A high-sensitivity bicontinuous thin film electrode and a preparation method thereof

By fabricating a dual-continuous thin-film electrode that mixes polymers and liquid metals, the problems of signal loss and transmission loss at the electrode-skin interface of epidermal electrode materials have been solved, enabling highly sensitive electrophysiological signal monitoring, which is suitable for wearable electronic devices and biosensors.

CN119505309BActive Publication Date: 2026-05-08NANJING UNIV
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
NANJING UNIV
Filing Date
2024-11-17
Publication Date
2026-05-08

AI Technical Summary

Technical Problem

Existing epidermal electrode materials suffer from signal loss at the electrode-skin interface and losses during transmission, resulting in insufficient electrode sensitivity and difficulty in accurately capturing minute changes in electrophysiological signals.

Method used

A highly sensitive dual-continuous thin-film electrode was prepared by mixing a polymer solution with liquid metal. The liquid metal served as the fluid phase of the electrode, while the polymer network formed a three-dimensional porous structure, ensuring close adhesion to the skin and reducing interfacial impedance.

Benefits of technology

It achieves high signal-to-noise ratio electrophysiological signal monitoring, improves electrode conductivity and interface stability, and can accurately monitor weak electrophysiological signals in dynamic environments, making it suitable for wearable electronic devices and biosensors.

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Abstract

The application discloses a kind of high-sensitivity bicontinuous film electrode and preparation method thereof, belong to wearable sensing technical field.It includes the following steps: preparation of polymer solution: high molecular weight powder is added to good solvent respectively, after dissolving it is stirred evenly, obtain polymer solution;Preparation of liquid metal-polymer mixed solution: liquid metal is added to polymer solution, mixed solution is evenly dispersed with homogenizer, obtain liquid metal-polymer mixed solution;Preparation of bicontinuous film electrode: after evenly dispersed mixed solution is removed good solvent by heating or freeze drying etc., obtain bicontinuous film electrode.Compared with prior art, the beneficial aspects of the present application can realize the stability of the monitoring signal of the skin electrode in the skin of various deformation scenarios and dynamic monitoring environment, and can monitor the characteristic electro-physiological signal in the disease scenario with high signal-to-noise ratio.
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Description

Technical Field

[0001] This invention relates to the field of wearable sensing technology, and more specifically, to a high-sensitivity dual-continuous thin-film electrode and its preparation method. Background Technology

[0002] Electrophysiological signals, as a direct manifestation of electrical activity within a living organism, contain a wealth of physiological and pathological information, making them irreplaceable for clinical diagnosis and health management. These signals are typically monitored non-invasively using epidermal electrodes, and even minute electrophysiological fluctuations can reflect complex physiological changes within the body. Early detection of potential micro-lesions (such as arrhythmias and early signs of myocardial infarction) can significantly reduce the risk of serious complications. Therefore, accurate capture of electrophysiological signals, especially in the early identification of potential micro-lesions such as arrhythmias and myocardial infarction, is crucial for preventing serious complications and improving treatment outcomes. Developing highly sensitive epidermal electrodes that accurately monitor these minute changes is key to improving medical diagnosis and health management.

[0003] However, the development of current epidermal electrode technology faces significant challenges. The main problems are signal loss at the electrode-skin interface and attenuation during electron transport. For high-sensitivity monitoring, ideal electrode materials should possess both high conductivity and low interfacial impedance. However, existing electrode materials have limitations in both aspects. Metal electrodes, such as gold and platinum, are renowned for their excellent conductivity, but in practical applications, they struggle to form a stable, low-impedance interface with the skin. This is primarily due to the difference in mechanical properties between metals and skin tissue. This difference leads to interfacial instability and high interfacial impedance, thus affecting signal transmission efficiency and accuracy. On the other hand, conductive polymer electrodes (such as polypyrrole and polyaniline) and conductive composite electrodes can form a tighter interface with the skin, reducing signal attenuation at the interface. However, the conductivity of these materials is relatively limited, resulting in some loss during signal transmission, thus limiting the electrode's sensitivity. In related technologies, such as Chinese patent CN106798556A, a portable electrocardiogram (ECG) measurement system based on an electronic skin is provided. This system includes an analog section, a main control MCU, and electronic skin ECG electrodes. The analog section and the main control MCU are made of a flexible circuit board and connected to the electronic skin ECG electrodes. The main control MCU includes a data processing and analysis circuit and a Bluetooth BLE communication section. To study the correlation between ECG signals and changes in human movement, a triaxial sensor is also integrated on the flexible circuit board. The electronic skin ECG electrodes have a serpentine interconnected island bridge structure. This solution aims to improve the measurement accuracy of ECG signals in both active and static states to suppress interference signals caused by human movement. However, a shortcoming of this solution is that it does not provide any technical guidance on how to reduce the loss of electrophysiological signals during transmission and when crossing interfaces.

