JP5704630B2 - Crystallization process control method and apparatus - Google Patents

Description

  The present invention relates to a crystallization process control method and apparatus used for a crystallization method for separating and purifying crystals.

  As a method for performing separation and purification of crystals, a crystallization method for performing precipitation purification from a solution can be mentioned. This is an operation in which nuclei are generated from a supersaturated solution and recrystallization is performed by crystal growth using temperature dependence of solubility, solvent evaporation, chemical equilibrium, chemical reaction, substance addition, and the like. Since the properties (melting point, solubility, purity, external shape) of the resulting crystals vary depending on the crystal polymorphs and crystal sizes of the different crystal forms, the target crystal form and its size must be controlled in the crystallization operation. Is very important (for example, Non-Patent Documents 1 and 2).

Moreover, as a crystallization process control method for controlling the target crystal form and its size, a method using FBRM (convergent beam reflection measurement method) can be mentioned. It measures particle size and number of particles in real time, and observes and measures changes in the particle size distribution over time, so that research and process control of the progress, change, and stability of crystallization, polymerization, emulsification, dispersion, aggregation, etc. (For example, Non-Patent Document 2).

Norihito Toki, Satoshi Ogawa, Shigeko Sasaki, Masaaki Yokota, Kenji Shimizu, “Optical resolution of racemic bodies by crystallization”, Journal of Japanese Society for Crystal Growth 35 (1) p31-36 2008 Hiroshi Takiyama, Yasuo Yamazaki, Takahiro Nishida “Special Issue: Crystallization Technology in Various Areas”, Chemical Engineering 71 (3) p130-134 2008

  However, since it is difficult to directly analyze the crystal structure of the conventional method, the crystal is converted into the desired polymorph and size while grasping the crystal structure change in each stage of the crystallization process such as supersaturation and metastable state. It was difficult to grow and precipitate. In particular, in the case of ultra-fine crystals with a few tens to hundreds of units constituting the crystal structure, the problem arises that the physical properties change more sensitively due to slight differences in polymorphs and sizes. Precision control of conditions is required. Although it is possible to confirm the crystal structure and purity by performing X-ray scattering and thermal analysis after obtaining the crystal, it is necessary to obtain a large number of samples with the same structure in order to perform such several types of analysis. was there. Furthermore, there has been a problem that the uniformity of the generated crystal structure tends to be lowered with the scale-up for producing a large number of samples having the same structure.

  The present invention has been made in view of the above circumstances, can control the crystallization conditions when crystallizing the sample, can control the crystal structure and size, and grow and precipitate the sample to the desired polymorph and size It is an object of the present invention to provide a method and apparatus for controlling a crystallization process that can be performed.

The method the crystallization析過according to a first aspect of the present invention includes the steps of emitting an electromagnetic wave of 0.1~10THz the sample solution the component amount of crystallization target the crystallization析過was constant included, the sample solution detecting the transmitted or reflected electromagnetic wave, comprising the steps of: by the detected electromagnetic wave to obtain the absorption spectrum of properties of the sample solution, based on the difference in the absorption intensity of a plurality of absorption bands in the obtained absorption spectrum of properties characterized by a step of controlling the crystallization conditions of the sample solution on the basis of obtaining a crystal structure of the sample solution, the resulting crystal structure.

According to a first aspect of the present invention, the electromagnetic wave components of crystallization target sample solution as the crystallization析過constant irradiated with electromagnetic waves 0.1～10THz, transmitted through or reflected by the sample solution contained Detecting, obtaining an absorption characteristic spectrum of the sample solution from the detected electromagnetic wave, obtaining a crystal structure of the sample solution based on a difference in absorption intensity of a plurality of absorption bands in the obtained absorption characteristic spectrum, By controlling the crystallization conditions of the sample solution based on the obtained crystal structure, the sample can be grown and precipitated into the desired polymorph or size.

  For example, if it is found that the crystal structure is supersaturated or metastable based on the absorption characteristic spectrum, the crystallization conditions are controlled so that the supercrystallization or metastable state is obtained. The sample can be grown and deposited to the desired polymorph and size.

  Theoretical calculation by molecular orbital calculation or molecular dynamics calculation for obtaining the crystal structure of the crystal based on the absorption characteristic spectrum can be performed, for example, during the crystallization process.

