A multifunctional intelligent electronic tattoo and its preparation method and application

Abstract

The present invention discloses a multifunctional smart electronic tattoo and its preparation method and application, specifically relating to the field of material technology. The smart electronic tattoo is prepared from MXene, nanocellulose and silver nanowires; wherein the weight ratio of MXene, nanocellulose and silver nanowires is 25:(1-10):1. The specific preparation method is: after MXene, nanocellulose and silver nanowires are evenly mixed, they are transferred to a substrate to obtain a smart electronic tattoo. The present invention also discloses the application of the above-mentioned smart electronic tattoo in the preparation of epidermal electronics and smart prostheses. The electrical conductivity of the smart electronic tattoo prepared by the present invention can reach 3688.4S / m, and it has excellent sensing capabilities for ambient temperature, humidity, distance and angle perception, material recognition and tensile strain. At the same time, it can realize self-powered distance perception and material recognition for moving objects, and has great application potential in the fields of epidermal electronics and smart prostheses.

Description

Technical Field

[0001] The present invention belongs to the field of material technology, and in particular relates to a multifunctional intelligent electronic tattoo and a preparation method and application thereof. Background Art

[0002] Wearable / implantable electronic systems can be tightly integrated with human tissue, enabling real-time monitoring of physiological and environmental signals, and will play an irreplaceable and important role in future society. Despite the growing global market demand for wearable electronics (expected to reach $74 billion by 2025), most current wearable devices are based on brittle silicon substrates. These silicon-based electronics cannot achieve conformal contact with human tissue, resulting in performance degradation and motion artifacts during dynamic testing. Electronic tattoos are a novel wearable bioelectronic system that are ultrathin, lightweight, and have a skin-like modulus, enabling noninvasive, high-fidelity monitoring. Furthermore, their exceptional flexibility and highly conformable adhesion to biological tissue make them promising candidates for multimodal sensing of physiological signals and environmental stimuli. However, most current electronic tattoos or epidermal electronics require complex design structures, multiple sensor combinations, and a large skin coverage area to achieve multi-signal sensing and multifunctional integration, which inevitably leads to cumbersome designs and increased discomfort.

[0003] MXenes are a new type of two-dimensional (2D) transition metal carbides or carbonitrides discovered by Professor Yury Gogotsi and others at Drexel University in the United States in 2011. Its chemical formula can be expressed as n+1 X n T x Indicates, where M refers to a transition metal, X refers to C and / or N, n is generally 1-3, T x Refers to surface groups (such as -F, =O, -OH, etc.). MXenes have demonstrated tremendous potential in energy storage, adsorption, sensors, and conductive fillers. While MXene-based printed electronics have been initially developed, existing research primarily focuses on energy storage, while research on multifunctional sensing integration and conformal electronics for biological tissues remains scarce. Summary of the Invention

[0004] In order to solve the above problems in the prior art, the present invention provides a multifunctional intelligent electronic tattoo and a preparation method and application thereof.

[0005] To achieve the above object, the present invention provides the following technical solutions:

[0006] The present invention provides a multifunctional smart electronic tattoo, which is prepared from MXene, nanocellulose and silver nanowires; wherein the weight ratio of the MXene, nanocellulose and silver nanowires is 25:(1-10):1.

[0007] Beneficial effects: The reason why the present invention adds nanocellulose when preparing smart electronic tattoos is that the addition of nanocellulose can make the prepared electronic tattoos more sensitive to changes in humidity and increase the humidity sensing ability. On this basis, the addition of silver nanowires can increase the temperature sensing ability of the electronic tattoos, making them have higher temperature sensitivity. At the same time, mixing nanocellulose, silver nanowires and MXene can increase the conductivity of the electronic tattoos and improve their electrical conductivity.

[0008] Furthermore, the weight ratio of the MXene, nanocellulose and silver nanowires is 25:(1-3):1.

[0009] More preferably, the weight ratio of the MXene, nanocellulose and silver nanowires is 25:3:1.

