtaining a high yield (yield) are sought for high efficiency. In the optimization step, each item is sequentially optimized, but as the index thereof, a yield and a reaction rate measured by sampling the concentration of the product in the reaction time are mainly used. For synthesis of the product, for example, a flow reactor is used in which the first solution and the second solution are injected into a supply device and mixed by a mixer (see, for example, japanese patent application laid-open No. 2020-11948).

However, in the conventional technique, in order to obtain a reaction rate by an experiment, it is necessary to sample a reaction fluid within a certain reaction time, and to perform processes such as extraction of a product and concentration measurement on the reaction fluid obtained by the sampling, and it takes at least several hours of work time to calculate a concentration under one condition. Conventionally, depending on the number of optimization items, it is necessary to repeat a trial and error (try and error) process of changing conditions and extracting the conditions several tens of times or more. In addition, in the conventional art, concentration data under a plurality of temperature conditions is required, and therefore, more man-hours are required.

Disclosure of Invention

In order to achieve the above object, a reaction analyzer according to an aspect of the present invention is a reaction analyzer for determining a reaction state of a reaction fluid flowing through a flow reactor, including: the processing unit determines the reaction state of the reaction fluid based on a reaction parameter indicating the reaction state of the reaction fluid obtained from a temperature distribution of the reaction fluid immediately after the start of the reaction along the flow direction of the reaction fluid.

In the reaction analysis device according to an aspect of the present invention, the processing unit may acquire the reaction parameter by comparing a measured result obtained by measuring a temperature of the reaction fluid with an estimated temperature distribution obtained by estimating a temperature distribution of the reaction fluid immediately after the start of the reaction.

In the reaction analyzer according to one aspect of the present invention, the estimated temperature distribution may be obtained by a control equation (calculation) for estimating a temperature distribution of the reaction fluid immediately after the start of the reaction, the control equation including a first reaction parameter related to a peak of the temperature distribution of the reaction fluid immediately after the start of the reaction and a second reaction parameter related to a peak position of the temperature distribution of the reaction fluid immediately after the start of the reaction.

In the reaction analyzer according to one aspect of the present invention, the first reaction parameter may represent a calorific value per unit mass, and the second reaction parameter may represent a temperature dependency of a reaction rate.

In the reaction analysis device according to an aspect of the present invention, the processing unit may adjust the first reaction parameter and the second reaction parameter so that a difference between the actual measurement result and the estimated temperature distribution is within a predetermined value, and store the adjusted first reaction parameter and second reaction parameter in the storage unit.

In the reaction analysis device according to an aspect of the present invention, the processing unit may calculate at least one of a reaction rate of the reaction fluid, a concentration of the plurality of reactants, and a concentration or a yield of the product contained in the reaction fluid, based on the first reaction parameter and the second reaction parameter stored in the storage unit.

In the reaction analysis device according to an aspect of the present invention, the reaction analysis device may further include a control unit that compares the reaction state of the reaction fluid specified by the processing unit with a target value of the reaction state, and controls the reaction conditions of the reaction fluid in the flow reactor.

In the reaction analyzer according to one aspect of the present invention, the control unit may perform first control for setting the reaction state at the flow channel outlet of the flow reactor to the target value or more.

In the reaction analyzer according to an aspect of the present invention, the control unit may perform a second control for minimizing a residence time of the reaction fluid from when the reaction state reaches the target value to when the reaction state reaches the outlet of the flow channel of the flow reactor.

In order to achieve the above object, a reaction analysis system according to an aspect of the present invention is a reaction analysis system for determining a reaction state of a reaction fluid flowing through a flow reactor, including: a temperature measuring unit that measures the temperature of the reaction fluid along the reaction flow path of the flow reactor; and the reaction analyzer described above, wherein the processing unit determines the reaction state of the reaction fluid based on a reaction parameter indicating the reaction state of the reaction fluid obtained from the actual measurement result obtained by the temperature measuring unit.

In the reaction analysis system according to an aspect of the present invention, the temperature measurement unit may be provided so as to sandwich at least a peak position of a temperature distribution of the reaction fluid in the reaction channel.

In the reaction analysis system according to one aspect of the present invention, the flow reactor may include: a plurality of supply channels that supply a plurality of reactants for chemical reactions, respectively; a mixer connected to the plurality of supply flow paths and mixing a plurality of reactants; and a reaction channel connected to the mixer and allowing a reaction fluid obtained by mixing a plurality of reactants to flow therethrough.

In the reaction analysis system according to one aspect of the present invention, the flow reactor may be provided with a catalyst for causing (promoting) a chemical reaction of the reaction fluid.

In the reaction analysis system according to an aspect of the present invention, the reaction analysis system may further include an electromagnetic wave irradiation device that irradiates the reaction fluid flowing through the flow reactor with electromagnetic waves.

In the reaction analysis system according to an aspect of the present invention, a heating device may be provided to heat the reaction fluid flowing through the flow reactor.

In the reaction analysis system according to one aspect of the present invention, the reaction analysis system may further include an energizing device that energizes the reaction fluid flowing through the flow reactor.

In order to achieve the above object, a reaction analysis method according to an aspect of the present invention is a reaction analysis method for determining a reaction state of a reaction fluid flowing through a flow reactor, including: the reaction state of the reaction fluid is determined by the processing unit based on a reaction parameter indicating the reaction state of the reaction fluid obtained from the temperature distribution of the reaction fluid immediately after the start of the reaction along the flow direction of the reaction fluid.

In the reaction analysis method according to an aspect of the present invention, the processing unit may obtain the reaction parameter by comparing a measured result obtained by measuring a temperature of the reaction fluid with an estimated temperature distribution obtained by estimating a temperature distribution of the reaction fluid immediately after the start of the reaction.

In the reaction analysis method according to the aspect of the present invention, the estimated temperature distribution may be obtained by a governing equation that estimates a temperature distribution of the reaction fluid immediately after the start of the reaction, the governing equation including a first reaction parameter related to a peak of the temperature distribution of the reaction fluid immediately after the start of the reaction and a second reaction parameter related to a peak position of the temperature distribution of the reaction fluid immediately after the start of the reaction.

In the reaction analysis method according to the aspect of the present invention, the first reaction parameter may represent a calorific value per unit mass, and the second reaction parameter may represent a temperature dependency of a reaction rate.

According to the present invention, a reaction state such as a reaction rate can be detected in a shorter time than before without performing a plurality of experiments.

Further features and aspects of the invention will become apparent from the detailed description of the embodiments given below with reference to the attached drawings.

Drawings

Fig. 1 is a block diagram showing a configuration example of a reaction analysis system according to a first embodiment.

Fig. 2 is a diagram showing a relationship between a position and a temperature and a relationship between time and a temperature.

Fig. 3 is a diagram for explaining a method of calculating a reaction parameter from a temperature distribution of a reaction field according to the first embodiment.

Fig. 4 is a flowchart for determining the reaction state of the reaction fluid based on the temperature distribution of the reaction fluid immediately after mixing along the flow direction of the reaction fluid, in the reaction analysis processing procedure of the first embodiment.

Fig. 5 is a graph showing the positional change (temporal change) of the concentrations of the reactant and the product.

Fig. 6 is a diagram showing a configuration example of the reaction analysis apparatus according to the first embodiment.

Fig. 7 is a diagram showing a connection example and a configuration example of the reaction analysis apparatus according to the first embodiment.

Fig. 8 is a block diagram showing a configuration example of the reaction analysis system according to the second embodiment.

Fig. 9 is a block diagram showing a configuration example of a reaction analysis system according to a modification of the second embodiment.

Fig. 10 is a block diagram showing a configuration example of a reaction analysis system according to a modification of the second embodiment.

Fig. 11 is a block diagram showing a configuration example of a reaction analysis system according to a modification of the second embodiment.

Fig. 12 is a block diagram showing a configuration example of a reaction analysis system according to a modification of the second embodiment.

Fig. 13 is a block diagram showing a configuration example of a reaction analysis system according to a modification of the second embodiment.

Fig. 14 is a block diagram showing a configuration example of a reaction analysis system according to a modification of the third embodiment.

Fig. 15 is a flowchart showing a procedure of reaction condition control from the start of reaction analysis according to the third embodiment.

