Electrodeposition device and system for preparing nano twin crystal copper-graphene composite material

Abstract

The invention discloses an electro-deposition preparation device and system for a graphene-twin crystal copper-based composite material. The preparation method of the graphene-twin-crystal copper composite material comprises the following steps: carrying out electro-deposition in a composite electroplating solution containing graphene and copper ions through a pulsed power supply by taking a copper-phosphorus plate as an anode, namely, directly obtaining the graphene-twin-crystal copper composite material on a cathode substrate. According to the preparation method, multiple parameters in the electrodeposition process are automatically adjusted through the upper computer, preparation of the graphene-twin crystal copper composite material with excellent dispersity and high homogenization degree is achieved, and further, multiple different parameter combinations can be set, so that the multi-layer multi-gradient composite material with different graphene volume fractions and different twin crystal lamellar thicknesses is achieved. The method has potential application value in the technical field of flexible electronics and the like.

Description

Technical Field

[0001] The invention relates to an electrodeposition device and system for preparing nano twinned copper-graphene composite materials, which utilizes constant current pulse electrodeposition to prepare graphene-nano twinned copper composite materials, and a control device and program for key parameters in the deposition process, belonging to the field of graphene composite material preparation. Background Art

[0002] Since its discovery, graphene has attracted much attention from researchers. Graphene has excellent thermal and electrical conductivity, and its theoretical specific surface area is as high as 2630 m 2 / g, and the charge mobility at room temperature is about 15000 cm 2 / (V·s), thermal conductivity as high as 5300W / mK and as low as 10 -6 Ω·cm resistivity. At the same time, graphene also has extremely high strength and Young's modulus, with a strength of up to 130GPa, making it the strongest material known so far.

[0003] Copper-based composite materials have shown a rapid growth trend in the past decade, due to their excellent thermal conductivity, good mechanical properties and higher electrical conductivity than other materials. The above advantages make them widely used in the field of electronic products. In 2006, studies have shown that pure copper foil with a twin structure made by electric pulse deposition can achieve a yield strength of up to 900MPa, a tensile strength of up to 1068MPa, and an electrical conductivity of 96.9±1.1% of the international standard annealed copper performance. The mechanical properties are improved by adding oxides and carbides as reinforcement materials in the copper matrix, but the electrical and thermal properties are difficult to meet the requirements of electronic component products. Therefore, new carbon derivatives such as carbon nanotubes, carbon nanofibers and graphene are regarded as ideal reinforcement materials for the matrix due to their excellent electrical, thermal and mechanical properties. They have received widespread attention from the academic community and have produced a large number of related commercial experiments.

[0004] There are two main methods for preparing copper-graphene composite materials, namely powder metallurgy and composite electrodeposition. In the powder metallurgy method, copper oxide particles and graphene oxide powder are mixed, reduced in a hydrogen atmosphere to obtain mixed particles of copper and graphene, and then the composite material is obtained by electric spark sintering. The defects of this method are that the high temperature and stirring process are easy to affect the interaction between graphene and the metal interface, and the incomplete reduction of some graphene oxide will also lead to material defects.

[0005] Electrodeposition method can obtain uniform and dense copper-graphene composite materials by depositing graphene and copper on cathode carrier. Compared with powder metallurgy method, it has the advantages of low energy consumption, low cost, rich adjustable process parameters, etc. However, the strength of copper-graphene composite materials obtained by traditional electrodeposition method is still not ideal, so it is necessary to develop a new electrodeposition method to obtain a copper matrix with higher strength. The invention of pulse electrodeposition method can make the substrate undergo electrodeposition process at a higher current density, which improves the structural strength of the deposited copper matrix to a certain extent. However, the experimental parameters of electrodeposition require that the pulse power supply has a short conduction time in one cycle, such as only set to conduct 0.02s, disconnect 2s, and constant current density. At present, the following problems are generally present in pulse electrodeposition devices.

[0006] Traditional pulse electroplating power supplies can only achieve a constant pulse voltage value, and the resistance of the plating solution will change during the electrodeposition process, so it is impossible to maintain a constant current density. The constant current module commonly used in pulsed DC power supplies cannot adjust the voltage to achieve constant current in such a short time of 0.02s, and the digital ammeter cannot obtain an accurate current value under short conduction time, making it impossible to achieve the constant current density required for the experiment. Therefore, an effective device and procedure are needed to achieve accurate current density control. Traditional pulse electroplating power supplies cannot meet the current preparation process requirements for various composite materials with organizational gradients, that is, multi-layer composite materials with different organizational structures, and various reinforcing layered materials with different contents.