[0010] Beneficial effect: The reason why the weight ratio of MXene, nanocellulose and silver nanowires in the present invention is preferably 25:3:1 is because nanocellulose plays an important role in humidity sensing. The greater the amount of nanocellulose added, the greater the resistance change value of the MXene / nanocellulose / silver nanowire electronic tattoo. However, when the amount of nanocellulose added is too large, the resistance of the electronic tattoo will be too high and the mechanical sensing performance will be reduced.

[0011] Furthermore, the MXene includes one or more of Ti3C2, Ta4C3, Nb2C and Ti2C mixed in any proportion; the lateral size of the MXene is 0.3-1.2 μm and the thickness is 0.8-1.5 nm.

[0012] Beneficial effects: The reason why the present invention selects Ti3C2, Ta4C3, Nb2C and Ti2C as MXene is that Ti3C2, Ta4C3, Nb2C and Ti2C have high electrical conductivity, among which Ti3C2 is relatively more mature and has higher electrical conductivity.

[0013] Furthermore, the nanocellulose (CNFs) is nanocellulose oxidized by 2,2,6,6-tetramethylpiperidine-1-oxydione; the diameter of the nanocellulose is 10-50 nm, and the aspect ratio is 10-100.

[0014] Beneficial effects: The present invention uses nanocellulose oxidized with 2,2,6,6-tetramethylpiperidine-1-oxydione because it has a large number of hydrophilic hydroxyl groups and carbonyl groups on its surface, which is beneficial to ensure the subsequent humidity sensing performance.

[0015] Furthermore, the silver nanowires (AgNWs) have a diameter of 10-50 nm and an aspect ratio of 10-100.

[0016] The present invention also provides a method for preparing a multifunctional smart electronic tattoo, comprising the following steps: uniformly mixing the MXene, nanocellulose and silver nanowires to obtain a mixed slurry, and then transferring the mixed slurry to a substrate to obtain the smart electronic tattoo.

[0017] Furthermore, before the transfer, the mixed slurry is placed in a vacuum environment and evacuated for 1 hour, and the vacuum degree of the vacuum environment is -0.1 MPa.

[0018] Beneficial effect: The mixed slurry is placed in a vacuum environment in the present invention to remove air bubbles and facilitate the subsequent preparation of a uniform electronic tattoo.

[0019] Furthermore, the transfer method is one of direct writing, seal transfer, screen printing or 3D printing.

[0020] Beneficial effects: The present invention can be transferred by direct writing, seal transfer, screen printing or 3D printing, etc., so as to diversify the prepared smart electronic tattoos.

[0021] Furthermore, the substrate is one of fabric, rubber, metal sheet, A4 paper or polyurethane surface.

[0022] Beneficial effects: The present invention selects different substrates in order to reflect the universality of the substrate of the electronic tattoo.

[0023] The present invention also provides an application of a multifunctional intelligent electronic tattoo in the preparation of epidermal electronics and intelligent prostheses.

[0024] In this invention, the smart electronic tattoo can distinguish different ambient temperatures. Specifically, at a constant input voltage of 4V, the currents flowing through the smart electronic tattoo at ambient temperatures of 30, 50, 70, and 90°C were 0.065, 0.071, 0.079, and 0.088A, respectively.

[0025] In the present invention, the smart electronic tattoo can distinguish different ambient humidity levels. Specifically, when the amount of nanocellulose in the smart electronic tattoo is 0.1-0.5g, and the relative humidity increases from 40% to 90%, the relative resistance of the smart electronic tattoo changes by 1.6-2.8, more preferably 2.1.

[0026] In this invention, the smart electronic tattoo can distinguish different tensile strains. Specifically, applying different axial strains (10%, 20%, 30%, 40%, and 50%) results in a relative resistance change of 0.24-0.56. Therefore, the smart electronic tattoo can monitor different human movements in real time.

