In-situ conductive biogel and preparation method thereof

Abstract

The invention provides in-situ conductive biogel and a preparation method thereof. The in-situ conductive biogel is prepared from the following raw materials: gelatin, a conductive polymer, a deep eutectic solvent and deionized water, the mass ratio of the gelatin to the conductive polymer to the deep eutectic solvent to the deionized water is (1-100): 1: (0.5-100): (1-300). The in-situ conductive biogel provided by the invention has the advantages of high mechanical property, strong adhesive force, high conductivity and low signal-to-noise ratio. The in-situ conductive biogel provided by the invention is simple in preparation method, low in raw material cost, pollution-free in preparation process and beneficial to large-scale production, and has huge industrial application potential.

Description

Technical Field

[0001] The present invention relates to the technical field of medical conductive materials, and in particular to an in-situ conductive biogel and a preparation method thereof. Background Art

[0002] Soft conductive materials play a vital role in smart medical devices, energy applications, and brain-computer interfaces. In healthcare, typical applications of soft conductive materials involve the acquisition of electrophysiological signals, such as electrocardiogram (ECG) and electromyogram (EMG) detection.

[0003] Common soft conductive materials include conductive elastomers, hydrogels, organic hydrogels, etc. However, the current formulations of these conductive gel materials result in the formation of solids, which often results in a weak interface between the conductive material and the skin, insufficient bonding, and thus a low signal-to-noise ratio (SNR).

[0004] In addition, conductive gels in an initial liquid state effectively solve the problem of insufficient adhesion in solid gels. However, after gelation, these conductive gels usually face problems such as fragility, weak adhesion to the skin, and low signal-to-noise ratio. These factors significantly affect accurate and long-term detection, especially under conditions involving mechanical stress, such as motion detection through electromyographic signals.

[0005] Therefore, an innovative formulation and method to create an in situ gelling liquid biogel with high mechanical properties, strong adhesion, high conductivity, and low signal-to-noise ratio is urgently needed. Such a biogel will be crucial for enhancing the detection of electrocardiogram (ECG) and electromyogram (EMG) signals. Summary of the invention

[0006] In view of the deficiencies in the prior art, the object of the present invention is to provide an in situ conductive biogel with high mechanical properties, strong adhesion, high conductivity and low signal-to-noise ratio, which is essential for enhancing the detection of electrocardiogram (ECG) and electromyogram (EMG) signals.

[0007] The first aspect of the present invention provides an in situ conductive biogel prepared from the following raw materials: gelatin, a conductive polymer, a deep eutectic solvent, and deionized water; the mass ratio of the gelatin, the conductive polymer, the deep eutectic solvent, and the deionized water is (1-100):1:(0.5-100):(1-300).

[0008] In one embodiment of the present invention, the conductive polymer is at least one of PEDOT:PSS, PANI, and PPy.

[0009] In one embodiment of the present invention, the conductive polymer is PEDOT:PSS.

[0010] In one embodiment of the present invention, the deep eutectic solvent comprises a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is at least one of glycerol, urea, ethylene glycol, vanillic acid, sebacic acid, acetamide, phenol, benzamide, benzoic acid, malonic acid, thiourea, succinic acid, 1,3-dimethylurea, oxalic acid, lactic acid, citric acid, glucose, 1-methylurea, 1,1-dimethylurea, 1,4-butanediol, capric acid, fructose, triethylene glycol, dodecanoic acid, menthol, thymol, and 1-naphthol;

[0011] The hydrogen bond acceptor is at least one of choline chloride, lactic acid, choline carbonate, 2-(chlorocarbonyloxy)-N,N,N-trimethylethyleneamine chloride, benzyltriphenylphosphonium chloride, lidocaine, proline, histidine, nicotinic acid, betaine and tetramethylammonium chloride.

[0012] In one embodiment of the present invention, the deep eutectic solvent consists of glycerol and choline chloride.

