Apparatus and method for synthesizing heterogeneous materials by using flow chemistry system integrated with PID feedback

Abstract

A synthesis apparatus is provided. The synthesis apparatus may comprise: a synthesis unit in which a plurality of reactants are synthesized into one product; and a control unit for feedback-controlling the flow rate of a specific reactant introduced into the synthesis unit by using measurement information of the product, wherein the compositions of each reactant constituting the product may be automatically adjusted by means of the control unit according to set conditions. An adjustment unit for adjusting the flow rate of the specific reactant outputted toward the synthesis unit is provided, and the adjustment unit may be feedback-controlled by means of the control unit.

Description

Heterogeneous material synthesis device and method using a flow chemistry system integrated with PID feedback

[0001] The present invention relates to a device and method for synthesizing heterogeneous materials using a fluid chemical system.

[0002] Mixed-metal nanoparticles (NPs) present a challenge to synthesize with high precision and reproducibility due to the complex interplay of compositional and reaction condition factors.

[0003] Highly precise and automated flow chemistry techniques are needed to synthesize nanoboxes containing heterogeneous materials such as AgAu alloys.

[0004] The synthesis process requires precise control of reaction parameters such as flow rate to achieve target AgAu nanoboxes with the desired UV-vis (Ultra violet-Visible Spectroscopy) absorbance wavelength.

[0005] The present invention provides a synthesis device and method for synthesizing a plurality of heterogeneous materials (reactants) into one product using PID feedback control.

[0006] A synthesis device and a synthesis method are provided. The synthesis device may include a synthesis unit in which a plurality of reactants are synthesized into a single product; and a control unit that feedback-controls the flow rate of a specific reactant flowing into the synthesis unit using measurement information of the product.

[0007] At this time, the composition of each reactant constituting the product can be automatically adjusted according to set conditions by the control unit.

[0008] A control unit may be provided to control the flow rate of a specific reactant flowing into a synthesis unit where synthesis of multiple reactants takes place. The control unit may be feedback-controlled by the control unit.

[0009] A first regulating means and a second regulating means may be provided.

[0010] The first control means can control a first flow rate of a first reactant output toward the synthesis unit, and the second control means can control a second flow rate of a second reactant output toward the synthesis unit.

[0011] The first reactant and the second reactant exist in a solution state, and the control unit can control the first control means and the second control means so that when the first flow rate increases, the second flow rate decreases.

[0012] By means of the above control unit, the product can always satisfy the preset capacity regardless of changes in the first flow rate or the second flow rate.

[0013] A light source that generates measurement light required for measuring the optical properties of the above product, a flow cell through which the product and the measurement light intersect, and a spectrometer that obtains a spectrum of the measurement light passing through the product may be provided.

[0014] At this time, the control unit can identify the optical characteristics through analysis of the spectrum and feedback-control the flow rate of the specific reactant according to the optical characteristics.

[0015] A measuring unit for measuring the optical properties of the above product is provided, and the control unit can feedback control the flow rate of the specific reactant so that the measured optical properties measured by the measuring unit follow the designed optical properties of the product having the designed composition.

[0016] A control unit for controlling the flow rate of the specific reactant output toward the synthesis unit may be provided, and a measurement unit for measuring the optical properties of the product output from the synthesis unit may be provided.

[0017] When the time taken for the specific reactant output from the control unit to reach the measurement unit via the synthesis unit is defined as the response time, the control unit generates a first control value corresponding to a feedback control value, provides the first control value to the control unit, and the control unit can determine the optical characteristics measured by the measurement unit as the result of executing the first control value after the response time has elapsed from the time at which the first control value is provided to the control unit.

[0018] The above control unit can generate a second control value corresponding to a new feedback control value using the execution result of the identified first control value, and provide the second control value to the adjustment unit.

[0019] A measuring unit for measuring the optical characteristics of the above product is provided, and the control unit can generate the feedback control value using the optical characteristics measured by the measuring unit.

[0020] Once the control unit provides the first control value to the first regulating unit, the control unit can maintain the feedback control value for the regulating unit as the first control value from the time of providing the first control value to the regulating unit until the generation of the second control value.

[0021] The control unit may not provide a new feedback control value corresponding to the changed optical characteristic to the control unit during the period from the time the first control value is provided to the control unit to the time the second control value is generated, even if the optical characteristic changes.

[0022] The control unit can provide the second control value based on the execution result of the first control value to the control unit instead of the first control value only when the response time has elapsed from the time at which the first control value is provided to the control unit and the execution result of the first control value is determined.

[0023] A first connector, a second connector, a reaction tube and a bubble trap may be provided.

[0024] The first connector is formed so that the plurality of reactants are merged into one, the second connector is formed so that the output product merged into one from the first connector and the auxiliary solution for providing a set flow rate are merged, the reaction tube is formed so that the merged solution is synthesized through the first connector and the second connector, and the bubble trap can be formed so as to remove bubbles included in the product synthesized through the reaction tube.

[0025] The above control unit can feedback control the flow rate of the specific reactant using measurement information of the product output from the bubble trap.

[0026] One of the plurality of reactants may include silver nanocubes (Ag NanoCubes), another of the plurality of reactants may include HAuCl4, and the auxiliary solution may include ascorbic acid (AA) and poly vinyl pyrrolidone (PVP).

[0027] The flow rate of the auxiliary solution is maintained constant at a first set value, and the flow rate of the reactant can be controlled by the control unit within a range higher than the first set value.

[0028]

[0029] When a control unit is provided that controls the flow rate of a specific reactant flowing into a synthesis unit where synthesis of a plurality of reactants is performed, the synthesis method may include a command step of providing a command to the control unit; an acquisition step of obtaining measurement information of a product synthesized from the plurality of reactants into one from the measurement unit after the response time has elapsed from the time of providing the command to the control unit when the time taken for the specific reactant output from the control unit to reach the measurement unit through the synthesis unit is defined as a response time; and a control step of performing PID control so that the measurement information follows the command.

[0030] The above control step can generate a first control value that resolves the difference between the measurement information and the command and provide it to the control unit.

[0031] The above control step can determine the measurement information measured after the response time has elapsed from the time at which the first control value is provided to the control unit as the execution result of the first control value.

[0032] The above control step can generate a new second control value that resolves the difference between the execution result of the first control value and the command and provide the new second control value to the control unit.