[0004] As can be seen from the above, although existing technologies have achieved monitoring of electrophysiological signals to a certain extent, the maximum sensitivity of currently reported epidermal electrodes is only 5 μV·N⁻¹, which is insufficient to accurately capture subtle changes in characteristic signals. Therefore, improving the conductivity and reducing the interfacial impedance of electrode materials to enhance their sensitivity is a pressing issue in this field. Summary of the Invention

[0005] 1. Technical problems to be solved

[0006] To address the issues of signal loss at the electrode-skin interface and signal loss during transmission in existing technologies, this invention provides a high-sensitivity dual-continuous thin-film electrode and its fabrication method. This electrode can stabilize the monitoring signal in various epidermal deformation scenarios and dynamic monitoring environments, enabling the detection of characteristic electrophysiological signals in disease scenarios with a high signal-to-noise ratio.

[0007] 2. Technical Solution

[0008] The objective of this invention is achieved through the following technical solutions.

[0009] The summary section of this application is intended to provide a brief overview of the concepts, which will be described in detail in the detailed description section below. This summary section is not intended to identify key or essential features of the claimed technical solutions, nor is it intended to limit the scope of the claimed technical solutions.

[0010] Some embodiments of this application propose a high-sensitivity dual-continuous thin-film electrode and its preparation method to solve the technical problems mentioned in the background section above.

[0011] As a first aspect of this application, some embodiments of this application provide a method for preparing a high-sensitivity dual-continuous thin-film electrode, the steps of which include: preparing a polymer solution: adding polymer powder to a good solvent, dissolving it and stirring it evenly to obtain a polymer solution; preparing a liquid metal-polymer mixed solution: adding liquid metal to the polymer solution, and uniformly dispersing the mixed solution using a homogenizer to obtain a liquid metal-polymer mixed solution; preparing a dual-continuous thin-film electrode: removing the good solvent from the uniformly dispersed mixed solution by means of heating or freeze-drying to obtain a dual-continuous thin-film electrode.

[0012] Furthermore, the prepared polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution.

[0013] Furthermore, the steps for preparing the polymer solution include preparing an ethylene / vinyl acetate solution and a polyethylene oxide solution.

[0014] Furthermore, the process for preparing the ethylene / vinyl acetate solution is as follows: 5.0 wt% to 10.0 wt% of ethylene / vinyl acetate particles are dissolved in anisole, and magnetic stirring is performed at a temperature of 90℃ to 98℃ until the ethylene / vinyl acetate particles dissolve to obtain the ethylene / vinyl acetate solution.

[0015] Furthermore, the process for preparing the polyethylene oxide solution is as follows: 0.2wt% to 4.0wt% of polyethylene oxide powder is dissolved in an ethylene / vinyl acetate solution, and magnetic stirring is performed at a temperature of 25℃ to 40℃ until the polyethylene oxide powder is dissolved to obtain an ethylene / vinyl acetate-polyethylene oxide solution.

[0016] Furthermore, the preparation of liquid metal-polymer mixed solutions includes the preparation of gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solutions, gallium-ethylene / vinyl acetate-polyethylene oxide mixed solutions, and gallium-indium-tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solutions.

[0017] Furthermore, the process for preparing the gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution is as follows: liquid gallium-indium alloy is mixed with ethylene / vinyl acetate-polyethylene oxide solution to obtain an initial mixed solution; the initial mixed solution is placed at a temperature of 25℃~40℃ and stirred and sheared at a speed of 8000rpm~15000rpm using a handheld homogenizer to obtain the gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0018] Furthermore, the process for preparing the gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution is as follows: liquid metallic gallium is mixed with an ethylene / vinyl acetate-polyethylene oxide solution to obtain an initial mixed solution; the initial mixed solution is placed at a temperature of 25℃~40℃, and a handheld homogenizer is used to stir and shear the initial mixed solution at a speed of 8000rpm~15000rpm to obtain the gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0019] Furthermore, the process for preparing the gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution is as follows: liquid gallium indium tin alloy is mixed with ethylene / vinyl acetate-polyethylene oxide solution to obtain an initial mixed solution; the initial mixed solution is placed at a temperature of 25℃~40℃ and stirred and sheared at a speed of 8000rpm~15000rpm using a handheld homogenizer to obtain the gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0020] As a second aspect of this application, some embodiments of this application provide a high-sensitivity dual-continuous thin-film electrode prepared by a high-sensitivity dual-continuous thin-film electrode preparation method, comprising liquid metal and a polymer network. The liquid metal serves as the fluid phase of the electrode and forms an interconnected continuum in the dual-continuous thin film. The polymer network exhibits a dispersed three-dimensional porous network structure, connecting the liquid metal oxide layer and adhering to the skin surface.

