Universal bioelectronic interface capable of being repeatedly assembled and preparation method thereof

Abstract

The invention provides a universal bioelectronic interface capable of being repeatedly assembled and a preparation method thereof, and relates to the technical field of bioelectronics, and the universal bioelectronic interface is formed by combining a self-healing bottle brush elastomer substrate composed of a monomer with amido and a nano-thickness conductive film prepared through a physical vapor deposition technology. The universal bioelectronic interface capable of being repeatedly assembled can be used for preparing various patterns through laser and other processing technologies, and has the advantages of high adhesion, high electrical stability, high assembly rate and the like, an electrode formed after assembly can meet the requirement for monitoring of various in-vivo and in-vitro electric signals, and the universal bioelectronic interface has a good application prospect and is suitable for popularization and application. And the preparation method is simple and has a good industrialization prospect.

Description

Technical Field

[0001] The present invention relates to the field of bioelectronic technology, and particularly to a reusable and general bioelectronic interface and a preparation method thereof. Background Art

[0002] Stretchable electronic devices have achieved high-fidelity bio-signal acquisition in the field of human physiological signal monitoring. Its system architecture consists of three core modules: a flexible module that is mechanically compatible with human tissues, a rigid functional module integrating silicon-based microelectronic devices, and a protective encapsulation module. Due to significant differences in material properties, geometric configurations, and processing technologies among the modules, commercially available conductive materials such as anisotropic conductive films or silver pastes are commonly used for inter-module assembly. However, the mismatch in mechanical properties between the modules causes the conductive material to be prone to interfacial peeling under dynamic stretching conditions, resulting in the failure of the conductive path. This key technical bottleneck severely restricts the complexity and robustness of stretchable electronic devices. Currently, researchers at home and abroad have tried various methods to solve the above problems. For example, all-soft electronic devices (without rigid silicon-based components) have been developed to eliminate mechanical mismatch at the interface. However, silicon-based components are still crucial for signal processing and wireless communication. Some studies have used liquid metals to replace rigid conductive materials, but their high surface tension results in low interfacial adhesion and may smear to unwanted places. Composites composed of self-healing polymers or hydrogel matrices and conductive fillers can also be used to replace rigid conductive materials. However, their large thickness (tens to hundreds of micrometers) leads to reduced mechanical mismatch and electrical stability. Moreover, these materials are assembled together by attaching them to the modules, and after disassembly, there will be residual conductive materials on the modules, making them unable to be reused. This preparation process is complex and greatly increases the cost. Therefore, developing a bioelectronic interface connection technology with reversible assembly characteristics and capable of withstanding dynamic deformation has become a key research direction for breaking through the existing technical barriers. Summary of the Invention

[0003] The purpose of the present invention is to provide a reusable and general bioelectronic interface and a preparation method thereof to solve the above technical problems.

[0004] To solve the above technical problems, the present invention adopts the following technical solutions:

[0005] A reusable self-adhesive general bioelectronic interface, which is composed of a self-healing bottlebrush elastomer substrate formed by monomers with amino groups and combined with a conductive thin film with a nanometer thickness prepared by physical vapor deposition technology.

[0006] Furthermore, the substrate comprises the following materials in parts by volume: 50 - 200 parts of a polymer with a single terminal double bond and an amino group, 1 part of a crosslinking agent, and 0.5 - 2 parts of a photoinitiator.

[0007] Further, the polymer with a single terminal double bond having an amino group is any one of 3-allylaminocarbonylphenylboronic acid and 6-(allyloxycarbonylamino)-1-hexanol, the crosslinking agent is poly(dimethylsiloxane) terminated with methacryloxypropyl, and the photoinitiator is 2-hydroxy-2-methylpropiophenone.

[0008] The method for preparing a reusable and general bioelectronic interface using the above materials includes the following steps:

[0009] 1) Place 50 - 200 parts by volume of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of poly(dimethylsiloxane) terminated with methacryloxypropyl, and 0.5 - 2 parts of 2-hydroxy-2-methylpropiophenone in a container to obtain a composite polymer solution for preparing the substrate;

[0010] 2) Vortex the composite polymer solution at room temperature for 1 minute to mix it evenly;

[0011] 3) Add the composite polymer solution into a customized Teflon mold, irradiate it with a 365 nm ultraviolet lamp for 10 minutes, then the polymer cures, and remove the polymer film;

[0012] 4) Pre-stretch the film, place it in a three-phase film evaporation and deposition system, and deposit gold nanoparticles by physical vapor deposition at a rate of 0.5 Å / s to form a gold nanometer film with a thickness of 20 - 100 nm;

[0013] 5) Take out the film from the evaporation and deposition system to obtain a reusable and self-adhesive general bioelectronic interface.

