Plate type microchannel reaction device and application thereof

Abstract

The invention relates to the technical field of micro-channel reaction devices, and discloses a plate type micro-channel reaction device and application thereof. The plate type microchannel reaction device comprises a first chip and second chips located on the two sides of the first chip, microscale grooves are formed in the first chip and the second chips, the microscale grooves are combined together to form one or more microchannels which are connected in series or in parallel, and each microchannel is of a three-dimensional streaming structure. The plate type microchannel reaction device can realize efficient mixing under the condition of low pressure drop, and can obtain higher target product selectivity and yield when being used for synthesizing caprolactone.

Description

Technical Field

[0001] The invention relates to the technical field of microchannel reaction devices, and in particular to a plate-type microchannel reaction device and applications thereof. Background Art

[0002] Micro-reaction technology refers to the process technology of continuous flow and reaction in a micro-device system with a microreactor as the core. The technology originated in the 1990s. Professor Wolfgang Ehrfeld, who worked at the Mainz Institute of Technology in Germany, was inspired by the "huge performance improvement and innovation brought by miniaturization in the field of microelectronics" and successfully applied the micro-mixer to the gas-phase synthesis of hydrocyanic acid for the first time, laying the foundation for the technology. Early microreactors used for reactions were usually made of glass, quartz glass, ceramics or stainless steel to achieve specific operating purposes such as rapid mixing, heat transfer or high-pressure operation, but they had high production costs and limited flexibility, and most of the application cases were relatively simple chemical processes. After more than 20 years of development, micro-reaction technology has gradually matured, from early laboratory devices and concepts to diversified commercial equipment and has been widely used.

[0003] There are many domestic enterprises that have carried out the research and development and production of ε-caprolactone, but most of them remain in the pilot stage and have not yet achieved industrialization. Baling Petrochemical built a 200-ton / year pilot plant in 2009. The product quality reached the standards of similar foreign products, and the purity of ε-caprolactone products was greater than 99.5%. Nanjing Red Sun New Materials Co., Ltd. built a 500-ton / year pilot production plant in Nanjing Chemical Industrial Park in 2014. It uses ionic liquid to catalyze the reaction of acetic acid and hydrogen peroxide to produce peracetic acid, which then reacts with cyclohexanone to produce ε-caprolactone. After distillation and purification, the ε-caprolactone product with a purity greater than 99.5% can be obtained. Zhongyuan Dahua also conducted a pilot test of synthesizing ε-caprolactone by the indirect method of hydrogen peroxide, but due to reaction control problems, the product polymerized during the distillation process, resulting in excessive viscosity of the material and blockage of the pump. Although it has been reported in China that many ε-caprolactone production units have opened up the process and produced qualified products, no domestic ε-caprolactone has been found for sale in the market. Domestic downstream users also have the intention to launch ε-caprolactone production lines, but due to the high safety risks, long reaction time, and cumbersome operation of traditional methods, they have not been implemented, which shows the difficulty of producing ε-caprolactone products. Chinese patent application CN103539770A discloses a microchannel reaction technology for preparing ε-caprolactone based on the oxidation of cyclohexanone with peracetic acid, and Chinese patent application CN106279093A discloses a microchannel reaction technology for preparing ε-caprolactone based on the oxidation of cyclohexanone with meta-chloroperbenzoic acid. The above two processes better achieve efficient mixing and reaction of heterogeneous systems, but there are no targeted measures for controlling the impurity content, which affects the selectivity of the final product and increases the subsequent separation cost, which is difficult to mass produce. Summary of the invention

[0004] The purpose of the present invention is to provide a plate-type microchannel reaction device and its application, in which a three-dimensional complex flow structure is configured, which can achieve efficient mixing of liquid materials and precise control of reactions under high throughput, shorten the residence time of easily decomposable materials in the reaction channel, and improve the utilization efficiency of raw materials.

[0005] In order to achieve the above-mentioned objectives, the present invention provides, on one hand, a plate-type microchannel reaction device, comprising a first chip and a second chip located on both sides of the first chip, wherein microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure.

[0006] Preferably, the microchannel comprises a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different.

[0007] Preferably, a transition module is provided between two adjacent mixing units, and each of the micro-sized flow paths in the mixing unit is communicated with the transition module.

[0008] Preferably, the mixing unit in the microchannel has at least two structures, and the structures of two adjacent mixing units on the same microchannel are different.

[0009] Preferably, the first structural form of the mixing unit in the microchannel is: it has 4 micro-sized flow paths, which are arranged in three layers from top to bottom, with 1 micro-sized flow path in the upper layer, 2 micro-sized flow paths in the middle layer, and 1 micro-sized flow path in the lower layer.

[0010] Preferably, in the mixing unit of the first structural form, each micro-sized flow path has 3 modules.

[0011] Preferably, on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right trapezoid respectively; on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right trapezoid, rectangle and isosceles trapezoid respectively.

[0012] Preferably, the second structural form of the mixing unit in the microchannel is: it has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths in the upper layer, 1 micro-sized flow path in the middle layer, and 2 micro-sized flow paths in the lower layer.

[0013] Preferably, in the mixing unit of the second structural form, each micro-sized flow path has 3 modules.

[0014] Preferably, on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are respectively a right-angled trapezoid, a rectangle and a right-angled trapezoid; on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are respectively an isosceles trapezoid, a rectangle and an isosceles trapezoid.