[0013] In one embodiment of the present invention, the mass ratio of gelatin to conductive polymer is (1-100):1.

[0014] In one embodiment of the present invention, the mass ratio of glycerol to gelatin is 1:(0.1-10).

[0015] In one embodiment of the present invention, the mass ratio of glycerol to choline chloride is 1:(0.1-10).

[0016] The second aspect of the present invention provides a method for preparing the above-mentioned in situ conductive biogel, comprising the following steps:

[0017] S1, mixing a hydrogen bond donor, a conductive polymer and deionized water in a deep eutectic solvent to obtain a first mixture;

[0018] S2, introducing gelatin into the first mixture, dissolving and mixing at high temperature to obtain a second mixture;

[0019] S3, adding the hydrogen bond acceptor in the deep eutectic solvent to the second mixture, placing it in a high temperature oven for 4-8 hours to eliminate residual bubbles, and obtaining a third mixture;

[0020] S4. The obtained third mixture is placed in an oven for drying for 4-8 hours to remove moisture and obtain an in-situ biogel.

[0021] In one embodiment of the present invention, step S1 specifically comprises: mixing the hydrogen bond donor in the deep eutectic solvent with deionized water, and then adding the hydrogen bond donor in the deep eutectic solvent to mix, to obtain a first mixture;

[0022] or,

[0023] Step S1 specifically includes: mixing a conductive polymer with deionized water, and then adding a hydrogen bond donor in a deep eutectic solvent to mix, so as to obtain a first mixture.

[0024] Compared with the prior art, the embodiments of the present invention have the following beneficial effects:

[0025] 1. The in situ conductive biogel provided by one embodiment of the present invention has high mechanical properties, strong adhesion, high conductivity and low signal-to-noise ratio, which is crucial for enhancing the detection of electrocardiogram (ECG) and electromyogram (EMG) signals.

[0026] 2. The in-situ conductive biogel provided by one embodiment of the present invention has better performance than existing commercial biogels in terms of electrocardiogram (ECG) and electromyogram (EMG) signal detection. Obviously, the in-situ biogel provided by the present invention has great industrial application potential.

[0027] 3. In the in-situ conductive biogel provided by one embodiment of the present invention, the conductive polymer is PEDOT:PSS, the hydrogen bond donor is glycerol, and the hydrogen bond acceptor is choline chloride. PEDOT:PSS helps to improve electronic conductivity, while the combination of choline chloride and glycerol forms a deep eutectic solvent, thereby establishing ionic conductivity. Gelatin contributes to the in-situ gel properties and adhesion. In particular, the semi-interpenetrating network formed by PEDOT:PSS and gelatin enhances mechanical strength, and these combined properties significantly improve the efficiency of electrocardiogram (ECG) and electromyogram (EMG) detection.

[0028] 4. The in-situ conductive biogel preparation method provided by one embodiment of the present invention is simple, has low-cost raw materials, and has a pollution-free manufacturing process, which is conducive to large-scale production and has great industrial application potential. BRIEF DESCRIPTION OF THE DRAWINGS

[0029] In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the following briefly introduces the drawings required for describing the embodiments. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative work. In the drawings:

[0030] Figure 1 The in-situ conductive biogel prepared in Example 1 is shown in FIG. 1 just taken out of the oven and one minute after being taken out;

[0031] Figure 2 The figure is a graph showing the mechanical properties test results of the in-situ conductive biogel prepared in Example 1; wherein, Figure 2 A is the tensile strength diagram of in situ biogels with different contents of deep eutectic solvent (0.37, 0.75, 1.12), Figure 2 B is the toughness diagram, Figure 2 C is the tensile modulus diagram, Figure 2 D is the stress-strain curve, Figure 2 E is a diagram of using the in situ biogel in Example 1 to pull a one kilogram weight;

[0032] Figure 3 This is a graph showing the in-situ adhesion performance test results of the in-situ conductive biogel prepared in Example 1;

