Continuous flow preparation system of graphene composite membrane

By employing a continuous flow preparation system for substrate pretreatment, multi-component layered composite, in-situ synergistic crosslinking, and online detection and feedback control, the problems of low efficiency, poor uniformity, and consistency in the preparation of graphene composite films have been solved, achieving efficient and uniform production of graphene composite films.

CN121623587APending Publication Date: 2026-03-10NORTHWESTERN POLYTECHNICAL UNIV
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2026-01-20
Publication Date
2026-03-10

AI Technical Summary

Technical Problem

The existing methods for preparing graphene composite films suffer from problems such as low preparation efficiency, poor uniformity of film thickness, easy agglomeration of graphene, weak interfacial bonding, weak compatibility of multiple components, and poor product consistency.

Method used

A continuous flow preparation system is adopted, including a substrate pretreatment module, a multi-component layered composite module, an in-situ synergistic crosslinking module, an online detection and feedback control module, and a roll-to-roll unwinding module. Through the synergistic treatment of coaxial flow channel dispersion, ultrasonic oscillation, plasma and ultraviolet crosslinking, combined with real-time detection and parameter adjustment, the efficient and uniform preparation of graphene composite films is achieved.

Benefits of technology

It improves production efficiency, enhances the uniformity of membrane thickness and interfacial bonding strength, improves product consistency and adaptability to multifunctional composite membranes, and increases application flexibility.

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Abstract

The invention relates to the technical field of membrane preparation, and discloses a continuous flow preparation system of a graphene composite membrane, the system comprises a base material pretreatment module, a multi-component layered compounding module, an in-situ synergistic crosslinking module, an online detection and feedback regulation and control module and a reel-to-reel winding and unwinding module which are sequentially connected in series; the multi-component layered composite module realizes uniform mixing and layered coating of graphene and functional components through a coaxial runner dispersion unit, and an ultrasonic oscillation assembly inhibits graphene agglomeration; the in-situ synergistic cross-linking module adopts plasma-ultraviolet series treatment to strengthen film interface bonding; the online detection and feedback regulation and control module is linked with the central controller through spectrum detection and thickness detection to realize real-time optimization of preparation parameters; and the reel-to-reel winding and unwinding module ensures the transmission stability of the base material. According to the invention, full-process continuous production of the graphene composite membrane is realized, the preparation efficiency, the membrane layer uniformity and the mechanical stability are improved, and the method is compatible with multi-component functional compounding and is suitable for membrane preparation in the fields of water treatment, energy storage and the like.
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Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of film preparation, more particularly to a continuous flow preparation system of graphene composite film. BACKGROUND

[0002] Graphene composite film has a wide application prospect in water treatment, gas separation, energy storage and other fields due to its excellent mechanical strength, permeability and selectivity. However, the existing preparation of graphene composite film mostly adopts an intermittent process (such as vacuum filtration, solution casting), which has problems such as low preparation efficiency, poor uniformity of film layer thickness, easy aggregation of graphene, and insufficient interface bonding strength of functional components and graphene.

[0003] Although the existing continuous flow preparation technology has been tried, it still has obvious defects: firstly, the graphene is unevenly dispersed in the composite process, resulting in fluctuation of film layer performance; secondly, the cross-linking method is single (such as only ultraviolet cross-linking or thermal cross-linking), and the interface bonding strength is insufficient; thirdly, there is a lack of real-time detection and feedback mechanism, which cannot dynamically adjust the preparation parameters, and the product consistency is poor; fourthly, the multi-component compatibility is weak, and it is difficult to realize the continuous preparation of multifunctional composite film.

[0004] Based on this, the present application provides a continuous flow preparation system of graphene composite film to solve the above problems. SUMMARY

[0005] In order to overcome the above defects of the prior art, the present application provides a continuous flow preparation system of graphene composite film to solve the problems existing in the background art.