[0027] In the present invention, based on the synergistic effect of electromagnetic induction and electrostatic induction, the intelligent electronic tattoo can sense the different distances and angles of the moving object from the tattoo.

[0028] In the present invention, based on the fact that different materials have different electronegativities, the smart electronic tattoo can distinguish the various materials of different objects.

[0029] Compared with the prior art, the present invention has the following beneficial effects:

[0030] (1) The intelligent electronic tattoo provided by the present invention has skin conformability and multi-sensing capabilities, overcoming the problem that traditional silicon-based flexible devices are difficult to adapt to biological tissue mechanics, and avoiding the subsequent multi-sensor integration and large-area coverage of the skin;

[0031] (2) The preparation method of the intelligent electronic tattoo provided by the present invention is convenient, has a wide range of applications, and is safe in process. The mixed slurry can be printed onto a variety of different substrate surfaces by direct writing, seal transfer, screen printing, or 3D printing, and electronic tattoo patterns of different shapes can be obtained;

[0032] (3) The intelligent electronic tattoo provided by the present invention exhibited a high conductivity of 3688.4 S / m in the conductivity test;

[0033] (4) The intelligent electronic tattoo prepared by the present invention has excellent multifunctional sensing capabilities, including temperature sensing, humidity sensing, tensile strain sensing, distance and angle sensing, and material recognition, and has great application potential in the fields of epidermal electronics and intelligent prostheses. BRIEF DESCRIPTION OF THE DRAWINGS

[0034] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the following briefly introduces the drawings required for use in the embodiments. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without paying any creative work.

[0035] Figure 1 This is a flow chart of preparing the smart electronic tattoo material of the present invention.

[0036] Figure 2 The graphs are rheological properties test graphs of the smart inks prepared in Example 1 and Comparative Example 1;

[0037] Figure 3 The texture patterns of the smart electronic tattoos prepared in Example 1 and Examples 8-14, wherein a is the texture pattern of the smart electronic tattoo prepared in Example 8, b is the texture pattern of the smart electronic tattoo prepared in Example 9, c is the texture pattern of the smart electronic tattoo prepared in Example 10, e is the texture pattern of the smart electronic tattoo prepared in Example 11, f is the texture pattern of the smart electronic tattoo prepared in Example 12, g is the texture pattern of the smart electronic tattoo prepared in Example 13, i is the texture pattern of the smart electronic tattoo prepared in Example 14, and d and h are the texture patterns of the smart electronic tattoo prepared in Example 1;

[0038] Figure 4 Conductivity test graph of the smart electronic tattoo prepared in Example 1 and Comparative Examples 1-2;

[0039] Figure 5 Schematic diagram of temperature sensing of the smart electronic tattoo prepared in Example 1 and Comparative Example 2;

[0040] Figure 6 This is a humidity sensor diagram of the smart electronic tattoo prepared in Example 1-3;

[0041] Figure 7 This is a tensile strain sensor image of the smart electronic tattoo prepared in Example 1;

[0042] Figure 8 This is a distance perception test chart of the smart electronic tattoo prepared in Example 1;

[0043] Figure 9 This is the angle perception test chart of the smart electronic tattoo prepared in Example 1;

[0044] Figure 10 This is a graph showing the material recognition test results of smart electronic tattoos prepared by transferring the mixed slurry obtained in Example 1 onto different substrates. DETAILED DESCRIPTION

[0045] Various exemplary embodiments of the present invention are now described in detail. This detailed description should not be considered as a limitation of the present invention, but should be understood as a more detailed description of certain aspects, features, and embodiments of the present invention. It should be understood that the terms used in the present invention are only for describing specific embodiments and are not intended to limit the present invention.

[0046] In addition, for numerical ranges in the present invention, it is understood that each intervening value between the upper and lower limits of the range is also specifically disclosed. Each smaller range between any stated value or intervening value in a stated range and any other stated value or intervening value in the stated range is also included in the present invention. The upper and lower limits of these smaller ranges may independently be included or excluded in the range.