Fig. 16 is a diagram showing a relationship between a position and an estimated temperature and a relationship between a position and an estimated concentration.

Detailed Description

The embodiments of the present invention will be described with reference to preferred embodiments. Those skilled in the art can implement the various alternative elements of the present embodiment using the teachings of the present invention, which is not limited to the preferred embodiment described herein.

One embodiment of the present invention provides a reaction analysis apparatus, a reaction analysis system, and a reaction analysis method, which can detect a reaction state such as a reaction rate in a shorter time than before without performing a plurality of experiments.

Hereinafter, embodiments of the present invention will be described with reference to the drawings. In the drawings used for the following description, the scale of each member is appropriately changed so that each member can be recognized.

(first embodiment)

First, a first embodiment of the present invention will be explained.

< construction of reaction analysis System 1 >

Fig. 1 is a block diagram showing a configuration example of a reaction analysis system 1 according to a first embodiment. As shown in fig. 1, the reaction analysis system 1 includes a first pump 11, a liquid feeding tube 111, a second pump 12, a liquid feeding tube 112, a mixer 13, a reaction tube 14 (reaction channel), a temperature regulator 15, a temperature measuring unit 16, and a reaction analysis device 20. The temperature measuring unit 16 includes a first temperature measuring unit 161 (temperature measuring unit), a second temperature measuring unit 162 (temperature measuring unit), a third temperature measuring unit 163 (temperature measuring unit), and a fourth temperature measuring unit 164 (temperature measuring unit). The flow reactor 10 includes a first pump 11, a liquid sending pipe 111, a second pump 12, a liquid sending pipe 112, a mixer 13, and a reaction pipe 14. The reaction analyzer 20 includes a CPU 23 (processing unit).

The flow reactor 10 shown in fig. 1 has a plurality of supply flow paths (the first pump 11 and the liquid sending tube 111, the second pump 12 and the liquid sending tube 112) for supplying a plurality of reactants for chemical reaction, respectively, and a mixer 13 connected to the plurality of supply flow paths and mixing the plurality of reactants, thereby forming a flow path shape.

The first pump 11 is connected to the first inlet of the mixer 13 via a liquid feeding pipe 111. The second pump 12 is connected to the second inlet of the mixer 13 via a liquid feeding pipe 112. The mixer 13 has two inlets and one outlet. The discharge port of the mixer 13 is connected to a reaction tube (reaction channel) 14 through which a reaction fluid obtained by mixing a plurality of reactants flows.

The temperature measuring unit 16 has, for example, a plurality of first temperature measuring units 161, second temperature measuring units 162, third temperature measuring units 163, and fourth temperature measuring units 164 arranged along the flow path in front of and behind the mixer 13 so as to be able to measure the temperature of the reaction fluid at a plurality of positions along the reaction tube 14.

The first temperature measuring unit 161 is provided on the input side of the mixer 13, and the initial temperature of the reaction fluid (the temperature of the reaction fluid at the discharge port of the mixer 13) obtained by mixing a plurality of reactants can be measured (estimated) by the first temperature measuring unit 161.

The second temperature measuring unit 162, the third temperature measuring unit 163, and the fourth temperature measuring unit 164 are provided in the reaction tube 14 on the output side of the mixer 13, and the temperature (temperature distribution) of the reaction fluid immediately after mixing (immediately after the start of the reaction) in the flow direction of the reaction fluid can be measured by these second temperature measuring unit 162 to fourth temperature measuring unit 164. Further, "immediately after the reaction" does not mean immediately after the reaction fluid actually starts the reaction, but means immediately after the reaction fluid is brought into a state where the reaction is started (immediately after a plurality of reactants are mixed in the first embodiment).

The liquid feeding pipe 111, the liquid feeding pipe 112, the mixer 13 and the reaction pipe 14 are provided in the temperature controller 15.

< operation of reaction analysis System 1 (reaction analysis method) >

The reaction analysis system 1 determines the reaction state of the reaction fluid in the chemical reaction apparatus of the flow synthesis type. The reaction analysis system 1 measures the temperature before the reaction and the temperatures of a plurality of portions after the reaction, and estimates the reaction parameters based on the measured temperatures. The reactant to be fed to the first pump 11 and the second pump 12 may be liquid or gas. The reaction parameter indicates a reaction state of the reaction fluid, and as described later, is, for example, a parameter that affects a temperature distribution of the chemical reaction field. The product generated by the reaction analysis system 1 is, for example, a peptide composition.

The first reactant a is fed into the first pump 11. The first pump 11 supplies the first reactant a, which is fed, to the mixer 13 via the liquid feeding tube 111 (first channel) at, for example, a first flow rate and a first flow rate.

The second reactant B is fed into the second pump 12. The second pump 12 supplies the second reactant B, which has been fed, to the mixer 13 through the liquid feeding tube 112 (second channel) at a second flow rate and a second flow rate.

The mixer 13 mixes the first reactant a supplied from the first pump 11 and the second reactant B supplied from the second pump 12, and supplies the mixed product to the reaction tube 14.

The product is supplied from the discharge port of the mixer 13 to the reaction tube 14. In the space inside the mixer 13, the mixing of the first reactant a and the second reactant B is started. In the flow reactor, a reaction is caused in the reaction tube 14 from the inside of the mixer 13, and a product-containing solution, for example, moves in the reaction tube 14. Further, in the flow reactor, for example, a solution containing the product is discharged to the outside of the reaction tube 14 through the reaction tube 14.

The temperature regulator 15 is, for example, a constant temperature water tank, and regulates the temperature of the mixer 13 and the reaction tube 14 to a predetermined temperature under the control of the reaction analyzer 20.

The temperature measuring unit 16 is a sensor for measuring the temperature of the chemical reaction field, and is, for example, a thermocouple. The temperature measuring unit 16 may be a non-contact type, for example, an optical temperature sensor. The temperature measuring unit 16 detects a temperature distribution of the reaction fluid along the reaction tube 14 (reaction channel), and outputs temperature information (actually measured temperature distribution) indicating the detected temperature to the reaction analyzer 20. The chemical reaction field is a region where the reactants mixed at the downstream side of the mixer are chemically reacted.

The first temperature measuring unit 161 is disposed at the position p1 before the reaction. The installation location may be at least one of the first pump 11 side and the second pump 12 side, or may be both the first pump 11 side and the second pump 12 side. In the case where the first temperature measuring unit 161 is provided on both the first pump 11 side and the second pump 12 side, the average value of the temperature on the first pump 11 side and the temperature on the second pump 12 side may be output to the reaction analyzer 20. The average value may be calculated by the reaction analyzer 20. In addition, it is not essential to measure the temperature on the upstream side of the mixer. For example, when the temperature of the reactant is kept constant, the first temperature measuring unit 161 is not necessary.

The second temperature measuring unit 162 is disposed at the position p2 after the reaction. The position p2 is the position closest to the discharge port of the mixer 13 among the positions p2 to p 4. The second temperature measuring unit 162 measures the temperature at the position p2, and outputs information indicating the measured temperature to the reaction analyzer 20.

The third temperature measuring unit 163 is disposed at the position p3 after the reaction. The position p3 is a position between the position p2 and the position p4, and is a longer distance from the discharge port of the mixer 13 than the position p 2. The third temperature measuring unit 163 measures the temperature at the position p3, and outputs information indicating the measured temperature to the reaction analyzer 20.

The fourth temperature measuring unit 164 is provided at the position p4 after the reaction. The position p4 is the farthest position from the discharge port of the mixer 13 among the positions p2 to p 4. The fourth temperature measuring unit 164 measures the temperature at the position p4, and outputs information indicating the measured temperature to the reaction analyzer 20.

The reaction analyzer 20 controls the temperature regulator 15. The reaction analysis device 20 controls the flow rates of the first pump 11 and the second pump 12. The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analyzer 20 uses the acquired information indicating the temperature to specify the reaction state of the reaction fluid obtained by mixing a plurality of reactants. The reaction state is, for example, the reaction rate of the reaction fluid, the concentration of a plurality of reactants, and the concentration or yield of a product contained in the reaction fluid. The reaction analysis means 20 analyzes the reaction, for example, by estimating a function of the position and the temperature. The estimation method and the like will be described later.