[0033]

[0034] The above synthesis method can obtain an initial controller tuning constant including at least one of a process gain (Kp), a process time constant (τp), and a process dead time (θp) using a First-Order Plus Dead-Time (FOPDT) model.

[0035] The above synthesis method determines P, I and D of PID control based on the obtained Kp, τp and θp values, and can change the flow rate of the reactants based on the determined P, I and D values ​​until the target nanomaterial is produced.

[0036] The above synthesis method can obtain a gain (KC) corresponding to the controller P and an integral reset time (τI) corresponding to the I using the IMC (Internal Model Control) method.

[0037] The above synthesis method sets the differentiation time constant (τD) corresponding to the above D to 0, and at least one of the initial flow rate of the reactant, TP (Target Peak), and sampling interval time (SIT) can be obtained from the user.

[0038] According to the present invention, a system can be provided in which the composition of a fluid chemical compound is automatically controlled by applying feedback control and PID control, which have not been introduced in the field of fluid chemistry.

[0039] According to the present invention, the composition of the reactants constituting the product can be automatically controlled through a control unit that feedback-controls the flow rate of a specific reactant flowing into the synthesis unit using measurement information of the product.

[0040] For example, mixed metal nanoparticles (NPs) as products are a challenging task to synthesize with high precision and reproducibility due to the complex interplay of compositional and reaction condition factors.

[0041] The synthetic apparatus and method of the present invention can provide a highly precise and automated flow chemistry technique for synthesizing AgAu alloy (gold-silver alloy) nanoboxes with tailored optical properties.

[0042] The synthesis apparatus and method of the present invention may include a proportional-integral-derivative (PID) feedback control mechanism that enables precise control of reaction parameters such as flow rate to achieve target AgAu nanoboxes having optical properties such as a desired UV-vis absorbance wavelength.

[0043] The PID control algorithm can be based on the First-Order Plus Dead-Time (FOPDT) model, which relates the maximum absorbance peak of the nanoalloy product to the flow rate of the precursor.

[0044] The synthesis device of the present invention can adjust the flow rate of the precursor (i.e., reagent concentration) through a repetitive process until the real-time absorbance wavelength of the AgAu alloy nanobox becomes the target wavelength based on the difference between the UV-vis absorbance wavelength measured in real time and the target wavelength.

[0045] Implementing a PID feedback control mechanism in a flow chemistry system can automatically adjust concentration changes, minimizing the need for user intervention. This provides a highly versatile and universal strategic environment for producing on-demand complex nanomaterials with significantly improved consistency and reliability.

[0046] Figure 1 is a block diagram showing a synthesis device according to an embodiment of the present invention.

[0047] Figure 2 is a schematic diagram showing a synthesis device according to an embodiment of the present invention.

[0048] Figure 3 is a flowchart showing a synthesis method according to an embodiment of the present invention.

[0049] Figure 4 is a schematic diagram showing the characteristics of an AgAu nano box.

[0050] Figure 5 is a flowchart illustrating the entire workflow from the screening and modeling stages to the synthesis stage.

[0051] Figure 6 is a formula for calculating the output flow rate of the Au precursor solution that allows the absorbance peak of the AgAu nanoalloy to approach the target peak (TP).

[0052] Figure 7 is K C It is a formula that calculates a value.

[0053] Figure 8 is a graph showing the results of a screening stage test experiment.

[0054] Figure 9 shows the K obtained through screening experiments. p , τ p , θ p This is a table showing the values.

[0055] Figure 10 is a schematic diagram showing a plot of data recorded in a blue shift experiment.

[0056] Figure 11 is a schematic diagram showing a plot of recorded data for AgAu nanoalloy synthesis using red-shifted PID feedback control.

[0057] Figure 12 is a schematic diagram showing an AgAu alloy nano box product having an absorbance wavelength of 450 nm obtained in a blue shift experiment and an AgAu alloy nano box product having an absorbance wavelength of 535 nm obtained in a red shift experiment.

[0058] FIG. 13 is a drawing showing a computing device according to an embodiment of the present invention.

[0059] Below, with reference to the attached drawings, embodiments of the present invention are described in detail so that those skilled in the art can easily implement the invention. However, the present invention can be implemented in various different forms and is not limited to the embodiments described herein. In addition, in the drawings, parts irrelevant to the description are omitted for clarity of description, and similar parts are designated with similar reference numerals throughout the specification.

[0060] In this specification, duplicate descriptions of identical components are omitted.

[0061] Additionally, when a component is referred to herein as being "connected" or "connected" to another component, it should be understood that while it may be directly connected or connected to that other component, there may be other components present in between. Conversely, when a component is referred to herein as being "directly connected" or "directly connected" to another component, it should be understood that there are no other components present in between.

[0062] Additionally, the terms used herein are only used to describe specific embodiments and are not intended to limit the present invention.

[0063] Also, in this specification, singular expressions may include plural expressions unless the context clearly indicates otherwise.

[0064] In addition, in this specification, it should be understood that terms such as “include” or “have” are intended to specify only the presence of a feature, number, step, operation, component, part, or combination thereof described in the specification, and do not exclude in advance the possibility of the presence or addition of one or more other features, numbers, steps, operations, components, parts, or combinations thereof.

[0065] Also, in this specification, the term 'and / or' includes a combination of multiple listed items or any item among multiple listed items. In this specification, 'A or B' can include 'A', 'B', or 'both A and B'.

[0066] Additionally, in this specification, detailed descriptions of known functions and configurations that may obscure the gist of the present invention will be omitted.

[0067] Flow chemistry is a technique for synthesizing fine chemicals using flow equipment such as pipelines. In the field of flow chemistry, large-scale or continuous flow synthesis for producing nanomaterials with desired chemical properties requires a trial-and-error approach, which is time-consuming and resource-intensive. Another significant challenge is that continuous flow synthesis is affected not only by controllable factors such as concentration and temperature, but also by minor perturbations in reaction conditions, such as solution aging, small changes in reagent concentration, and flow fluctuations, resulting in dramatic deviations from the desired properties.

[0068] These discrepancies (differences) are related to the routine fluctuations and irregularities that occur during continuous synthesis due to the unavoidable instability of the experimental parameters mentioned above. Automated synthesis can be utilized to optimize reaction conditions and improve reaction stability. However, automation without closed-loop feedback control cannot eliminate the instability of precursor concentrations, so a trial-and-error approach is still necessary to obtain the desired product.

[0069] Instead of a trial-and-error approach that relies on manual intervention by the user, PID control can be used to generate control signals that adjust the output of the system in response to changes in input or disturbance for automatic synthesis.