[0006] The present application provides the following technical scheme: a continuous flow preparation system of graphene composite film, comprising a substrate pretreatment module, a multi-component layered composite module, an in-situ synergistic cross-linking module, an online detection and feedback regulation module, and a roll-to-roll winding and unwinding module which are connected in series along the material transmission direction; The multi-component layered composite module comprises a coaxial flow channel dispersion unit and a dynamic coating unit, the coaxial flow channel dispersion unit is provided with an inner tube, an outer tube and an ultrasonic oscillation assembly surrounding the outer tube, the inner tube inlet is connected with a graphene dispersion liquid, the outer tube inlet is connected with a functional component solution, and the inner tube outlet and the outer tube outlet form a coaxial jet structure; the dynamic coating unit comprises a pair of elastic coating rollers with adjustable gap, and the surface of the coating roller is provided with micron-level flow guide grooves; The in-situ synergistic cross-linking module comprises a plasma treatment cavity and a ultraviolet light cross-linking cavity which are connected in series, the plasma treatment cavity is provided with an inert gas inlet and a plasma generator, and the ultraviolet light cross-linking cavity is internally provided with an array type ultraviolet lamp tube and a temperature regulation assembly; The online detection and feedback control module includes a spectral detection unit, a thickness detection unit, and a central controller. The spectral detection unit is used to monitor the distribution of film components in real time, the thickness detection unit is used to collect film thickness data, and the central controller is electrically connected to the substrate pretreatment module, the multi-component layered composite module, the in-situ synergistic crosslinking module, and the roll-to-roll unwinding module, and dynamically adjusts the working parameters of each module according to the detection data. The roll-to-roll unwinding module includes an unwinding roller, a winding roller, and a tension adjustment component. The substrate output by the unwinding roller is processed by each module in sequence and then recovered by the winding roller. The tension adjustment component maintains a constant tension during substrate transmission.

[0007] This solution enables complete and uninterrupted production of graphene composite films from substrate processing to finished product winding, eliminating the pauses, conversions, and material transfers between processes in traditional intermittent processes. This significantly improves overall production efficiency and reduces product inconsistencies caused by human intervention or environmental changes. As a further aspect of the present invention: the substrate pretreatment module includes a plasma cleaning chamber and a corona treatment unit. The plasma cleaning chamber is equipped with a gas distribution plate, and the electrode gap of the corona treatment unit is 0.5-2mm, and the processing power is 30-80W.

[0008] This solution effectively removes organic contaminants from the substrate surface through plasma cleaning and improves the surface energy and roughness of the substrate through corona treatment. This combined treatment provides a cleaner and more active bonding interface for subsequent film layers, which helps to enhance the adhesion between the composite film and the substrate and reduce the risk of film peeling during use.

[0009] As a further aspect of the present invention: the substrate pretreatment module includes a plasma cleaning chamber and a corona treatment unit. The plasma cleaning chamber is equipped with a gas distribution plate, and the electrode gap of the corona treatment unit is 0.5-2mm, and the processing power is 30-80W.

[0010] The ultrasonic oscillation at specific frequencies and powers effectively suppresses the aggregation tendency of graphene nanosheets in fluids. Combined with the shear force generated by the helical turbulence protrusions, it promotes uniform mixing and micro-region distribution of the graphene dispersion and functional component solution during the flow process, laying the foundation for the formation of a composite film with uniform component distribution.

[0011] As a further aspect of the present invention: the gap adjustment range of the coating roller of the dynamic coating unit is 10-200μm, the adjustment accuracy is ±1μm, the cross section of the guide groove on the surface of the coating roller is V-shaped, the groove width is 50-200μm, and the groove depth is 20-50μm.

[0012] This solution's high-precision gap adjustment capability allows for precise control of the wet film coating thickness according to process requirements. The V-shaped guide grooves on the coating roller surface facilitate uniform spread and flow control of the slurry between the rollers, thereby enabling the production of a wet film with good thickness uniformity and low edge effects on high-speed substrates, improving the final film thickness consistency. As a further aspect of the present invention: the plasma generator of the plasma processing cavity is a dielectric barrier discharge type with a discharge power of 50-150W, the inert gas is argon, nitrogen or helium, and the gas flow rate is 10-50 sccm; the ultraviolet lamp of the ultraviolet crosslinking cavity has a wavelength of 200-300nm, a power of 30-100W, and a temperature control range of 25-80℃ for the temperature control component.