The structure shown in fig. 1 is an example, and is not limited to this. For example, the following structure is also possible: the first reactant and the second reactant are mixed in the first mixer to produce a first product, and the first product and the third reactant are mixed in the second mixer to produce a second product. In this case, by installing temperature measuring units before and after (upstream and downstream sides) or only on the downstream side of the first mixer and installing temperature measuring units before and after (upstream and downstream sides) or only on the downstream side of the second mixer, the temperature distribution of the reaction fluid immediately after mixing of the first reactant and the second reactant by the first mixer is detected, and the temperature distribution of the reaction fluid immediately after mixing of the first product and the third reactant by the second mixer is detected.

< example of temperature distribution >

Next, an example of the relationship between the position x and the temperature will be described.

Fig. 2 is a graph showing a relationship between a position and a temperature and a relationship between time and a temperature, and specifically shows a temperature distribution of the reaction fluid with respect to a flow path distance from the mixer 13 in the reaction tube 14 and a temperature distribution of the reaction fluid with respect to an elapsed time (reaction time) after mixing by the mixer 13. In FIG. 2, the lower horizontal axis represents time, the upper horizontal axis represents position, and the vertical axis represents temperature (. degree. C.).

The curve g21 is a curve showing the measured temperature distribution obtained by the temperature measuring unit 16 when the first reactant a and the second reactant B are mixed in the flow reactor 10. At this time, the measured temperature after about T11 (position from the outlet L11 of the mixer 13) was T12, the measured temperature after T12 (position from the outlet L12 of the mixer 13) was T13, and the measured temperature after T13 (position from the outlet L13 of the mixer 13) was T14. Regarding the reaction parameters when the first reactant A and the second reactant B are mixed, Δ H (first reaction parameter) is, for example, 180kJ/mol,

(second reaction parameter) is, for example, 74 kJ/mol. In addition, the reaction parameters Δ H,

As will be described later.

Here, the mounting position of the temperature measuring unit 16 will be described.

In the temperature measuring unit 16, the first temperature measuring unit 161 is attached to a position before the reaction (p1 in fig. 1). The second to fourth temperature measuring units 162 to 164 are installed at positions (p2 to p4 in fig. 1) after the reaction. As shown in fig. 2, the positions where the second to fourth temperature measuring units 162 to 164 are installed are preferably positions where temperature changes of the reaction fluid immediately after the reaction due to the reaction heat of the first and second reactants a and B are captured. The temperature change of the reaction fluid immediately after the reaction is a temperature change in a short time such as a maximum value or a maximum value of the temperature change. Immediately after the reaction, the reaction rate is high because the concentration of the reactant is highest, and the amount of heat generated per unit time is large, so that a temperature change in a short time is likely to occur. The portion for capturing the temperature change of the reaction fluid immediately after the reaction is an arrangement portion that includes at least a portion that increases in temperature toward the peak of the temperature change (the temperature value of the maximum value or the maximum value) and a portion that decreases in temperature from the peak of the temperature change, with the peak position of the temperature change (the position of the maximum value or the maximum value that is the distance from the flow path of the mixer 13 or the elapsed time after the mixing) interposed therebetween.

Therefore, when the position of the maximum value is L4, the second temperature measurement unit 162 to the fourth temperature measurement unit 164 are attached to positions at which the change in the maximum value at the position is captured, for example, positions L3, L5, and L6.

In addition, in the case where the time or position at which the maximum value occurs is unknown, for example, 3 or more temperature measurement units 16 may be installed after the reaction. Further, the reaction analyzer 20 may select the temperature measuring unit 16 that captures a change in temperature immediately after the reaction based on the measured temperature.

< method for calculating reaction parameters based on temperature distribution of reaction field >

Next, a method of calculating a reaction parameter from the temperature distribution of the reaction field will be described.

Fig. 3 is a diagram for explaining a method of calculating a reaction parameter from a temperature distribution of a reaction field according to the first embodiment. The graph of the region denoted by reference numeral g1 shows an example of the temperature distribution before or during the parameter adjustment. In the graph of the region denoted by reference character g1, the horizontal axis represents position and the vertical axis represents temperature.

Found T1 is the temperature at position p 1. Found T2 is the temperature at position p 2. Found T3 is the temperature at position p 3. Found T4 is the temperature at position p 4.

Function T₁(x) Is thatThe solution of the governing equation (govering equation) for estimating the temperature distribution of the reaction fluid immediately after mixing is a function of temperature with respect to position x.

Estimate T₁(p1) is based on the function T₁(x) Is estimated from the temperature at position p 1. Estimate T₁(p2) is based on the function T₁(x) Is estimated from the temperature at position p 2. Estimate T₁(p3) is based on the function T₁(x) Is estimated from the temperature at position p 3. Estimate T₁(p4) is based on the function T₁(x) Is estimated from the temperature at position p 4.

I.e. the diagram of the region labeled g1 in fig. 3 (function T)₁(x) Graph of (d) represents an estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after mixing.

Δ T1 is the estimated value T at position p1₁(p1) and the measured value T1. Δ T2 is the estimated value T at position p2₁(p2) and the measured value T2. Δ T3 is the estimated value T at position p3₁(p3) and the measured value T3. Δ T4 is the estimated value T at position p4₁(p4) and the measured value T4.

That is, if the actual measurement result obtained by actually measuring the temperature of the reaction fluid (in this case, the actual measured temperature distribution) and the estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after mixing are compared, in the example shown in the region of reference numeral g1, the function T used is due to₁(x) Is inappropriate and therefore a large difference is generated between the estimated value and the measured value.

The graph of the area denoted by reference numeral g2 is an example of the temperature distribution after parameter adjustment. In the graph of the region denoted by reference character g2, the horizontal axis represents position and the vertical axis represents temperature.

Function T_n(x) Is the solution of the governing equation that estimates the temperature distribution of the reactive fluid immediately after mixing and is a function of temperature with respect to position x.

Estimate T_n(p1) is based on the function T_n(x) Is estimated from the temperature at position p 1. Estimate T_n(p2) is based on the function T_n(x) Is estimated from the temperature at position p 2. Estimate T_n(p3) is based onFunction T_n(x) Is estimated from the temperature at position p 3. Estimate T_n(p4) is based on the function T_n(x) Is estimated from the temperature at position p 4.

I.e. the diagram of the region labeled g1 in fig. 3 (function T)_n(x) Graph of (d) represents an estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after mixing.

Diagram of the region labeled g2 in FIG. 3 (function T)_n(x) Graph of (d), the estimated value T at the position p1_n(p1) and the difference between the measured value T1, i.e., Δ T1, the estimated value T at the position p2_n(p2) difference Δ T2 from measured value T2, estimated value T at position p3_n(p3) and the difference between the measured value T3, i.e., Δ T3, and the estimated value T at position p4_nThe difference between (p4) and the actually measured value T4, Δ T4, is very small within a predetermined value, and therefore, is not shown.

That is, if the measured temperature distribution obtained by measuring the temperature of the reaction fluid is compared with the estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after mixing, the function T used in the example shown in the region of reference numeral g2 is used_n(x) Therefore, the difference between the estimated value and the measured value is within a predetermined value. In the first embodiment, the difference between the estimated value and the measured value within the predetermined value is regarded as the measured value and the function T_n(x) And (5) the consistency is achieved.

In the first embodiment, the following reaction parameters are set: the reaction parameters are determined by a function T based on the measured values of the temperatures of the reaction fluids at the temperature measurement positions (corresponding to the positions x) by the temperature measurement unit 16 (the second temperature measurement unit 162 to the fourth temperature measurement unit 164)_n(x) The difference between the estimated values of the temperature of the reaction fluid at each position x is within a prescribed value.

Here, for the reaction parameter, function T_n(x) The description is given.

Function T_n(x) Is a solution of a governing equation for estimating the temperature distribution of the reaction fluid immediately after mixing, and is represented by the following formula (1) where the position x, the reaction parameter Δ H, and,

As a function of (c).

[ mathematical formula 1 ]

Or, function T_n(x) As shown in the following formula (2), the position x and the reaction parameter Δ H, E_aAs a function of (c).