[0021] 3. Beneficial effects

[0022] Compared with existing technologies, the advantages of this invention are: it develops a novel epidermal electrode that reduces the loss of electrophysiological signals when crossing interfaces and during transmission; it constructs a dual-continuous structure for the epidermal electrode, which can simultaneously achieve high electronic conductivity and good adhesion to the skin; the constructed epidermal electrode can achieve high signal-to-noise ratio monitoring of characteristic signals in electrophysiological tests; and the electrophysiological signals acquired by the epidermal electrode can be further combined with deep learning to achieve material recognition based on electrophysiological signals. Attached Figure Description

[0023] Figure 1 This is a schematic diagram of a dual continuous thin-film electrode structure in one embodiment of the present invention;

[0024] Figure 2 This is an SEM image of the polymer network in a dual continuous thin-film electrode according to an embodiment of the present invention.

[0025] Figure 3 This is a force diagram of the interaction between liquid metal and polymer in a dual continuous thin-film electrode according to an embodiment of the present invention;

[0026] Figure 4 This is a graph showing the effect of liquid metal content on the conductivity of a dual continuous thin-film electrode in one embodiment of the present invention;

[0027] Figure 5 This is an adhesion force diagram of a dual continuous thin-film electrode with different polyethylene oxide contents and skin in one embodiment of the present invention;

[0028] Figure 6 This is a graph showing the resistance variation of a dual continuous thin-film electrode under various deformation conditions in one embodiment of the present invention.

[0029] Figure 7 This is an electrocardiogram of a dual continuous thin-film electrode in a mouse model of myocardial infarction, according to one embodiment of the present invention.

[0030] Figure 8 This is an electromyography (EMG) monitoring diagram of a dual continuous thin-film electrode in one embodiment of the present invention when a finger touches different materials;

[0031] Figure 9This is a diagram of a deep learning model for material recognition based on electromyography signals in one embodiment of the present invention;

[0032] Figure 10 This is a schematic diagram of the fabrication process of a high-sensitivity dual-continuous thin-film electrode in one embodiment of the present invention. Detailed Implementation

[0033] The present invention will now be described in detail with reference to the accompanying drawings and specific embodiments.

[0034] Example 1

[0035] like Figure 1 As shown, this embodiment provides a high-sensitivity dual-continuous thin-film electrode, comprising a liquid metal and a polymer network.

[0036] Liquid metal serves as the fluid phase of the electrode, forming an interconnected continuum in a bicontinuous thin film; a polymer network connects the liquid metal oxide layer and adheres to the skin surface.

[0037] Specifically, liquid metal, as the fluid phase in the bicontinuous thin film, occupies 85.1% to 92.4% of the total volume of the bicontinuous thin film, forming a continuous body that is interconnected within the bicontinuous thin film. This structure ensures that the liquid metal can flow freely inside the film without affecting its conductivity, providing a broad and efficient channel for the transmission of electronic signals.

[0038] like Figure 2 and Figure 3 As shown, Figure 2 The microstructure of the polymer network in the dual-continuous thin-film electrode is shown. Figure 3 This demonstrates the interaction forces between liquid metal and polymer in a thin film.

[0039] Specifically, the polymer network exhibits a dispersed three-dimensional porous network structure, which can uniformly and stably fix the liquid metal fluid and serve as a stable support for the liquid metal. Hydrogen bonds exist between the polymer network and the liquid metal, enabling effective fixation of the liquid metal and ensuring that leakage does not occur.

[0040] Meanwhile, the tunable mechanical properties of the polymer network allow for customized design based on specific application needs, ensuring the stability and durability of the bicontinuous film. The polymer network also interacts with proteins on the skin surface through hydrogen bonding; this unique adhesion mechanism enables the electrodes to adhere tightly to the skin, maintaining good contact even during prolonged wear or exercise. This further enhances the accuracy and reliability of electrophysiological signal monitoring.

[0041] like Figure 4As shown, the effect of liquid metal content on the conductivity of a dual continuous thin-film electrode is illustrated.

[0042] Specifically, within the bicontinuous thin film, the liquid metal continuum serves as the fluid phase, providing an excellent electronic pathway for the bicontinuous thin film electrode, achieving a conductivity as high as 1.2 × 10⁻⁶. 6 The S / m ratio makes it perform well in electrophysiological signal monitoring, especially significantly improving its ability to capture weak signals.

[0043] like Figure 5 The figure shows the adhesion curves between the bicontinuous film and skin with different polyethylene oxide contents. By adjusting the polyethylene oxide content in the bicontinuous film, different adhesion strengths were observed, with the highest reaching 45 N / m. This indicates that the film electrode can form a good adhesion interface with the skin, which helps to reduce the impedance of electrophysiological signals across the tissue-electrode interface, thereby improving the quality and signal-to-noise ratio of the monitored electrophysiological signals.

[0044] like Figure 6 As shown, it further demonstrates the resistance variation of the dual continuous thin film electrode under various deformation conditions.

[0045] Specifically, under simulated skin deformation conditions such as bending, torsion, friction, and compression, the resistance of the dual continuous thin-film electrode hardly changed. This indicates that the thin-film electrode can maintain stable electrical performance even during dynamic monitoring and output consistent electrophysiological signals.