[0013] This approach utilizes plasma treatment to activate surface molecules of the membrane under mild conditions, introducing active sites. Subsequent ultraviolet light crosslinking then efficiently initiates covalent bonding reactions. This tandem "activation-crosslinking" model, compared to a single crosslinking method, achieves stronger interfacial bonding between graphene sheets and functional components with a lower thermal budget, thus enhancing the mechanical integrity and stability of the membrane.

[0014] As a further aspect of the present invention: the spectral detection unit is a Raman spectrometer or an infrared spectrometer with a detection accuracy of ±0.1%; the thickness detection unit is a laser thickness gauge with a measurement range of 1-500μm and a measurement error of ±0.5μm.

[0015] This method uses Raman or infrared spectroscopy to reflect the chemical state and distribution of graphene in the film layer in a non-contact, real-time manner, while a laser thickness gauge can monitor the physical thickness of the film layer with high precision. The combination of these two detection methods provides multi-dimensional quantitative data for online quality monitoring, making real-time evaluation of key product performance indicators possible.

[0016] As a further aspect of the present invention: the multi-component stratified composite module is further provided with a dispersion circulation unit, including a storage tank, a booster pump and a filter, the filter having a filtration accuracy of 0.1-1μm, and the storage tank being provided with an ultrasonic dispersant and a temperature sensor.

[0017] This solution maintains a stable slurry supply through a circulation unit, and the built-in filter effectively removes trace large particles or secondary agglomerates that may be introduced or generated during the circulation process. This ensures that the slurry entering the coating unit always maintains good dispersion and consistency, thereby guaranteeing process stability and product quality for long-term continuous production. As a further aspect of the present invention: the central controller has a built-in PID adjustment algorithm, and the adjustable parameters include: substrate conveying speed 0.5-5m / min, ultrasonic oscillation power, coating roller gap, plasma power, ultraviolet light power, inert gas flow rate and substrate pretreatment power.

[0018] Based on real-time detection data, this solution uses a PID control algorithm to dynamically adjust key parameters such as transmission speed, coating gap, and energy input in a closed loop. This allows the system to automatically compensate for interference caused by raw material fluctuations or minor environmental changes, helping to stabilize the process state near the set target and thus improving the repeatability and consistency of product performance across different batches.

[0019] As a further aspect of the present invention: the tension adjustment component of the roll-to-roll winding and unwinding module includes a tension sensor and a magnetic powder brake, with a tension control range of 5-50N and a control accuracy of ±0.5N.

[0020] This solution's high-precision closed-loop tension control ensures that the substrate tension remains constant and controllable throughout the entire transport path. This avoids problems such as substrate stretching and deformation due to excessive tension or substrate loosening and wrinkling due to insufficient tension, and is key to ensuring coating uniformity, interlayer alignment, and stable operation in continuous production.

[0021] As a further aspect of the present invention: a cooling unit is provided between the in-situ co-crosslinking module and the online detection and feedback control module. The cooling unit adopts air cooling or water cooling and the cooling temperature is 15-30℃.

[0022] The cooling unit of this solution can reduce the temperature of the thermally cross-linked membrane to near room temperature. This helps protect subsequent precision optical inspection equipment (such as spectrometers) from the effects of heat radiation, ensuring the stability and accuracy of the detection signal; it also helps the membrane morphology stabilize before inspection, making the online measurement results more reflective of the final state of the product.