[ mathematical formula 2 ]

T_n(x)≈f(x，ΔH，E_a)···(2)

The reaction parameter Δ H is the molar reaction enthalpy (kJ/mol). The molar reaction enthalpy is an amount representing the heat of reaction per mole (amount per unit substance). The maximum value (or maximum value) in the graph of fig. 3 of the relationship between the position and the temperature of the reaction parameter Δ H, that is, the peak value of the temperature distribution of the reaction fluid immediately after mixing.

Reaction parameters

Is activation free energy (kJ/mol). The activation free energy is the difference between the free energy before the reaction and the free energy in the transition state of the reaction, and indicates the temperature dependence of the reaction rate. Reaction parameters

The peak value and the peak position of the temperature distribution of the reaction fluid immediately after mixing.

Reaction parameter E_aIs the activation energy (kJ/mol). The activation energy is a parameter of an Arrhenius (Arrhenius) formula representing the relationship between the reaction rate and the temperature, and is the difference between the energy before the reaction and the energy in the transition state of the reaction, and represents the temperature dependence of the reaction rate. Reaction parameter E_aThe peak value and the peak position of the temperature distribution of the reaction fluid immediately after mixing.

In the following description, an actual measurement value (temperature distribution measurement value) T of temperature₀(x) Represented by the following formula (3).

[ mathematical formula 3 ]

T₀(x)＝(T1，T2，T3，T4)…(3)

Next, an example of a process of reaction analysis in the reaction analysis system 1 will be described.

Fig. 4 is a processing procedure of the reaction analysis of the first embodiment, and is a flowchart for determining the reaction state of the reaction fluid based on the temperature distribution of the reaction fluid immediately after mixing along the flow direction of the reaction fluid. In the following processing, the reaction parameters Δ H,

The case (1).

(step S11) the reaction analyzer 20 acquires information on the temperature measured by the temperature measuring unit 16 (measured temperature distribution obtained by measuring the temperature of the reaction fluid). In this way, the reaction analyzer 20 reads the temperature distribution measurement value T₀(x) In that respect In addition, the reaction analysis apparatus 20 stores the position x (p1 to p4 in fig. 1) where the temperature measurement unit 16 is installed.

(step S12) the reaction analyzer 20 temporarily sets the reaction parameters Δ Hn,

And calculating a temperature distribution calculation value T_n(x) (an estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after mixing is obtained). When the process of step S12 is the first time, the reaction analyzer 20 changes the reaction parameter Δ H₁、

Set to an initial value stored therein, for example, and calculate a temperature distribution calculation value T₁(x)。

(step S13) the reaction analyzer 20 calculates the function T_n(x) The difference Δ Tm between the estimated temperature value of each position pm (m is an integer of 1 to 4, for example) and the measured temperature value Tm of each position pm actually measured by the temperature measuring unit 16 (the actually measured temperature distribution and the estimated temperature distribution are compared). The reaction analyzer 20 discriminates Δ T1 (T1-T) when 4 measurement sites of temperature are present_n(p1))、Δt2(＝T2－T_n(p2))、Δt3(＝T3－T_n(p3))、Δt4(＝T4－T_n(p4)) is within the predetermined value stored in the device, and T is determined_n(x) Whether or not to be associated with T₀(x) Are substantially identical. The reaction analyzer 20 judges that T is present_n(x) And T₀(x) If they are substantially the same (step S13; y), the process proceeds to step S15. The reaction analyzer 20 judges that T is present_n(x) And T₀(x) If the two pieces do not substantially match (step S13; n), the process proceeds to step S14. The predetermined value used for the comparison between the measured temperature distribution and the estimated temperature distribution may be set for each measurement site in common or may be set for each measurement site individually.

(step S14) the reaction analyzer 20 adjusts the value of the reaction parameter. For example, when all of Δ t1 to Δ t4 are positive, the reaction parameter Δ H is set to be the ratio Δ H₁Large value to increase the height of the maximum. For example, when Δ t1 to Δ t4 are all negative, the reaction parameter Δ H is set to be the ratio Δ H₁Small value to reduce the height of the maximum. After the processing, the reaction analyzer 20 returns to the processing of step S12. In addition, if only Δ t2 is negative and the other is positive (for example, if the peak position of the estimated temperature distribution is located rearward of the measured temperature distribution), the peak position is assumed to be set to be negative

To a smaller value so that the peak position of the estimated temperature distribution is located forward.

(step S15) the reaction analyzer 20 outputs the reaction parameters Δ H,

(step S16) the reaction analyzer 20 calculates the concentration distribution p (x) of the product and the reactant, and outputs the calculated concentration distribution p (x) of the product and the reactant.

Further, the reaction parameters are Δ H,

In the case of (3), the concentration distribution p (x) of the product and the reactant calculated and outputted by the reaction analyzer 20 is obtained by solving the differential equation of the following formula (4).

[ mathematical formula 4 ]

In formula (4) [ A ]]Is the concentration of the first reactant A, [ B ]]Is the concentration of the second reactant B, h is the Planckian constant (6.62607004X 10)^-34(m²kg/s))，k_BIs Boltzmann constant (1.380649 × 10)^-23(JK^-1) R is the gas constant and T is the temperature of the fluid.

In addition, the reaction parameter is Δ H, E_aIn the case of (3), the concentration distribution p (x) of the product and the reactant calculated and outputted by the reaction analyzer 20 is represented by the following formula (5).

[ math figure 5 ]

In the formula (5), [ A ] is the concentration of the first reactant A, [ B ] is the concentration of the second reactant B, A is the frequency factor in the Arrhenius formula (Arrhenius equalisation), R is the gas constant, and T is the temperature of the fluid.

Fig. 5 is a graph showing the positional change (temporal change) of the concentrations of the reactant and the product. In fig. 5, the lower horizontal axis represents time, the upper horizontal axis represents position, and the vertical axis represents concentrations of the reactant and the product. In addition, the value relative to the vertical axis of the first reactant a and the second reactant B represents the concentration of the reactants. Fig. 5 shows an example of the result of the reaction analyzer 20 converting the obtained concentration into the yield by obtaining the concentration distribution p (x) of the product and the reactant using the obtained reaction parameter and the formula (4) or the formula (5). The yield is a ratio of the yield in the reaction to the theoretical yield. The yield is the amount of the product actually obtained. The theoretical yield is the maximum amount theoretically attainable relative to the substrate (based-pouenin) or reagent used.

Curve g31 is the time versus concentration, the location versus concentration of the first reactant a after mixing.

Curve g32 is the time versus concentration, the location versus concentration of the second reactant B after mixing.

The curve g33 shows the relationship between the time and yield of the product after mixing and the relationship between the position and yield.

In the example of fig. 5, the concentration of the first reactant a is approximately 0 at t1 to t2, the concentration of the second reactant B converges to [ B ] x at t1 to t2, and the concentration of the product converges to [ P ] x at t1 to t 2.

In this way, in the first embodiment, by estimating the reaction parameters using the actual measurement values, the concentrations of the reactants and the products and the reaction speed at an arbitrary position and an arbitrary time in the flow reactor can be estimated.

Further, by estimating the concentration, the yield of the product at an arbitrary position and an arbitrary time in the flow reactor can be estimated.

< example of construction of reaction Analyzer 20 >

Next, a configuration example of the reaction analyzer 20 will be described.

Fig. 6 is a diagram showing a configuration example of the reaction analyzer 20 according to the first embodiment. As shown in fig. 6, the reaction analyzer 20 includes an external storage device 21, an internal storage device 22, a CPU 23, an input device 24, and an output device 25. The external storage device 21 includes an experimental data storage unit 211, a fluid physical property data storage unit 212, a reactor thermal characteristic data storage unit 213, a reaction data storage unit 214, a calculation data storage unit 215, and a reaction analysis program storage unit 216.

The external storage device 21, the internal storage device 22, the CPU 23, the input device 24, and the output device 25 are connected via a system bus 26.