[0007] Stirring rate and ultrasonic vibration are also very important links in the composite electrodeposition process, affecting the dispersion effect and embedding efficiency of graphene. Lack of stirring and ultrasonic vibration will lead to graphene agglomeration and low embedding efficiency. However, too high a stirring rate will form a high-speed liquid flow that destroys the uniform electrodeposition process. Too long ultrasonic vibration will lead to temperature rise and poor electrodeposition quality. How to accurately maintain the dispersion of graphene in the plating solution is a problem that needs to be solved urgently. Summary of the invention

[0008] In order to overcome the above-mentioned process problems, the present invention provides a method for obtaining a nano-twinned copper-based graphene composite material by electrodeposition, wherein the method makes the graphene uniformly dispersed in the gradient nano-scale columnar twinned copper matrix by regulating the frequency, current density, plating solution composition, stirring rate, etc. of the pulse power supply. A general-purpose PC is used as the control host computer, and the 485 interface under the MODBUS protocol is used for inter-device communication to realize the use of program control of the stirring rate and current density. The stirring rate and ultrasonic homogenization frequency are automatically controlled. The current density is automatically controlled using a self-made PID algorithm. The obtained nano-twinned copper-graphene composite material has the characteristics of high hardness, uniform and dense organization, etc. The method is simple and economical in process and suitable for large-scale industrial applications.

[0009] The technical solution provided by the present invention is specifically as follows:

[0010] The present invention provides a device for preparing rice-twinned copper-graphene composite materials by pulse electrodeposition, the device comprising a pulse constant voltage power supply, a host computer, a communication module, an electromagnetic stirrer, an oscilloscope, an electroplating tank, and a sampling resistor:

[0011] The pulse power supply, the electroplating tank and the sampling resistor are connected in series, and the oscilloscope is connected in parallel with the sampling resistor.

[0012] The host computer is connected to the pulse power supply, oscilloscope and electromagnetic stirrer respectively through the communication module.

[0013] The pulse constant voltage power supply is used to provide pulse current for electroplating, and it is provided with a voltage display module, and can output the current current value to the host computer through the communication module, and accept the host computer's instructions to adjust the voltage.

[0014] The host computer is used to monitor the current current density and adjust the voltage in real time. It has a program that can realize intermittent PID control.

[0015] The program execution steps are as follows: 1. The oscilloscope uses the trigger mode to read the oscilloscope pulse voltage value, and the current current is obtained according to the sampling resistor value. 2. Compare with the target current, use the automatic control algorithm to get the expected adjustment value of the voltage. 3. Issue a voltage adjustment command to the pulse power supply. 4. Read the oscilloscope pulse voltage value to achieve feedback closed-loop control.

[0016] The communication module is used to realize the communication between the host computer and the pulse power supply, oscilloscope, and electromagnetic stirrer, and realize data monitoring and adjustment.

[0017] The electromagnetic stirrer is used for stirring the electroplating solution, and has a built-in communicative power supply to realize the control of the stirring rate of the electromagnetic stirring process.

[0018] Among them, the electromagnetic stirrer has a built-in communicative power supply that can be switched on and off and output a constant current value under the control of the host computer. According to the current at the current stirring rate, the purpose of changing the stirring rate can be achieved by adjusting the current.

[0019] The oscilloscope is used to collect the current in the electroplating circuit. The implementation method is to use the oscilloscope to collect the sampling resistor voltage, obtain the current current value according to Ohm's law and feed it back to the host computer.

[0020] Optionally, the sampling resistor uses a variable resistor to match plating solutions with different resistance values, which is convenient for pulse voltage monitoring.

[0021] The graphene / gradient nano-twin copper composite material prepared by the present invention has a hardness of up to 3 GPa, and has good mechanical properties and a fine twin structure with a gradient.

[0022] The principle of the present invention is as follows:

[0023] The present invention utilizes the composite electrodeposition principle and adds graphene powder to the original pulse deposition copper plating solution. The anode copper phosphorus plate loses electrons under the action of the pulse power supply, and the copper atoms lose electrons to become copper ions and cuprous ions. The cuprous ions can be further oxidized to cupric ions during the stirring process. The thin graphene sheets can adsorb copper ions around them, and under the action of the electric field force, they are reduced and deposited together with the copper ions at the cathode. Thus, a graphene / gradient nano-twin copper composite material with a columnar twin structure and graphene attached to the grain boundary and the twin boundary is formed.