  Or, prior to crystallization, theoretical calculation by molecular orbital calculation or molecular dynamics calculation is performed, and the absorption characteristic spectrum or its change state is associated with the crystal structure or its change state (assignment). If the absorption characteristic spectrum and the state of change are found during crystallization, the crystal structure stored and the state of change may be obtained in association with each other.

For example, in the step of obtaining the crystal structure, an arrangement structure between molecules or ions of a component to be crystallized contained in the sample solution is obtained based on a difference in absorption intensity of the plurality of absorption bands .

The crystallizing process control device according to the second aspect of the present invention includes a placing part for placing a sample solution with a constant amount of components to be crystallized, and 0.1 to 10 THz in the sample solution in the crystallization process. absorption characteristics of an irradiation unit for irradiating an electromagnetic wave, and a detector for detecting the electromagnetic wave transmitted through or reflected by the sample solution, for the sample solution with constant component of crystallization object included in advance the sample solution wherein the crystal structure of the sample solution in association with storing each other, the sample solution by detected electromagnetic wave by the detector when the difference between the differences and the absorption intensity of the absorption intensities of a plurality of absorption bands in the spectrum was obtained to obtain the absorption spectrum of properties, with the crystal structure of the sample solution stored in association with the difference in the absorption intensity of a plurality of absorption bands in the obtained absorption spectrum of properties, before on the basis of the crystal structure Characterized in that it comprises a calculation control unit for controlling the crystallization conditions of the sample solution.

For example, crystallization析過as control device includes a temperature adjustment unit for adjusting the temperature of the sample solution, and a pressure adjustment unit for adjusting the pressure of the atmosphere of the sample solution, the calculation control unit, based on the crystal structure And controlling at least one of the temperature adjusting unit and the pressure adjusting unit.

According to the present invention, the components of the crystallization object included irradiated with electromagnetic waves 0.1~10THz the sample solution as the crystallization析過constant, and detecting the electromagnetic wave transmitted through or reflected by the sample solution, to obtain the absorption spectrum of properties of the sample solution by the detected electromagnetic wave, with the crystal structure of the sample solution based on differences in absorption intensities of a plurality of absorption bands definitive in the obtained absorption spectrum of properties, the resulting By controlling the crystallization conditions of the sample solution based on the obtained crystal structure, the sample can be grown and precipitated to the desired polymorph or size.

It is a block diagram which shows one Embodiment of the crystallization process control apparatus of this invention. It is a figure which shows the absorption characteristic spectrum which tracked the change of the crystal structure in each step of a crystallization process for demonstrating Example 1 of this invention.

  Hereinafter, embodiments of the present invention will be described with reference to the drawings.

  An example of the crystallization process control method and apparatus of the present invention will be described with reference to FIG.

  FIG. 1 is a configuration diagram showing a crystallization process control device 10 (hereinafter simply referred to as device 10) according to an embodiment of the present invention.

  The apparatus 10 includes a mounting unit 2 that mounts a chamber 11 that stores the sample solution 1, an irradiation unit 3 that irradiates the sample solution 1 with electromagnetic waves, a detection unit 4 that detects the electromagnetic waves transmitted through the sample solution 1, A calculation control unit 5 for assigning a structure based on the absorption characteristic spectrum of the sample solution 1 based on the electromagnetic wave detected by the detection unit 4, a pressure adjusting unit 6 for controlling the pressure of the sample solution atmosphere, and the sample And a temperature adjusting unit 7 for controlling the temperature of the solution. In addition, the detection part 4 may detect the electromagnetic waves reflected by the thought solution 1.

  The placement unit 2 is a stage arranged substantially horizontally, and the placement unit 2 has a size that allows the chamber 11 to be placed.

  The irradiation unit 3 includes a light source 8 and a pulse generator 9. The light source 8 is only required to excite an electromagnetic wave of 0.1 to 10 THz (hereinafter, appropriately referred to as a terahertz wave), and the light source 8 is, for example, a femtosecond mode-locked titanium sapphire laser or a femtosecond fiber laser.

  The pulse generator 9 only needs to receive excitation light from the light source 8 and generate a terahertz wave. The pulse generator 9 is, for example, a nonlinear optical crystal, a photoconductive antenna, a semiconductor, a quantum well, a high-temperature conductive thin film, or the like.

