WO2024065074A1 - Réacteur à flux continu à microcanaux combinés dynamique - Google Patents

Réacteur à flux continu à microcanaux combinés dynamique Download PDF

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Publication number
WO2024065074A1
WO2024065074A1 PCT/CN2022/121198 CN2022121198W WO2024065074A1 WO 2024065074 A1 WO2024065074 A1 WO 2024065074A1 CN 2022121198 W CN2022121198 W CN 2022121198W WO 2024065074 A1 WO2024065074 A1 WO 2024065074A1
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WO
WIPO (PCT)
Prior art keywords
reaction tube
rotating shaft
baffle
heat exchanger
baffles
Prior art date
Application number
PCT/CN2022/121198
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English (en)
Chinese (zh)
Inventor
叶伟平
周宏宇
费安杰
王扬
吴杰
傅利
罗富元
林柳君
周章涛
Original Assignee
广东莱佛士制药技术有限公司
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Application filed by 广东莱佛士制药技术有限公司 filed Critical 广东莱佛士制药技术有限公司
Priority to PCT/CN2022/121198 priority Critical patent/WO2024065074A1/fr
Publication of WO2024065074A1 publication Critical patent/WO2024065074A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F27/00—Mixers with rotary stirring devices in fixed receptacles; Kneaders
    • B01F27/80—Mixers with rotary stirring devices in fixed receptacles; Kneaders with stirrers rotating about a substantially vertical axis
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01L—CHEMICAL OR PHYSICAL LABORATORY APPARATUS FOR GENERAL USE
    • B01L3/00—Containers or dishes for laboratory use, e.g. laboratory glassware; Droppers