[0047] Unless otherwise indicated, all technical and scientific terms used herein have the same meaning as commonly understood by those skilled in the art. Although only preferred methods and materials are described herein, any methods and materials similar or equivalent to those described herein may also be used in the practice or testing of the present invention. All documents mentioned in this specification are incorporated by reference to disclose and describe the methods and / or materials associated with the documents. In the event of any conflict with any incorporated document, the contents of this specification shall prevail.

[0048] It will be apparent to those skilled in the art that various modifications and variations may be made to the specific embodiments described herein without departing from the scope or spirit of the invention. Other embodiments will be apparent to those skilled in the art from the description of the invention. The description and examples are intended to be exemplary only.

[0049] The words “include,” “including,” “have,” “contain,” etc. used in this document are open-ended terms, meaning including but not limited to.

[0050] The raw materials used in the examples of the present invention were all commercially available, including MXene purchased from Jilin Yiyi Technology Co., Ltd., 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose purchased from Tianjin Mujingling Biotechnology Co., Ltd., and silver nanowires (AgNWs) purchased from Zhejiang Xinglong New Materials Technology Co., Ltd.

[0051] A multifunctional smart electronic tattoo is prepared from MXene, nanocellulose and silver nanowires; wherein the weight ratio of the MXene, nanocellulose and silver nanowires is 25:(1-10):1.

[0052] Furthermore, the weight ratio of the MXene, nanocellulose and silver nanowires is 25:(1-3):1.

[0053] More preferably, the weight ratio of MXene, nanocellulose and silver nanowires is 25:3:1.

[0054] The MXene includes one or more of Ti3C2, Ta4C3, Nb2C and Ti2C mixed in any proportion; the lateral size of the MXene is 0.3-1.2 μm and the thickness is 0.8-1.5 nm.

[0055] The nanocellulose (CNFs) is nanocellulose oxidized by 2,2,6,6-tetramethylpiperidine-1-oxydione; the diameter of the nanocellulose is 10-50nm, and the aspect ratio is 10-100.

[0056] The silver nanowires (AgNWs) have a diameter of 10-50 nm and an aspect ratio of 10-100.

[0057] The present invention also provides a method for preparing a multifunctional smart electronic tattoo, comprising the following steps: uniformly mixing the MXene, nanocellulose and silver nanowires to obtain a mixed slurry, and then transferring the mixed slurry to a substrate to obtain the smart electronic tattoo.

[0058] In some preferred embodiments, the mixed slurry is placed in a vacuum environment for 1 hour before the transfer, and the vacuum degree of the vacuum environment is -0.1 MPa;

[0059] The transfer method is one of direct writing, seal transfer, screen printing or 3D printing.

[0060] The substrate is one of fabric, rubber, metal sheet, A4 paper or polyurethane surface.

[0061] The present invention also provides an application of a multifunctional intelligent electronic tattoo in the preparation of epidermal electronics and intelligent prostheses.

[0062] In this invention, the smart electronic tattoo can distinguish different ambient temperatures. Specifically, at a constant input voltage of 4V, the currents flowing through the smart electronic tattoo at ambient temperatures of 30, 50, 70, and 90°C were 0.065, 0.071, 0.079, and 0.088A, respectively.

[0063] In the present invention, the smart electronic tattoo can distinguish different ambient humidity levels. Specifically, when the amount of nanocellulose in the smart electronic tattoo is 0.1-0.5g, and the relative humidity increases from 40% to 90%, the relative resistance of the smart electronic tattoo changes by 1.6-2.8, more preferably 2.1.

[0064] In this invention, the smart electronic tattoo can distinguish different tensile strains. Specifically, applying different axial strains (10%, 20%, 30%, 40%, and 50%) results in a relative resistance change of 0.24-0.56. Therefore, the smart electronic tattoo can monitor different human movements in real time.