[0024] During the electroplating process, due to the agglomeration of graphene in the plating solution, the ion concentration in the local area decreases, which often leads to changes in the resistance of the plating solution during the electroplating process. When the current density is constant, the current situation of the plating solution can be indirectly reflected by the voltage. Therefore, it is necessary to monitor the voltage to adjust the frequency of stirring and ultrasound to achieve the homogenization of graphene and copper ions in the plating solution. The principle of achieving constant current density by connecting the plating solution in series with a standard resistor is Ohm's law. The pulse power supply is the total voltage, and the oscilloscope can obtain the divided voltage of the standard resistor. The current on the entire closed loop is obtained by dividing the divided voltage by the resistance of the standard resistor. The current value is divided by the area of ​​the electroplating sheet to obtain the current current density. Then, based on the total voltage, the divided voltage obtained by the oscilloscope, and the current value, the current resistance of the plating solution is obtained. Multiply the target current by the sum of the resistance of the plating solution and the standard resistor to obtain the recommended value of the pulse power supply at the set current density. PID is an automatic control algorithm. In this program, the operating variable adjusted by PID is the voltage of the pulse power supply. When the operating variable is 100%, it corresponds to the pulse power supply voltage +1V. Each time the pulse voltage amplitude sampled by the oscilloscope is measured, the pulse power supply voltage is automatically adjusted by calculation to achieve a stable current density within a few short cycles. Then the stirring motor is controlled by a communicative DC power supply to achieve program-controlled stirring rate. The pulse voltage is detected and adjusted to achieve a constant current of the pulse current. The formula is:

[0025] V=((V a -V b ) / V a *R+R ) *I set (1-1)

[0026] Where V is the pulse power supply voltage adjustment target value controlled by the host computer, V a is the current setting voltage value of the pulse voltage, V bis the voltage value measured by the oscilloscope, I set is the set target current value, and R is the resistance value of the standard resistor.

[0027] The formulas for the key PID parameters are shown in the attached Figure 6

[0028] Where u(t) is the output control signal of the PID module, and its value is equal to V in formula (1-1). p ) is set to 1; T i The integral time constant value of the PID module is set to 0; T d The differential time constant of PID is set to 0.001. e(t) is the output signal V of the pulse voltage control module and the feedback signal V of the pulse power supply output a The difference between .

[0029] The MODBUS protocol 485 communication module is used to read the oscilloscope measurement value, control the pulse power supply voltage and the current value of the DC power supply that supplies power to the stirring motor.

[0030] Compared with the prior art, the advantages of the present invention are:

[0031] 1. The present invention enables the equipment to automatically adjust parameters such as stirring rate and ultrasonic homogenization time according to changes in the plating solution during the electrodeposition process, thereby ensuring stable and uniform dispersion of graphene during the electrodeposition process and accurately constructing a twinned copper-based graphene composite material with a uniform organizational structure.

[0032] 2. The various process parameters of the present invention can be adjusted at any time during the electrodeposition process to prepare multilayer gradient tissue materials with different twin spacings. Further, multilayer composite materials with different twin spacings and different graphene volume fractions can be prepared.

[0033] 3. The present invention can realize accurate control of current density, and in the later stage, it can also realize a composite material with a gradient structure by changing the current density and stirring rate during the electrodeposition process. It overcomes the problem that the graphene content of the sample cannot be increased by increasing the graphene concentration of the plating solution in the traditional composite electrodeposition. It provides a technical basis for the manufacture of a variety of high-content graphene composite electrodeposition materials.

[0034] 4. The present invention realizes current regulation of the electrodeposition cell whose resistance value changes with time, voltage, and DC / pulse mode by implementing reading and control. Compared with the traditional constant voltage regulation, it can more accurately control the electrodeposition structure. It successfully introduces graphene into the electrodeposition twinned copper without destroying the process.

[0035] 5. The present invention provides a real-time record of changes in the resistance of the plating solution during the pulse electrodeposition process, providing a rich data basis for analyzing the changes in the components in the plating solution over time and the influence of the stirring rate on the resistance of the plating solution.