[0070] Proportional-Integral-Derivative (PID) control is simple and very effective, especially when paired with a descriptive dynamic model. Dynamic models are essential for understanding system dynamics in open-loop (manual) or closed-loop (automatic) control. In particular, the First-Order Plus Dead-Time (FOPDT) model is a standard empirical model used for stable dynamic control in various industrial processes. The FOPDT model is based on the process gain (K p ), process time constant (τ p ) and process dead time (θ p) can be used to obtain initial controller tuning constants such as K. These values ​​can be used in a predefined tuning algorithm to design a PID controller. p , τ p and θ p Based on the values, P, I and D can be determined, and based on these values, the flow rate of the precursor solution can be continuously changed until the target nanomaterial is produced.

[0071] In this context, the feasibility of PID control in flow chemistry can be demonstrated by proposing a continuous microfluidic system (e.g., the synthesis device of the present invention) for synthesizing on-demand AgAu alloy nanoboxes as a model. Considering the balance between the chemical stability of Ag and the high activity of Au as a catalyst, the target maximum absorbance wavelength of the AgAu nanoalloy can be predefined. At this time, the compositions of Ag and Au can be automatically adjusted by a PID algorithm. While the following description primarily focuses on absorbance-based feedback, the synthesis device of the present invention can also be applied to fluorescence-based feedback, such as in perovskite synthesis.

[0072] Fig. 1 is a block diagram illustrating a synthesis device according to an embodiment of the present invention. Fig. 2 is a schematic diagram illustrating a synthesis device according to an embodiment of the present invention.

[0073] The synthesis device illustrated in FIG. 1 may include a synthesis unit (130), a control unit (170), a regulation unit (110), and a measurement unit (150). The synthesis device may be applied in the field of flow chemistry.

[0074] In the synthesis unit (130), multiple reactants can be synthesized into one product.

[0075] For example, the synthesis unit (130) may be provided with a first connector (131), a second connector (132), a reaction tube (133), and a bubble trap (135).

[0076] The first connector (131) may be formed to merge a plurality of reactants into one. For example, the first connector (131) may include a first pipe portion extending in a straight line and a second pipe portion protruding from the center of the first pipe portion. In terms of the flow path, the first pipe portion and the second pipe portion may be formed to be connected to each other. At this time, a first inlet into which the first reactant is input and a second inlet into which the second reactant is input may be formed at both ends of the first connector (131). An outlet through which an output product in which the first reactant and the second reactant are mixed may be output may be formed at the end of the second pipe portion. Since the connection shape of the first pipe portion and the second pipe portion has a 'T' shape, the first connector (131) may be referred to as a T-shaped connector.

[0077] The second connector (132) may be formed to merge the output from the first connector (131) into one and the auxiliary solution for providing the set flow rate. The second connector (132) may also include a T-shaped connector.

[0078] One of the inlets of the second connector (132) may receive the output from the outlet of the first connector (131), and the other may receive an auxiliary solution. A solution that combines the output from the outlet of the first connector (131) and the auxiliary solution may be output from the outlet of the second connector (132).

[0079] The reaction tube (133) may be formed so that the combined solution is synthesized through the first connector (131) and the second connector (132). As an example, the reaction tube (133) may include a flexible tube with a length of 1 to 5 m formed to be submerged in a water tank.

[0080] A bubble trap (135) can be formed to remove bubbles contained in the product synthesized through the reaction tube (133).

[0081] The auxiliary solution may contain ascorbic acid (AA) and poly vinyl pyrrolidone (PVP).

[0082] The flow rate of the auxiliary solution can be maintained constant at the first set value. An injection means (139), such as a pump, for injecting the auxiliary solution into the second connector (132) can be provided.

[0083] The flow rate of the reactant can be controlled by the control unit (170) within a range higher than the first set value.

[0084] As an example, FIG. 2 may represent a synthesis device corresponding to an integrated flow chemical synthesis system operated under PID control to synthesize AgAu alloy nano boxes.

[0085] A customized syringe pump module (included in the control unit (110)) for controlling the flow rate of the reagent, a flow cell (159) (included in the measurement unit (150)) for measuring the UV-vis absorbance of the produced AgAu alloy nano boxes in real time, a feedback controller (included in the control unit (170)) for resetting the reaction conditions, and a sample collector (90) may be provided.

[0086] In the experiment, the syringe pump module was designed using Cut2D version 10.5 software (Vectric, USA) and fabricated from PMMA sheet (Acrytals, South Korea) by a TinyCNC-6060C milling machine (Tinyrobo, South Korea). The syringe pump module was equipped with a 51 / 1 reduction gear for fine-tuning the flow rate and was controlled by a TMCM-3110 motor driver (TRINAMIC, Germany) via a Python API (pyTMCL). The Seabreeze package was used to interface with the portable spectrometer (153), and the matplotlib package was used for process monitoring. The absorbance flow cell (159) can be provided with a 10 mm optical path to mimic a standard cuvette. A balanced light source (151) using a deuterium and tungsten halogen lamp can pass through a filter to remove alpha deuterium lines in the visible region. Two optical cables were used, 2 m long, multimode optical fibers with a diameter of 400 μm for the enhanced transmission optical signal (QP400-2-UV-vis, Ocean Optics, UK). The first cable was connected from the light source (151) to the absorbance flow cell (159). The second cable was aligned with the first cable and plugged into the other end of the flow cell (159), which was then connected to a portable spectrometer (153) (USB4000, Ocean Optics, UK). A single-board computer, Raspberry Pi 4, was used for signal processing, visualization, and PID feedback control. Peak detection was performed by fitting the upper half of the spectrum to a polynomial after raw signal processing using a 1D Box filter (width = 10).

[0087] The flow rate f3 of the auxiliary solution was maintained at 150 μL / min, and the total flow rate of the Ag nanocubes and HAuCl4 precursor solution was maintained at 300 μL / min, which was twice that of the AA-PVP solution.

[0088] The tube length between the first connector (131) and the second connector (132) was set to 500 mm.

[0089] The solution output from the second connector (132) was passed through a reaction tube (133) immersed in water at a temperature of 70 degrees.

[0090] The total flow rate ft of the solution output from the second connector (132) is 450 μL / min, and the tube length from the outlet of the second connector (132) to the flow cell (159) is set to 1750 mm (approximately 2 minutes). When the AgAu alloy nano box passes through the flow cell (159), real-time absorbance measurements can be displayed on the monitor screen.