[0065] In the present invention, based on the synergistic effect of electromagnetic induction and electrostatic induction, the intelligent electronic tattoo can sense the different distances and angles of the moving object from the tattoo.

[0066] In the present invention, based on the fact that different materials have different electronegativities, the smart electronic tattoo can distinguish the various materials of different objects.

[0067] Example 1

[0068] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0069] Ti3C2, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:3:1, wherein the lateral size of Ti3C2 was 0.8 μm and the thickness was 1.2 nm, the diameter of the nanocellulose oxidized 2,2,6,6-tetramethylpiperidine-1-oxydione was 35 nm, the aspect ratio was 15, and the diameter of the silver nanowire was 35 nm, the aspect ratio was 15. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 h to obtain a mixed slurry (MXene / CNFs / AgNWs-0.3). The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and vacuumed for 1 h to remove bubbles. Subsequently, the mixed slurry was transferred to A4 paper by screen printing and dried at 25 ° C for 12 h to obtain a uniform smart electronic tattoo. The obtained smart electronic tattoo pattern is Figure 3 The d and h in .

[0070] Example 2

[0071] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0072] Ti3C2, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:1:1, wherein the lateral size of Ti3C2 was 0.8 μm and the thickness was 1.2 nm, the diameter of the 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose was 35 nm and the aspect ratio was 15, and the diameter of the silver nanowires was 35 nm and the aspect ratio was 15. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 h to obtain a mixed slurry (MXene / CNFs / AgNWs-0.1). The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and evacuated for 1 h to remove bubbles. Subsequently, the mixed slurry was transferred to A4 paper by screen printing and dried at 25°C for 12 h to obtain a uniform smart electronic tattoo.

[0073] Example 3

[0074] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0075] Ti3C2, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:5:1, wherein the lateral size of Ti3C2 was 0.8 μm and the thickness was 1.2 nm, the diameter of the 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose was 35 nm and the aspect ratio was 15, and the diameter of the silver nanowires was 35 nm and the aspect ratio was 15. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 h to obtain a mixed slurry (MXene / CNFs / AgNWs-0.5). The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and evacuated for 1 h to remove bubbles. Subsequently, the mixed slurry was transferred to A4 paper by screen printing and dried at 25°C for 12 h to obtain a uniform smart electronic tattoo.

[0076] Example 4

[0077] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0078] Ta4C3, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:3:1, wherein the lateral size of Ta4C3 was 0.4 μm and the thickness was 0.9 nm, the diameter of the 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose was 12 nm and the aspect ratio was 10, and the diameter of the silver nanowires was 12 nm and the aspect ratio was 10. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 hours to obtain a mixed slurry. The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and evacuated for 1 hour to remove bubbles. Subsequently, the mixed slurry was transferred to the fabric by direct writing, and dried at 25°C for 12 hours to obtain a uniform smart electronic tattoo.

[0079] Example 5

[0080] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0081] Nb2C, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:3:1, wherein the lateral size of Nb2C was 1.0 μm and the thickness was 1.5 nm, the diameter of the 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose was 50 nm and the aspect ratio was 60, and the diameter of the silver nanowires was 50 nm and the aspect ratio was 60. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 hours to obtain a mixed slurry. The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and evacuated for 1 hour to remove bubbles. Subsequently, the mixed slurry was transferred to rubber by stamp transfer, and dried at 25°C for 12 hours to obtain a uniform smart electronic tattoo.

[0082] Example 6

[0083] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0084] Ti2C, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:3:1, wherein the lateral size of Ti2C was 0.6 μm and the thickness was 1.0 nm, the diameter of the 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose was 20 nm and the aspect ratio was 15, and the diameter of the silver nanowires was 20 nm and the aspect ratio was 15. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 hours to obtain a mixed slurry. The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and evacuated for 1 hour to remove bubbles. Subsequently, the mixed slurry was transferred to a metal sheet by 3D printing, and dried at 25°C for 12 hours to obtain a uniform smart electronic tattoo.