[0036] 6. The present invention adopts an innovative PID control algorithm based on host computer control, and uses a general-purpose computer to implement PID control based on a software program. It does not require additional PID control hardware, is more convenient and easy to maintain, and is flexible to adjust. The PID algorithm used in the field of continuous control is expanded to the intermittent control field of pulses. The operating variable is set to a pulse voltage of plus or minus 1V, which has good robustness. When the oscilloscope occasionally reads a value that is too high or too low, the erroneous adjustment value of the pulse voltage will not exceed 1V, so that after the oscilloscope reads the correct value in multiple cycles, it can return to the correct target current density, and avoid the situation where the target current oscillates greatly but cannot stabilize. BRIEF DESCRIPTION OF THE DRAWINGS

[0038] In order to more clearly illustrate the technical solutions in the embodiments of the present invention, the drawings required for use in the description of the embodiments will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative work.

[0039] Figure 1 A circuit diagram of an embodiment of a device for preparing composite materials by constant current pulse electrodeposition provided by the present invention.

[0040] Figure 2 A schematic diagram of the communication structure and data transmission sequence of an embodiment of a device for preparing a composite material by constant current pulse electrodeposition provided by the present invention.

[0041] Figure 3 A schematic block diagram of the program implementation of a constant current pulse electrodeposition device and system for preparing composite materials provided by the present invention.

[0042] Figure 4 A schematic diagram of the LabView program structure of a constant current pulse electrodeposition system for preparing composite materials provided by the present invention.

[0043] Figure 5 The invention is made at 400mA / cm 2 The organizational structure diagram of the graphene-nano-twinned copper composite material sample prepared by composite electrodeposition under current density and plating solution concentration of 0.1g / L graphene.

[0044] Figure 6 This is the key parameter formula diagram of PID control. DETAILED DESCRIPTION

[0046] The technical solutions in the embodiments of the present invention will be described clearly and completely below in conjunction with the drawings in the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, rather than all of the embodiments. Based on the embodiments in the present invention, all other embodiments obtained by those skilled in the art without creative work are within the scope of protection of the present invention. It should be understood that the schematic drawings are not drawn in real proportion. The flowcharts used in the present invention illustrate the operations implemented according to some embodiments of the present invention.

[0047] It should be understood that the operations of the flow chart may not be implemented in order, and steps without logical contextual relationships may be reversed in order or implemented simultaneously. In addition, those skilled in the art may add one or more other operations to the flow chart, or may remove one or more operations from the flow chart under the guidance of the content of the present invention.

[0048] Reference to "embodiments" herein means that a particular feature, structure, or characteristic described in conjunction with the embodiments may be included in at least one embodiment of the present invention. The appearance of the phrase in various places in the specification does not necessarily refer to the same embodiment, nor is it an independent or alternative embodiment that is mutually exclusive with other embodiments. It is explicitly and implicitly understood by those skilled in the art that the embodiments described herein may be combined with other embodiments.

[0049] The embodiments of the present invention provide a precision constant current pulse composite electrodeposition device and method, which are described below respectively.

[0050] Figure 1 This is a schematic diagram of the device circuit connection, in which the pulse electrodeposition cell is connected in series with the pulse power supply and the standard resistor, and the oscilloscope is connected in parallel with the standard resistor. The electromagnetic stirrer and the ultrasonic vibration platform are independently powered and are used to stir the electrodeposition cell, which are not specifically marked in the figure.

[0051] Figure 2 It is the communication structure connection diagram of the system. Figure 3is the execution order of the program. The principle of achieving constant current density by connecting the plating solution in series with the standard resistor is Ohm's law. The pulse power supply is the total voltage. The oscilloscope can obtain the divided voltage of the standard resistor. The current on the entire closed loop is obtained by dividing the divided voltage by the resistance of the standard resistor. The current value is divided by the area of ​​the electroplating sheet to obtain the current current density. Then, according to the total voltage, the divided voltage obtained by the oscilloscope, and the current value, the current resistance of the plating solution is obtained. Multiply the target current by the sum of the resistance of the plating solution and the standard resistor to obtain the recommended voltage value of the pulse power supply under the set current density. PID is an automatic control algorithm. In this program, the operating variable adjusted by PID is the voltage of the pulse power supply. When the operating variable is 100%, it corresponds to the pulse power supply voltage +1V. Each time the pulse voltage amplitude obtained by the oscilloscope is measured, the pulse power supply voltage is automatically adjusted by calculation to achieve a stable current density within a few short cycles. Then, the stirring motor is controlled by a communicative DC power supply to realize program-controlled stirring rate.