[0091] The control unit (170) can feedback control the flow rate of a specific reactant flowing into the synthesis unit (130) using the measurement information of the product output from the bubble trap (135).

[0092] The composition of each reactant constituting the product can be automatically controlled by the control unit (170) according to set conditions or commands.

[0093] The control unit (110) can control the flow rate of a specific reactant output toward the synthesis unit (130). The control unit (110) can be closed-loop feedback controlled by the control unit (170).

[0094] The control unit (110) may be provided with a first control means (111) and a second control means (112).

[0095] The first control means (111) can control the first flow rate f1 of the first reactant output toward the synthesis unit (130).

[0096] The second control means (112) can control the second flow rate f2 of the second reactant output toward the synthesis unit (130).

[0097] The first control means (111) and the second control means (112) may include a syringe pump module, etc.

[0098] The first reactant and the second reactant may be in a solution state. For example, the first reactant may include silver (Ag). Specifically, the first reactant may include nanocubes (Ag NanoCubes). The second reactant may include gold (Au). Specifically, the second reactant may include HAuCl4.

[0099] The product synthesized by combining the first and second reactants may include AgAu (silver-gold or gold-silver) alloy nano boxes.

[0100] The control unit (170) can control the first control means (111) and the second control means (112) so that when the first flow rate f1 increases, the second flow rate f2 decreases.

[0101] The product can always satisfy the preset capacity regardless of the change in the first flow rate f1 or the second flow rate f2 by the control unit (170).

[0102] The measuring unit (150) can measure the optical properties of the product. The optical properties may include absorbance or fluorescence measurements.

[0103] The measuring unit (150) may be provided with a light source (151), a flow cell (159), and a spectrometer (153).

[0104] The light source (151) can generate measurement light necessary for measuring the optical properties of a product.

[0105] The flow cell (159) can be formed so that a product synthesized from multiple reactants and a measurement light cross-pass through it.

[0106] The spectrometer (153) can obtain a measured light spectrum passing through the product.

[0107] At this time, the control unit (170) can determine the optical characteristics (including absorbance) of the product through spectrum analysis, and can feedback control the flow rate of a specific reactant, for example, the first flow rate f1 or the second flow rate f2, according to the optical characteristics. For example, the control unit (170) can feedback control the flow rate of a specific reactant so that the measured optical characteristics measured by the measurement unit (150) follow the designed optical characteristics of a product having a pre-designed composition.

[0108] The pre-designed composition may be a composition set by the user, i.e., may correspond to the user's instructions. To compare the optical characteristics obtained by the measurement unit (150), the control unit (170) may convert and transform the pre-designed composition into optical characteristics, and the optical characteristics corresponding to the pre-designed composition may correspond to the design optical characteristics.

[0109] The time it takes for a specific reactant (e.g., a first reactant or a second reactant) output from the control unit (110) to pass through the synthesis unit (130) and reach the measurement unit (150) can be defined as the response time.

[0110] At this time, the control unit (170) can generate a first control value corresponding to the feedback control value and provide the first control value to the adjustment unit (110). The control unit (170) can determine the optical characteristics measured by the measurement unit (150) as the execution result of the first control value after a response time has elapsed from the time at which the first control value is provided to the adjustment unit (110).

[0111] The control unit (170) can generate a second control value corresponding to a new feedback control value using the execution result of the first control value, and provide the second control value to the adjustment unit (110). As with the first control value, after a response time has elapsed from the time the second control value is provided to the adjustment unit (110), the optical characteristics measured by the measurement unit (150) can be determined as the execution result of the second control value by the control unit (170).

[0112] As described above, the control unit (170) can generate a feedback control value using the optical characteristics measured by the measurement unit (150).

[0113] Once the control unit (170) provides the first control value to the first control unit (110), the feedback control value for the control unit (110) can be maintained as the first control value from the time of providing the first control value to the control unit (110) until the generation of the second control value. In other words, even if the optical characteristic changes during the period from the time of providing the first control value to the control unit (110) until the generation of the second control value, the control unit (170) can not provide a new feedback control value corresponding to the changed optical characteristic to the control unit (110).

[0114] The control unit (170) can provide the second control value based on the execution result of the first control value to the control unit (110) only after the response time has elapsed from the time at which the first control value is provided to the control unit (110) and the execution result of the first control value is determined.

[0115] To ensure high reliability, the control unit (170) can determine the measured optical characteristics after a set time has additionally elapsed from the point at which the response time has elapsed as the execution result of the first control value.

[0116] Figure 3 is a flowchart showing a synthesis method according to an embodiment of the present invention.

[0117] The synthesis method of FIG. 3 can be performed by the synthesis device illustrated in FIG. 1, specifically, the control unit (170).

[0118] The synthesis method may include a command step (S 510), an acquisition step (S 520), and a control step (S 530).

[0119] The control unit (170) can perform a command step (S 510) of providing a command to the control unit (110). The command step (S 510) can obtain the composition of a desired product from the user and provide the command value or command information for achieving the corresponding input value or input value to the control unit (110).

[0120] The control unit (170) may perform an acquisition step (S 520) of acquiring measurement information of a product synthesized from multiple reactants from the measurement unit (150) after a response time has elapsed from the time a command is provided to the control unit (110). In order to maintain control consistency, the control unit (170) may ignore measurement information of a product acquired in the period from the time a command is provided to before the response time has elapsed.

[0121] The control unit (170) may perform a control step (S 530) of performing PID control so that the measurement information follows the command. In most cases, the measurement information differs from the command, and PID control may be performed by the control unit (170) to resolve the difference (error value) at this time. The control unit (170) may control the adjustment unit (110) with a first control value to reduce and correct the error value. After the response time has elapsed, the measurement information based on the first control value may be obtained, and the error value may be determined again. The control unit (170) may control the adjustment unit (110) with a second control value to reduce and correct the error value. This process may be repeated until the error value is reduced to within the target range (command tracking is completed).

[0122] In other words, the control step (S 530) can generate a first control value that resolves the difference between the measurement information and the command, and provide the first control value to the control unit (110).

[0123] The control step (S 530) can determine the measurement information measured after the response time has elapsed from the time the first control value is provided to the control unit (110) as the execution result of the first control value.

[0124] The control step (S 530) can generate a new second control value that resolves the difference between the execution result of the first control value and the command and provide it to the control unit (110).

[0125] Figure 4 is a schematic diagram showing the characteristics of an AgAu nano box.