[0085] Example 7

[0086] A method for preparing a multifunctional intelligent electronic tattoo comprises the following steps:

[0087] Ti2C, 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose and silver nanowires were weighed in a weight ratio of 25:3:1, wherein the lateral size of Ti2C was 1.0 μm and the thickness was 1.0 nm, the diameter of the 2,2,6,6-tetramethylpiperidine-1-oxydione oxidized nanocellulose was 20 nm and the aspect ratio was 15, and the diameter of the silver nanowire was 20 nm and the aspect ratio was 15. After mixing and stirring evenly, the mixture was stirred at room temperature for 24 hours to obtain a mixed slurry. The obtained mixed slurry was placed in a vacuum bottle with a vacuum degree of -0.1 MPa and evacuated for 1 hour to remove bubbles. Subsequently, the mixed slurry was transferred to the polyurethane surface by 3D printing, and dried at 25°C for 12 hours to obtain a uniform smart electronic tattoo.

[0088] Example 8

[0089] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0090] The vacuumed mixed slurry is transferred to the fabric by screen printing. The remaining steps and parameters are the same as those in Example 1 to obtain a smart electronic tattoo. Figure 3 a in .

[0091] Example 9

[0092] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0093] The vacuumed mixed slurry is transferred to the rubber by screen printing. The remaining steps and parameters are the same as those in Example 1 to obtain the smart electronic tattoo. Figure 3 The b in.

[0094] Example 10

[0095] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0096] The vacuumed mixed slurry is transferred to the metal sheet by screen printing. The remaining steps and parameters are the same as those in Example 1 to obtain a smart electronic tattoo. Figure 3 c in.

[0097] Example 11

[0098] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0099] The vacuumed mixed slurry is transferred to the polyurethane surface by screen printing. The remaining steps and parameters are the same as those in Example 1 to obtain a smart electronic tattoo. Figure 3 The e in.

[0100] Example 12

[0101] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0102] The mixed slurry after vacuuming was transferred to A4 paper by direct writing. The remaining steps and parameters were the same as those in Example 1 to obtain a smart electronic tattoo. Figure 3 The f in.

[0103] Example 13

[0104] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0105] The vacuumed mixed slurry is transferred onto A4 paper using a stamp transfer method. The remaining steps and parameters are the same as in Example 1 to obtain a smart electronic tattoo. The obtained smart electronic tattoo pattern is Figure 3 The g in.

[0106] Example 14

[0107] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0108] The vacuumed mixed slurry is transferred to A4 paper by 3D printing. The remaining steps and parameters are the same as those in Example 1 to obtain a smart electronic tattoo. Figure 3 The i in .

[0109] Comparative Example 1

[0110] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0111] Without adding CNFs and AgNWs, the remaining steps and parameters were the same as in Example 1 to prepare a pure MXene electronic tattoo.

[0112] Comparative Example 2

[0113] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0114] Without adding AgNWs, the remaining steps and parameters were the same as in Example 1, and an electronic tattoo with a weight ratio of MXene to CNFs of 25:3 was prepared.

[0115] Comparative Example 3

[0116] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0117] Without adding CNFs, the remaining steps and parameters were the same as in Example 1, and an electronic tattoo with a weight ratio of MXene to AgNWs of 25:1 was prepared.

[0118] Comparative Example 4

[0119] A method for preparing a multifunctional intelligent electronic tattoo differs from Example 1 in that:

[0120] The A4 paper substrate was replaced with a silicon substrate, and the remaining steps and parameters were the same as in Example 1 to produce a smart electronic tattoo.