Definitions

  • the invention relates to the field of continuous flow reaction devices, in particular to a dynamic mixing microchannel continuous flow reactor.
  • Common microchannel reactors are planar structures and belong to static mixers. Although they have good mass transfer and heat exchange effects, their solid content carrying capacity for the reactor is relatively weak (generally, the solid loading must be less than 10%, and the solid particle size must be less than 0.5 mm). For tubular reactors with relatively good solid content carrying capacity, their mass transfer effect is poor, and the larger the tube diameter, the worse the mass transfer and heat transfer effect, and the more obvious the amplification effect, resulting in low production efficiency. Even if the tubular reactor is designed in the form of dynamic rotating shaft mixing, turbulence is increased, and the mass transfer effect is enhanced, its mass transfer and heat transfer effect is still far from that of the traditional microchannel continuous flow reactor.
  • the conventional continuous flow reactor has strong specificity and weak universality, and production equipment needs to be customized for different processes, and the related investment is high. Therefore, the industry is in urgent need of a type of continuous flow reactor with strong process universality and can be assembled quickly.
  • the purpose of the present invention is to provide a dynamic mixing microchannel continuous flow reactor, aiming to solve the shortcomings of low solid loading capacity of microchannels, easy channel clogging, poor mixing effect and weak heat exchange capacity of common tubular reactors, so as to achieve one reactor to cover multiple reaction types, increase equipment utilization, improve production efficiency and reduce production costs.
  • the present invention is implemented through the following technical solutions:
  • the inner curved surface of the reaction tube and the rotating shaft are designed as a continuous multi-level structure with uneven surfaces.
  • the inner wall of the reaction tube and the rotating shaft are nested with each other to form a tiny reaction channel.
  • the rotating shaft provides lateral shear force as the driving force for dynamic mixing.
  • the reaction tube is designed as a two-in-one split structure. On the one hand, it is easy to disassemble and repair. On the other hand, higher protrusions can be designed on the inner surface of the reaction tube and the surface of the rotating shaft, so that a smaller microchannel can be formed, further enhancing the mass transfer effect.
  • the rotating shaft is designed to be a multi-tooth structure with high and low protrusions, the height of the high protrusion is 3.0-20.0 mm, the height of the concave part is 1.0-3.0 mm, and the overall concave part is nested with the protrusion of the reaction tube to allow fluid to pass through, and it is a multi-tooth structure when viewed from the side;
  • the main body of the reaction tube is a reactant container cavity, which is a split structure and can be divided into two. There is a sealing gasket at the joint.
  • the inner wall of the container cavity is designed as a split-type continuous flow multi-stage structure.
  • the protruding part is used as a baffle.
  • the height of the baffle is between 3.0 and 20.0 mm.
  • the depth of the concave structure here is 1.00 to 3.00 mm.
  • the distance between the top of the rotating shaft protrusion and the bottom of the overall depression of the reaction tube is between 1.0 and 3.0 mm, and the distance between the top of the reaction tube protrusion and the bottom of the overall depression of the rotating shaft is between 1.0 and 3.0 mm;
  • a detachable, split-type return flow channel type jacket heat exchanger is used outside the reaction tube, which can be divided into two parts, with a sealing gasket at the joint, and is integrated with the reaction tube by overlapping with fixing bolts.
  • the groove inside the heat exchanger is tightly fitted with the outer wall of the reaction tube to form a heat exchange passage;
  • Both ends of the reaction tube are composed of quick-release flanges, which are used for overall sealing, as well as bearing mechanical seals and fixing the rotating shaft;
  • the driving device adopts a servo motor or a pneumatic motor to drive the rotating shaft to rotate, and can realize multi-level speed adjustment.
  • the beneficial effect of the present invention lies in that the present invention adopts a unique structural design, namely: on the one hand, the reactor pipe size adopted by the present invention is the size of a common tubular reactor, and a micro-reaction channel is formed in the reaction tube through the inner wall of the tube and the concave baffle structure on the rotating shaft, thereby greatly improving the mass transfer and heat transfer efficiency of the tubular reactor, and at the same time having the advantages of high mass transfer efficiency of the microchannel continuous flow reactor and large flux of the tubular reactor, but avoiding the disadvantages of low solid carrying capacity of the microchannel reactor and poor mass transfer and heat transfer of the conventional tubular reactor.
  • the reaction tube is designed as a split structure, which is convenient for disassembly and assembly, and thus the concave baffle structure on the inner wall of the tube and the convex structure on the rotating shaft can be designed to be larger in size, so that a smaller microchannel can be formed, back-mixing phenomenon can be avoided, and the mass transfer effect is further enhanced.