[0015] Preferably, the base angle of the isosceles trapezoidal module is 15-75°, the base length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the base angle of the right-angled trapezoidal module is 15-75°, the base length is 0.2-2.5mm, the top length is 0.1-1mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, and the depth is 0.5-3mm; and the angle between adjacent faces of adjacent modules is 5-20°.

[0016] Preferably, an inlet module is provided at the feed end of at least one of the microchannels, the inlet module having three inlets arranged from top to bottom, the upper inlet and the lower inlet serving as high-flux raw material inlets, and the middle inlet serving as low-flux raw material inlet.

[0017] Preferably, the dimensions of each inlet include: 0.5-5 mm in length, 0.1-2 mm in width, and 2-10 mm in depth.

[0018] Preferably, the inlet module is connected to the subsequent mixing unit via a transition module.

[0019] Preferably, the dimensions of the transition module include: length of 0.5-5 mm, width of 0.5-5 mm, and depth of 2-4 mm.

[0020] Preferably, two adjacent microchannels are connected via a connecting module.

[0021] Preferably, the dimensions of the connection module include: 0.5-5 mm in length, 1-10 mm in width, and 1-4 mm in depth.

[0022] Preferably, an outlet module is provided at the discharge end of at least one of the microchannels.

[0023] Preferably, the dimensions of the outlet module include: length of 0.5-8 mm, width of 0.5-5 mm, and depth of 4-10 mm.

[0024] Preferably, the number of the microchannels is 3-30.

[0025] Preferably, the length of a single microchannel is 6-60 cm, preferably 10-48 cm, more preferably 24-36 cm.

[0026] Preferably, the liquid holding capacity of the plate-type microchannel reaction device is 10-50 mL, preferably 16-30 mL.

[0027] Preferably, the material of the first chip and the second chip is respectively selected from at least one of borosilicate glass, stainless steel, silicon carbide and polytetrafluoroethylene, and the sealing material between the first chip and the second chip is selected from at least one of polytetrafluoroethylene, EPDM rubber, perfluororubber and graphite.

[0028] The second aspect of the present invention provides a method for liquid phase mixing reaction, which comprises: injecting a reaction substrate raw material and an oxidant into a reaction system respectively to carry out an oxidative rearrangement reaction, wherein the reaction system comprises at least one plate-type microchannel reaction device as described above.

[0029] Preferably, the reaction system comprises a plurality of the plate-type microchannel reaction devices connected in series or in parallel.

[0030] Preferably, the number of the plate-type microchannel reaction devices in the reaction system is 2-10, preferably 4-6.

[0031] Preferably, the reaction substrate raw material is cyclohexanone, and the oxidant is at least one of peroxypropionic acid, peroxyacetic acid and cumene hydroperoxide.

[0032] In the plate-type microchannel reaction device described in the present invention, microscale grooves are formed on multiple chips and the microscale grooves of these chips are combined to form a number of microchannels. By utilizing the three-dimensional flow structure in the microchannel, precise reactions between materials can be achieved, and multiple streams of liquid phase materials can be efficiently mixed at a lower channel pressure drop, thereby ensuring efficient mixing reaction efficiency and good economy in the entire process. BRIEF DESCRIPTION OF THE DRAWINGS

[0033] Figure 1 It is a schematic diagram of the three-dimensional structure of the microchannel in the plate-type microchannel reaction device of the present invention;

[0034] Figure 2 is a top view of a microchannel in the plate-type microchannel reaction device of the present invention;

[0035] Figure 3 is a side view of a microchannel in the plate-type microchannel reaction device of the present invention;

[0036] Figure 4 is a schematic structural diagram of the second chip in the plate-type microchannel reaction device of the present invention;

[0037] Figure 5 It is a schematic structural diagram of the first chip in the plate-type microchannel reaction device of the present invention;

[0038] Figure 6 This is a schematic diagram of the three-dimensional structure of the microchannel structure in the plate-type microchannel reaction device used in Comparative Example 1.

[0039] Description of Reference Numerals

[0040] a, entrance module; b, transition module; c-first mixing unit; d-second mixing unit; e, connection module. DETAILED DESCRIPTION

[0041] The specific implementation of the present invention is described in detail below in conjunction with the accompanying drawings. It should be understood that the specific implementation described here is only used to illustrate and explain the present invention, and is not used to limit the present invention.

[0042] The endpoints and any values ​​of the ranges disclosed in this article are not limited to the precise ranges or values, and these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of each range, the endpoint values ​​of each range and the individual point values, and the individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed in this article.

[0043] In the description of this application, the terms "first" and "second" are used for descriptive purposes only and should not be understood as indicating relative importance or implicitly indicating the number of technical features indicated. Therefore, unless otherwise specified, features defined as "first" and "second" may explicitly or implicitly include one or more of the features; "plurality" means two or more. The term "including" and any variation thereof means non-exclusive inclusion, and one or more other features, integers, steps, operations, units, components and / or combinations thereof may exist or be added.

[0044] In addition, terms indicating orientation or positional relationships such as "upper", "lower", "inside", and "outside" are described based on the orientation or relative positional relationships shown in the drawings, and are only for the convenience of describing the simplified description of the present application, and do not indicate that the device or element referred to must have a specific orientation, be constructed and operated in a specific orientation, and therefore should not be understood as a limitation on the present application.

[0045] In addition, unless otherwise clearly specified and limited, the terms "connected" and "connection" should be understood in a broad sense, for example, it can be a fixed connection, a detachable connection, or an integral connection; it can be a mechanical connection or an electrical connection; it can be a direct connection, or it can be indirectly connected through an intermediate medium, or it can be internally connected between two elements. For ordinary technicians in this field, the specific meanings of the above terms in this application can be understood according to specific circumstances.