[0052] It should be noted that in addition to adjusting the pulse voltage to match the set current value, the program can also set multiple time periods, each with a different target current value, to achieve the electrodeposition process under variable current density and construct a gradient twin structure. It is also possible to set the timing of the electrodeposition stirring to switch between electrodeposited twinned copper and electrodeposited twinned copper composite materials.

[0053] Example 1

[0054] During the pulse electrodeposition of nanotwinned copper-graphene composites, the current density needs to be maintained at 400 mA / cm 2 The current density is first measured by measuring the area of ​​the deposition sheet to be 4cm 2 , immersed in the electroplating tank, and then connected to the entire pulse electrodeposition circuit. The program reads that the pulse voltage is 15V at this time and the voltage at the sampling resistor is 1V. According to the sampling resistor value of 0.5 ohms, the current in the entire circuit is 2A at this time. Therefore, the current density is higher than 400mA / cm 2 , the program now determines that the voltage needs to be lowered. The pulse power supply outputs a voltage reduction instruction, and the voltage drops to 14V. At this time, the current in the entire circuit is 1.8A. The voltage is then adjusted until the sampled voltage value reaches 0.8V, that is, the current reaches 1.6A. During this process, the program controls the constant stirring rate. After the electrodeposition reaches the target time, the program stops, the pulse power supply automatically turns off, and the stirring stops.

[0055] Example 2

[0056] In the process of pulse electrodeposition of multilayer composite materials of nano twinned copper-graphene layer and nano twinned copper layer, it is necessary to maintain a current density of 400mA / cm2. First, the area of ​​the deposited sheet is 4cm2 by measuring, immersed in the electroplating tank, and then the entire pulse electrodeposition circuit is connected. The program reads that the pulse voltage is 15V at the sampling resistor and the voltage is 1V. According to the sampling resistor resistance of 0.5 ohm, the current in the entire circuit is 2A at this time. Therefore, the current density is higher than 400mA / cm2 at this time. The program judges that the voltage needs to be reduced at this time. The pulse power supply outputs an instruction to reduce the voltage, and the voltage is reduced to 14V. At this time, the current in the entire circuit is 1.8A, and the voltage is adjusted again until the sampling voltage value reaches 0.8V, that is, the current reaches 1.6A. During this process, the program controls the constant stirring rate.

[0057] After 2 hours of electrodeposition, the program automatically changes the target value of the electrodeposition current density to 200 mA / cm2. At this time, the program still automatically adjusts the current density to the target value through the control cycle of this program, and the program controls to stop stirring. The above operation of the program realizes the switch from pulse electrodeposition of twinned copper composite materials to electrodeposition of twinned copper. Electrodeposition of composite materials with two layer structures of nano-twinned copper-graphene layer and pure nano-twinned copper is realized.

[0058] Example 3

[0059] In the process of pulse electrodeposition of nano-twinned copper-graphene layer and multi-layer composite material of nano-twinned copper layer, the current density is controlled to be constant as shown in Examples 1 and 2. Furthermore, in the composite electrodeposition process with a graphene concentration of 0.3 g / L in the plating solution, electromagnetic stirring and ultrasonic homogenization are controlled to take effect in different time periods. The device automatically measures and records the current resistance of the plating solution. When the resistance change is detected to be higher than 0.5%, the ultrasonic homogenization and electromagnetic stirring time distribution ratio are automatically adjusted to achieve a stable resistance of the plating solution and ensure good dispersion of graphene.

[0060] Figure 5 It is shown that in Example 1, the composite material sample with the graphene concentration controlled at 0.1 g / L has a dense columnar twin structure. The twin spacing reaches the nanometer level and is distributed in almost all columnar crystals, indicating that the twin density is extremely high. The graphene is distributed evenly at the twin boundaries of the material, indicating that the device ensures the dispersion of graphene and the close fit of graphene and the electrodeposited twin copper structure.

[0061] It should be noted that in the embodiment of the present invention, the monitoring interface deployed on the host computer can be designed by a variety of programming languages. The embodiment of the present invention is designed using the graphical editing language Labview, and the numerical control constant current source device can be monitored with the help of the virtual instrument control provided by Labview. The software includes user login, current regulation and monitoring, communication status display, overcurrent self-protection, and automatic storage of voltage data, which facilitates the intelligent control of the constant current source device, increases the safety of the constant current source device, and can also quickly locate the problem by analyzing the stored data for maintenance, thereby reducing maintenance costs.