  • FIG1 is an exploded view of a dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • FIG2 is a schematic diagram of the overall structure of a dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • FIG 3 is a longitudinal cross-sectional view of the overall structure of a dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • FIG. 4 is a schematic diagram of the structure of a heat exchanger in a dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • FIG5 is a schematic diagram of the reaction tube structure in a dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • FIG6 is a schematic diagram of the structure of the rotating shaft in the dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • FIG. 7 is a schematic diagram of the flange cover structure in a dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • orientation or positional relationship indicated by the terms “length”, “width”, “upper”, “lower”, “far”, “near”, etc. is based on the orientation or positional relationship shown in the drawings, which is only for the convenience of describing the invention and simplifying the description, and does not indicate or imply that the device or element referred to must have a specific orientation, be constructed and operated in a specific orientation, and cannot be understood as limiting the specific protection scope of the invention.
  • first and second are only used for descriptive purposes to distinguish technical features, and do not have substantial meanings, and cannot be understood as indicating or implying relative importance or implicitly indicating the number of technical features.
  • the dynamic mixing microchannel continuous flow reactor includes a reaction tube, a rotating shaft 30, a first heat exchanger 10 and a second heat exchanger 11, a coupling 60 and a driving device 70.
  • the reaction tube includes a first half reaction tube 20 and a second half reaction tube 21, the inner diameter of the reaction tube is greater than the outer diameter of the rotating shaft 30, the rotating shaft 30 is coaxially arranged inside the reaction tube 20, and the driving device 70 is configured to be able to drive the rotating shaft 30 to rotate relative to the reaction tube.
  • the first half reaction tube 20 and the second half reaction tube 21 are two semi-cylinders of the same shape and size, and the two are assembled together to form a reaction tube with a cylindrical space inside (see Figure 4).
  • the first half reaction tube 20 and the second half reaction tube 21 are fixed as a whole by bolts in the transverse position, and the radial fitting surfaces of the two are provided with PTFE sealing gaskets.
  • At least one stopper is provided on the inner surface of the reaction tube formed by the first half reaction tube 20 and the second half reaction tube 21.
  • the stopper is in a circular shape and close to the inner surface of the reaction tube.
  • the height of the at least one stopper on the inner surface of the reaction tube is between 3.0 and 20.0 mm.
  • At least one depression is provided on the stopper, and the depth of the depression is 1.00 to 3.00 mm.
  • at least one stopper is provided on the rotating shaft 30.
  • the stopper is in a circular shape and close to the surface of the rotating shaft 30.
  • the height of the at least one stopper on the rotating shaft 30 is between 3.0 and 20.0 mm.
  • At least one depression is provided on the stopper, and the depth of the depression is 1.00 to 3.00 mm.
  • the at least one stopper provided on the inner surface of the reaction tube and the at least one stopper provided on the rotating shaft 30 are staggered with each other, so that the rotational movement between the reaction tube and the rotating shaft 30 is not affected.
  • the height of the at least one stopper provided on the inner surface of the reaction tube can be flexibly set according to the size of the reaction tube and the rotating shaft 30, but the height of the stopper cannot be too high, at least it cannot contact the surface of the rotating shaft 30, so as not to affect the rotation of the rotating shaft 30.
  • the height of at least one stopper provided on the rotating shaft 30 can be flexibly set according to the size of the reaction tube and the rotating shaft 30 , but the height of the stopper cannot be too high, at least it cannot contact the inner surface of the reaction tube to avoid affecting the rotation of the rotating shaft 30 .
  • At least two baffles are arranged on the inner surface of the reaction tube, and at least two baffles are spaced apart from each other in the radial direction and arranged on the inner surface of the reaction tube.
  • Each baffle includes at least two depressions, and the at least two depressions are evenly arranged on the baffle.
  • 6 baffles are arranged on the inner surface of the reaction tube, and the 6 baffles are spaced apart from each other in the radial direction and arranged on the inner surface of the reaction tube.
  • Each baffle includes 8 depressions, and the 8 depressions are evenly arranged on the same baffle.
  • the depth of the depression is 1.0 to 3.0 mm
  • the width is 1.0 to 3.0 mm
  • the depression is in the shape of a cuboid
  • the length is between 2.0 and 10.0 mm
  • the height of the baffle is between 3.0 and 20.0 mm
  • the interval between one baffle and another baffle is 4.0 to 22.0 mm.