[0126] Figure 4 (a) shows the color of AgAu alloy nano boxes according to the ratio between Ag and Au elements (from left to right, the flow ratio of Ag / Au = 290 / 10, 270 / 30, 250 / 50, 230 / 70, 210 / 90, 90 / 110, 170 / 130).

[0127] Figure 4 (b) shows the UV-vis absorbance spectrum of the resulting AgAu alloy nanoboxes manufactured by adjusting the flow rates of Ag nanocubes and Au ion solutions in a continuous flow synthesis system.

[0128] Figure 4(c) shows a schematic diagram of the reaction of AgAu alloy nanoboxes with Au ions coated on Ag nanocubes and the corresponding TEM image. Void nucleation was first observed in the Ag nanoboxes, followed by void propagation and shell deposition.

[0129] Figure 4 (d) shows a nonlinear curve indicating the maximum absorbance wavelength based on the flow rate of the Au ion solution.

[0130] To produce on-demand AgAu alloy nanoboxes via PID feedback control in continuous flow chemical synthesis, three target peaks (TPs) were selected for blue-shifted (440, 450, and 460 nm) and red-shifted (525, 535, and 545 nm) experiments.

[0131] Seven types of AgAu alloy nanoboxes were synthesized in a continuous flow synthesis system by varying the flow ratio of Ag nanocubes and HAuCl4 precursor solution. As the flow rate of the HAuCl4 precursor solution gradually increased, the color of the synthesized AgAu alloy nanoboxes changed from yellow to brown, purple, and blue. Since the produced AgAu alloy nanoboxes had different metal compositions between Ag and Au, the AgAu nanoalloys exhibited different UV-vis absorbance wavelengths under irradiation with deuterium and tungsten halogen lamps.

[0132] In Fig. 4(b), the shortest UV-vis absorbance wavelength of 434 nm was observed at a flow rate ratio of 290 μL / min: 10 μL / min for the Ag NC (nanocube) and Au ion solutions, respectively. Meanwhile, the longest wavelength of 615 nm was detected when the flow rate ratio of the two solutions was 170:130. As the flow rate of the HAuCl4 precursor solution gradually increased, Au ions were coated on the Ag nanocubes, and then void nucleation was formed in the Ag nanoboxes, followed by void propagation and shell deposition (Fig. 2(c)). Fig. 2(d) shows a nonlinear graph showing the shift of the maximum absorbance peak according to the flow rate of the Au ion solution. The synthesis device of the present invention can aim to automatically produce AgAu alloy nanoboxes with a desired maximum absorbance wavelength using a continuous flow synthesis system with PID control applied. To demonstrate the validity of automatic PID control, three target peaks (TP) (525, 535, and 545 nm) for redshift experiments and three target peaks (TP) (440, 450, and 460 nm) for blueshift experiments were set.

[0133] Figure 5 is a flowchart illustrating the entire workflow from the screening and modeling stages to the synthesis stage. Figure 6 is a formula for calculating the output flow rate of the Au precursor solution that allows the absorbance peak of the AgAu nanoalloy to approach the target peak (TP).

[0134] First, step tests were performed to correlate UV-vis absorbance peaks with the flow rate of the Au ion solution during the screening and modeling stages. During the step tests, the flow rate of the Au ion precursor (reactant) solution was systematically varied, and the absorbance peaks were differentiated stepwise (corresponding to the number of flow rate tunings) according to the change in flow rate step applied to the precursor solution. Each step lasted 600 s, and the final step was maintained for 1,200 s to stabilize the output (maximum absorbance wavelength).

[0135] K in step test data p , τ p and θ p The value can be calculated using the FOPDT model as shown in Equation 1 below with the Sequential Least Squares Programming (SLSQP) optimizer (S 531).

[0136] ...Formula 1

[0137] Here, y(t) is the maximum absorbance peak recorded, and u(t) is the flow rate of the Au ion solution.

[0138] In the next step, the controller gain (K) is adjusted by the IMC (Internal Model Control) method. C ) and the integral reset time (τ I ) was obtained. τ I The values ​​were initially generated by the IMC method, but were experimentally optimized to minimize the fluctuation of the maximum absorbance peak after reaching the target peak (TP). The differentiation time constant (τ D ) value was set to 0 because the TP (Target Peak) did not change during the synthesis run. Through this process, K corresponding to P, I, and D C , τ I , τ D The values ​​were determined (S 552). The suitability of these values ​​for PID feedback control was evaluated in blue-shift and red-shift experiments.

[0139] The synthesis step may be controlled (performed by inputting specific values) or the progress may be displayed via a graphical user interface (GUI) provided to the user. The synthesis device of the present invention may additionally be provided with a display (179) that displays the GUI required for the synthesis step.

[0140] The user can set the initial flow rate of the precursor solution, TP (Target Peak), SIT (Sampling Interval Time), K through the GUI. C and τ I The values ​​and other necessary information can be input (S 511, Parameter Definition). The initial flow rate was kept constant for 240 s to stabilize the entire synthesis system before triggering the PID control. Then, an infinite loop was started with an arbitrary initial flow rate of the precursor solution, and the generated absorbance spectra were recorded and compared with the target peak (TP) (S 521, Spectrum Detection). The wavelength difference between the target peak and the currently observed absorbance peak (denoted as e(t) in the equation of Fig. 6) was calculated, and the PID control considered the e(t) value as input (S 523). Then, a new set of output flow rates (i.e., u(t) in the equation of Fig. 6) of the Au precursor solution was provided, which allows the absorbance peak of the resulting AgAu nanoalloy to approach the target peak (TP). A predefined K C , τ I and τ D The adjusted flow rates of Ag nanocubes and Au ion precursor solutions were calculated using the formula in Fig. 6 using the values.

[0141] Here, u bias is the current flow rate, e(t) is the wavelength difference, Δt is the sampling interval time, PV is the process variable, and u(t) is the new flow rate of the Au ion solution. Differential (D) control is TP(τ D = 0) is equal to 0 because there is no change.

[0142] A command for adjusted flow rates received from the PID controller can be transmitted to the motor driver to change the flow rates of the customized syringe pump for the Ag NC (nanocube) and Au ion solutions. A new set of precursor solutions can synthesize a new AgAu nanoalloy whose absorbance wavelength is closer to the TP than before. Again, the synthesis device can measure the wavelength difference between the TP and the current peak (i.e., the e(t) value) and generate a new u(t) value based on the equation in Figure 6. This flow rate adjustment of the precursor solutions can be repeated until the current UV-vis absorbance peak finally coincides with the TP (S 530, PID control).