[0023] The technical effects and advantages of this invention are as follows: This system enables continuous operation from substrate pretreatment to finished product winding, reducing gaps between processes in intermittent processes and improving the continuity and efficiency of the production process. Through coaxial flow channel dispersion, synergistic ultrasonic oscillation, and the structural design of the dynamic coating roller, the dispersion of graphene in the composite system is improved, enhancing film thickness and the uniformity of component distribution. A synergistic treatment method combining plasma and ultraviolet crosslinking first activates surface groups in the film layer, then promotes the crosslinking reaction, enhancing the interfacial bonding between graphene, functional components, and the substrate. Relying on an online detection and feedback control mechanism, it adapts to parameter fluctuations during the preparation process in real time, reducing product performance differences and improving the consistency of different batches. The coaxial flow channel design allows for flexible adaptation to different types of functional component solutions, broadening the system's adaptability to the preparation of multifunctional graphene composite films and enhancing application flexibility. Attached Figure Description

[0024] The invention will now be further described with reference to the accompanying drawings.

[0025] Figure 1 This is a system block diagram of a continuous flow preparation system for a graphene composite film according to the present invention. Detailed Implementation

[0026] The technical solution of the present invention will be described in detail below with reference to the accompanying drawings and specific embodiments. These embodiments are only used to explain the present invention and are not intended to limit the scope of protection of the present invention.

[0027] Please see Figure 1 As shown, a continuous flow preparation system for graphene composite films includes a substrate pretreatment module, a multi-component layered composite module, an in-situ synergistic crosslinking module, an online detection and feedback control module, and a roll-to-roll unwinding module, which are connected in series along the material transport direction. The multi-component layered composite module includes a coaxial flow channel dispersion unit and a dynamic coating unit. The coaxial flow channel dispersion unit is equipped with an inner tube, an outer tube, and an ultrasonic oscillation component surrounding the outer tube. The graphene dispersion liquid is introduced into the inlet of the inner tube, and the functional component solution is introduced into the inlet of the outer tube. The outlets of the inner tube and the outer tube form a coaxial jet structure. The dynamic coating unit includes a pair of elastic coating rollers with adjustable gaps. The surface of the coating rollers is provided with micron-level guide grooves. The in-situ synergistic crosslinking module includes a plasma processing chamber and an ultraviolet crosslinking chamber connected in sequence. The plasma processing chamber is equipped with an inert gas inlet and a plasma generator. The ultraviolet crosslinking chamber is equipped with an array of ultraviolet lamps and a temperature control component. The online detection and feedback control module includes a spectral detection unit, a thickness detection unit, and a central controller. The spectral detection unit is used to monitor the distribution of film components in real time, the thickness detection unit is used to collect film thickness data, and the central controller is electrically connected to the substrate pretreatment module, the multi-component layered composite module, the in-situ synergistic crosslinking module, and the roll-to-roll unwinding module, and dynamically adjusts the working parameters of each module according to the detection data. The roll-to-roll unwinding module includes an unwinding roller, a winding roller, and a tension adjustment component. The substrate output from the unwinding roller is processed by each module in sequence and then recovered by the winding roller. The tension adjustment component maintains a constant tension during substrate transmission.

[0028] In one specific embodiment, the system is arranged linearly according to the material flow. The substrate (such as a polymer film or metal foil) first enters the substrate pretreatment module for surface activation and cleaning. Subsequently, the substrate enters the multi-component layered composite module, which first uniformly mixes and initially layers the graphene dispersion (such as an aqueous dispersion of graphene oxide) with the functional component solution (such as a solution containing crosslinking agents or nanoparticles) through its coaxial flow channel dispersion unit. Then, the mixture is uniformly coated onto the substrate surface through the dynamic coating unit. The coated wet film is then conveyed to the in-situ co-crosslinking module, where it passes through the plasma treatment chamber and the ultraviolet light crosslinking chamber in sequence to achieve interfacial activation and crosslinking curing of the film layer. Afterward, the film material enters the online detection and feedback control module, where the film quality is analyzed in real time through spectral and thickness detection, and the central controller dynamically adjusts the process parameters of the preceding modules based on the analysis results. Finally, the prepared composite film is collected by the winding roller of the roll-to-roll unwinding module. Throughout the process, the tension adjustment component ensures smooth substrate transmission and constant tension, realizing continuous and automated production from raw materials to finished products.