[0046] like Figure 1-5 As shown, the plate-type microchannel reaction device described in the present invention includes a first chip and a second chip located on both sides of the first chip, and microscale grooves are formed on the first chip and the second chip. These microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure.

[0047] In the plate-type microchannel reaction device described in the present invention, a plurality of microchannels are formed by combining the microscale grooves in the first chip and the second chip, and the three-dimensional flow structure in the microchannel can realize efficient mixing of multiple liquid phase materials. In the present invention, the microscale grooves on the first chip and the second chip can be formed by high-precision machining or etching process.

[0048] In the plate-type microchannel reaction device of the present invention, in a preferred case, the microchannel includes a plurality of mixing units, each of which has a plurality of micro-sized flow paths, each of which has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different. In each of the micro-sized flow paths, through the combination of modules of different shapes and / or sizes, the liquid phase material in each micro-sized flow path entering the mixing unit changes its flow direction and flow velocity between each module, thereby achieving efficient mixing.

[0049] Further preferably, a transition module b is provided between two adjacent mixing units, and each of the micro-sized flow paths in the mixing unit is connected to the transition module b. Through this structural arrangement, the liquid phase materials in the micro-sized flow paths of the previous mixing unit are merged in the transition module b, and then divided into the micro-sized flow paths of the next mixing unit. Through multiple repeated processes of merging and dividing, efficient mixing of liquid phase materials can be achieved.

[0050] More preferably, the mixing unit in the microchannel has at least two structures, and the structures of two adjacent mixing units in the same microchannel are different. Through this structural arrangement, the liquid phase material is mixed in two adjacent mixing units in different mixing modes, thereby further promoting uniform mixing of the liquid phase material.

[0051] In some embodiments, the first structural form of the mixing unit in the microchannel (i.e., the first mixing unit c) is: having 4 micro-sized flow paths, which are arranged in three layers from top to bottom, with 1 micro-sized flow path in the upper layer, 2 micro-sized flow paths in the middle layer, and 1 micro-sized flow path in the lower layer. Further, in the mixing unit of the first structural form, each micro-sized flow path has 3 modules. Furthermore, on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right-angled trapezoid in sequence; on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and isosceles trapezoid in sequence. Specifically, the base angle of the isosceles trapezoidal module is 15-75°, the base length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the base angle of the right-angled trapezoidal module is 15-75°, the base length is 0.2-2.5mm, the top length is 0.1-1mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, and the depth is 0.5-3mm; and the angle between adjacent faces of adjacent modules is 5-20°.

[0052] In other embodiments, the second structural form of the mixing unit in the microchannel (i.e., the second mixing unit d) is: having 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths in the upper layer, 1 micro-sized flow path in the middle layer, and 2 micro-sized flow paths in the lower layer. Further, in the mixing unit of the second structural form, each micro-sized flow path has 3 modules. Furthermore, on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoids, rectangles, and right-angled trapezoids, respectively; on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoids, rectangles, and isosceles trapezoids, respectively. Specifically, the base angle of the isosceles trapezoidal module is 15-75°, the base length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the base angle of the right-angled trapezoidal module is 15-75°, the base length is 0.2-2.5mm, the top length is 0.1-1mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, and the depth is 0.5-3mm; and the angle between adjacent faces of adjacent modules is 5-20°.

[0053] According to a preferred embodiment of the present invention, the microchannel has a plurality of the first mixing units c and a plurality of the second mixing units d, and along the flow direction of the logistics, the next mixing unit of each of the first mixing units c is the second mixing unit d, and the next mixing unit of each of the second mixing units d is the first mixing unit c, and the adjacent first mixing units c and second mixing units d are connected through the transition module b.

[0054] In the plate-type microchannel reaction device of the present invention, in a preferred case, an inlet module a is provided at the feed end of at least one of the microchannels, and the inlet module a has three inlets arranged from top to bottom, the upper inlet and the lower inlet are used as high-flux raw material inlets, and the middle inlet is used as a low-flux raw material inlet. Further preferably, the dimensions of each inlet include: length 0.5-5mm, width 0.1-2mm, depth 2-10mm.

[0055] According to a preferred embodiment of the present invention, the inlet module a is connected to the subsequent mixing unit through the transition module b. With this structural arrangement, the multiple streams of liquid phase materials injected through the inlet module a are first preliminarily mixed in the transition module b, and then divided and injected into each micro-sized flow path of the subsequent mixing unit for further circumferential mixing.

[0056] In the plate-type microchannel reaction device of the present invention, the dimensions of the transition module b include: length of 0.5-5 mm, width of 0.5-5 mm, and depth of 1-4 mm.

[0057] In the plate-type microchannel reaction device of the present invention, in a preferred case, two adjacent microchannels are connected via a connecting module e. The dimensions of the connecting module e include: 0.5-8 mm in length, 1-10 mm in width, and 2-4 mm in depth.

[0058] In the plate-type microchannel reaction device of the present invention, an outlet module is provided at the discharge end of at least one of the microchannels, and the dimensions of the outlet module include: 0.5-5 mm in length, 0.5-5 mm in width, and 4-10 mm in depth.