  The detection unit 4 only needs to detect the terahertz wave that has passed through the sample solution 1, and the detection unit 4 is, for example, a photoconductive antenna.

  The pressure adjustment unit 6 includes a gas pressure control valve 14 for feeding dry nitrogen or dry air, a vacuum pump 15, and a vacuum gauge 16 so that the pressure inside the chamber 11 can be reduced through a path 15 a that leads to the vacuum pump 15. It has become. By sending dry nitrogen or dry air through the gas introduction pipe 14a, the atmosphere inside the chamber 11 is replaced with a desired gas.

  The pressure adjustment unit 6 preferably has a performance of adjusting the pressure inside the chamber 11 to 0.1 Pa to atmospheric pressure. Further, the accuracy of the pressure control preferably has a stability of ± 0.1 to 1 Pa.

  The temperature adjusting unit 7 includes a refrigerant tank 17 such as liquid nitrogen, a heater 18, and a temperature sensor 19, and sends a refrigerant such as liquid nitrogen into the chamber 11 from the path 17 a and the heater 18 a introduced into the chamber 11. , The chamber 11 is cooled or heated to control the crystallization process conditions of the sample solution 1.

  It is preferable that the temperature adjusting unit 7 has a heating / cooling performance capable of setting the temperature of the chamber 11 to −200 to 100 ° C. The temperature control accuracy preferably has a stability of ± 0.1 to 1.0 ° C.

  In the chamber 11, an upper part facing the irradiation unit 3 and a lower part facing the detection unit 4 are optical windows 11 a through which the terahertz wave can be transmitted.

  The apparatus 10 is provided with parabolic mirrors 12 and 14.

  Next, an example of a crystallization process control method performed by the apparatus 10 for the sample solution 1 will be described.

  The sample solution 1 is, for example, a saturated NaCl solution or a saturated KCl solution. The sample solution 1 preferably has a thickness in the electromagnetic wave irradiation direction (vertical direction in FIG. 1) of 0.1 to 15 mm (desirably 0.5 to 2 mm).

  If the sample solution 1 is too thin, the amount of the target component is reduced, so that the detection accuracy is lowered. If the sample solution 1 is too thick, the terahertz wave is hardly transmitted. On the other hand, by setting the thickness within the above range, the detection accuracy can be improved and the terahertz wave can be transmitted with certainty. In addition, multiple reflection and interference are less likely to occur. Therefore, highly accurate analysis is possible.

  The sample solution 1 preferably has a maximum dimension in a plane (the above-described in-plane direction) intersecting with the electromagnetic wave irradiation direction of 3 to 15 mm. If this maximum dimension is too large, precise control of the crystallization conditions becomes difficult due to uneven temperature and pressure. On the other hand, the precision of crystallization condition control can be improved by making a maximum dimension into the said range.

  The calculation control unit 5 drives the temperature adjustment unit 7 in accordance with the temperature in the chamber 11 detected by the temperature sensor 19 to heat or cool the chamber 11 to a predetermined temperature.

When the sample solution 1 is frozen, the cooling rate is preferably −0.1 to −5 ° C./second (desirably −1 to −1.5 ° C./second). In order to prevent condensation of water vapor inside due to cooling, it is preferable to reduce the pressure to about 10 ⁴ Pa using the pressure adjusting unit 6 before the start of cooling. After the temperature reaches about −20 ° C., it is replaced with a vacuum atmosphere or dry nitrogen or dry air. By setting the cooling rate within this range, the structure of the crystallization process is reflected in the sample solution 1 without the substances in the sample solution 1 being deposited outside, and the components to be crystallized in the sample solution 1 are Intermolecular interaction is exhibited with solvent molecules (such as water) in the sample solution 1.

  When the sample solution 1 is to be frozen, the ultimate cooling temperature is first left at −100 to −20 ° C. (preferably −80 to −70 ° C.) for 10 to 360 minutes (preferably 60 to 180 minutes). Measure structural changes. By setting the cooling temperature within this range, molecular movement and structural changes are unlikely to occur in a macro region, but it is necessary to form ultrafine crystals with a very small number of units constituting the crystal structure. Only simple microscopic molecular movements are possible. After that, it is preferable to re-cool to -200 to -150 ° C (desirably -200 to -180 ° C). By setting the cooling temperature within this range, it is possible to stop molecular movement and structural change even in the formed ultrafine crystal structure, and to take out a desired crystal polymorph and size.