[0046] like Figure 7 The image shows an electrocardiogram (ECG) monitoring result of a dual-continuous thin-film electrode in a mouse model of myocardial infarction. The dual-continuous thin-film electrode can accurately monitor ECG changes in mice at different stages of myocardial damage, such as ST segment elevation, T wave prominence, and P wave prominence. This indicates that the dual-continuous thin-film electrode has broad application potential in high-quality ECG monitoring.

[0047] like Figure 8 The image shows electromyography (EMG) monitoring data obtained by a dual-continuous thin-film electrode when a finger touches different materials. The dual-continuous thin-film electrode can monitor the electrophysiological signals of the finger when touching different materials, and each group of electrophysiological signals exhibits similar group characteristics. This indicates that even weak EMG changes caused by touching different materials can be monitored by the dual-continuous thin-film electrode, which greatly improves the monitoring capability of existing epidermal electrodes for weak electrophysiological signals.

[0048] like Figure 9 As shown, it demonstrates a deep learning model for material recognition built based on electromyographic signals from touching different materials.

[0049] Specifically, by using different electromyographic signals collected by dual continuous thin-film electrodes and combining them with data feature processing, a deep learning model can be constructed to efficiently distinguish between different materials.

[0050] The dual-continuous thin-film electrode in this embodiment not only enables highly sensitive monitoring of characteristic electrophysiological signals but also effectively enhances the ability to capture weak electrophysiological signals. It has broad application prospects in wearable electronic devices, and can be used for highly sensitive monitoring of characteristic electrophysiological signals and improving the monitoring capability of weak electrophysiological signals.

[0051] Example 2

[0052] like Figures 1 to 10 As shown, this embodiment discloses a method for fabricating a high-sensitivity dual-continuous thin-film electrode, including the following steps:

[0053] Preparation of polymer solutions:

[0054] The preparation of a polymer solution involves gradually adding the polymer to a good solvent, allowing the polymer to dissolve, and then stirring until a homogeneous solution is obtained.

[0055] Specifically, the prepared polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution. The steps for preparing the polymer solution include preparing an ethylene / vinyl acetate (EVA) solution and preparing a polyethylene oxide (PEO) solution.

[0056] In one specific embodiment, the process for preparing the polymer solution is as follows:

[0057] Preparation of ethylene / vinyl acetate (EVA) solution: Dissolve 10.0 wt% of ethylene / vinyl acetate particles in anisole liquid; perform continuous magnetic stirring at 90°C for 3 hours until the ethylene / vinyl acetate particles dissolve, thereby obtaining an ethylene / vinyl acetate solution;

[0058] Preparation of polyethylene oxide (PEO) solution: Dissolve 2.0 wt% polyethylene oxide powder in the prepared ethylene / vinyl acetate (EVA) solution; perform continuous magnetic stirring at 40°C for 2 hours until the polyethylene oxide powder dissolves, thereby obtaining an ethylene / vinyl acetate-polyethylene oxide solution.

[0059] Preparation of liquid metal-polymer mixed solution:

[0060] The preparation of a liquid metal-polymer mixed solution involves adding liquid metal to a polymer solution to obtain an initial mixed solution; then using a homogenizer to uniformly disperse the initial mixed solution to obtain the liquid metal-polymer mixed solution.

[0061] Specifically, the preparation of liquid metal-polymer mixed solutions is based on three different liquid metals, and three liquid metal-polymer mixed solutions are prepared separately.

[0062] In a specific embodiment, the process for preparing the liquid metal-polymer mixed solution is as follows:

[0063] Liquid gallium indium alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 8:2 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 10,000 rpm for 5 minutes using a handheld homogenizer to obtain a gallium indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0064] Liquid gallium metal was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 8:2 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 10,000 rpm for 5 minutes using a handheld homogenizer to obtain a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0065] Liquid gallium indium tin alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 8:2 to obtain an initial mixed solution. The mixed solution was placed at 25°C and stirred and sheared at 10,000 rpm for 5 minutes using a handheld homogenizer to obtain a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0066] Specifically, in the above mixing process, the liquid metal is dispersed in the solution as small droplets after being subjected to high-speed stirring and shearing by the homogenizer, while the polymer network is dispersed on the metal surface and in the good solvent.

[0067] Processing liquid metal-polymer mixed solutions:

[0068] The uniformly dispersed mixed solution is subjected to heat or freeze-drying to remove the good solvent, thereby obtaining a dual continuous thin film electrode.

[0069] Specifically, the three liquid metal-polymer mixed solutions prepared during the preparation of the liquid metal-polymer mixed solution were added to a polytetrafluoroethylene petri dish and placed in a vacuum environment at 80°C to remove the good solvent, thus obtaining the three prepared dual continuous thin film electrodes.