[0062] The present invention is not limited to the above-mentioned embodiments. For ordinary technicians in this technical field, several improvements and modifications can be made without departing from the principle of the present invention, and these improvements and modifications are also considered to be within the scope of protection of the present invention. The contents not described in detail in this specification belong to the prior art known to professional and technical personnel in this field.

Claims

1. An electrodeposition device and system for preparing nano twin copper-graphene composite materials, characterized in that a program based on a general-purpose computer is developed to realize pulsed electrodeposition of PID constant pulse current value, so as to obtain a stable nano twin organizational structure. And the program controls the sample stirring rate and stirring time, controls the ultrasonic vibration time, and realizes the composite electrodeposition of twin copper-graphene. By setting the stirring rate to 0 and high stirring rate, switching between the electrodeposition of pure nano twin copper and nano twin copper-graphene composite materials is realized. By setting different current densities, stirring rates and ultrasonic vibration times in different time periods, a composite material with a gradient twin structure of 10-100nm twin spacing and graphene embedded in the common grain boundary of the twin boundary is realized, and a multilayer composite material can be realized, each layer having different twin spacing and graphene content.

2. An electrodeposition device and system for preparing nano-twinned copper-graphene composite materials, characterized in that: The pulse current density control program can make the electrodeposition device 0.001mA to 1000mA / cm 2 Electrodeposition is carried out at a current density of 10000 r / min, and its pulse frequency can be set from 0.001-10s on and 0.001-10s off. The control program can control the electromagnetic stirring device to carry out electrodeposition at a stirring rate of 0-2000 r / min, and control its switching time, so as to achieve control functions such as a cycle time of 10min on and 1min off and a variety of different on-off time combinations. The control program can control the switching time of the ultrasonic vibration platform, so as to achieve control functions such as a cycle time of 10min on and 1min off and a variety of different on-off time combinations. The upper limit of the time control of stirring and ultrasonic vibration depends on the program itself, and can reach up to 10h.

3. An electrodeposition device and system for preparing nano-twinned copper-graphene composite materials, characterized in that: It can automatically monitor and record the resistance change of the plating solution during the composite electrodeposition process, thereby reflecting the agglomeration of graphene therein. The stirring time and ultrasonic homogenization frequency are automatically adjusted according to the change in resistance value to ensure that the dispersion of graphene remains consistent and uniform during the long-term electrodeposition process.

4. An electrodeposition device and system for preparing nano-twinned copper-graphene composite materials, characterized in that: The device comprises a pulse current sampling module, a communication-controlled pulse power supply, a controllable electromagnetic stirring device, a controllable ultrasonic vibration platform, a data communication module, and a host computer including a current control program.

5. Among them, the pulse power supply should be able to transmit the real-time voltage value to the host computer and accept the host computer's instructions to adjust the voltage.

6. The pulse current sampling module is used to read the current value in the entire electrodeposition circuit, which includes an adjustable resistor and an oscilloscope connected in parallel. The adjustable resistor can match the electroplating solution with different resistance values ​​by changing the resistance value. A larger resistance value can more accurately estimate the current value.

7. The pulse power supply is connected in series with the electroplating tank and the sampling resistor, and the oscilloscope is connected in parallel with the sampling resistor to apply a pulse current to the electroplating tank to achieve electrodeposition and monitor the real-time current value.

8. The data communication module can adopt a variety of communication protocols, such as RS485, etc., to realize data acquisition and control between the host computer and the oscilloscope, pulse power supply, electromagnetic stirrer, and ultrasonic vibration platform.

9. The electrodeposition device and system for preparing nano-twinned copper-graphene composite materials according to claim 1, characterized in that: The host computer control program includes structures such as a target setting module, a program execution module, and a data recording module.

10. The target setting module includes setting the tuning parameters of the PID program, setting the current density target value, setting the electrodeposition cathode area, setting the electromagnetic stirring rate, and setting the working time. Multiple working time periods can be set, and each time period has a different stirring rate and current density.

11. The input parameter of the program execution module is the current voltage of the oscilloscope, the target parameter is the target voltage under the set current density, and the output parameter is the voltage value increase or decrease of the pulse power supply. The tuning method adopted can be PID self-tuning, etc.

12. The data recording module can record the real-time voltage value, and can obtain the current resistance of the plating solution according to the pulse voltage value and the real-time voltage value of the sampling resistor, and record the change of the resistance of the plating solution over time for subsequent research.

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