[0059] In the plate-type microchannel reaction device of the present invention, the number of the microchannels may be 3-30, preferably 5-20. The length of a single microchannel may be 6-60 cm, preferably 10-48 cm, more preferably 24-36 cm. The liquid holding capacity of the plate-type microchannel reaction device may be 10-50 mL, preferably 16-30 mL.

[0060] In the plate-type microchannel reaction device of the present invention, the material of the first chip and the second chip can be selected from at least one of borosilicate glass, stainless steel, silicon carbide and polytetrafluoroethylene.

[0061] In the plate-type microchannel reaction device of the present invention, the sealing material between the first chip and the second chip can be selected from at least one of polytetrafluoroethylene, EPDM rubber, perfluororubber and graphite.

[0062] According to some embodiments of the present invention, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip, microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure. Specifically, the microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different; a transition module b is arranged between two adjacent mixing units, and each of the micro-sized flow paths in the mixing unit is connected to the transition module b; an inlet module a is arranged at the feed end of at least one of the microchannels, and the inlet module a is connected to the subsequent mixing unit through the transition module b; two adjacent microchannels are connected through a connecting module e, and an outlet module is arranged at the discharge end of at least one of the microchannels.

[0063] According to some other embodiments of the present invention, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip, microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure. Specifically, the microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different; a transition module b is arranged between two adjacent mixing units, and each of the micro-sized flow paths in the mixing unit is connected to the transition module b; the mixing unit in the microchannel has at least two structures, and the structures of two adjacent mixing units on the same microchannel are different; an inlet module a is arranged at the feed end of at least one of the microchannels, and the inlet module a is connected to the subsequent mixing unit through the transition module b; two adjacent microchannels are connected through a connecting module e, and an outlet module is arranged at the discharge end of at least one of the microchannels.

[0064] According to some other embodiments of the present invention, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip, microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure. Specifically, the microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different; the microchannel has a plurality of the first mixing units c and a plurality of the second mixing units d, and along the flow direction of the logistics, the next mixing unit of each of the first mixing units c is the second mixing unit d, and the next mixing unit of each of the second mixing units d is the first mixing unit c, and the mixing units are mutually The adjacent first mixing unit c and the second mixing unit d are connected through the transition module b, wherein the first mixing unit c has 4 micro-sized flow paths, which are arranged in three layers from top to bottom, with 1 micro-sized flow path in the upper layer, 2 micro-sized flow paths in the middle layer, and 1 micro-sized flow path in the lower layer, and each micro-sized flow path has 3 modules; the second mixing unit d has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths in the upper layer, 1 micro-sized flow path in the middle layer, and 2 micro-sized flow paths in the lower layer, and each micro-sized flow path has 3 modules; an inlet module a is provided at the feed end of at least one of the microchannels, and the inlet module a is connected to the subsequent mixing unit through the transition module b; two adjacent microchannels are connected through a connecting module e, and an outlet module is provided at the discharge end of at least one of the microchannels.

[0065] According to some other embodiments of the present invention, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip, and microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure. Specifically, the microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different; the microchannel has a plurality of the first mixing units c and A plurality of second mixing units d, along the flow direction of the logistics, the next mixing unit of each first mixing unit c is the second mixing unit d, and the next mixing unit of each second mixing unit d is the first mixing unit c, and the first mixing unit c and the second mixing unit d adjacent to each other are connected through the transition module b, wherein the first mixing unit c has 4 micro-sized flow paths, and these micro-sized flow paths are arranged in three layers from top to bottom, the upper layer is 1 micro-sized flow path, the middle layer is 2 micro-sized flow paths, and the lower layer is 1 micro-sized flow path, and each micro-sized flow path has 3 modules, and the upper layer has 4 micro-sized flow paths. On the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right-angled trapezoid respectively; on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and isosceles trapezoid respectively; the second mixing unit d has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths in the upper layer, 1 micro-sized flow path in the middle layer, and 2 micro-sized flow paths in the lower layer, and each micro-sized flow path has 3 modules, and on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and isosceles trapezoid respectively. The shapes are right-angled trapezoid, rectangle and right-angled trapezoid respectively; on the micro-sized flow path of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and isosceles trapezoid respectively; an inlet module a is arranged at the feed end of at least one of the microchannels, and the inlet module a has three inlets arranged from top to bottom, the upper inlet and the lower inlet are used as high-throughput raw material inlets, and the middle inlet is used as a low-throughput raw material inlet; the inlet module a is connected to the subsequent mixing unit through the transition module b; two adjacent microchannels are connected through a connecting module e, and an outlet module is arranged at the discharge end of at least one of the microchannels.