[0070] The three types of bicontinuous thin-film electrodes prepared through the above steps all achieve high electronic conductivity, ensuring excellent conductivity during electron transport. They also exhibit good adhesion to the skin, meaning they can adhere tightly to the skin surface and are not easily detached, providing an important material basis for applications such as wearable electronic devices, biosensors, and medical monitoring devices. Furthermore, the excellent adhesion properties of these bicontinuous thin-film electrodes help enhance the interfacial stability between the electrode and the skin, reducing signal interference and thus improving the accuracy and reliability of the device under long-term use.

[0071] In one specific embodiment, the process of processing the liquid metal-polymer mixed solution is as follows:

[0072] The prepared gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0073] The prepared gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous film.

[0074] The prepared gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0075] Specifically, in this step, liquid metal droplets are initially dispersed in droplet form, where entangled polymer chains form physically cross-linked networks that simultaneously trap a large amount of good solvent. As drying proceeds, the good solvent in these networks is gradually replaced by liquid metal, and the micropores between the liquid metal droplets that were originally filled with solvent are transformed into nanopores filled with liquid metal. Ultimately, the liquid metal fluid becomes the dominant component, forming a continuous structure in which the polymer network is embedded.

[0076] Example 3

[0077] This embodiment discloses a method for preparing a high-sensitivity dual-continuous thin-film electrode, including the following steps:

[0078] Preparation of polymer solutions:

[0079] The preparation of a polymer solution involves gradually adding the polymer to a good solvent, dissolving it, and then stirring until a homogeneous solution is obtained.

[0080] Specifically, the prepared polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution. The steps for preparing the polymer solution include preparing an ethylene / vinyl acetate (EVA) solution and preparing a polyethylene oxide (PEO) solution.

[0081] In one specific embodiment, the process for preparing the polymer solution is as follows:

[0082] Preparation of ethylene / vinyl acetate (EVA) solution: Dissolve 5.0 wt% of ethylene / vinyl acetate particles in anisole liquid; perform continuous magnetic stirring at 90°C for 3 hours until the ethylene / vinyl acetate particles dissolve to obtain an ethylene / vinyl acetate solution;

[0083] Preparation of polyethylene oxide (PEO) solution: Dissolve 0.2 wt% of polyethylene oxide powder in the prepared ethylene / vinyl acetate (EVA) solution, and perform continuous magnetic stirring at 40°C for 2 hours until the polyethylene oxide powder dissolves to obtain an ethylene / vinyl acetate-polyethylene oxide solution.

[0084] Preparation of liquid metal-polymer mixed solution:

[0085] The preparation of a liquid metal-polymer mixed solution involves adding liquid metal to a polymer solution to obtain an initial mixed solution; then using a homogenizer to uniformly disperse the initial mixed solution to obtain the liquid metal-polymer mixed solution.

[0086] Specifically, the preparation of liquid metal-polymer mixed solutions is based on three different liquid metals, and three liquid metal-polymer mixed solutions are prepared separately.

[0087] In a specific embodiment, the process for preparing the liquid metal-polymer mixed solution is as follows:

[0088] Liquid gallium indium alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 1:1 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 8000 rpm for 3 minutes using a handheld homogenizer to obtain a gallium indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0089] Liquid gallium metal was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 1:1 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 8000 rpm for 3 minutes using a handheld homogenizer to obtain a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0090] Liquid gallium indium tin alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 1:1 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 8000 rpm for 3 minutes using a handheld homogenizer to obtain a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0091] Specifically, in the above mixing process, the liquid metal is dispersed in the solution as small droplets after being subjected to high-speed stirring and shearing by the homogenizer, while the polymer network is dispersed on the metal surface and in the good solvent.

[0092] Processing liquid metal-polymer mixed solutions:

[0093] The uniformly dispersed mixed solution is subjected to heat or freeze-drying to remove the good solvent, thereby obtaining a dual continuous thin film electrode.

[0094] Specifically, the three liquid metal-polymer mixed solutions prepared during the preparation of the liquid metal-polymer mixed solution were added to a polytetrafluoroethylene petri dish and placed in a vacuum environment at 80°C to remove the good solvent, thus obtaining three kinds of dual continuous thin film electrodes.

[0095] In one specific embodiment, the process of processing the liquid metal-polymer mixed solution is as follows:

[0096] The prepared gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0097] The prepared gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous film.

[0098] The prepared gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0099] Specifically, in this step, liquid metal droplets are initially dispersed in droplet form, where entangled polymer chains form physically cross-linked networks that simultaneously capture a large amount of good solvent. As drying proceeds, the good solvent in these networks is gradually replaced by liquid metal, and the micropores between the liquid metal droplets that were originally filled with solvent are transformed into nanopores filled with liquid metal. Ultimately, the liquid metal fluid becomes the dominant component, forming a continuous structure in which the polymer network is embedded.

[0100] Example 4

[0101] This embodiment discloses a method for preparing a high-sensitivity dual-continuous thin-film electrode, including the following steps:

[0102] Preparation of polymer solutions:

[0103] The preparation of a polymer solution involves gradually adding the polymer to a good solvent, dissolving it, and then stirring until a homogeneous solution is obtained.