  In this process, the pulse generator 9 is irradiated with excitation light from the light source 8 at appropriate times. The pulse generator 9 generates a terahertz wave W1, is focused by a parabolic mirror 12, and is irradiated onto the subject 1.

  When the sample solution 1 is irradiated with the terahertz wave W1, it resonates with energy of weak interaction such as hydrogen bond, van der Waals bond, π electron interaction, electrostatic interaction and the like.

  The terahertz wave W <b> 2 that has passed through the sample solution 1 becomes parallel light by the parabolic mirror 13 and reaches the detection unit 4.

  The detector 4 detects the terahertz wave W <b> 2 and the detected value is sent to the calculation control unit 5.

  The calculation control unit 5 converts the detected value into a function of a frequency of 0.1 to 10 THz by Fourier transform.

  Based on this, the calculation control unit 5 obtains the absorption characteristic spectrum normalized so as to correspond to the unit thickness of the sample solution 1 and the unit concentration of the target component and its change.

  For example, if it is found that the crystal structure is supersaturated or metastable based on the obtained absorption characteristic spectrum or change, the calculation control unit 5 sets crystallization conditions suitable for the supersaturation or metastable state. To grow and deposit the sample to the desired polymorph and size.

  For example, in order to obtain a crystal structure based on the absorption characteristic spectrum, the calculation control unit 5 performs calculation by molecular orbital calculation or molecular dynamics calculation during the crystallization process. The crystal structure is, for example, an array structure between sample molecules or an array structure between sample ions.

  Or, prior to crystallization, perform theoretical calculations by molecular orbital calculation or molecular dynamics calculation, and the crystal structure in solution at each stage of the crystallization process and its change, absorption characteristic spectrum or its change Are stored in association with each other, and if an absorption characteristic spectrum or a change is obtained during crystallization, the calculation control unit 5 can change the stored crystal structure in association with each other. The crystallization conditions may be adjusted based on this.

  That is, since the resonance frequency and absorption intensity of the energy of the interaction are in accordance with the structure of the crystallization process in the sample solution 1, this absorption characteristic spectrum can be used as an index of crystal polymorphism or size. It is.

  According to the apparatus 10 according to the present embodiment, that is, according to the crystallization process control method, the sample solution 1 in the crystallization process is irradiated with electromagnetic waves, and the terahertz wave W2 transmitted through the sample solution 1 is detected. Since the absorption characteristic spectrum of the sample solution 1 is obtained by the terahertz wave W2, the crystal structure of the sample solution 1 is obtained based on the absorption characteristic spectrum, and the crystallization conditions of the sample solution 1 are controlled based on the crystal structure. Measure particle size and number of particles in real time and observe and measure changes in particle size distribution over time to conduct research and process control of crystallization, polymerization, emulsification, dispersion, aggregation, etc. Compared to the method, fine control of the crystallization conditions is facilitated, and it becomes easy to grow and precipitate the crystal to the desired polymorph and size. In addition, even for ultra-fine crystals with a few tens to hundreds of units that make up the crystal structure, the physical properties of which tend to change more sensitively due to slight differences in polymorphs and sizes. It is possible to grow and precipitate.

  Even in the case of an ultrafine crystal having a very small number of units (the number of lattices) constituting the crystal structure, such as 1 to several tens, it can be grown and precipitated into the desired polymorph or size.

  In addition, there is no need to obtain a crystal structure or purity by performing X-ray scattering or thermal analysis after obtaining the crystal structure (conventional procedure), so there is no need to obtain a large number of samples with the same structure, which can be scaled up. Along with this, it becomes easy to prevent a decrease in the uniformity of the crystal structure to be generated.

  Examples of the present invention will be specifically described below with reference to FIGS. In addition, this Example is an example and does not limit this invention.

  An analytical test was performed using the apparatus 10 shown in FIG. The apparatus 10 includes a pulse generator 9 (manufactured by Infrared Inc., photoconductive antenna), and a spectroscopic device (manufactured by Advanced Infrared Inc., THz-TDS2004) provided with a detection unit 4 (manufactured by Infrared IR, photoconductive antenna) It was produced using. The light source 8 used was Ti-sapphire laser Vitesse (100 femtosecond type, manufactured by Coherent).

  As the sample solution 1, a 1 mol / L NaCl solution was introduced to a depth of 1.5 mm.