[0066] According to some other embodiments of the present invention, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip, microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure. Specifically, the microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different; the microchannel has a plurality of the first mixing units c and a plurality of the second mixing units d, and along the flow direction of the logistics, the next mixing unit of each of the first mixing units c is The second mixing unit d, and the next mixing unit of each of the second mixing units d is the first mixing unit c, and the adjacent first mixing units c and second mixing units d are connected through the transition module b, wherein the first mixing unit c has 4 micro-sized flow paths, and these micro-sized flow paths are arranged in three layers from top to bottom, the upper layer is 1 micro-sized flow path, the middle layer is 2 micro-sized flow paths, and the lower layer is 1 micro-sized flow path, and each micro-sized flow path has 3 modules, and on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right-angle trapezoid respectively, and on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled respectively. Trapezoid, rectangle and isosceles trapezoid, wherein the bottom angle of the isosceles trapezoid module is 15-75°, the bottom length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the bottom angle of the right-angle trapezoidal module is 15-75°, the bottom length is 0.2-2.5mm, the top length is 0.1-1mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, the depth is 0.5-3mm, and the angle between adjacent faces of each adjacent module is 5-20°; the second mixing unit d has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths on the upper layer. The micro-sized flow path has one micro-sized flow path in the middle layer and two micro-sized flow paths in the lower layer, and each micro-sized flow path has three modules. On the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid in turn. On the micro-sized flow path of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and isosceles trapezoid in turn. Among them, the bottom angle of the isosceles trapezoidal module is 15-75°, the bottom length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the bottom angle of the right-angled trapezoidal module is 15-75°, the bottom length is 0.2-2.5mm, the top length is 0.The length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, the depth is 0.5-3mm, and the angle between the adjacent faces of each adjacent module is 5-20°; an inlet module a is arranged at the feed end of at least one of the microchannels, and the inlet module a has three inlets arranged from top to bottom, the upper inlet and the lower inlet are used as high-throughput raw material inlets, and the middle inlet is used as a low-throughput raw material inlet, and the dimensions of each inlet include: a length of 0.5-5mm, a width of 0.1-2mm, and a depth of 2-10mm; the inlet module a is connected to the subsequent mixing unit through the transition module b. The transition module b has the following dimensions: length 0.5-5mm, width 0.5-5mm, depth 1-4mm; two adjacent microchannels are connected by a connection module e, and the connection module e has the following dimensions: length 0.5-8mm, width 1-10mm, depth 2-4mm; an outlet module is provided at the discharge end of at least one of the microchannels, and the dimensions of the outlet module include: length 0.5-5mm, width 0.5-5mm, depth 4-10mm; the number of the microchannels is 3-30, the length of a single microchannel is 6-60cm, and the liquid holding capacity of the plate-type microchannel reaction device is 10-50mL.

[0067] According to some other embodiments of the present invention, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip, microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form one or more microchannels connected in series or in parallel, and the microchannel has a three-dimensional flow structure. Specifically, the microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different; the microchannel has a plurality of the first mixing units c and a plurality of the second mixing units d, and along the flow direction of the logistics, the next mixing unit of each of the first mixing units c is The second mixing unit d, and the next mixing unit of each of the second mixing units d is the first mixing unit c, and the adjacent first mixing units c and second mixing units d are connected through the transition module b, wherein the first mixing unit c has 4 micro-sized flow paths, and these micro-sized flow paths are arranged in three layers from top to bottom, the upper layer is 1 micro-sized flow path, the middle layer is 2 micro-sized flow paths, and the lower layer is 1 micro-sized flow path, and each micro-sized flow path has 3 modules, and on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right-angle trapezoid respectively, and on the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled respectively. Trapezoid, rectangle and isosceles trapezoid, wherein the bottom angle of the isosceles trapezoid module is 15-75°, the bottom length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the bottom angle of the right-angle trapezoidal module is 15-75°, the bottom length is 0.2-2.5mm, the top length is 0.1-1mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, the depth is 0.5-3mm, and the angle between adjacent faces of each adjacent module is 5-20°; the second mixing unit d has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths on the upper layer. The micro-sized flow path has one micro-sized flow path in the middle layer and two micro-sized flow paths in the lower layer, and each micro-sized flow path has three modules. On the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid in turn. On the micro-sized flow path of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and isosceles trapezoid in turn. Among them, the bottom angle of the isosceles trapezoidal module is 15-75°, the bottom length is 0.5-5mm, the top length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the bottom angle of the right-angled trapezoidal module is 15-75°, the bottom length is 0.2-2.5mm, the top length is 0.1-1mm, 0.5-3mm high, 0.5-3mm deep; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, the depth is 0.5-3mm, and the angle between adjacent faces of each adjacent module is 5-20°; an inlet module a is provided at the feed end of at least one of the microchannels, the inlet module a has three inlets arranged from top to bottom, the upper inlet and the lower inlet are used as high-throughput raw material inlets, the middle inlet is used as a low-throughput raw material inlet, and the dimensions of each inlet include: length 0.5-5mm, width 0.1-2mm, depth 2-10mm; the inlet module a is connected to the subsequent mixing unit through the transition module b; the dimensions of the transition module b include: length 0.5-5mm, width 0.5-5mm, depth 1-4mm; adjacent The two microchannels are connected by a connecting module e, and the dimensions of the connecting module e include: length 0.5-8mm, width 1-10mm, depth 2-4mm; an outlet module is provided at the discharge end of at least one of the microchannels, and the dimensions of the outlet module include: length 0.5-5mm, width 0.5-5mm, depth 4-10mm; the number of the microchannels is 5-20, the length of a single microchannel is 10-48cm, and the liquid holding capacity of the plate-type microchannel reaction device is 16-30mL; the materials of the first chip and the second chip are each selected from at least one of borosilicate glass, stainless steel, silicon carbide and polytetrafluoroethylene, and the sealing material between the first chip and the second chip is selected from at least one of polytetrafluoroethylene, EPDM rubber, perfluororubber and graphite. .

[0068] The present invention also provides a method for liquid phase mixing reaction, which comprises: injecting a reaction substrate raw material and an oxidant into a reaction system respectively to carry out an oxidative rearrangement reaction, wherein the reaction system comprises at least one plate-type microchannel reaction device as described above.

[0069] In the method of the present invention, the reaction system comprises a plurality of the plate-type microchannel reaction devices connected in series or in parallel. Preferably, the number of the plate-type microchannel reaction devices in the reaction system is 2-10, preferably 4-6.