[0104] Specifically, the prepared polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution. The steps for preparing the polymer solution include preparing an ethylene / vinyl acetate (EVA) solution and preparing a polyethylene oxide (PEO) solution.

[0105] In one specific embodiment, the process for preparing the polymer solution is as follows:

[0106] Preparation of ethylene / vinyl acetate (EVA) solution: Dissolve 10.0 wt% of ethylene / vinyl acetate particles in anisole liquid and stir magnetically for 3 hours at 90°C until the ethylene / vinyl acetate particles are dissolved to obtain ethylene / vinyl acetate solution.

[0107] Preparation of polyethylene oxide (PEO) solution: Dissolve 4.0 wt% of polyethylene oxide powder in the prepared ethylene / vinyl acetate (EVA) solution, and perform continuous magnetic stirring at 40°C for 2 hours until the polyethylene oxide powder dissolves to obtain an ethylene / vinyl acetate-polyethylene oxide solution.

[0108] Preparation of liquid metal-polymer mixed solution:

[0109] The preparation of a liquid metal-polymer mixed solution involves adding liquid metal to a polymer solution and then uniformly dispersing the mixed solution using a homogenizer to obtain the liquid metal-polymer mixed solution.

[0110] Specifically, the preparation of liquid metal-polymer mixed solutions is based on three different liquid metals, and three liquid metal-polymer mixed solutions are prepared separately.

[0111] In a specific embodiment, the process for preparing the liquid metal-polymer mixed solution is as follows:

[0112] Liquid gallium indium alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 8:2 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 15000 rpm for 15 minutes using a handheld homogenizer to obtain a gallium indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0113] Liquid gallium metal was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 8:2 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 15000 rpm for 15 minutes using a handheld homogenizer to obtain a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0114] Liquid gallium indium tin alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 8:2 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 15000 rpm for 15 minutes using a handheld homogenizer to obtain a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0115] Specifically, in the above mixing process, the liquid metal is dispersed in the solution as small droplets after being subjected to high-speed stirring and shearing by the homogenizer, while the polymer network is dispersed on the metal surface and in the good solvent.

[0116] Processing liquid metal-polymer mixed solutions:

[0117] The uniformly dispersed mixed solution is subjected to heat or freeze-drying to remove the good solvent, thereby obtaining a dual continuous thin film electrode.

[0118] Specifically, the three liquid metal-polymer mixed solutions prepared during the preparation of the liquid metal-polymer mixed solution were added to a polytetrafluoroethylene petri dish and placed in a vacuum environment at 80°C to remove the good solvent, thus obtaining three kinds of dual continuous thin film electrodes.

[0119] In one specific embodiment, the process of processing the liquid metal-polymer mixed solution is as follows:

[0120] The prepared gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0121] The prepared gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous film.

[0122] The prepared gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0123] Example 5

[0124] This embodiment discloses a method for preparing a high-sensitivity dual-continuous thin-film electrode, including the following steps:

[0125] Preparation of polymer solutions:

[0126] The preparation of a polymer solution involves gradually adding the polymer to a good solvent, dissolving it, and then stirring until a homogeneous solution is obtained.

[0127] Specifically, the prepared polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution. The steps for preparing the polymer solution include preparing an ethylene / vinyl acetate (EVA) solution and preparing a polyethylene oxide (PEO) solution.

[0128] In one specific embodiment, the process for preparing the polymer solution is as follows:

[0129] Preparation of ethylene / vinyl acetate (EVA) solution: Dissolve 10.0 wt% of ethylene / vinyl acetate particles in anisole liquid, and perform continuous magnetic stirring at 90°C for 3 hours until the ethylene / vinyl acetate particles dissolve to obtain an ethylene / vinyl acetate solution.

[0130] Preparation of polyethylene oxide (PEO) solution: Dissolve 2.0 wt% polyethylene oxide powder in the prepared ethylene / vinyl acetate (EVA) solution, and perform continuous magnetic stirring at 40°C for 2 hours until the polyethylene oxide powder dissolves to obtain an ethylene / vinyl acetate-polyethylene oxide solution.

[0131] Preparation of liquid metal-polymer mixed solution:

[0132] The preparation of a liquid metal-polymer mixed solution involves adding liquid metal to a polymer solution and then uniformly dispersing the mixed solution using a homogenizer to obtain the liquid metal-polymer mixed solution.

[0133] Specifically, the preparation of liquid metal-polymer mixed solutions is based on three different liquid metals, and three liquid metal-polymer mixed solutions are prepared separately.