[0143] The display (179) provided in the control unit (170) can display the current flow rates of the Ag and Au precursor solutions, the change in the maximum absorbance spectrum, and the current spectrum based on the change in the flow rate of the Au ion solution. During this infinitely repeating process, all data of the absorbance spectrum and the flow rate of the precursor solution can be automatically recorded in CSV (Comma Separated Values) format. Even if a sudden change in the precursor concentration, such as precipitation, occurs, the system can self-correct through the repeating process. The user can close the GUI window displayed on the display (179) and terminate the experiment at any time without losing data.

[0144] To observe the effect of stepwise changes in the Au ion flow rate on the maximum absorbance peak of AgAu alloy nanoboxes, four types of step tests were performed. The first experiment was a step-up experiment, in which the flow rate of the Au ion solution was gradually increased from 10 μL / min to 110 μL / min, with incremental steps of 20 μL / min. The second experiment decreased the flow rate from 110 μL / min to 10 μL / min, with six incremental steps of 20 μL / min. In the third and fourth experiments, the flow rate of the Au ion solution was randomly varied in six steps.

[0145] Figure 8 is a graph showing the results of a screening stage test experiment.

[0146] In the pressure-assisted test of Fig. 8(a), the maximum absorbance peak increased with increasing flow rate, whereas in the pressure-assisted test of Fig. 8(b), the absorbance peak gradually decreased in proportion to the flow rate of the Au ion solution. In the two random step tests, the profiles of the absorbance peaks were similar to the profiles of the flow rates. Therefore, in all four experimental trials, the measured maximum absorbance peak of the AgAu alloy nanoboxes correlated with the flow rate of the Au ion solution with a time delay of about 2 minutes, which was consistent with the calculated total reaction time. Each step test was performed using the FOPDT model with the SLSQP optimizer to obtain a unique K p , τ p and θ p We generated a set of values. Therefore, K p , τ p , θ p Four sets of values ​​and their averages were obtained after four screening experiments, as shown in Fig. 9.

[0147] Figure 9 shows the K obtained through screening experiments. p , τ p , θ p This is a table showing the values.

[0148] Through the above screening and synthesis processes, an explanatory model can be established that accurately characterizes the correlation between the measured maximum absorbance peak of the AgAu alloy nanobox and the flow rate of the Au ion solution.

[0149] Then the average K p , τ p and θ p The values ​​were used in the next step to adjust the correlation using the IMC method. Through the IMC-based tuning process, τ C Enter a value for K C I got the value τ CThe parameter controls the degree of response (aggressive, moderate, or conservative) of the PID control system in response to deviations between the current peak and TP. Thus, τ C can be selected with the following options and K accordingly C The value can be calculated as in the formula in Fig. 7.

[0150] The selection rules among aggressive, moderate, or conservative tuning, as shown in Figure 7, can generally be applied to industrial processes with low dead times and high tolerance for overshooting of inputs (control variables) and outputs (process variables). However, current flow synthesis systems have low tolerance for input (flow rate) overshooting and long dead times (i.e., relatively long response times). For example, since the total flow rates of the Ag and Au precursor solutions were maintained at 300 μL / min, an excess flow rate of Au would lead to a negative flow rate of the Ag precursor solution. Therefore, an extremely conservative tuning approach may be appropriate in this case to minimize overshoot of the adjusted flow rate during the long response time. Consequently, the PID control system may exhibit a relatively slow response to the difference between the current peak and the target peak (TP), but such an algorithm prevents overshooting problems or negative flow rates. Taking all these factors into account, τ c The value is 120θ p Set to 22868.793 and K C The value was obtained as 0.01. Through experimental optimization, τ I The optimal value was determined to be 5000. This value was chosen based on the balance between the time taken to reach TP and the variation of the maximum absorbance peak observed after reaching TP.

[0151] For blue shift feedback control, use GUI to set TP values ​​(440, 450 and 460 nm) and PID values ​​(K C = 0.01, τ I = 5000, τ D = 0) was set.

[0152] Figure 10 is a schematic diagram showing a plot of data recorded in a blue shift experiment.

[0153] Figure 10(a) shows the change in the flow rate of the Au ion solution, and Figure 10(b) shows the maximum UV-vis absorbance peak of the generated AgAu nanoalloy. The initial flow rates of the Ag NC and HAuCl4 precursor solutions were set to 150 μL / min, producing AgAu alloy nanoboxes with an absorbance wavelength of approximately 560 nm. The initial flow rate was maintained for 240 s to stabilize the entire synthesis system. Then, the flow rate of the precursor solution was adjusted by PID feedback control based on the difference between the observed and target wavelengths. This iteration was repeated every 10 s for 5,000 s of the synthesis experiment. As the flow rate of the Au ion solution gradually decreased, the maximum UV-vis absorbance wavelength of the generated AgAu nanoalloy decreased in a pattern similar to that of the flow rate. For TPs of 440, 450, and 460 nm, all flow rates decreased and decreased to about 50 μL / min at 1500 s, and then stabilized at distinct flow rates of 62.7, 54.6, and 49.3 μL / min, respectively (Fig. 10(c)). Simultaneously, the absorbance peak gradually approached the TP with slight overshoot and undershoot and then stabilized around the TP (Fig. 10(d)). The complete changes in the absorbance spectra during the experiment are shown in Fig. 10(e) for the TP of 440 nm, Fig. 10(f) for the TP of 450 nm, and Fig. 10(g) for the TP of 460 nm.

[0154] Inspection revealed that the PID feedback-controlled flow chemistry operates rapidly and accurately, with the UV-vis absorbance wavelength starting at approximately 560 nm and blue-shifting to reach each target wavelength after 1600 s, while maintaining stability. The spacing between the three TP wavelengths is only 10 nm, demonstrating the high precision of the proposed synthesis methodology.

[0155] After completing the blueshift experiments, the proposed synthetic device was further tested in redshift experiments using TPs of 525 nm, 535 nm, and 545 nm.

[0156] Figure 11 is a schematic diagram showing a plot of recorded data for AgAu nanoalloy synthesis using red-shifted PID feedback control.