The experiment data storage unit 211 stores experiment data (for example, temperatures measured by various sensors and the like). The fluid physical property data storage portion 212 stores fluid physical property data (for example, density, specific heat, thermal conductivity, viscosity coefficient, and the like) as constants or variables necessary for analysis. The reactor thermal characteristic data storage unit 213 stores reactor thermal characteristic data (for example, thermal conductivity, specific heat, and the like of a wall surface in the flow reactor) as constants or variables necessary for analysis. The reaction data storage unit 214 stores reaction data (for example, data relating to a chemical reaction formula, that is, reaction parameters). The operation data storage unit 215 stores operation data (for example, various distributions such as temperature, flow rate, and concentration obtained by an equation). The reaction analysis program storage unit 216 stores a reaction analysis program (for example, a program for solving a simulation for calculating an estimated temperature distribution).

The internal storage device 22 temporarily stores data under analysis (e.g., reaction parameters, various distributions, etc.).

The CPU 23 is, for example, a personal computer, and performs control of the reaction analysis system 1, acquisition of data, analysis and estimation of data.

The input device 24 is, for example, a keyboard, a mouse, a touch panel sensor provided on the display device, or the like, and is a device for detecting an operation by a user.

The output device 25 is an output device such as a liquid crystal display device, an organic EL (Electro Luminescence) display device, or a printer.

Fig. 7 is a diagram showing a connection example and a configuration example of the reaction analyzer 20 according to the first embodiment. As shown in fig. 7, the CPU 23 includes a control unit 231, a calculation unit 232, a determination unit 233, and a parameter adjustment unit 234. The experimental data storage unit 211, the fluid physical property data storage unit 212, the reactor thermal property data storage unit 213, the reaction data storage unit 214, and the calculation data storage unit 215 are connected to the control unit 231.

The control unit 231 acquires the actual measurement value of the temperature of the reaction fluid in the temperature measurement unit 16 (the process of step S11 in fig. 4). The controller 231 calculates the estimated reaction parameters Δ H,

(or E)_a) And outputs the result to the reaction data storage unit 214 (step S15 in fig. 4). The control unit 231 may control the set temperature (reactant and reaction) of the temperature regulator 15The temperature of the fluid). The control unit 231 may control the set flow rates (flow rates of the reactant and the reaction fluid) of the first pump 11 and the second pump 12.

The calculating part 232 calculates the temperature distribution calculation value T_n(x) (the process of step S12 of fig. 4). The calculation unit 232 calculates the concentration distribution p (x) of the product and the reactant (the process of step S16 in fig. 4).

The determination unit 233 determines the temperature measured by the temperature measurement unit 16 from the temperature distribution_n(x) Whether all the differences between the estimated values of the temperatures of (1) are within the predetermined values stored in the device itself, to thereby determine T_n(x) Whether or not to be associated with T₀(x) Substantially match each other (step S13 in fig. 4).

The parameter adjusting unit 234 adjusts the reaction parameter Δ H,

(or E)_a) (the process of step S14 of fig. 4).

The configurations shown in fig. 6 and 7 are merely examples, and are not limited thereto. For example, the external storage device 21 may be connected to the internal storage device 22, the CPU 23, the input device 24, and the output device 25 via a network. The internal storage device 22 may include each storage unit of the external storage device 21.

<Function T representing temperature distribution_n(x)>

Here, the function T representing the temperature distribution is explained_n(x) An example of the method of (1) is described.

The CPU 23 solves the following 3 equations, for example, approximation (approximation), as a one-dimensional space to obtain a function T representing the temperature distribution_n(x) In that respect In addition, the CPU 23 may approximate the 3 expressions to, for example, a two-dimensional space or more to solve the approximation.

The governing equations in the fluid simulation include 3 of the mass conservation equation of the following equation (6), the momentum conservation equation of the following equation (7), and the energy conservation equation of the following equation (8).

[ mathematical formula 6 ]

[ mathematical formula 7 ]

[ mathematical formula 8 ]

In the formulae (6) to (8), ρ_sIs the density of the chemical species s, u is the flow velocity vector of the reaction fluid, M_sIs the molecular weight of chemical species s, J_sIs the diffusion mass flux of chemical species s, omega_sIs the molar production rate of the chemical species s, ρ is the density of the reaction fluid, and p is the pressure of the reaction fluid. I is the unit tensor, V is the viscous stress tensor, T is the temperature of the reaction fluid, h_sIs the molar enthalpy of formation of the chemical species s, N is the number (type) of product, and cv is the volumetric specific heat of the reaction fluid.

In the above example, the example in which the number of products obtained by mixing the first reactant and the second reactant is 1 was described, but the number of products may be 2 or more.

When the concentration of the reactant, the concentration of the product, and the yield in the flow reactor and the reaction rate thereof are estimated by a conventional method, the treatment takes about 1 day because the concentration and the yield are estimated by a successive approximation method (cut and try). According to the first embodiment, by measuring the temperature distribution of the flow-path-shaped reactor (flow reactor), the reaction parameters such as the activation free energy of the chemical reaction can be calculated in a short time without performing a plurality of experiments. According to the first embodiment, by performing a reaction simulation using the calculated reaction parameters, even when the operating conditions such as concentration and temperature and the structure of the reactor are changed, the rate and concentration of the product generated at an arbitrary position in the reaction can be analyzed.

In addition, according to the first embodiment, by measuring the temperature before and after the mixer, it is possible to cope with the reaction immediately after the mixing.

In addition, according to the first embodiment, even a subject having a large change in flow velocity such as a gas in which the fluid itself is a reactant can be dealt with by using a fluid simulation including a law of conservation of momentum.

Further, according to the first embodiment, the concentration of the product at an arbitrary position in the channel shape can be estimated in real time in several seconds or so using the estimated reaction parameters.

Further, according to the first embodiment, since the concentration of the product at an arbitrary position in the flow path shape can be estimated in real time in several seconds or so, the number of steps required for optimizing the reaction conditions can be reduced to about 1/100 or less in the related art. In addition, in the conventional method, since there are many parameters, successive approximation is required, and thus, there are many man-hours.

Further, according to the first embodiment, since the number of steps for measuring the concentration, calculating the parameter, and the like can be reduced, it is possible to realize a high throughput, that is, to make the efficiency of data acquisition 100 times or more under the conditions that have been a problem in chemical informatics (cheminformatics).

Further, according to the first embodiment, the estimated concentration of the product at an arbitrary position in the flow path shape can be converted into the yield, and thus the present invention can be applied to the hardware design of the reactor such as the optimum flow path length, the flow path inner diameter of the reactor, the flow path wall thickness, and the thermal characteristics such as the material.

Here, regarding the yield, the yield at time t when 1 product P is produced from the first reactant a and the second reactant B is as shown in the following formula (9).

[ mathematical formula 9 ]

Yield (t) ═ P](t)/min{[A]₀，[B]₀}…(9)

In the above formula, [ P ]](t) is the concentration of product P at time t, [ A ]]₀Is the input concentration of the first reactant A, [ B ]]₀Is the input concentration of the second reactant B and min is a function of the extraction minimum.

< application example >

The reaction analysis system 1 of the first embodiment can be applied to, for example, the following apparatuses or systems.

A first application example is a soft sensor for reaction monitoring. In this application example, the concentrations of the reactant and the product can be calculated in real time from the temperature measurement result.

The second application example is a system that controls a chemical reaction by controlling operating conditions such as temperature, flow rate, material concentration, and switching of a reaction channel described later, based on the output result of the soft sensor of the first application example. In this application example, the reaction can be controlled while monitoring the reaction on-line in real time without sampling the reaction fluid and measuring the concentration of the product.

The third application example is a production technique for producing a raw material of a pharmaceutical product or a functional raw material of a fine chemical by using the reaction control system of the second application example. In this application example, the raw material can be produced while monitoring the reaction fluid (reaction) on-line in real time without sampling the reaction fluid and measuring the concentration of the product.

The above application example is an example, and is not limited to this. The reaction analysis system 1 may be applied to other systems, apparatuses, processes, and the like.

The reaction analysis system 1 and the reaction analysis apparatus 20 as described above can be applied not only to the flow reactor 10 in which a chemical reaction of a reaction fluid is performed by mixing a plurality of reactants but also to the flow reactor 10 described in the second embodiment below.