[0134] In a specific embodiment, the process for preparing the liquid metal-polymer mixed solution is as follows:

[0135] Liquid gallium indium alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 7:3 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 10,000 rpm for 5 minutes using a handheld homogenizer to obtain a gallium indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0136] Liquid gallium metal was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 7:3 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 10,000 rpm for 5 minutes using a handheld homogenizer to obtain a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0137] Liquid gallium indium tin alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 7:3 to obtain an initial mixed solution. The initial mixed solution was placed at 25°C and stirred and sheared at 10,000 rpm for 5 minutes using a handheld homogenizer to obtain a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0138] Specifically, in the above mixing process, the liquid metal is dispersed in the solution as small droplets after being subjected to high-speed stirring and shearing by the homogenizer, while the polymer network is dispersed on the metal surface and in the good solvent.

[0139] Processing liquid metal-polymer mixed solutions:

[0140] The uniformly dispersed mixed solution is subjected to heat or freeze-drying to remove the good solvent, thereby obtaining a dual continuous thin film electrode.

[0141] Specifically, the three liquid metal-polymer mixed solutions prepared during the preparation of the liquid metal-polymer mixed solution were added to a polytetrafluoroethylene petri dish and placed in a vacuum environment at 80°C to remove the good solvent, thus obtaining three kinds of dual continuous thin film electrodes.

[0142] In one specific embodiment, the process of processing the liquid metal-polymer mixed solution is as follows:

[0143] The prepared gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0144] The prepared gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous film.

[0145] The prepared gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 80°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0146] Example 6

[0147] This embodiment discloses a method for preparing a high-sensitivity dual-continuous thin-film electrode, including the following steps:

[0148] Preparation of polymer solutions:

[0149] The preparation of a polymer solution involves gradually adding the polymer to a good solvent, dissolving it, and then stirring until a homogeneous solution is obtained.

[0150] Specifically, the prepared polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution. The steps for preparing the polymer solution include preparing an ethylene / vinyl acetate (EVA) solution and preparing a polyethylene oxide (PEO) solution.

[0151] In one specific embodiment, the process for preparing the polymer solution is as follows:

[0152] Preparation of ethylene / vinyl acetate (EVA) solution: Dissolve 5.0 wt% of ethylene / vinyl acetate particles in anisole liquid; perform continuous magnetic stirring at 98°C for 3 hours until the ethylene / vinyl acetate particles dissolve to obtain an ethylene / vinyl acetate solution;

[0153] Preparation of polyethylene oxide (PEO) solution: Dissolve 0.2 wt% of polyethylene oxide powder in the prepared ethylene / vinyl acetate (EVA) solution, and perform continuous magnetic stirring at 25°C for 2 hours until the polyethylene oxide powder dissolves to obtain an ethylene / vinyl acetate-polyethylene oxide solution.

[0154] Preparation of liquid metal-polymer mixed solution:

[0155] The preparation of a liquid metal-polymer mixed solution involves adding liquid metal to a polymer solution to obtain an initial mixed solution; then using a homogenizer to uniformly disperse the initial mixed solution to obtain the liquid metal-polymer mixed solution.

[0156] Specifically, the preparation of liquid metal-polymer mixed solutions is based on three different liquid metals, and three liquid metal-polymer mixed solutions are prepared separately.

[0157] In a specific embodiment, the process for preparing the liquid metal-polymer mixed solution is as follows:

[0158] Liquid gallium indium alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 1:1 to obtain an initial mixed solution. The initial mixed solution was placed at a temperature of 40°C and stirred and sheared at a speed of 8000 rpm for 3 minutes using a handheld homogenizer to obtain a gallium indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0159] Liquid gallium metal was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 1:1 to obtain an initial mixed solution. The initial mixed solution was placed at a temperature of 40°C and stirred and sheared at a speed of 8000 rpm for 3 minutes using a handheld homogenizer to obtain a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0160] Liquid gallium indium tin alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution at a weight ratio of 1:1 to obtain an initial mixed solution. The initial mixed solution was placed at a temperature of 40°C and stirred and sheared at 8000 rpm for 3 minutes using a handheld homogenizer to obtain a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

[0161] Specifically, in the above mixing process, the liquid metal is dispersed in the solution as small droplets after being subjected to high-speed stirring and shearing by the homogenizer, while the polymer network is dispersed on the metal surface and in the good solvent.

[0162] Processing liquid metal-polymer mixed solutions:

[0163] The uniformly dispersed mixed solution is subjected to heat or freeze-drying to remove the good solvent, thereby obtaining a dual continuous thin film electrode.

[0164] Specifically, the three liquid metal-polymer mixed solutions prepared during the preparation of the liquid metal-polymer mixed solution were added to a polytetrafluoroethylene petri dish and placed in a vacuum environment at 25°C to remove the good solvent, thus obtaining three kinds of dual continuous thin film electrodes.

[0165] In one specific embodiment, the process of processing the liquid metal-polymer mixed solution is as follows:

[0166] The prepared gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 25°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0167] The prepared gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 25°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0168] The prepared gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution was added to a polytetrafluoroethylene petri dish, and then placed in a vacuum environment at 25°C to remove the good solvent, thereby obtaining a bicontinuous thin film.