  The sample solution 1 was irradiated with the terahertz wave W1 using the irradiation unit 3, and the terahertz wave W2 was detected by the detection unit 4. If the sample solution 1 is too thin, the amount of the target component is reduced, so that the detection accuracy is reduced. If the sample solution 1 is too thick, the terahertz wave is not easily transmitted. However, in this example, such a decrease in the detection accuracy did not occur. The thickness of Solution 1 was judged reasonable.

  The in-plane dimension (the in-plane direction) intersecting the electromagnetic wave irradiation direction was 10 mm. If this maximum dimension is too large, it becomes difficult to precisely control the crystallization conditions due to uneven temperature and pressure. However, in this example, the unevenness of the sample due to such unevenness did not occur. The inside dimensions were judged to be reasonable.

  The sample solution 1 was rapidly cooled to -70 ° C. and frozen at a cooling rate of −1.5 ° C./second, and an absorption characteristic spectrum was measured in order to measure the arrangement structure between molecules and ions in the sample. . At this time, a broad absorption band was observed in the vicinity of about 1.6 THz (FIG. 2 (a)). This absorption band shows a structure in which sodium ions and chloride ions in ice are more disordered than the cubic crystal structure by molecular orbital calculation using a model in which a single unit of sodium chloride type (cube) is formed. When taken, it was assigned to be a peak derived from an interaction with water molecules.

  While maintaining the temperature at −70 ° C., the absorption characteristic spectrum was measured at regular intervals. After several hours, an absorption band near about 2.4 THz began to appear and was gradually observed as a sharp peak (FIG. 2 (b)). This absorption band is based on molecular orbital calculation using a model in which sodium ions and chloride ions in ice constitute a single unit of sodium chloride type (cube). When they took a slightly more disturbed structure than the cubic crystal structure in ice, they were assigned as peaks derived from interactions with water molecules. Compared with the peak at about 1.6 THz, the timing at which observation begins is different because the order formation process of the crystal structure gradually proceeds in the state of being kept at −70 ° C., and is observed as a new structure. It is thought that it became.

  Thereafter, the sample was rapidly cooled to −196 ° C. at a cooling rate of −1.5 ° C./second, and an absorption characteristic spectrum was measured. Absorption bands around 1.6 THz and around 2.4 THz were observed in the same manner as when the temperature was kept at -70 ° C., but this resulted in low background absorption intensity and constituted a single unit. This is because water molecules with little interaction with sodium ions and chloride ions have changed to more stable and ordered ice structures.

  Thereafter, the sample was gently heated at a heating rate of 1 ° C./min, and the absorption characteristic spectrum was measured at a step of 10 ° C. in the range from −110 ° C. to 20 ° C. Up to a temperature of −20 ° C., an absorption spectrum almost identical to the absorption characteristic spectrum obtained at −196 ° C. was obtained, indicating that the crystal structure was retained, but when the temperature reached −10 ° C., Only absorption bands near about 1.6 THz and about 2.5 THz were observed, and the absorption intensity due to the background disappeared (FIG. 2 (c)). This is presumably because water molecules with little interaction with sodium ions and chloride ions constituting a single unit were evaporated by heating, and only NaCl crystals having the same structure as in ice at −196 ° C. remained.

  Using this technique, NaCl crystals are obtained as fine particles having a particle size of about 10 to 100 nm, and it is found that these are ultrafine crystals with a few tens to hundreds of units constituting the crystal structure. It was. These fine particles were found to have superior solubility in water as compared with normal NaCl crystals mechanically pulverized.

  Here, when performing rapid cooling to -196 ° C without performing the process of maintaining at -70 ° C, a broad absorption band is observed around 1.6 THz, but the absorption band around 2.5 THz is Not observed. This is because the order formation process of the crystal structure, which occurs in a state of being held at -70 ° C. for a certain period of time, did not go through a process of gradually changing to a new structure, and thus the desired polymorph was not obtained. It is. In this case, the crystal obtained by evaporating the surrounding water molecules by heating has a large particle size of about 1-100 μm, and the solubility in water is only the same level as that of a normal NaCl crystal. It was.