[0014] Further, in the above preparation method, it is preferred to use 200 parts by volume of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of poly(dimethylsiloxane) terminated with methacryloxypropyl, and 1 part of 2-hydroxy-2-methylpropiophenone.

[0015] Further, the conductive layer of the bioelectronic interface prepared by the above preparation method is gold nanoparticles, and the thickness of the conductive layer is preferably 80 nm.

[0016] The reusable and general bioelectronic interface is applied to in-vivo and in-vitro electrical signal monitoring.

[0017] Further, the reusable and general bioelectronic interface can be applied to peripheral nerve electrodes, epidermal electrodes, etc.

[0018] The reusable and self-adhesive general bioelectronic interface can be prepared with various patterns through processing techniques such as laser.

[0019] The beneficial effects of the present invention are:

[0020] 1. The reusable and general bioelectronic interface prepared by the present invention can be processed by laser or other processing techniques to prepare various patterns, and has the advantages of high adhesion, high electrical stability, high assembly rate, etc. The electrodes formed after assembly can meet the requirements of various electrical signal monitoring in vivo and in vitro, have good application prospects, and the preparation method is simple, with good industrialization prospects.

[0021] 2. The reusable and general bioelectronic interface prepared by the present invention can be customized in shape and size according to different parts and application scenarios, and can be repeatedly bonded and removed. It can be widely used in the monitoring of human electrophysiological signals, and can be connected to silicon-based electronic components to realize signal post-processing and analysis, improving the overall performance and data processing efficiency of the monitoring system. Brief Description of the Drawings

[0022] Figure 1 It is the preparation flow chart of the reusable and general bioelectronic interface;

[0023] Figure 2 It is the self-healing principle diagram of the substrate;

[0024] Figure 3 It is the schematic principle diagram of the bioelectronic interface structure;

[0025] Figure 4 It is the substrate modulus diagram in Example 1;

[0026] Figure 5 It is the comparison diagram of the sheet resistance of Sample 4 in Example 1 after evaporating gold nanoparticles with different thicknesses;

[0027] Figure 6 It is the tensile schematic diagram after the interface is assembled;

[0028] Figure 7 It is the relative resistance change of the independent interface and the assembled interface;

[0029] Figure 8 It is the relative resistance change between the assembled interface and the traditional interface assembled with commercial conductive materials;

[0030] Figure 9 It is the resistance change of the interface during repeated use;

[0031] Figure 10 It is the schematic diagram of the repeated self-assembly of the interface. Detailed Embodiments

[0032] To facilitate the understanding of the present invention, the present invention will be described more comprehensively below with reference to the relevant drawings. Preferred embodiments of the present invention are shown in the drawings. However, the present invention can be implemented in many different forms and is not limited to the embodiments described herein. On the contrary, these embodiments are provided to make the understanding of the disclosure of the present invention more thorough and comprehensive.

[0033] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by those of ordinary skill in the technical field to which the present invention belongs. The terms used in the description of the present invention herein are only for the purpose of describing specific embodiments and are not intended to limit the present invention.

[0034] Specific embodiments of the present invention will be described below with reference to the drawings.

[0035] Example 1

[0036] In this embodiment, four examples for preparing the substrate are provided by volume parts. All four examples use the same materials, but the volume parts between the materials are different. For details, please refer to Table 1.

[0037] Table 1: Material Table for Preparing the Substrate

[0038]

[0039] The above four examples all prepare the substrate according to the following method: 1) Put 6-(allyloxycarbonylamino)-1-hexanol, methacryloxypropyl-terminated polydimethylsiloxane, and 2-hydroxy-2-methylpropiophenone into a container according to volume parts to obtain a composite polymer solution for preparing the substrate; 2) Vortex the composite polymer solution at room temperature for 1 minute to mix it evenly; 3) Add the composite polymer solution into a customized Teflon mold, and after irradiating it with a 365 nm ultraviolet lamp for 10 minutes, the polymer cures, and the polymer film is peeled off.