[0070] In a more preferred embodiment, the liquid phase mixing reaction method comprises the following steps:

[0071] (1) filling the entire plate-type microchannel reaction device with a solvent as an inert medium and raising the reaction environment in the plate-type microchannel reaction device to a specified reaction temperature and pressure, wherein the inert medium circulates between the units and controls the flow rate to a required flow rate for the reaction by a mass flow meter, wherein the solvent is selected from at least one of acetone, ethyl acetate, ethyl propionate and propionic acid;

[0072] (2) The reaction substrate raw material (liquid phase) and the oxidant raw material (liquid phase) enter the microchannel through the inlet module according to the stoichiometric ratio, mix and react, and the reacted materials are discharged through the outlet module;

[0073] The plate-type microchannel reaction devices are used in multiple stages in series or in parallel. Specifically, the number of the plate-type microchannel reaction devices is 2-10, preferably 4-6.

[0074] According to a preferred embodiment of the present invention, the liquid phase mixed reaction method is used to synthesize ε-caprolactone. Specifically, the reaction substrate raw material is cyclohexanone, and the oxidant is at least one of peroxypropionic acid, peroxyacetic acid and cumene hydroperoxide.

[0075] The plate-type microchannel reaction device and its application described in the present invention are further described below by way of examples. The examples are implemented based on the technical solution of the present invention, and detailed implementation methods and specific operation processes are given, but the protection scope of the present invention is not limited to the following examples.

[0076] The experimental methods in the following examples, unless otherwise specified, are all conventional methods in the art. The experimental materials used in the following examples, unless otherwise specified, are all commercially available.

[0077] In the following examples and comparative examples, the mixing index is calculated by the following formula,

[0078]

[0079] Where N represents the value of N different points of the detection outlet, C i Indicates the component concentration value at each point in the channel outlet cross section, in mol / m 3 , It represents the average value of the component concentration at the channel outlet, in mol / m 3 .

[0080] Example 1

[0081] (1) Construction of plate-type microchannel reaction device and reaction system

[0082] like Figure 1-5As shown, the plate-type microchannel reaction device includes a first chip and a second chip located on both sides of the first chip (that is, the first chip and the second chip are arranged alternately), microscale grooves are formed on the first chip and the second chip, and these microscale grooves are combined to form 20 microchannels connected in series, the length of a single microchannel is 10 cm, the total length is 200 cm, the liquid holding capacity is 16 mL, the material of the first chip and the second chip is borosilicate glass, and the sealing material between the first chip and the second chip is perfluororubber.The microchannel includes a plurality of first mixing units c and a plurality of second mixing units d, and the first mixing units c and the second mixing units d are arranged alternately with each other, and the adjacent first mixing units c and the second mixing units d are connected through a transition module b, wherein the first mixing unit c has 4 micro-sized flow paths, and these micro-sized flow paths are arranged in three layers from top to bottom, the upper layer is 1 micro-sized flow path, the middle layer is 2 micro-sized flow paths, and the lower layer is 1 micro-sized flow path, and each micro-sized flow path has 3 modules, and on the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right-angle trapezoid respectively, and on the micro-sized flow path of the middle layer, along the flow direction of the logistics, the three modules The main cross-sectional shapes are right-angled trapezoid, rectangle and isosceles trapezoid, wherein the base angle of the isosceles trapezoid module is 45°, the base length is 3mm, the top length is 1mm, the height is 1mm, and the depth is 1mm; the base angle of the right-angled trapezoid module is 45°, the base length is 1mm, the top length is 0.5mm, the height is 1mm, and the depth is 1mm; the length of the rectangular module is 1mm, the width is 0.5mm, the depth is 1mm, and the angle between adjacent faces of each adjacent module is 15°; the second mixing unit d has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths in the upper layer, 1 micro-sized flow path in the middle layer, and 2 micro-sized flow paths in the lower layer, and each micro-sized flow path has There are three modules. On the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid respectively. On the micro-sized flow paths of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and isosceles trapezoid respectively. Among them, the bottom angle of the isosceles trapezoid module is 45°, the bottom length is 3mm, the top length is 1mm, the height is 1mm, and the depth is 1mm; the bottom angle of the right-angled trapezoid module is 45°, the bottom length is 1mm, the top length is 0.5mm, the height is 1mm, and the depth is 1mm; the length of the rectangular module is 1mm, the width is 0.5mm, the depth is 1mm, and the angle between adjacent faces of each adjacent module is 15 °; An inlet module a is provided at the feed end of the outer microchannel, and the inlet module a has three inlets arranged from top to bottom, and the dimensions of each inlet include: 3 mm in length, 2 / 3 mm in width, and 5 mm in depth; the inlet module a is connected to the subsequent mixing unit through a transition module b; the dimensions of the transition module b include: 3 mm in length, 2 mm in width, and 1 mm in depth; two adjacent microchannels are connected through a connecting module e, and the dimensions of the connecting module e include: 6 mm in length, 2 mm in width, and 2 mm in depth; an outlet module is provided at the discharge end of another outer microchannel (on the side opposite to the inlet module), and the dimensions of the outlet module include: 3 mm in length, 2 mm in width, and 5 mm in depth.

[0083] The reaction system is formed by integrating six of the above-mentioned plate-type microchannel reaction devices in series, and external heating is provided by a circulating oil bath.