(second embodiment)

A second embodiment of the present invention will be described below. In the following description, the same or equivalent structures as those of the above-described embodiment are denoted by the same reference numerals, and the description thereof is simplified or omitted.

Fig. 8 is a block diagram showing a configuration example of a reaction analysis system 1A according to a second embodiment. The reaction analysis system 1A shown in fig. 8 includes a flow reactor 10 for performing a chemical reaction of a reaction fluid by contact of the reaction fluid with a catalyst 30. The flow reactor 10 includes a liquid feeding pipe 111, a reaction pipe 14, a discharge pipe 113, and a catalyst 30.

The reaction tube 14 accommodates a catalyst 30. The reaction tube 14 has an inlet and an outlet. A liquid feeding pipe 111 is connected to the inlet of the reaction tube 14. A discharge pipe 113 is connected to the discharge port of the reaction tube 14.

The temperature measuring unit 16 includes first to fifth temperature measuring units 161 to 165. The first temperature measuring unit 161 is provided at a position p1 of the liquid feeding tube 111 on the upstream side (before the reaction) of the reaction tube 14. The second to fifth temperature measuring units 162 to 165 are provided in the reaction tube 14 in the order of the position p2 to the position p5 along the flow of the reaction fluid. The second to fifth temperature measuring units 162 to 165 can measure the temperature (temperature distribution) of the reaction fluid immediately after contact with the catalyst 30 (immediately after the start of the reaction) in the flow direction of the reaction fluid.

The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analysis device 20 determines the reaction state of the reaction fluid caused by the contact of the reaction fluid with the catalyst 30 using the acquired information indicating the temperature.

Fig. 9 is a block diagram showing a configuration example of a reaction analysis system 1B according to a modification of the second embodiment.

The reaction analysis system 1B shown in fig. 9 includes a flow reactor 10 that performs a chemical reaction of a reaction fluid by irradiating the reaction fluid with an electromagnetic wave 31A. The reaction analysis system 1B includes an electromagnetic wave irradiation device 31. The electromagnetic wave irradiation device 31 irradiates the reaction flow path of the flow reactor 10 with an electromagnetic wave 31A.

The temperature measuring unit 16 includes first to fifth temperature measuring units 161 to 165. The first temperature measuring unit 161 is provided at a position p1 on the upstream side (before reaction) of the irradiation range of the electromagnetic wave 31A. The second temperature measuring unit 162 to the fifth temperature measuring unit 165 are provided in the order of the position p2 to the position p5 along the flow of the reaction fluid within the irradiation range of the electromagnetic wave 31A. The second to fifth temperature measuring units 162 to 165 can measure the temperature (temperature distribution) of the reaction fluid immediately after the irradiation of the electromagnetic wave 31A (immediately after the start of the reaction) along the flow direction of the reaction fluid.

The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analysis device 20 determines the reaction state of the reaction fluid by irradiating the reaction fluid with the electromagnetic wave 31A using the acquired information indicating the temperature.

Fig. 10 is a block diagram showing a configuration example of a reaction analysis system 1C according to a modification of the second embodiment.

The reaction analysis system 1C shown in fig. 10 includes a reactor flow 10 for performing a chemical reaction of a reaction fluid by irradiating the reaction fluid with an electromagnetic wave 31A, similarly to the reaction analysis system 1B shown in fig. 9. The flow reactor 10 includes a liquid feeding tube 111, a spiral reaction tube 14, a discharge tube 113, and an electromagnetic wave irradiation device 31.

The reaction tube 14 spirally surrounds the electromagnetic wave irradiation device 31. The electromagnetic wave irradiation device 31 irradiates electromagnetic waves 31A from the radially inner side to the radially outer side of the spiral reaction tube 14.

The temperature measuring unit 16 includes first to fifth temperature measuring units 161 to 165. The first temperature measuring unit 161 is disposed at a position p1 of the liquid feeding tube 111 on the upstream side (before reaction) of the irradiation range of the electromagnetic wave 31A. The second temperature measuring unit 162 to the fifth temperature measuring unit 165 are provided in the reaction tube 14, which is the irradiation range of the electromagnetic wave 31A, in the order of the position p2 to the position p5 along the flow of the reaction fluid. The second to fifth temperature measuring units 162 to 165 can measure the temperature (temperature distribution) of the reaction fluid immediately after the irradiation of the electromagnetic wave 31A (immediately after the start of the reaction) along the flow direction of the reaction fluid.

The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analysis device 20 determines the reaction state of the reaction fluid by irradiating the reaction fluid with the electromagnetic wave 31A using the acquired information indicating the temperature.

Fig. 11 is a block diagram showing a configuration example of a reaction analysis system 1D according to a modification of the second embodiment.

The reaction analysis system 1D shown in fig. 11 includes a flow reactor 10 that heats a reaction fluid to cause a chemical reaction of the reaction fluid. The reaction analysis system 1D includes a heating device 32 (heater) for heating the reaction fluid flowing through the flow reactor 10. The heating device 32 is disposed along the reaction flow path of the flow reactor 10.

The temperature measuring unit 16 includes first to fourth temperature measuring units 161 to 164. The first temperature measuring unit 161 is provided at a position p1 on the upstream side (before reaction) of the region opposed to the heating device 32. The second to fourth temperature measuring units 162 to 164 are provided in the order of position p2 to position p4 along the flow of the reaction fluid in the region facing the heating device 32. The second to fourth temperature measuring units 162 to 164 can measure the temperature (temperature distribution) of the reaction fluid immediately after heating (immediately after the start of the reaction) in the flow direction of the reaction fluid.

The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analyzer 20 determines the reaction state of the reaction fluid caused by heating the reaction fluid, using the acquired information indicating the temperature.

Fig. 12 is a block diagram showing a configuration example of a reaction analysis system 1E according to a modification of the second embodiment.

Like the reaction analysis system 1D shown in fig. 11, the reaction analysis system 1E shown in fig. 12 includes a flow reactor 10 that heats the reaction fluid to cause a chemical reaction of the reaction fluid. The flow reactor 10 includes a liquid feeding pipe 111, a spiral reaction pipe 14, a discharge pipe 113, and a heating device 32.

The reaction tube 14 is helically wrapped around the heating device 32. The heating device 32 heats the spiral reaction tube 14 from the radially inner side.

The temperature measuring unit 16 includes first to fifth temperature measuring units 161 to 165. The first temperature measuring unit 161 is provided at a position p1 of the liquid feeding tube 111 on the upstream side (before the reaction) of the reaction tube 14. The second to fifth temperature measuring units 162 to 165 are provided in the reaction tube 14, which is an area facing the heating device 32, in the order of the position p2 to the position p5 along the flow of the reaction fluid. The second to fifth temperature measuring units 162 to 165 can measure the temperature (temperature distribution) of the reaction fluid immediately after heating (immediately after the reaction) along the flow direction of the reaction fluid.

The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analysis device 20 determines the reaction state of the reaction fluid caused by heating the reaction fluid using the acquired information indicating the temperature.

Fig. 13 is a block diagram showing a configuration example of a reaction analysis system 1F according to a modification of the second embodiment.

The reaction analysis system 1F shown in fig. 13 includes a flow reactor 10 that performs a chemical reaction of a reaction fluid by applying an electric current to the reaction fluid. The reaction analysis system 1F includes an energization device 33 for energizing the reaction fluid flowing through the flow reactor 10. The energization unit 33 includes a pair of electrodes 33a disposed so as to sandwich the reaction flow path of the flow reactor 10.

The temperature measuring unit 16 includes first to fifth temperature measuring units 161 to 165. The first temperature measuring unit 161 is provided at a position p1 on the upstream side (before reaction) of the region where the pair of electrodes 33a face each other. The second to fifth temperature measuring units 162 to 165 are provided in the order of position p2 to position p5 along the flow of the reaction fluid in the region where the pair of electrodes 33a face each other. The second to fifth temperature measuring units 162 to 165 can measure the temperature (temperature distribution) of the reaction fluid immediately after the energization (after the reaction starts) along the flow direction of the reaction fluid.

The reaction analyzer 20 acquires information indicating the measured temperature output from the temperature measuring unit 16. The reaction analysis device 20 determines the reaction state of the reaction fluid caused by the current applied to the reaction fluid using the acquired information indicating the temperature.