[0029] The substrate pretreatment module includes a plasma cleaning chamber and a corona treatment unit. The plasma cleaning chamber is equipped with a gas distribution plate. The electrode gap of the corona treatment unit is 0.5-2mm, and the processing power is 30-80W.

[0030] Specifically, the substrate pretreatment module can employ a plasma cleaning chamber and a corona treatment unit arranged in series. The substrate first enters a sealed plasma cleaning chamber, into which process gases such as argon or oxygen are introduced, with a gas distribution plate ensuring uniform gas distribution. After the plasma generator (e.g., an RF power supply) is activated, low-temperature plasma is generated within the chamber, effectively removing organic contaminants from the substrate surface and introducing active groups. Subsequently, the substrate passes through the corona treatment unit, which is equipped with high-voltage electrodes and a grounding roller. The electrode gap can be precisely adjusted to, for example, 1.0 mm, and the processing power is set to 50 W. Corona discharge further roughens the substrate surface and increases its surface energy, thereby significantly enhancing the adhesion between the subsequent composite film layer and the substrate.

[0031] The substrate pretreatment module includes a plasma cleaning chamber and a corona treatment unit. The plasma cleaning chamber is equipped with a gas distribution plate. The electrode gap of the corona treatment unit is 0.5-2mm, and the processing power is 30-80W.

[0032] In the coaxial flow channel dispersion unit of the multi-component stratified composite module, the ultrasonic oscillation component is tightly fitted to the outside of the outer tube. During implementation, the oscillation frequency can be set to 40 kHz and the power density to 1.0 W / cm². When the graphene dispersion is pumped simultaneously from the inner tube and the functional component solution from the outer tube, the ultrasonic cavitation effect effectively breaks up any graphene agglomerates that may form. Simultaneously, the spiral-shaped turbulence protrusions (e.g., with a protrusion height of 0.3 mm) on the inner wall of the outer tube apply rotational shear force to the passing solution, working synergistically with the ultrasonic oscillation to further enhance the turbulent mixing effect of the two liquids. This ensures that the graphene and functional components are uniformly dispersed at the microscale, forming a stable laminar or micro-stratified structure.

[0033] The gap between the coating rollers in the dynamic coating unit can be adjusted from 10 to 200 μm with an adjustment accuracy of ±1 μm. The cross-section of the guide groove on the surface of the coating roller is V-shaped, with a groove width of 50 to 200 μm and a groove depth of 20 to 50 μm.

[0034] The gap between a pair of flexible coating rollers (such as silicone rollers) in the dynamic coating unit is adjusted via a precision servo mechanism. Depending on the target film thickness, the gap can be set to, for example, 50 μm, with an adjustment accuracy of ±1 μm. The coating roller surfaces are machined with densely arranged V-shaped guide grooves, for example, 100 μm wide and 30 μm deep. When the premixed slurry passes through the gap between the coating rollers, the V-shaped grooves guide the slurry to spread evenly and restrict its lateral flow, while the flexible roller surface adapts to the slight undulations of the substrate. This design, combined with precise gap control, enables the formation of a highly uniform, defect-free wet film coating on substrates transported at high speeds (e.g., 2 m / min).

[0035] The plasma generator in the plasma processing chamber is a dielectric barrier discharge type with a discharge power of 50-150W. The inert gas is argon, nitrogen, or helium, and the gas flow rate is 10-50 sccm. The ultraviolet lamp in the ultraviolet cross-linking chamber has a wavelength of 200-300nm and a power of 30-100W. The temperature control component has a temperature control range of 25-80℃.