[0033] Figure 4 The figure is a test result of the adhesion between the in-situ conductive biogel prepared in Example 1 and the pig skin and the electrode; wherein, Figure 4 A is the adhesion strength diagram of in-situ biogels with different contents of deep eutectic solvent on pig skin. Figure 4 B is the adhesion strength diagram with the electrode, Figure 4 C is the adhesion strength diagram with pig skin in the case of sodium chloride solution, Figure 4 D is the adhesion strength diagram with the electrode in the case of sodium chloride solution;

[0034] Figure 5 This is a data graph of an electrocardiogram (ECG) signal test using the in-situ conductive biogel provided in Example 1, wherein: Figure 5 A is a test diagram of a commercial electrode sheet and an electrode prepared by in-situ biogel provided in Example 1, Figure 5 B is a graph showing the measured signal-to-noise ratio using the commercial patch and the in situ biogel provided in Example 1, as well as the signal-to-noise ratio after long-term application;

[0035] Figure 6 This is a data graph of electrocardiogram and electromyogram (EMG) testing using the in situ conductive biogel provided in Example 1, wherein: Figure 6 A is a graph showing the electromyographic signal of the electrode arm prepared by the commercial patch and the in situ biogel provided in Example 1 under multiple grasping conditions, as well as the electromyographic signal graph in the presence of sodium chloride solution. Figure 6 B is the corresponding myoelectric noise ratio diagram. DETAILED DESCRIPTION

[0036] The present invention is described in detail below in conjunction with specific embodiments. The following embodiments will help those skilled in the art to further understand the present invention, but are not intended to limit the present invention in any form. It should be noted that, for those of ordinary skill in the art, several changes and improvements can also be made without departing from the concept of the present invention. These all belong to the protection scope of the present invention.

[0037] The invention provides an in-situ conductive biogel, which is prepared from the following raw materials: gelatin, conductive polymer, deep eutectic solvent, and deionized water.

[0038] In order to provide electronic conductivity, the conductive polymer PEDOT:PSS is added to the in-situ conductive biogel material system of the present invention to help improve the electronic conductivity. Alternatively, the conductive polymer in the present invention can also be PANI or PPy.

[0039] In order to provide ionic conductivity, the present invention introduces a deep eutectic solvent. The deep eutectic solvent includes a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is at least one of glycerol, urea, ethylene glycol, vanillic acid, sebacic acid, acetamide, phenol, benzamide, benzoic acid, malonic acid, thiourea, succinic acid, 1,3-dimethylurea, oxalic acid, lactic acid, citric acid, glucose, 1-methylurea, 1,1-dimethylurea, 1,4-butanediol, capric acid, fructose, triethylene glycol, dodecanoic acid, menthol, thymol, and 1-naphthol; and the hydrogen bond acceptor is at least one of choline chloride, lactic acid, choline carbonate, 2-(chlorocarbonyl)-N,N,N-trimethylethyleneamine chloride, benzyltriphenylphosphonium chloride, lidocaine, proline, histidine, nicotinic acid, betaine, and tetramethylammonium chloride.

[0040] In one embodiment, glycerol acts as a hydrogen bond donor and choline chloride acts as a hydrogen bond acceptor. In another embodiment, the hydrogen bond donor may be urea and the hydrogen bond acceptor may be choline fluoride. In another embodiment, the hydrogen bond donor may be ethylene glycol and the hydrogen bond acceptor may be lactic acid. In another embodiment, the hydrogen bond donor may be vanillic acid and the hydrogen bond acceptor may be choline carbonate.

[0041] In one embodiment, the conductive polymer is PEDOT:PSS, the hydrogen bond donor is glycerol, and the hydrogen bond acceptor is choline chloride. PEDOT:PSS contributes to electronic conductivity, while the combination of choline chloride and glycerol forms a deep eutectic solvent, thereby establishing ionic conductivity. Gelatin contributes to in-situ gel properties and adhesion. In particular, the semi-interpenetrating network formed by PEDOT:PSS and gelatin enhances mechanical strength, and these combined properties significantly improve the efficiency of electrocardiogram (ECG) and electromyogram (EMG) detection.