The reaction analysis system 1(1A to 1F) and the reaction analysis device 20 as described above can be applied not only to the determination of the reaction state of the reaction fluid in each flow reactor 10, but also to the control of the reaction conditions of the reaction fluid based on the estimated value of the determined reaction state (the estimated concentration of the reactant, etc.) as described in the following third embodiment.

(third embodiment)

A third embodiment of the present invention will be explained below. In the following description, the same or equivalent structures as those of the above-described embodiment are denoted by the same reference numerals, and the description thereof is simplified or omitted.

Fig. 14 is a block diagram showing a configuration example of a reaction analysis system 1G according to the third embodiment.

The reaction analysis system 1G shown in fig. 14 includes a liquid feeding tube 111, a reaction tube 14, and a plurality of discharge tubes 113A to 113D. The reaction tube 14 is provided with any one of the catalyst 30, the electromagnetic wave irradiation device 31, the heating device 32, and the energization device 33.

The temperature measuring unit 16 includes first to tenth temperature measuring units 161 to 170. The first temperature measuring unit 161 is provided at a position p1 of the liquid feeding tube 111 on the upstream side (before the reaction) of the reaction tube 14. The second temperature measuring unit 162 to the first 0 temperature measuring unit 170 are provided in the reaction tube 14 in the order of the position p2 to the position p10 along the flow of the reaction fluid.

A plurality of valves 114a to 114c are provided on the reaction tube 14. Specifically, the valve 114a is disposed between the position p4 and the position p 5. The valve 114b is disposed between the position p7 and the position p 8. The valve 114c is disposed on the downstream side of the position p 10.

The discharge pipe 113A is connected to the upstream side of the valve 114a of the reaction tube 14, i.e., between the position p3 and the position p 4. Discharge pipe 113A is provided with a valve 113A. The discharge pipe 113B is connected to the reaction tube 14 on the downstream side of the valve 114a and on the upstream side of the valve 114B, i.e., between the position p6 and the position p 7. Discharge pipe 113B is provided with a valve 113B.

The discharge pipe 113C is connected to the reaction tube 14 on the downstream side of the valve 114b and on the upstream side of the valve 114C, i.e., between the position p9 and the position p 10. A valve 113b is provided in the discharge pipe 113C. The discharge pipe 113D is connected to the discharge port of the reaction tube 14 on the downstream side of the valve 114c of the reaction tube 14.

The valves 113a to 113c and the valves 114a to 114c are connected to the reaction analyzer 20, and are controlled by a control unit 231 (see fig. 7 described above) to switch the reaction flow paths and adjust the flow rates of the reaction fluids. The controller 231 compares the estimated value indicating the reaction state of the reaction fluid thus determined with a predetermined target value, and controls the reaction conditions of the reaction fluid in the flow reactor 10.

For example, in the case where the catalyst 30 is provided in the reaction tube 14, the reaction conditions of the reaction fluid may be controlled by switching the reaction flow path in the flow reactor 10. Specifically, the reaction fluid is discharged from the discharge pipe 113A by closing the valve 114a of the reaction tube 14 and opening the valve 113A of the discharge pipe 113A, whereby the distance that the reaction fluid contacts the catalyst 30 in the reaction tube 14 can be shortened. Similarly, in order to discharge the reaction fluid from any one of the discharge pipes 113A to 113D, the reaction conditions of the reaction fluid can be controlled by opening and closing the valves 113A to 113c and the valves 114a to 114 c.

In addition, in the case where any one of the electromagnetic wave irradiation device 31, the heating device 32, and the energization device 33 is provided in the reaction tube 14, similarly, the reaction conditions of the reaction fluid can be controlled by switching the reaction flow path in the flow reactor 10. In the case of the electromagnetic wave irradiation device 31, the heating device 32, and the energization device 33, the reaction conditions of the reaction fluid can be controlled without switching the reaction flow path. For example, in the case of the electromagnetic wave irradiation device 31, the reaction conditions can be controlled by moving an electromagnetic wave shielding wall, not shown, to vary the irradiation range of the electromagnetic wave 31A or to vary the output of the irradiation of the electromagnetic wave. In the case of the heating device 32, the reaction conditions can be controlled by varying the heating temperature. In the case of the energization device 33, the reaction conditions can be controlled by varying the energization amount.

Fig. 15 is a flowchart showing a procedure of reaction condition control from the start of reaction analysis according to the third embodiment. Fig. 16 is a graph showing a relationship between a position and an estimated temperature and a relationship between a position and an estimated concentration.

The control unit 231 controls the reaction conditions of the reaction fluid according to the flowchart shown in fig. 15. In the third embodiment, the control equation in the fluid simulation uses an energy conservation equation represented by the following formula (10) in which the above formula (8) is improved.

[ MATHEMATICAL FORMULATION 10 ]

The expression (10) is the expression (8) with Q added thereto. In the flow reactor 10, when a chemical reaction of the reaction fluid is performed by irradiating the reaction fluid with electromagnetic waves, Q is represented by the following formula (11). In the flow reactor 10, when a chemical reaction of the reaction fluid is performed by applying an electric current to the reaction fluid, Q is represented by the following formula (12). In addition, Q is 0 (zero) in the other cases.

[ mathematical formula 11 ]

Q＝f(κ，I)…(11)

[ MATHEMATICAL FORMULATION 12 ]

Q＝f(σ，i)…(12)

Equation (11) considers heat generation due to radiation heat generation caused by irradiation of electromagnetic waves to the reaction fluid, κ is an absorption coefficient of radiation, and I is an output of the electromagnetic wave irradiation device 31. In addition, equation (11) can be calculated strictly from radiation analysis or electromagnetic field analysis. Equation (12) considers electrothermal heat generation by energization of the reaction fluid, where σ is the electrical conductivity and i is the current value. In addition, equation (12) can be calculated strictly from electromagnetic field analysis.

The flowchart shown in fig. 15 is a flowchart in which step S17 and step S18 are added to step S11 to step S16 shown in fig. 4. Therefore, the explanation of step S11 to step S16 is omitted for redundancy.

(step S17) the controller 231 determines an estimated value P at the outlet of the flow channel of the flow reactor 10 (x is the outlet of the reaction tube 14) based on the concentration distribution P (x) of the product and the reactant calculated in step S16, and determines whether or not the estimated value P is at a predetermined target value P_setThe above. Further, it is judged that the estimated value P has reached a predetermined target value P_setWhether or not the residence time (time) of the reaction fluid up to the outlet of the flow path of the flow reactor 10 is minimized (minimum). Determination of step S17 by control unit 231 "If no, the process proceeds to step S18.

(step S18) the control unit 231 sets the estimated value P of the outlet of the flow path of the flow reactor 10 to the target value P_setThe first control described above and the process of making the estimated value P reach the target value P_setA second control for minimizing the residence time of the reaction fluid at the outlet of the flow path of the flow reactor 10. In addition, the second control is control for suppressing a side reaction of the reaction fluid.

As a specific example of the first control, the estimated value P (estimated concentration) at the outlet of the flow path of the flow reactor 10 is lower than the target value P_set(target concentration) in the case of (P! (x)<P_setIn the case of (3), the control unit 231 controls the valves 114a to 114c to reduce the flow rate of the reaction fluid and extend the residence time in the reaction channel, thereby extending the reaction time. For example, the control unit 231 controls the valves 113a to 113c and 114a to 114c to switch the reaction channels and extend the channel length, thereby extending the reaction time. For example, the control unit 231 increases the output of the actuators (the electromagnetic wave irradiation device 31, the heating device 32, and the energization device 33) to increase the reactivity of the reaction fluid.

As a specific example of the second control, when the estimated value P (estimated concentration) reaches the target value P_setWhen the residence time from the (target concentration) to the outlet of the flow channel of the flow reactor 10 is long, the control unit 231 controls the valves 114a to 114c to increase the flow rate of the reaction fluid and shorten the residence time in the reaction flow channel. For example, the control unit 231 controls the valves 113a to 113c and 114a to 114c to switch the reaction flow paths and shorten the flow path length, thereby shortening the reaction time. For example, the control unit 231 decreases the output of the actuators (the electromagnetic wave irradiation device 31, the heating device 32, and the energization device 33) to decrease the reactivity of the reaction fluid, thereby extending the time until the target value P is reached_set(target concentration).