[0036] In the in-situ co-crosslinking module, the plasma processing chamber is equipped with a dielectric barrier discharge (DBD) plasma generator, with a discharge power set to 100W. Argon gas is introduced into the chamber as the working gas, with a flow rate controlled at 30 sccm. The DBD plasma is generated under normal pressure or low vacuum, which can efficiently activate the molecules on the wet film surface, forming free radicals or introducing oxygen / nitrogen-containing groups. Subsequently, the film material enters the ultraviolet crosslinking chamber, where several 254nm ultraviolet lamps are uniformly arranged, each with a power of 50W. Temperature control components (such as a built-in circulating water cooling plate or infrared heater) maintain the ambient temperature in the chamber at 60°C. Under these conditions, ultraviolet light excites the photoinitiator in the film layer, and synergistically interacts with the active sites generated by plasma pretreatment, promoting efficient covalent crosslinking reactions between graphene sheets and between graphene and functional components.

[0037] The spectral detection unit is a Raman spectrometer or an infrared spectrometer with a detection accuracy of ±0.1%. The thickness detection unit is a laser thickness gauge with a measurement range of 1-500μm and a measurement error of ±0.5μm.

[0038] In the online detection and feedback control module, the spectral detection unit can utilize an online Raman spectrometer. During implementation, the spectral probe is non-contactly aligned with the film surface during transmission, acquiring Raman spectra of specific regions in real time. By analyzing the intensity ratio of the characteristic G and D peaks of graphene, the dispersion state and defect degree of graphene can be semi-quantitatively monitored. The thickness detection unit employs a laser triangular reflection thickness gauge, whose laser beam scans the film surface at a fixed angle. The film thickness is calculated by receiving the reflected light signal, with a measurement range covering 1-500 μm and real-time data accuracy reaching ±0.5 μm. The detection data is synchronously transmitted to the central controller.

[0039] The multi-component stratified composite module also includes a dispersion circulation unit, comprising a storage tank, a booster pump, and a filter. The filter has a filtration accuracy of 0.1-1μm, and the storage tank is equipped with ultrasonic dispersers and a temperature sensor.

[0040] To ensure a continuous and stable supply of slurry, the multi-component stratified composite module is equipped with a dispersion circulation unit. Specifically, the circulation unit for storing and supplying the graphene dispersion includes a jacketed storage tank containing ultrasonic dispersers and an integrated temperature sensor to maintain the dispersion temperature at 25°C and prevent sedimentation. A booster pump is connected to the tank outlet to pump the dispersion out at a constant pressure. A precision filter (0.5 μm filtration accuracy) is installed on the pump outlet line to trap trace amounts of large particle agglomerates or impurities that may form during storage or circulation, ensuring that the slurry entering the coating unit is of uniform and stable quality.

[0041] The central controller has a built-in PID control algorithm, and the adjustable parameters include: substrate conveying speed (0.5-5 m / min), ultrasonic oscillation power, coating roller gap, plasma power, ultraviolet light power, inert gas flow rate, and substrate pretreatment power.

[0042] The central controller, as the core of the system, can utilize an industrial PLC or industrial computer in its hardware, with a built-in PID (Proportional-Integral-Derivative) control algorithm in its software. The implementation process is as follows: When the online detection unit reports that the film thickness is too thin, the controller calculates the adjustment amount based on the PID algorithm and issues commands: on the one hand, it moderately reduces the gap between the coating rollers of the dynamic coating unit (e.g., by 5 μm); on the other hand, it simultaneously fine-tunes (e.g., reduces) the substrate's transport speed (e.g., from 2.0 m / min to 1.8 m / min). Similarly, if spectral detection shows uneven component distribution, the controller can instruct to increase the power of the ultrasonic oscillation component or adjust the gas flow rate in the plasma processing chamber. This multi-parameter linkage, real-time feedback-based PID closed-loop control is the core of achieving consistent product performance.

[0043] The tension adjustment components of the roll-to-roll take-up and unwind module include a tension sensor and a magnetic powder brake. The tension control range is 5-50N, and the control accuracy is ±0.5N.