  • the number of baffles, the number of depressions in each baffle, the shape of each depression, and the size of each depression do not need to be set strictly according to the above embodiments.
  • the general principle is to disturb the reactant flow flowing through the reaction tube by the baffles and depressions on the inner surface of the reaction tube to avoid back mixing and enhance the mixing effect and mass transfer effect of the reactants.
  • baffles it is better to set more than 3 groups of baffles on the inner surface of the reaction tube. Generally, 3-20 baffles are set. If the reaction tube is long, more baffles can be set, such as 30, 50, or even 100. 6-12 depressions are set on each baffle, but more depressions can also be set according to the circumference of the shaft and the tube. The interval between each depression is 2.0-5.0 mm, which can achieve better results.
  • At least two baffles are provided on the surface of the rotating shaft 30, and the at least two baffles are spaced apart from each other in the radial direction and are provided on the surface of the rotating shaft 30.
  • Each baffle includes at least two depressions, and the at least two depressions are evenly provided on the surface of the rotating shaft 30 at the same radial position.
  • six baffles are provided on the surface of the rotating shaft 30, and the six baffles are spaced apart from each other in the radial direction and are provided on the surface of the rotating shaft 30.
  • Each baffle includes eight depressions, and the eight depressions are evenly provided on the same baffle.
  • the width of the depression is 1.0 to 3.0 mm
  • the depth of the depression is 1.0 to 3.0 mm
  • the depression is in the shape of a cuboid
  • the length is between 2.0 and 10.0 mm
  • the height of the baffle is between 3.0 and 20.0 mm
  • the interval between one baffle and another baffle is 4.0 to 22.0 mm.
  • the number of baffles, the number of depressions in each baffle, the shape of each depression, and the size of each depression do not need to be set strictly according to the above embodiments.
  • the general principle is to disturb the reactant flow flowing through the reaction tube 20 by the baffles and depressions on the surface of the rotating shaft 30 to avoid back mixing and enhance the mixing effect and mass transfer effect of the reactants.
  • baffles According to the experience of the inventors of this application, it is better to set more than 3 baffles on the inner surface of the rotating shaft 30, and generally 3-20 baffles are set. If the reaction tube is long, more baffles can be set, such as 30, 50, or even 100. Each baffle is set with 6-12 depressions, which can achieve better results.
  • the first heat exchanger 10 and the second heat exchanger 11 are assembled into a cylinder, the inner diameter of which is the same as the outer diameter of the reaction tube, and the length of which is equal to the length of the reaction tube.
  • the first heat exchanger 10 and the second heat exchanger 11 are tightly fitted on the outside of the reaction tube and fixed on the reaction tube by the first outer ring flange clamp 50, the second outer ring flange clamp 51, the third outer ring flange clamp 52, and the fourth outer ring flange clamp 53.
  • Sealing gaskets are provided at the places where the first heat exchanger 10 and the second heat exchanger 11 are fitted to each other, and at the places where the first heat exchanger 10 and the second heat exchanger 11 are fitted to the reaction tube at both ends.
  • the inner walls of the first heat exchanger 10 and the second heat exchanger 11 have grooved passages, the passages are 5.0 to 20.0 mm wide and 2.0 to 20.0 mm deep.
  • the first flange cover 40 and the second flange cover 41 are installed at both ends of the reaction tube and seal the reaction tube.
  • FIG7 is a structural diagram of the flange cover of the dynamic mixing microchannel continuous flow reactor provided in an embodiment of the present invention.
  • four inlet/outlet ports are arranged on the first flange cover 40: the first inlet/outlet port 400, the second inlet/outlet port 401, the third inlet/outlet port 402, and the fourth inlet/outlet port 403, and these four inlet/outlet ports can also be used as temperature detection ports.
  • inlet/outlet ports are arranged on the second flange cover 41: the fifth inlet/outlet port 410, the sixth inlet/outlet port 411, the seventh inlet/outlet port 412, and the eighth inlet/outlet port 413.
  • the drive device 70 is configured to be able to drive the rotating shaft 30 to rotate relative to the reaction tube.
  • the output shaft of the drive device 70 is coaxially connected to the rotating shaft 30 through a coupling 60, so that when the drive device 70 rotates, it can drive the rotating shaft 30 to rotate together, so that the baffles on the inner surface of the reaction tube (staggered and adjacent to each other) and the baffles on the surface of the rotating shaft 30 also move relative to each other, and the reactant fluid flowing through the inner cavity of the reaction tube is subjected to the lateral shear force of the rotating shaft 30, which will passively form turbulence, and enter the convex and concave parts of the adjacent reaction tube surface baffles through the tiny gap between the top of the baffle on the surface of the rotating shaft 30 and the reaction tube, and is further blocked, diverted, and mixed again.