[0084] The mixing performance of the plate-type microchannel reaction device was tested with propionic acid and cyclohexanone as test liquids at a flow rate required for the reaction. As a result, the pressure drop was 0.81 kPa and the mixing index was 0.998. It can be seen that the plate-type microchannel reaction device of the present invention achieves efficient mixing under low pressure drop conditions.

[0085] (2) Caprolactone synthesis

[0086] The entire device is filled with propionic acid as an inert medium and the reaction environment in the device is raised to the specified reaction temperature and pressure. The inert medium circulates between the units and the flow rate is controlled by a mass flow meter to the required flow rate for the reaction. Cyclohexanone and 20% peroxy propionic acid solution enter the microchannel from the middle inlet and the upper and lower inlets at equal volume flow rates to mix the three liquid phase materials and react, and finally flow out from the outlet channel to enter the next stage reaction device; the mixing reaction process continues in the next stage reaction device, and the total input amount of fresh 20% peroxy propionic acid solution is consistent with the first stage, and enters the microchannel from the upper and lower inlets in equal proportions for mixing reaction, and finally flows out from the outlet channel to enter the next stage reaction device; after going through 4 stages of reaction devices according to the above model, the synthesis of caprolactone is completed, and crude caprolactone is obtained at the outlet channel of the reaction system. According to gas chromatography analysis, the caprolactone selectivity in the reaction process is 99.8%, and the time-space yield is 5.0kt / m 3 / a.

[0087] Comparative Example 1

[0088] (1) Construction of plate-type microchannel reaction device and reaction system

[0089] The plate-type microchannel reaction device includes two upper and lower chips, each of which is formed with microscale grooves, which are combined to form 20 microchannels connected in series, with a single microchannel having a length of 10 cm, a total length of 20 cm, a liquid holding capacity of 16 mL, a chip material of borosilicate glass, and a sealing material between chips of perfluororubber. The microchannel structure is as follows Figure 6As shown, it includes a plurality of first mixing units and a plurality of second mixing units, and the first mixing units and the second mixing units are arranged alternately with each other, and the first mixing units and the second mixing units adjacent to each other are connected through a transition module, wherein the first mixing unit has three micro-sized flow paths, and these micro-sized flow paths are arranged in two layers from top to bottom, the upper layer is one micro-sized flow path, and the lower layer is two micro-sized flow paths, and each micro-sized flow path has three modules, and on the micro-sized flow path of the upper layer, along the flow direction of the logistics The main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid, respectively. On the micro-sized flow path of the lower layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid, respectively. Among them, the right-angled trapezoidal module has a bottom angle of 45°, a bottom length of 1mm, a top length of 0.5mm, a height of 1mm and a depth of 1mm; the rectangular module has a length of 1mm, a width of 0.5mm and a depth of 1mm, and the angle between adjacent faces of adjacent modules is 15°; the second mixing unit has three micro-sized flow paths, which are arranged in two layers from left to right, with one micro-sized flow path on the left and two micro-sized flow paths on the right, and each micro-sized flow path has three modules. On the micro-sized flow path on the left, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and isosceles trapezoid, respectively. On the micro-sized flow path on the right, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid, respectively, wherein The isosceles trapezoidal module has a bottom angle of 45°, a bottom length of 3mm, a top length of 1mm, a height of 1mm, and a depth of 1mm; the right-angled trapezoidal module has a bottom angle of 45°, a bottom length of 1mm, a top length of 0.5mm, a height of 1mm, and a depth of 1mm; the rectangular module has a length of 1mm, a width of 0.5mm, a depth of 1mm, and an angle between adjacent faces of adjacent modules is 15°; the remaining structures and dimensions are the same as those of the plate-type microchannel reaction device of Example 1.

[0090] The reaction system is formed by integrating six of the above-mentioned plate-type microchannel reaction devices in series, and external heating is provided by a circulating oil bath.

[0091] The mixing performance of the plate-type microchannel reaction device was tested using propionic acid and cyclohexanone as test liquids at a flow rate required for the reaction. As a result, the pressure drop was 0.80 kPa and the mixing index was 0.829. It can be seen that the plate-type microchannel reaction device of the present invention achieves efficient mixing under low pressure drop conditions.

[0092] (2) Caprolactone synthesis

[0093] The above reaction system was used to synthesize caprolactone according to the process steps of Example 1. As a result, the caprolactone selectivity in the reaction process was 99.5%, and the space-time yield was 3.2 kt / m 3 / a.

[0094] It can be seen from the results of the above examples and comparative examples that the plate-type microchannel reaction device of the present invention can achieve efficient mixing under low pressure drop conditions, and can obtain higher target product selectivity and yield when used for synthesizing caprolactone.

[0095] The preferred embodiments of the present invention are described in detail above, but the present invention is not limited thereto. Within the technical concept of the present invention, the technical solution of the present invention can be subjected to a variety of simple modifications, including the combination of various technical features in any other suitable manner, and these simple modifications and combinations should also be regarded as the contents disclosed by the present invention and belong to the protection scope of the present invention.

Claims

1. A plate-type microchannel reaction device, characterized in that: The invention comprises a first chip and a second chip located on both sides of the first chip, wherein the first chip and the second chip are both formed with micro-scale grooves, and the micro-scale grooves are combined to form one or more micro-channels connected in series or in parallel, and the micro-channels have a three-dimensional flow structure.

2. The plate-type microchannel reaction device according to claim 1, characterized in that: The microchannel includes a plurality of mixing units, each mixing unit has a plurality of micro-sized flow paths, each of the micro-sized flow paths has a plurality of modules, and the shapes and / or sizes of two adjacent modules are different.