[0040] Please refer to Figure 4 , after testing the modulus and self-adhesion performance of the substrate, Example 4, that is, the substrate made of 200 parts by volume of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of methacryloxypropyl-terminated polydimethylsiloxane, and 1 part of 2-hydroxy-2-methylpropiophenone has the smallest modulus. As is well known, the smaller the modulus, the softer the substrate, and it is also easier to bend or stretch. Therefore, Example 4 is the optimal example among all examples.

[0041] Example 2

[0042] In this embodiment, a reusable and assembleable general bioelectronic interface is prepared using Sample 4 in Embodiment 1, including the following steps: 1) Put 200 parts of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of methacryloxypropyl-terminated polydimethylsiloxane, and 1 part of 2-hydroxy-2-methylpropiophenone in a container according to volume parts to obtain a composite polymer solution for preparing the substrate; 2) Vortex the composite polymer solution at room temperature for 1 minute to mix it evenly; 3) Add the composite polymer solution into a customized Teflon mold, irradiate it with a UV lamp in the 365nm band for 10 minutes, then the polymer cures, and peel off the polymer film; 4) Pre-stretch the film, place it in a three-phase film evaporation and plating system, and deposit gold nanoparticles by physical vapor deposition at a rate of 0.5 angstroms per second to form a gold nanometer film with a thickness of 20-100nm; 5) Take out the film from the evaporation and plating system to obtain a reusable self-adhesive general bioelectronic interface.

[0043] In this embodiment, the substrates prepared in steps 1) to 3) are respectively plated with gold nanometer films with thicknesses of 20nm, 40nm, 60nm, 80nm, and 100nm. In addition, this embodiment also provides 5 samples. For details, please refer to Table 2.

[0044] Table 2: Thickness table of gold nanometer films plated on the substrate

[0045]

[0046] Please refer to Figure 5 , when the thickness of the interface conductive layer (gold nanometer film) is 80nm, the interface can simultaneously meet good adhesion and conductivity. When the thickness is less than 80nm, although assembly can be achieved, due to the large resistance, the conductivity is poor; while when the thickness is greater than 80nm, although the conductivity is good, due to too few exposed polymer sites on the surface, effective assembly cannot be achieved.

[0047] Embodiment 3

[0048] This example uses Sample 4 in Example 2 to prepare a reusable and assembled general bioelectronic interface, including the following steps: 1) Put 200 parts of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of methacryloxypropyl-terminated polydimethylsiloxane, and 1 part of 2-hydroxy-2-methylpropiophenone in a container by volume to obtain a composite polymer solution for preparing the substrate; 2) Vortex the composite polymer solution at room temperature for 1 minute to mix it evenly; 3) Add the composite polymer solution into a customized Teflon mold, irradiate it with a 365-nm ultraviolet lamp for 10 minutes, then the polymer cures, and peel off the polymer film; 4) Pre-stretch the film, place it in a three-phase thin film evaporation system, and deposit gold nanoparticles by physical vapor deposition at a rate of 0.5 angstroms per second to form a gold nanoparticle film with a thickness of 80 nm; 5) Take out the film from the evaporation system to obtain a reusable self-adhesive general bioelectronic interface.

[0049] In this example, the resistance of the independent interface and the assembled interface is measured. Measurement process: Clamp both ends of the independent interface or the assembled interface on the fixture of a universal tensile testing machine (C42.503, MTS), measure the length with a vernier caliper, connect the sample to a Keithley 2450 source meter with conductive tape on the fixture, set the tensile speed of the universal testing machine to 10 mm / min, and synchronously collect the strain and resistance signals to obtain the relative resistance change of the interface. The test results are as Figure 7 shown. It can be clearly observed from Figure 7 that when the interface is assembled, the change in its relative resistance does not show a significant increase compared to the individual interface. This result fully demonstrates that the assembled interface performs excellently in terms of performance, and its assembly method can effectively ensure the transmission quality of electrical signals and will not damage the transmission effect of the signals.

[0050] Example 4

[0051] This example uses the reusable and assembled general bioelectronic interface prepared in Example 3. This example focuses on testing the relative resistance change between the assembled interface and the traditional interface assembled with commercial conductive materials. Among them, the commercial conductive materials are conductive copper tape (Nisshin EM 733, Japan) and conductive silver paint (Electrolube ESCP03B, Conduction CD-03). The test method is as follows: Regarding the assembly of the traditional interface, the traditional interface interface is mainly combined by using the same-sized commercial conductive paste and tape sandwiched in the middle to obtain the connection. The assembled interface is directly assembled by pressing the conductive surfaces of the two interfaces. The test results are as Figure 8As shown, the results indicate that, compared with traditional interfaces (such as those using commercial conductive materials like double-sided copper tape or silver pastes of different models for connection), under tensile conditions, the change in its resistance is significantly reduced.