After step S18, the process returns to step S11, and the concentration distribution p (x) of the product and the reactant is obtained in the same manner as in the first embodiment. If yes is determined in step S17, the process is terminated as an ideal reaction condition is obtained.

According to the third embodiment as described above, not only the reaction states of the reaction fluids in the respective flow reactors 10 can be determined, but also the reaction conditions in the flow reactor 10 can be controlled so as to suppress side reactions of the reaction fluids and obtain the reactant of the target concentration.

While the embodiments for carrying out the present invention have been described above with reference to the embodiments, the present invention is not limited to the embodiments, and various modifications and substitutions can be made without departing from the spirit of the present invention.

For example, in the above-described one embodiment, in order to grasp the peak position of the temperature distribution of the reaction fluid, the peak position of the temperature distribution of the reaction fluid is detected from a part of the temperature measuring unit 16 (for example, the second temperature measuring unit 162 and the third temperature measuring unit 163 disposed so as to sandwich the peak position of the temperature distribution of the reaction fluid). In this way, although the temperature measuring unit is provided at a plurality of positions in the reaction flow path of the flow reactor, when it is assumed that the peak position of the temperature distribution of the reaction fluid is located before and after the first temperature measuring unit, the temperature measuring unit may be the first temperature measuring unit alone. Specifically, this corresponds to a case where the first temperature measuring unit is provided in the vicinity of the reaction start point of the reaction fluid. In this case, when the flow velocity of the reaction fluid is sufficiently high, it is assumed that a temperature peak appears behind the first temperature measurement unit, and therefore, even if there is only one temperature measurement unit, the estimated temperature distribution can be obtained from the control equation described above based on the measurement result thereof.

In the above-described embodiment, in step S18 shown in fig. 15, the estimated value P of the outlet of the flow path of the flow reactor 10 is set to the target value P_setThe first control described above and the estimated value P to the target value P_setThe second control for minimizing the residence time of the reaction fluid up to the outlet of the flow path of the flow reactor 10 is not necessary in some cases, and therefore, only the first control may be performed.

In this specification, words such as "front, rear, up, down, right, left, vertical, horizontal, vertical, transverse, row and column" refer to these directions in the apparatus of the invention. Therefore, these words in the description of the invention should be interpreted relatively in the device of the invention.

The term "configured" is used to indicate a structure, an element, or a part of a device, and is configured to perform a function of the present invention.

Furthermore, the term "Means plus function" in the claims shall include all configurations that can be used to perform the function included in the present invention.

The term "unit" is used to indicate a component, unit, hardware, or part of software that is programmed to perform a desired function. Typical examples of hardware are, but not limited to, devices or circuits.

The preferred embodiments of the present invention have been described above, but the present invention is not limited to these embodiments. Additions, omissions, substitutions, and other modifications can be made in the structure without departing from the spirit of the invention. The invention is not limited by the foregoing description but is only limited by the appended claims.

Claims (20)

1. A reaction analysis apparatus for determining a reaction state of a reaction fluid flowing in a flow reactor, comprising:

the processing unit determines the reaction state of the reaction fluid based on a reaction parameter indicating the reaction state of the reaction fluid obtained from a temperature distribution of the reaction fluid immediately after the start of the reaction along the flow direction of the reaction fluid.

2. The reaction analysis apparatus according to claim 1,

the processing unit obtains the reaction parameter by comparing a measured result obtained by measuring the temperature of the reaction fluid with an estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after the start of the reaction.

3. The reaction analysis apparatus according to claim 2,

the estimated temperature distribution is obtained by a governing equation that estimates the temperature distribution of the reaction fluid immediately after the start of the reaction,

the governing equation has a first reaction parameter related to a peak of a temperature distribution of the reaction fluid immediately after the start of the reaction, and a second reaction parameter related to a peak position of the temperature distribution of the reaction fluid immediately after the start of the reaction.

4. The reaction analysis apparatus according to claim 3,

the first reaction parameter represents a calorific value per unit amount of a substance,

the second reaction parameter represents a temperature dependence of the reaction rate.

5. The reaction analysis apparatus according to claim 3,

the processing unit adjusts the first reaction parameter and the second reaction parameter so that a difference between the actual measurement result and the estimated temperature distribution is within a predetermined value, and stores the adjusted first reaction parameter and second reaction parameter in a storage unit.

6. The reaction analysis apparatus according to claim 5,

the processing unit calculates at least one of a reaction rate of the reaction fluid, a concentration of the plurality of reactants, and a concentration or a yield of a product contained in the reaction fluid, based on the first reaction parameter and the second reaction parameter stored in the storage unit.

7. The reaction analysis apparatus according to any one of claims 1 to 6,

the reaction device is provided with a control unit that compares the reaction state of the reaction fluid determined by the processing unit with a target value of the reaction state, and controls the reaction conditions of the reaction fluid in the flow reactor.

8. The reaction analysis apparatus according to claim 7,

the control unit performs first control for setting the reaction state at the flow path outlet of the flow reactor to the target value or more.

9. The reaction analysis apparatus according to claim 8,

the control unit performs a second control that minimizes a residence time until the reaction fluid reaches the outlet of the flow path of the flow reactor after the reaction state reaches the target value.

10. A reaction analysis system for determining a reaction state of a reaction fluid flowing in a flow reactor, comprising:

a temperature measuring unit that measures the temperature of the reaction fluid along the reaction flow path of the flow reactor; and

the reaction analysis apparatus according to claim 1,

the processing unit determines the reaction state of the reaction fluid based on a reaction parameter indicating the reaction state of the reaction fluid obtained from the actual measurement result obtained by the temperature measuring unit.

11. The reaction analysis system of claim 10,

the temperature measuring unit is provided so as to sandwich at least a peak position of a temperature distribution of the reaction fluid in the reaction channel.

12. The reaction analysis system according to claim 10 or 11,

the flow reactor is provided with:

a plurality of supply channels that supply a plurality of reactants for chemical reactions, respectively;

a mixer connected to the plurality of supply flow paths and mixing a plurality of reactants; and

and a reaction channel connected to the mixer and through which a reaction fluid obtained by mixing a plurality of reactants flows.

13. The reaction analysis system according to claim 10 or 11,

the flow reactor is provided with a catalyst for causing a chemical reaction of a reaction fluid to proceed.

14. The reaction analysis system according to claim 10 or 11,

the reactor is provided with an electromagnetic wave irradiation device for irradiating the reaction fluid flowing in the flow reactor with electromagnetic waves.

15. The reaction analysis system according to claim 10 or 11,

the reactor is provided with a heating device for heating the reaction fluid flowing through the flow reactor.

16. The reaction analysis system according to claim 10 or 11,

the reactor is provided with an energizing means for energizing the reaction fluid flowing through the flow reactor.

17. A reaction analysis method for determining a reaction state of a reaction fluid flowing in a flow reactor, comprising:

the reaction state of the reaction fluid is determined by the processing unit based on a reaction parameter indicating the reaction state of the reaction fluid obtained from the temperature distribution of the reaction fluid immediately after the start of the reaction along the flow direction of the reaction fluid.

18. The reaction analysis method according to claim 17,

the reaction parameter is acquired by comparing, by the processing unit, an actual measurement result obtained by actually measuring the temperature of the reaction fluid with an estimated temperature distribution obtained by estimating the temperature distribution of the reaction fluid immediately after the start of the reaction.

19. The reaction analysis method according to claim 18,

the estimated temperature distribution is obtained by a governing equation that estimates the temperature distribution of the reaction fluid immediately after the start of the reaction,

the governing equation has a first reaction parameter related to a peak of a temperature distribution of the reaction fluid immediately after the start of the reaction, and a second reaction parameter related to a peak position of the temperature distribution of the reaction fluid immediately after the start of the reaction.

20. The reaction analysis method according to claim 19,

the first reaction parameter represents a calorific value per unit amount of a substance,

the second reaction parameter represents a temperature dependence of the reaction rate.

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