3. The plate-type microchannel reaction device according to claim 2, characterized in that: A transition module (b) is provided between two adjacent mixing units, and each of the micro-sized flow paths in the mixing unit is communicated with the transition module (b).

4. The plate-type microchannel reaction device according to claim 2 or 3, characterized in that: The mixing unit in the microchannel has at least two structures, and the structures of two adjacent mixing units on the same microchannel are different.

5. The plate-type microchannel reaction device according to claim 4, characterized in that: The first structural form of the mixing unit in the microchannel is: it has 4 micro-sized flow paths, which are arranged in three layers from top to bottom, with 1 micro-sized flow path in the upper layer, 2 micro-sized flow paths in the middle layer, and 1 micro-sized flow path in the lower layer.

6. The plate-type microchannel reaction device according to claim 5, characterized in that: In the mixing unit of the first structural form, each micro-sized flow path has three modules.

7. The plate-type microchannel reaction device according to claim 6, characterized in that: On the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and right-angle trapezoid respectively; In the micro-sized flow path of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and isosceles trapezoid respectively.

8. The plate-type microchannel reaction device according to claim 4, characterized in that: The second structural form of the mixing unit in the microchannel is: it has 5 micro-sized flow paths, which are arranged in three layers from top to bottom, with 2 micro-sized flow paths in the upper layer, 1 micro-sized flow path in the middle layer, and 2 micro-sized flow paths in the lower layer.

9. The plate-type microchannel reaction device according to claim 8, characterized in that: In the mixing unit of the second structural form, each micro-sized flow path has three modules.

10. The plate-type microchannel reaction device according to claim 9, characterized in that: On the micro-sized flow paths of the upper and lower layers, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are right-angled trapezoid, rectangle and right-angled trapezoid respectively; In the micro-sized flow path of the middle layer, along the flow direction of the logistics, the main cross-sectional shapes of the three modules are isosceles trapezoid, rectangle and isosceles trapezoid respectively.

11. The plate-type microchannel reaction device according to claim 7 or 10, characterized in that: The bottom side angle of the isosceles trapezoidal module is 15-75°, the bottom side length is 0.5-5mm, the top side length is 0.1-2mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the bottom side angle of the right-angled trapezoidal module is 15-75°, the bottom side length is 0.2-2.5mm, the top side length is 0.1-1mm, the height is 0.5-3mm, and the depth is 0.5-3mm; the length of the rectangular parallelepiped module is 0.1-2mm, the width is 0.1-2mm, and the depth is 0.5-3mm; and the angle between adjacent faces of adjacent modules is 5-20°.

12. The plate-type microchannel reaction device according to any one of claims 1 to 11, characterized in that: An inlet module (a) is provided at the feed end of at least one of the microchannels, wherein the inlet module (a) has three inlets arranged from top to bottom, the upper inlet and the lower inlet serve as high-flux raw material inlets, and the middle inlet serves as a low-flux raw material inlet; Preferably, the dimensions of each inlet include: 0.5-5 mm in length, 0.1-2 mm in width, and 2-10 mm in depth; Preferably, the inlet module (a) is connected to the subsequent mixing unit via a transition module (b).

13. The plate-type microchannel reaction device according to any one of claims 3 to 12, characterized in that: The dimensions of the transition module (b) include: length 0.5-5 mm, width 0.5-5 mm, and depth 1-4 mm.

14. The plate-type microchannel reaction device according to any one of claims 1 to 13, characterized in that: Two adjacent microchannels are connected via a connecting module (e); Preferably, the dimensions of the connection module (e) include: length 0.5-8 mm, width 1-10 mm, and depth 2-4 mm.

15. The plate-type microchannel reaction device according to any one of claims 1 to 14, characterized in that: An outlet module is provided at the discharge end of at least one of the microchannels; Preferably, the dimensions of the outlet module include: length 0.5-5 mm, width 0.5-5 mm, and depth 4-10 mm.

16. The plate-type microchannel reaction device according to any one of claims 1 to 15, characterized in that: The number of the microchannels is 3-30; Preferably, the length of a single microchannel is 6-60 cm, preferably 10-48 cm, more preferably 24-36 cm; Preferably, the liquid holding capacity of the plate-type microchannel reaction device is 10-50 mL, preferably 16-30 mL.

17. The plate-type microchannel reaction device according to any one of claims 1 to 16, characterized in that: The material of the first chip and the second chip is respectively selected from at least one of borosilicate glass, stainless steel, silicon carbide and polytetrafluoroethylene, and the sealing material between the first chip and the second chip is selected from at least one of polytetrafluoroethylene, EPDM rubber, perfluororubber and graphite.

18. A method for liquid phase mixing reaction, characterized in that: The method comprises: injecting a reaction substrate raw material and an oxidant into a reaction system respectively to carry out an oxidative rearrangement reaction, wherein the reaction system comprises at least one plate-type microchannel reaction device according to any one of claims 1 to 18.

19. The method according to claim 18, characterized in that The reaction system comprises a plurality of the plate-type microchannel reaction devices connected in series or in parallel; Preferably, the number of the plate-type microchannel reaction devices in the reaction system is 2-10, preferably 4-6.

20. The method according to claim 18 or 19, characterized in that The reaction substrate raw material is cyclohexanone, and the oxidant is at least one of peroxypropionic acid, peroxyacetic acid and cumene hydroperoxide.

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