  • the above reactors were integrated, and the specific reactor parameters were as follows: 1) The diameter of the rotating shaft 30 was 15.0 mm, the height of the baffle was 4.0 mm, the width was 4.0 mm, the width of the teeth on the baffle was 2.0 mm, the number of depressions on each baffle was 8, the depth of each depression was 1.0 mm, there were 6 baffles in total, the length of each repeating unit (including a baffle and an adjacent cavity) was 12.0 mm, the length of the shaft 30 was 90 mm, and the rotation speed was 200 rpm; 2) The wall thickness of the reaction tube 20 was 4.0 mm, the height of the baffle was 4.0 mm, the width was 4.0 mm, the width of the teeth on the baffle was 2.0 mm, the number of depressions on each baffle was 8 , each depression has a depth of 1.0 mm, there are 6 sets of baffles in total, the length of each repeating unit (including a baffle and an adjacent cavity) is 12.0 mm, the outer diameter of the
  • the water emulsion is prepared by using three fluid feeds of vegetable oil (fluid one), emulsifier (fluid two) and water (fluid three).
  • the feed rate of vegetable oil is 10mL/min
  • the emulsifier is 15mL/min
  • the water feed rate is 30mL/min.
  • the three fluids are fed from the feed port at the same end at 20-25°C. After mixing by the shear force of the rotating shaft, a water emulsion is obtained. Analysis and detection show that the oil droplet size is about 0.9 ⁇ m.
  • the heat exchange capacity was verified. 60°C water was used as the only fluid to be injected into the reactor from the feed port and out of the other end of the discharge port.
  • the fluid flow rate was 50mL/min
  • the heat exchange jacket temperature was set to 30°C
  • the heat transfer oil flow rate in the heat exchanger was 35L/min.
  • the temperature information of the hot water fluid entering and leaving the reactor was monitored. After the overall working conditions were stabilized, after the 60°C hot water passed through the reactor, the actual measured fluid temperature at the discharge port was 31°C, which was +1.0°C lower than the temperature of the heat exchanger jacket, and the error range was less than 4.0%.
  • the interior of the reaction tube 20 is designed to be smooth without continuous protrusions, and the remaining components, such as heat exchangers 10 and 11, shaft 30, flange covers 40 and 41, and flange clamps 50-53, are the same as those in Example 1.
  • This scheme is used to test the mixing effect, and three fluids, vegetable oil (fluid one), emulsifier (fluid two) and water (fluid three), are fed at 20-25°C to prepare an aqueous emulsion.
  • the feed rate of vegetable oil is 10mL/min
  • the emulsifier is 15mL/min
  • the feed rate of water is 30mL/min.
  • the three fluids are fed from the feed port at the same end, and the aqueous emulsion is obtained after mixing by the shear force of the shaft.
  • the oil droplet size is about 2.5 ⁇ m after analysis.
  • 60°C water is used as the only fluid to be injected into the reactor from the feed port and out of the other end of the discharge port.
  • the fluid flow rate is 50mL/min
  • the heat exchange jacket temperature is set to 30°C
  • the heat transfer oil flow rate in the heat exchanger is 35L/min. Monitor the temperature information of the hot water fluid entering and leaving the reactor. After the overall working conditions are stable, after the 60°C hot water passes through the reactor, the actual measured fluid temperature at the discharge port is 35°C, which is +5.0°C different from the heat exchanger jacket temperature, and the error range is about 17%.
  • the grooves inside the heat exchanger are removed, and the inner surface of the heat exchanger is a smooth structure.
  • the remaining components, such as the reaction tube 20, the rotating shaft 30, the flange covers 40 and 41, and the flange clamps 50-53 are the same as those in Example 1.
  • 60°C water is used as the only fluid to be injected into the reactor from the feed port and out of the other end of the discharge port.
  • the fluid flow rate is 50mL/min
  • the heat exchange jacket temperature is set to 30°C
  • the heat transfer oil flow rate in the heat exchanger is 35L/min. Monitor the temperature information of the hot water fluid when it enters and exits the reactor. After the overall working conditions are stable, after the 60°C hot water passes through the reactor, the actual measured fluid temperature at the discharge port is 31.5°C, which is +1.5°C different from the heat exchanger jacket temperature, and the error range is less than 5.0%.
  • Example 1 The dynamic microchannel tubular continuous reactor provided by the embodiment of the present invention has a better oil-water mixing emulsification effect than that of the ordinary tubular reactor. Under the test conditions, the particle size of the emulsified oil droplets is reduced by 178% (0.9 ⁇ m vs. 2.5 ⁇ m), and the overall emulsification is more sufficient; 2) The concave-convex design of the reaction tube and the grooved reflux flow design of the heat exchanger increase the heat exchange area inside the reactor, and the overall heat exchange capacity of the reactor is improved. Under the test conditions, the fluid inlet temperature of Example 1 is closest to the temperature of the heat exchanger oil, and the temperature control is more precise.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Health & Medical Sciences (AREA)
  • Clinical Laboratory Science (AREA)
  • Organic Chemistry (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)