  Therefore, according to the present embodiment, it is possible to obtain and feed back the crystal structure in the solution at each stage of the crystallization process based on the absorption characteristic spectrum obtained by detecting the terahertz wave transmitted through the sample solution 1. It became clear that we could do it. In this example, it was possible to confirm the change to the target crystal structure by observing the occurrence of an absorption band near about 2.4 THz while maintaining the temperature at -70 ° C. That is, when an absorption band near about 2.4 THz is not developed, the control of heating the temperature control to the high temperature region and cooling to the low temperature region is repeated again so that the order formation process of the crystal structure proceeds. . Moreover, you may perform control which increases / decreases the pressure in those processes suitably, and control of a cooling rate. In this way, fine control of the crystallization conditions is facilitated, and it becomes easy to grow and precipitate crystals to the desired polymorph and size. In addition, ultrafine crystals with very few tens to hundreds of units that make up the crystal structure, where the physical properties such as solubility in water are more sensitive to changes due to slight differences in polymorphs and sizes. It has become clear that it is possible to grow and precipitate to the desired polymorph and size.

DESCRIPTION OF SYMBOLS 1 ... Sample solution 2 ... Placement part 3 ... Irradiation part 4 ... Detection part 5 ... Calculation control part 6 ... Pressure adjustment part 7 ... Temperature adjustment part 8 ... Light source 9 ... Pulse generator 10 ... Crystallization process control apparatus 11 ... Chamber DESCRIPTION OF SYMBOLS 11a ... Optical window 12, 13 ... Parabolic mirror 14 ... Gas pressure control valve 14a ... Gas introduction pipe 15 ... Vacuum pump 15a ... Path | route 16 ... Vacuum gauge 17 ... Refrigerant tank 17a ... Path | route 18, 18a ... Heater 19 ... Temperature sensor

Claims (5)

Irradiating an electromagnetic wave of 0.1 to 10 THz to a sample solution in a crystallization process in which the amount of a component to be crystallized is constant ;
Detecting the electromagnetic wave transmitted through or reflected by the sample solution,
Obtaining an absorption characteristic spectrum of the sample solution from the detected electromagnetic wave;
Obtaining a crystal structure of the sample solution based on a difference in absorption intensity of a plurality of absorption bands in the obtained absorption characteristic spectrum;
Controlling the crystallization conditions of the sample solution based on the obtained crystal structure. The step of obtaining the crystal structure is to obtain an arrangement structure between molecules or ions of a component to be crystallized contained in the sample solution based on a difference in absorption intensity of the plurality of absorption bands. The crystallization process control method according to claim 1. For the sample solution the component amount of crystallization subject to a constant included, the manner and the absorption intensity change of the difference of differences or the absorption intensity of the absorption intensities of a plurality of absorption bands in the absorption spectrum of properties of the previously said sample solution A difference or a change in the absorption intensity is observed in association with the crystal structure of the sample solution or the change in the crystal structure when the change is observed.
In the step of obtaining the crystal structure, the difference in the absorption intensity of the plurality of absorption bands in the obtained absorption characteristic spectrum or the change in the crystal structure or the crystal structure stored corresponding to the change in the difference in the absorption intensity is stored. The method for controlling a crystallization process according to claim 1 or 2, wherein: A placement unit for placing a sample solution in which the amount of a component to be crystallized is constant ;
An irradiation unit for irradiating the sample solution in the crystallization process with an electromagnetic wave of 0.1 to 10 THz ;
A detector for detecting the electromagnetic wave transmitted through or reflected by the sample solution,
For the sample solution the component amount of crystallization subject to a constant included, the sample solution when the pre-difference between differences and the absorption intensity of the absorption intensities of a plurality of absorption bands in the absorption spectrum of properties of the sample solution was obtained Are stored in association with each other, the absorption characteristic spectrum of the sample solution is obtained from the electromagnetic wave detected by the detection unit, and the difference in absorption intensity of a plurality of absorption bands in the obtained absorption characteristic spectrum is obtained. A crystallization process control apparatus, comprising: a calculation control unit that obtains a crystal structure of the sample solution stored in association with each other and controls a crystallization condition of the sample solution based on the crystal structure. A temperature adjusting unit for adjusting the temperature of the sample solution ;
A pressure adjustment unit for adjusting the pressure of the atmosphere of the sample solution ,
The calculation control unit
The crystallization process control device according to claim 4, wherein at least one of the temperature adjustment unit and the pressure adjustment unit is controlled based on the crystal structure.

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