[0157] Similar to Fig. 10(a), the change in the flow rate of the Au ion solution is shown in Fig. 11(a). Through the experiment, target nanomaterials with TPs of 525 nm, 535 nm, and 545 nm were generated. Simultaneously, the transition of the maximum UV-vis absorbance peak of the generated AgAu nanoalloy is shown in Fig. 11(b).

[0158] Compared to the blue-shifted PID control experiment, additional modifications made for the red-shifted PID control experiment were the initial flow rate and the TP of the GUI. All other parameters, such as the PID value, sampling interval time (SIT), total run time (5000 s), and monitoring plot parameters, were the same as those for the blue-shifted PID control experiment. The initial flow rates of the Ag NCs and HAuCl4 precursor solution were set to 290 μL / min and 10 μL / min, respectively, to produce AgAu alloy nanoboxes with an absorbance wavelength of 420 nm. Subsequently, the flow rate of the Ag NCs was decreased and the flow rate of the HAuCl4 precursor solution was increased by PID control, red-shifting the absorbance peak of the AgAu nanoalloy. The flow rate of the Au ion solution was increased from 10 μL / min to over 90 μL / min and then stabilized at different flow rates, producing distinct AgAu nanoalloys with different TPs (Figure 11 (c)). Because the gap between the TP of 545 nm and the initial peak (420 nm) was the largest, the slope of the flow rate showed the steepest slope among the three TPs. As the flow rate of the Au ion solution stabilized, the UV-vis absorbance peak gradually approached the TP and oscillated around the TP (Fig. 11(d)). The time required to reach the TP was approximately 1200 s for all cases. Although the TP was far from the initial value of 420 nm, the absorbance peak of the synthesized AgAu nanoalloy reached the TP quickly and smoothly without a large overshoot, highlighting one of the advantages of PID control. The synthesized AgAu nanoalloys at equilibrium exhibited distinct absorbance peaks at 525, 535, and 545 nm, respectively (Fig. 11(d)), indicating another advantage of PID control in reducing the steady-state error. Unlike other methods such as proportional control or integral control, PID control integrates both proportional and integral components, allowing it to respond to accumulated past errors as well as current errors.This allows the system to accurately track the target setpoint and compensate for persistent errors that may arise due to system disturbances or other external factors. The full absorbance spectra for redshift experiments using three different TPs are shown in Figure 11 (e)–(g).

[0159] The 3D graph provides an overall view of the overall evolution of the absorbance spectrum and the stability of the entire spectrum at equilibrium.

[0160] Both blue-shifted and red-shifted experiments successfully demonstrated the feasibility of adopting PID control to produce on-demand nanomaterials with TP. Figures 11(a) and (b) are similar to Figures 10(a) and (b) with vertically flipped patterns.

[0161] Compared to the blue-shift experiment, the red-shift experiment showed less variation in precursor solution flow rate and absorbance TP. The standard deviation (SD) of the average absorbance wavelength across the three TPs was 8.8 nm for the red-shift experiment, while the blue-shifted counterpart showed 19.8 nm. Furthermore, the average standard deviation of the HAuCl4 precursor solution flow rate was 1.8 μL / min in the red-shift experiment, which was lower than the corresponding 2.6 μL / min in the blue-shift experiment. This phenomenon may be due to the influence of the unstable region of the light source (151).

[0162] Because PID control is a closed-loop control, the flow rate and absorbance peak can be linked. Flow rate adjustment is guided by the absorbance peak, which in turn promotes flow rate stabilization. As shown in Figures 10(c) and 11(c), the equilibrium flow rate fluctuates less at redshift than at blueshift. These results suggest that flow chemistry using PID feedback control can reduce the time required to reach TP, minimize overshooting issues, and increase the stability of the entire synthesis device after reaching TP. These characteristics can be a powerful advantage in automated flow chemistry platforms.

[0163] Figure 12 is a schematic diagram showing an AgAu alloy nano box product having an absorbance wavelength of 450 nm obtained in a blue shift experiment and an AgAu alloy nano box product having an absorbance wavelength of 535 nm obtained in a red shift experiment.

[0164] Figure 12 (a) shows an AgAu alloy nanobox product having an absorbance wavelength of 450 nm obtained from a blue-shift experiment. Figure 12 (b) shows a product having an absorbance wavelength of 535 nm obtained from a red-shift experiment.

[0165] The size, morphology, and composition were analyzed using FE-TEM and Energy Dispersive X-ray Spectroscopy (EDS) mapping.

[0166] TEM images of both samples show a cubic shape with good crystallinity. The resulting AgAu nanoalloy had an average size of 50 ± 5 nm. EDS data shows the mapping of Au and Ag elements in the AgAu nanoalloy. The elemental proportions of Ag and Au were 97.56% and 2.44%, respectively, for the blue-shifted product, while they were 81.97% and 18.03%, respectively, for the red-shifted product. The observed relationship between the flow rate of the Au ion precursor and the elemental composition of the synthesized nanoparticles may be due to the kinetics of the reduction process. A higher flow rate of Au ions could increase the concentration of Au ions in the reaction mixture, resulting in a higher reduction rate and a higher percentage of Au atoms in the final red-shifted product.

[0167] FIG. 13 is a diagram illustrating a computing device according to an embodiment of the present invention. The computing device (TN100) of FIG. 13 may be a device described herein (e.g., a synthesis device or a control unit (170), etc.).

[0168] In the embodiment of FIG. 13, the computing device (TN100) may include at least one processor (TN110), a transceiver (TN120), and a memory (TN130). In addition, the computing device (TN100) may further include a storage device (TN140), an input interface device (TN150), an output interface device (TN160), and the like. The components included in the computing device (TN100) may be connected by a bus (TN170) to communicate with each other.

[0169] The processor (TN110) can execute program commands stored in at least one of the memory (TN130) and the storage device (TN140). The processor (TN110) may refer to a central processing unit (CPU), a graphics processing unit (GPU), or a dedicated processor in which methods according to embodiments of the present invention are performed. The processor (TN110) may be configured to implement procedures, functions, methods, etc. described in relation to embodiments of the present invention. The processor (TN110) may control each component of the computing device (TN100).

[0170] The memory (TN130) and the storage device (TN140) can each store various information related to the operation of the processor (TN110). The memory (TN130) and the storage device (TN140) can each be configured with at least one of a volatile storage medium and a non-volatile storage medium. For example, the memory (TN130) can be configured with at least one of a read-only memory (ROM) and a random access memory (RAM).

[0171] The transceiver (TN120) can transmit or receive wired or wireless signals. The transceiver (TN120) can be connected to a network to perform communication.