[0121] Technical effects:

[0122] The smart electronic tattoos prepared in Examples 1-14 and Comparative Examples 1-4 were subjected to rheological performance tests, multi-pattern design and applicable substrate tests, conductivity tests, temperature sensing performance tests, humidity sensing performance tests, tensile strain sensing performance tests, distance / angle perception tests, and material recognition performance tests. Specifically:

[0123] 1. Rheological properties test

[0124] The rheological properties of the smart inks prepared in Example 1 and Comparative Example 1 were studied using a rheometer (Physica MCR301). Figure 2 The rheological properties test diagram of the smart ink prepared in Example 1 and Comparative Example 1 shows that both the MXene / CNFs / AgNWs mixed slurry and the pure MXene ink have obvious non-Newtonian fluid shear thinning behavior, and after adding CNFs and AgNWs, the viscosity of the mixed slurry is significantly improved compared with the pure MXene ink, which ensures that the mixed slurry can be smoothly extruded, printed and quickly solidified in subsequent operations.

[0125] 2. Multi-patterning design and applicable substrate testing

[0126] The patterns are planned and designed in advance, and printing templates or stamps with different patterns are prepared. The electronic tattoos with different patterns are obtained using the preparation methods of Example 1 and Examples 8-14. Figure 3 According to the preparation method of Example 1 and Examples 8-14, the mixed slurry is transferred to different substrates (including fabric, rubber, metal sheet, A4 paper, polyurethane surface, etc.), and electronic tattoos with different patterns can be obtained after drying.

[0127] 3. Conductivity test

[0128] The electrical conductivity of the smart electronic tattoos prepared in Example 1 and Comparative Examples 1-2 at room temperature was studied using a comprehensive physical property measurement system (Quantum). Figure 4 This is a graph showing the conductivity test results of the smart electronic tattoos prepared in Example 1 and Comparative Examples 1-2. It can be seen that after the addition of CNFs, the conductivity of the MXene / CNFs electronic tattoo is significantly reduced, but after the addition of AgNWs, the conductivity of the MXene / CNFs / AgNWs electronic tattoo is significantly improved compared to the MXene / CNFs electronic tattoo.

[0129] 4. Temperature sensing performance test

[0130] The MXene / CNFs / AgNWs electronic tattoo was printed on the surface of a heating platform, and the change in resistance of the electronic tattoo during temperature change was monitored using an electrochemical workstation (CHI600E). Figure 5 This is a test result diagram of temperature sensing performed on the smart electronic tattoos prepared in Example 1 and Comparative Example 2. It can be seen from the figure that within the same temperature change range (30°C to 90°C), the MXene / CNFs / AgNWs electronic tattoo is more sensitive to temperature changes than the MXene / CNFs electronic tattoo, indicating that AgNWs plays an important role in temperature sensing.

[0131] 5. Humidity sensing performance test

[0132] The MXene / CNFs / AgNWs electronic tattoo was printed on the surface of a latex film and placed in a sealed glove box, and a humidifier was used to control the humidity changes in the box. Figure 6 This is a test result diagram of humidity sensing performed on the smart electronic tattoo prepared in Examples 1-3. It can be seen from the figure that within the same relative humidity change range (40% to 90%), the greater the amount of CNFs added, the greater the resistance change value of the MXene / CNFs / AgNWs electronic tattoo, indicating that CNFs play an important role in humidity sensing.

[0133] 6. Tensile strain sensing performance test

[0134] The MXene / CNFs / AgNWs electronic tattoo was printed on the surface of a polyurethane film to make a sensor. The sensor was stretched using a universal mechanical testing machine (Instron 5966), and the change in resistance of the sensor during the stretching process was monitored using an electrochemical workstation (CHI600E). Figure 7 This is a test result diagram of tensile strain sensing performed on the smart electronic tattoo prepared according to Example 1. It can be seen from the figure that the smart electronic tattoo sensor has different resistance change rates for different deformations, indicating its good sensing performance.