Abstract

L'invention concerne un réacteur à flux continu à microcanaux combinés dynamique, comprenant un tube de réaction, un arbre rotatif (30), un premier échangeur de chaleur (10), un second échangeur de chaleur (11), un coupleur (60) et un dispositif d'entraînement (70), le tube de réaction comprenant une première moitié de tube de réaction (20) et une seconde moitié de tube de réaction (21) ; le diamètre interne du tube de réaction est supérieur au diamètre externe de l'arbre rotatif (30), et l'arbre rotatif (30) est agencé de manière coaxiale à l'intérieur du tube de réaction ; le dispositif d'entraînement (70) est conçu pour pouvoir entraîner l'arbre rotatif (30) en rotation par rapport au tube de réaction ; et la première moitié de tube de réaction (20) et la seconde moitié de tube de réaction (21) constituent deux demi-cylindres de même forme et de même taille, et sont assemblés ensemble afin de former le tube de réaction comportant un espace cylindrique à l'intérieur de celui-ci. Une conduite de réacteur présente la même taille qu'un réacteur tubulaire commun, et des microcanaux de réaction sont formés dans le tube de réaction au moyen de structures de déflecteur, qui comportent des évidements, sur la paroi interne de tube et l'arbre rotatif (30), de sorte que l'efficacité de transfert de masse et chaleur du réacteur tubulaire soit améliorée.
PCT/CN2022/121198 2022-09-26 2022-09-26 Réacteur à flux continu à microcanaux combinés dynamique WO2024065074A1 (fr)

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PCT/CN2022/121198 WO2024065074A1 (fr) 2022-09-26 2022-09-26 Réacteur à flux continu à microcanaux combinés dynamique

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PCT/CN2022/121198 WO2024065074A1 (fr) 2022-09-26 2022-09-26 Réacteur à flux continu à microcanaux combinés dynamique

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20140073498A1 (en) * 2012-09-06 2014-03-13 Eppendorf Ag Rotor Device, Centrifuge Bowl, and Centrifuge, and the Production Method Thereof
CN105854685A (zh) * 2016-06-15 2016-08-17 浙江大学 一种动态细胞打印微混合器
CN110548463A (zh) * 2019-08-27 2019-12-10 济南泺沣医药科技有限公司 一种连续流反应模块及装置
CN211436155U (zh) * 2019-11-22 2020-09-08 江苏方圆芳纶研究院有限公司 一种微反应器
CN112403414A (zh) * 2020-11-16 2021-02-26 徐州亚兴医疗科技有限公司 一种微通道连续催化装置及其工作方法
CN114632487A (zh) * 2022-03-29 2022-06-17 浙江工业大学 一种微通道超重力旋转床

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20140073498A1 (en) * 2012-09-06 2014-03-13 Eppendorf Ag Rotor Device, Centrifuge Bowl, and Centrifuge, and the Production Method Thereof
CN105854685A (zh) * 2016-06-15 2016-08-17 浙江大学 一种动态细胞打印微混合器
CN110548463A (zh) * 2019-08-27 2019-12-10 济南泺沣医药科技有限公司 一种连续流反应模块及装置
CN211436155U (zh) * 2019-11-22 2020-09-08 江苏方圆芳纶研究院有限公司 一种微反应器
CN112403414A (zh) * 2020-11-16 2021-02-26 徐州亚兴医疗科技有限公司 一种微通道连续催化装置及其工作方法
CN114632487A (zh) * 2022-03-29 2022-06-17 浙江工业大学 一种微通道超重力旋转床

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