[0172] Meanwhile, the embodiments of the present invention are not implemented only through the devices and / or methods described so far, but may also be implemented through a program that realizes a function corresponding to the configuration of the embodiments of the present invention or a recording medium on which the program is recorded, and such implementation can be easily implemented by a person skilled in the art to which the present invention pertains based on the description of the embodiments described above.

[0173] Although the embodiments of the present invention have been described in detail above, the scope of the present invention is not limited thereto, and various modifications and improvements made by those skilled in the art using the basic concept of the present invention defined in the following claims also fall within the scope of the present invention.

Claims

1. A synthesis unit in which multiple reactants are synthesized into one product; A control unit that feedback-controls the flow rate of a specific reactant flowing into the synthesis unit using measurement information of the product; A synthesis device in which the composition of each reactant constituting the above product is automatically controlled by the control unit according to set conditions.

2. In paragraph 1, A control unit is provided to control the flow rate of the specific reactant output toward the above synthesis unit, The above-mentioned control unit is a synthetic device that is feedback-controlled by the above-mentioned control unit.

3. In paragraph 1, A first regulating means and a second regulating means are provided, The first control means controls the first flow rate of the first reactant output toward the synthesis unit, The second control means controls the second flow rate of the second reactant output toward the synthesis unit, The first reactant and the second reactant are present in a solution state, The above control unit controls the first control means and the second control means so that when the first flow rate increases, the second flow rate decreases, A synthetic device in which the product always satisfies the preset capacity regardless of changes in the first flow rate or the second flow rate by the above control unit.

4. In paragraph 1, A light source for generating measurement light required for measuring the optical properties of the product, a flow cell through which the product and the measurement light intersect, and a spectrometer for obtaining a spectrum of the measurement light passing through the product are provided. The above control unit is a synthetic device that determines the optical characteristics through analysis of the above spectrum and feedback-controls the flow rate of the specific reactant according to the optical characteristics.

5. In paragraph 1, A measuring unit for measuring the optical properties of the above product is provided, The above control unit is a synthesis device that feedback controls the flow rate of the specific reactant so that the measured optical characteristics measured in the above measurement unit follow the designed optical characteristics of a product having a pre-designed composition.

6. In paragraph 1, A control unit is provided to control the flow rate of the specific reactant output toward the above synthesis unit, A measuring unit is provided for measuring the optical characteristics of the product output from the above synthesis unit, When the time taken for the specific reactant output from the above control unit to pass through the synthesis unit and reach the measurement unit is defined as the response time, The above control unit generates a first control value corresponding to a feedback control value and provides the first control value to the regulating unit, The control unit is a synthesis device that determines the optical characteristics measured by the measurement unit as the execution result of the first control value after the response time has elapsed from the time at which the first control value is provided to the adjustment unit.

7. In paragraph 6, The control unit is a synthesis device that generates a second control value corresponding to a new feedback control value using the execution result of the identified first control value and provides the second control value to the regulation unit.

8. In paragraph 7, A measuring unit for measuring the optical properties of the above product is provided, The above control unit generates the feedback control value using the optical characteristics measured by the above measurement unit, Once the control unit provides the first control value to the first control unit, the control unit maintains the feedback control value for the control unit as the first control value from the time of providing the first control value to the control unit until the generation of the second control value. A synthetic device in which the control unit does not provide a new feedback control value corresponding to the changed optical characteristic to the control unit even if the optical characteristic changes during the period from the time the first control value is provided to the control unit to the time the second control value is generated.

9. In paragraph 8, A synthetic device in which the control unit provides the second control value based on the execution result of the first control value to the control unit instead of the first control value only when the execution result of the first control value is determined after the response time has elapsed from the time at which the first control value is provided to the control unit.

10. In paragraph 1, A first connector, a second connector, a reaction tube and a bubble trap are provided, The above first connector is formed so that the plurality of reactants are merged into one, The second connector is formed so that the output that is merged into one from the first connector and the auxiliary solution for providing the set flow rate are merged, The above reaction tube is formed so that the solution merged through the first connector and the second connector is synthesized, The above bubble trap is formed to remove bubbles contained in the product synthesized through the reaction tube, The above control unit is a synthesis device that feedback controls the flow rate of the specific reactant using measurement information of the product output from the bubble trap.

11. In paragraph 10, One of the plurality of reactants includes silver nanocubes (Ag NanoCubes), and another of the plurality of reactants includes HAuCl4, The above auxiliary solution contains ascorbic acid (AA) and poly vinyl pyrrolidone (PVP).

12. In paragraph 11, The flow rate of the above auxiliary solution is maintained constant at the first set value, A synthesis device in which the flow rate of the above reactant is controlled by the control unit within a range higher than the first set value.

13. In a synthesis method performed by a synthesis device, When a control unit is provided to control the flow rate of a specific reactant flowing into a synthesis unit where synthesis of multiple reactants takes place, A command step for providing a command to the above control unit; When the time taken for the specific reactant output from the control unit according to the above instruction to reach the measurement unit through the synthesis unit is defined as the response time, An acquisition step of acquiring measurement information of a product synthesized from the plurality of reactants from the measurement unit after the response time has elapsed from the time at which the command is provided to the control unit; A control step for performing PID control so that the above measurement information follows the above command; A synthetic method comprising:

14. In paragraph 13, The above control step generates a first control value that resolves the difference between the measurement information and the command and provides it to the control unit, The above control step determines the measurement information measured after the response time has elapsed from the time when the first control value is provided to the control unit as the execution result of the first control value, A synthesis method in which the above control step generates a new second control value that resolves the difference between the execution result of the first control value and the command and provides the new second control value to the control unit.

15. In a synthesis method performed by a synthesis device, Process gain (K) is calculated using the FOPDT (First-Order Plus Dead-Time) model. p ), process time constant (τ p ) and process dead time (θ p ) to obtain an initial controller tuning constant that includes at least one of the following: K obtained p , τ p and θ p Determine P, I and D of PID control based on the values, Based on the determined P, I and D values, the flow rate of the reactants is changed until the target nanomaterial is produced, Using the IMC (Internal Model Control) method, the gain (K) corresponding to the controller P C ) and the integral reset time (τ) corresponding to the above I I ) and obtain Differential time constant (τ) corresponding to the above D D ) is set to 0, A synthesis method wherein at least one of the initial flow rate of the above reactants, the target peak (TP) and the sampling interval time (SIT) is obtained from the user.

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