[0135] 7. Distance / angle perception test

[0136] The MXene / CNFs / AgNWs electronic tattoo was printed on the surface of a polyurethane film and fixed to a substrate. A modal exciter (SA-JZ020) was used to simulate a moving object, and an electrometer (Keithley 6514) was used to test the electrical output performance of the electronic tattoo at different distances and angles from the moving object. Figure 8 This is a test result diagram of distance perception conducted on the smart electronic tattoo prepared in Example 1. It can be seen from the figure that the output voltage values ​​of the smart electronic tattoo are different at different distances to the moving object, indicating that the smart electronic tattoo can accurately measure the distance between the moving object and the electronic tattoo. Figure 9 This is a test result diagram of the angle perception between the smart electronic tattoo prepared in Example 1 and a moving object. It can be seen from the figure that the output voltage values ​​of the smart electronic tattoo and the moving object are different at different angles, indicating that the smart electronic tattoo can accurately measure the angle between the moving object and the electronic tattoo.

[0137] 8. Material identification performance test

[0138] The mixed slurry obtained in Example 1 was transferred onto textile (cotton), rubber, metal sheet (Al), A4 paper, and polyurethane film surfaces (PET, PTFE, and Kapton) to obtain electronic tattoos, which were then fixed to substrates. These tattoos were then attached to the surface of an exciter, and an electrometer (Keithley 6514) was used to test the electrical output performance of the electronic tattoos when in contact with different substrates. Figure 10 This figure shows the material recognition test results of the smart electronic tattoo prepared by transferring the mixed slurry obtained in Example 1 onto different substrates. It can be seen from the figure that the output voltage values ​​of the smart electronic tattoo are different when it contacts substrates of different materials, indicating that the smart electronic tattoo can accurately identify different materials.

[0139] Through the above performance tests, it can be known that the smart electronic tattoo prepared by the method of the present invention not only has high conductivity, but also has excellent multifunctional sensing capabilities, including temperature sensing, humidity sensing, tensile strain sensing, distance and angle perception, and material recognition, etc., and also has good rheological properties.

[0140] The above description is only a preferred specific embodiment of the present invention, and the scope of protection of the present invention is not limited thereto. Any technician familiar with the technical field can make equivalent replacements or changes based on the technical solutions and inventive concepts of the present invention within the technical scope disclosed in the present invention, and these changes should be covered by the scope of protection of the present invention.

Claims

1. A multifunctional intelligent electronic tattoo, characterized in that: The smart electronic tattoo is prepared from MXene, nanocellulose and silver nanowires; wherein the weight ratio of the MXene, nanocellulose and silver nanowires is 25:(1-10):1; The MXene includes one or more of Ti3C2, Ta4C3, Nb2C and Ti2C in any proportion; the lateral size of the MXene is 0.3-1.2 μm and the thickness is 0.8-1.5 nm; The preparation method of the multifunctional smart electronic tattoo includes the following steps: uniformly mixing the MXene, nanocellulose and silver nanowires to obtain a mixed slurry, and then transferring the mixed slurry onto a substrate to obtain the smart electronic tattoo; the transfer method is one of direct writing, seal transfer, screen printing or 3D printing.

2. A multifunctional smart electronic tattoo according to claim 1, characterized in that: The nanocellulose is nanocellulose oxidized from 2,2,6,6-tetramethylpiperidine-1-oxydione; the diameter of the nanocellulose is 10-50 nm, and the aspect ratio is 10-100.

3. A multifunctional smart electronic tattoo according to claim 1, characterized in that: The silver nanowires have a diameter of 10-50 nm and an aspect ratio of 10-100.

4. The multifunctional smart electronic tattoo according to claim 1, characterized in that: Before the transfer, the mixed slurry was placed in a vacuum environment and evacuated for 1 hour, and the vacuum degree of the vacuum environment was -0.1 MPa.

5. The multifunctional smart electronic tattoo according to claim 1, characterized in that: The substrate is one of fabric, rubber, metal sheet, A4 paper or polyurethane surface.

6. Use of a multifunctional intelligent electronic tattoo according to any one of claims 1 to 5 in the preparation of epidermal electronics and intelligent prostheses.

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