[0044] Tension control in the roll-to-roll unwinding module is achieved through a closed-loop system. A tension sensor (such as a floating roller or strain gauge sensor) is installed between the unwinding roller and the first processing module to detect the actual tension value of the substrate in real time. This measurement is transmitted to the central controller and compared with a preset tension value (e.g., 20N). If the detected tension is too high, the controller adjusts the excitation current of the magnetic powder brake (mounted on the unwinding roller shaft) to reduce its braking torque, thereby reducing the unwinding tension; conversely, the same applies. Through this real-time feedback and adjustment, substrate tension fluctuations throughout the entire production path can be controlled within ±0.5N, effectively avoiding problems such as film wrinkling, stretching, or uneven coating caused by unstable tension.

[0045] A cooling unit is provided between the in-situ co-crosslinking module and the online detection and feedback control module. The cooling unit adopts air cooling or water cooling and the cooling temperature is 15-30℃.

[0046] After high-temperature treatment in the UV crosslinking chamber, the membrane temperature may rise to 70-80℃. To protect the subsequent online detection unit (especially precision optical components) from thermal interference and to stabilize the membrane morphology for accurate measurement, a cooling unit is installed between the two modules. Specifically, forced air cooling can be used, with a set of vortex tubes or cooling coils installed in a closed air duct to control the cooling air temperature at around 20℃. The air is then blown across the upper and lower surfaces of the membrane at a uniform speed, ensuring its temperature stabilizes below 30℃ before entering the detection zone. This cooling process is physical and does not affect the chemical structure of the formed membrane layer.

[0047] The above are merely specific embodiments of this application, but the scope of protection of this application is not limited thereto. Any variations or substitutions that can be easily conceived by those skilled in the art within the scope of the technology disclosed in this application should be included within the scope of protection of this application. Therefore, the scope of protection of this application should be determined by the scope of the claims.

Claims

1. A continuous flow system for the preparation of graphene composite membranes, characterized in that, The substrate pretreatment module, the multi-component layered composite module, the in-situ synergistic crosslinking module, the online detection and feedback control module and the roll-to-roll winding and unwinding module are connected in series along the material conveying direction. The multi-component layered composite module comprises a coaxial flow channel dispersion unit and a dynamic coating unit. The in-situ synergistic crosslinking module comprises a plasma treatment cavity and a UV crosslinking cavity connected in series. The online detection and feedback control module comprises a spectral detection unit, a thickness detection unit and a central controller. The substrate pretreatment module comprises a plasma cleaning cavity and a corona treatment unit.

2. The continuous flow system for the preparation of graphene composite films according to claim 1, characterized in that, The ultrasonic oscillation assembly has an oscillation frequency of 20-60 kHz and a power density of 0.5-2 W / cm².

3. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The dynamic coating unit has a coating roller gap adjustment range of 10-200 μm and an adjustment accuracy of ±1 μm.

4. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The plasma treatment cavity has a dielectric barrier discharge type plasma generator with a discharge power of 50-150 W.

5. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The spectral detection unit is a Raman spectrometer or an infrared spectrometer with a detection accuracy of ±0.1%.

6. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The multi-component layered composite module further comprises a dispersion liquid circulation unit comprising a liquid storage tank, a booster pump and a filter.

7. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The filter has a filtering accuracy of 0.1-1 μm, and the liquid storage tank is provided with an ultrasonic dispersion subunit and a temperature sensor.

8. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The central controller is built-in PID regulation algorithm, and adjustable parameters include: substrate transmission speed 0.5-5 m / min, ultrasonic oscillation power, coating roller gap, plasma power, ultraviolet light power, inert gas flow rate and substrate pretreatment power.

9. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The tension adjusting component of the roll-to-roll winding and unwinding module comprises a tension sensor and a magnetic powder brake, the tension control range is 5-50 N, and the control precision is ±0.5 N.

10. The continuous flow system for the preparation of graphene composite films according to claim 1, wherein, The cooling unit is arranged between the in-situ synergistic crosslinking module and the online detection and feedback regulation module, the cooling unit adopts air cooling or water cooling mode, and the cooling temperature is 15-30 DEG C.