[0169] Specifically, in this step, liquid metal droplets are initially dispersed in droplet form, where entangled polymer chains form physically cross-linked networks that simultaneously capture a large amount of good solvent. As drying proceeds, the good solvent in these networks is gradually replaced by liquid metal, and the micropores between the liquid metal droplets that were originally filled with solvent are transformed into nanopores filled with liquid metal. Ultimately, the liquid metal fluid becomes the dominant component, forming a continuous structure in which the polymer network is embedded.

[0170] The invention and its embodiments have been described above illustratively. This description is not restrictive, and the invention can be implemented in other specific forms without departing from its spirit or essential characteristics. The accompanying drawings are only one embodiment of the invention, and the actual structure is not limited thereto. No reference numerals in the claims should limit the scope of the claims. Therefore, if a person skilled in the art is inspired by this description and designs a similar structure and embodiment without departing from the spirit of the invention, such design should fall within the scope of protection of this patent. Furthermore, the word "comprising" does not exclude other elements or steps, and the word "a" preceding an element does not exclude the inclusion of "a plurality" of that element. Multiple elements stated in the product claims may also be implemented by a single element through software or hardware. The terms "first," "second," etc., are used to indicate names and do not indicate any specific order.

Claims

1. A method for fabricating a high-sensitivity dual-continuous thin-film electrode, comprising the following steps: Preparation of polymer solutions: Polymer powders are added to a good solvent, dissolved, and stirred until homogeneous to obtain polymer solutions; wherein, The polymer solution is an ethylene / vinyl acetate-polyethylene oxide solution, and the preparation process includes: dissolving 5.0wt%~10.0wt% of ethylene / vinyl acetate particles in anisole and magnetically stirring at a temperature of 90℃~98℃ to obtain an ethylene / vinyl acetate solution; dissolving 0.2wt%~4.0wt% of polyethylene oxide powder in the ethylene / vinyl acetate solution and magnetically stirring at a temperature of 25℃~40℃ to obtain an ethylene / vinyl acetate-polyethylene oxide solution; Preparation of liquid metal-polymer mixed solution: Liquid metal is added to polymer solution, and the mixed solution is uniformly dispersed using a homogenizer to obtain liquid metal-polymer mixed solution; Preparation of a dual continuous thin-film electrode: The uniformly dispersed mixed solution is heated or freeze-dried to remove the good solvent, thereby obtaining a dual continuous thin-film electrode; wherein, the dual continuous thin-film electrode comprises a liquid metal and a polymer network, wherein the liquid metal serves as the fluid phase of the electrode and forms an interconnected continuum in the dual continuous film; the polymer network exhibits a dispersed three-dimensional porous network structure, connecting the liquid metal oxide layer and adhering to the skin surface.

2. The method for preparing a high-sensitivity dual-continuous thin-film electrode according to claim 1, characterized in that, The preparation of liquid metal-polymer mixed solutions includes the preparation of gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solutions, gallium-ethylene / vinyl acetate-polyethylene oxide mixed solutions, and gallium-indium-tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solutions.

3. The method for preparing a high-sensitivity dual-continuous thin-film electrode according to claim 2, characterized in that, The process for preparing a gallium-indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution is as follows: Liquid gallium-indium alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution to obtain an initial mixed solution; The initial mixed solution was placed at a temperature of 25℃~40℃ and stirred and sheared using a handheld homogenizer at a speed of 8000rpm~15000rpm to obtain a gallium indium alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

4. The method for preparing a high-sensitivity dual-continuous thin-film electrode according to claim 2, characterized in that, The process for preparing a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution is as follows: Liquid gallium metal was mixed with an ethylene / vinyl acetate-polyethylene oxide solution to obtain an initial mixed solution; The initial mixed solution was placed at a temperature of 25℃~40℃ and stirred and sheared using a handheld homogenizer at a speed of 8000rpm~15000rpm to obtain a gallium-ethylene / vinyl acetate-polyethylene oxide mixed solution.

5. The method for preparing a high-sensitivity dual-continuous thin-film electrode according to claim 2, characterized in that, The process for preparing a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution is as follows: Liquid gallium indium tin alloy was mixed with an ethylene / vinyl acetate-polyethylene oxide solution to obtain an initial mixed solution; The initial mixed solution was placed at a temperature of 25℃~40℃ and stirred and sheared using a handheld homogenizer at a speed of 8000rpm~15000rpm to obtain a gallium indium tin alloy-ethylene / vinyl acetate-polyethylene oxide mixed solution.

6. The high-sensitivity dual-continuous thin-film electrode prepared by the method for preparing a high-sensitivity dual-continuous thin-film electrode according to any one of claims 1-5, characterized in that, It includes a liquid metal and a polymer network. The liquid metal serves as the fluid phase of the electrode and forms an interconnected continuum in a bicontinuous thin film. The polymer network presents a dispersed three-dimensional porous network structure, connecting the liquid metal oxide layer and adhering to the skin surface.

Citation Information

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