[0052] Example 5

[0053] This example uses the reusable and general bioelectronic interface prepared in Example 3. This example focuses on testing the resistance change of the assembled interface during repeated use. The testing method is as follows: During the experiment, first connect both ends of the assembled interface to a Keithley 2450 source meter through conductive tape. After the connection is completed, firmly fix the entire device on the test platform to isolate potential interference from external factors on the measurement results. Subsequently, Figure 10 as shown, repeatedly assemble the interface multiple times and use the source meter to record the resistance value after each assembly. Please refer to Figure 9 , the experimental results show that this interface can not only be successfully assembled repeatedly, but also maintain stable conductive performance after each assembly, demonstrating its reusability and fully proving its reliability and durability in practical applications.

[0054] The technical features of the above-described embodiments can be combined arbitrarily. For the sake of brevity of description, not all possible combinations of the technical features in the above embodiments are described. However, as long as there is no contradiction in the combination of these technical features, it should be considered as the scope described in this specification.

[0055] The above-described embodiments only represent several implementation manners of the present invention. Their descriptions are relatively specific and detailed, but they should not be construed as limiting the scope of the invention patent. It should be noted that for those of ordinary skill in the art, without departing from the concept of the present invention, several modifications and improvements can still be made, and these all belong to the protection scope of the present invention. Therefore, the protection scope of the present invention patent should be subject to the appended claims.

Claims

1. A reusable self - adhesive general bio - electronic interface, characterized in that, It includes a self-healing bottlebrush elastomer substrate composed of monomers with amino groups, combined with a nano-thick conductive film prepared by physical vapor deposition technology.

2. A reusable self - adhesive general bio - electronic interface according to claim 1, characterized in that, The substrate includes the following materials in parts by volume: 50 - 200 parts of a polymer with a single terminal double bond and an amino group, 1 part of a crosslinking agent, and 0.5 - 2 parts of a photoinitiator.

3. A reusable self - adhering general bio - electronic interface according to claim 2, characterized in that, The polymer with a single terminal double bond and an amino group is any one of 3-allylaminocarbonylphenylboronic acid and 6-(allyloxycarbonylamino)-1-hexanol, the crosslinking agent is methacryloxypropyl-terminated polydimethylsiloxane, and the photoinitiator is 2-hydroxy-2-methylpropiophenone.

4. A method for preparing a reusable and assembled general bioelectronic interface using the material according to claim 3, characterized in that, It includes the following steps: 1) Put 50 - 200 parts of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of methacryloxypropyl-terminated polydimethylsiloxane, and 0.5 - 2 parts of 2-hydroxy-2-methylpropiophenone in a container by parts by volume to obtain a composite polymer solution for preparing the substrate film; 2) Vortex the composite polymer solution at room temperature for 1 minute to mix it evenly; 3) Add the composite polymer solution into a customized Teflon mold, irradiate it with a UV lamp to cure the polymer, and then peel off the polymer film; 4) Pre-stretch the film, place it in a three-phase thin film evaporation and plating system, deposit gold nanoparticles by physical vapor deposition at a rate of 0.5 Å / s to form a gold nano-film with a thickness of 20 - 100 nm; 5) Take out the film from the evaporation and plating system to obtain a reusable self-bonding general bioelectronic interface.

5. The preparation method of the reusable and assembled general bioelectronic interface according to claim 4, wherein The materials are 200 parts of 6-(allyloxycarbonylamino)-1-hexanol, 1 part of methacryloxypropyl-terminated polydimethylsiloxane, and 1 part of 2-hydroxy-2-methylpropiophenone by parts by volume.

6. The preparation method of the reusable and assembled general bioelectronic interface according to claim 5, characterized in that, The conductive layer of the bioelectronic interface is gold nanoparticles, and the thickness of the conductive layer is 80 nm.

7. The preparation method of the reusable and assembled general bioelectronic interface according to claim 4, characterized in that, The wavelength band of the UV lamp is 365 nm, and the irradiation time is 10 min.

8. The reusable assembled general bioelectronic interface prepared in claim 4 is applied to in vivo and in vitro electrical signal monitoring.

9. The reusable assembled general bioelectronic interface prepared in claim 4 can be used to prepare various patterns by laser processing technology.

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