[0042] The in-situ conductive biogel provided by the present invention is in liquid state at a temperature exceeding 40°C.

[0043] The present invention provides an in-situ conductive biogel. In the present invention, "in-situ" means that in actual use, liquid is usually applied to the skin, and the liquid gel undergoes a gelation process and adheres to the skin in the form of a soft biogel.

[0044] In one embodiment, the weight ratio of gelatin to PEDOT:PSS disclosed herein is 100: 1. In another embodiment, the weight ratio of gelatin to PEDOT:PSS is 50: 1. In another embodiment, the weight ratio of gelatin to PEDOT:PSS is 25: 1. In another embodiment, the weight ratio of gelatin to PEDOT is from 1: 1 to 100: 1.

[0045] In one embodiment, the weight ratio of glycerol to water disclosed herein is 1:3. In one embodiment, the weight ratio of glycerol to water is 1:2. In another example, the weight ratio of glycerol to water is 1:1. In another embodiment, the weight ratio of glycerol to water is 1:0.5. In another example, the weight ratio of glycerol to water is 1:5. In another embodiment, the weight ratio of glycerol to water is 1:0 to 1:10.

[0046] In one embodiment, the molar ratio of glycerol to choline chloride disclosed herein is 1: 1. In another embodiment, the molar ratio of glycerol to choline chloride is 1: 2. In another embodiment, the molar ratio of glycerol to choline chloride is 1: 0.5. In another embodiment, the molar ratio of glycerol to choline chloride is 1: 0.25.

[0047] In one embodiment, the weight ratio of glycerin to gelatin disclosed herein is 1:4. In one embodiment, the weight ratio of glycerin to gelatin is 1:2. In another example, the weight ratio of glycerin to gelatin is 1:1. In another embodiment, the weight ratio of glycerin to gelatin is 1:0.5. In another embodiment, the weight ratio of glycerin to gelatin is 1:5.

[0048] In the present invention, "high temperature" refers to a temperature exceeding the liquid-solid transition temperature. Usually, the temperature exceeds 40°C, and may also exceed 37°C.

[0049] The present invention is further described below in conjunction with specific embodiments:

[0050] Example 1

[0051] This embodiment provides an in situ conductive biogel, which is prepared by the following raw materials: gelatin, conductive polymer, deep eutectic solvent, and deionized water. In this embodiment, the mass ratio of gelatin, conductive polymer, deep eutectic solvent, and deionized water is 2:0.02:1.75:3.

[0052] The conductive polymer in this embodiment is PEDOT:PSS, and the PEDOT:PSS in this embodiment is purchased from Sigma.

[0053] The deep eutectic solvent in this embodiment includes a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is glycerol and the hydrogen bond acceptor is choline chloride.

[0054] The gelatin and glycerol in this example were purchased from Sigma, and choline chloride was purchased from Macklin Inc.

[0055] The method for preparing the in situ conductive biogel in this embodiment comprises the following steps:

[0056] S1, mixing glycerol and deionized water evenly, and then mixing with PEDOT:PSS to obtain a first mixture;

[0057] S2, introducing gelatin into the first mixture, dissolving and mixing at high temperature to obtain a second mixture;

[0058] S3, adding choline chloride to the second mixture, putting it into a sealed bottle, and placing it in a high-temperature oven for 8 hours to eliminate residual bubbles, thereby obtaining a third mixture;

[0059] S4. Put the obtained third mixture into an oven, open the cap of the sealed bottle, and dry it for 4 hours to remove moisture, thereby obtaining an in-situ conductive biogel.

[0060] Figure 1 The state diagram of the in-situ conductive biogel prepared in this example when it is just taken out of the oven and one minute after it is taken out, as shown in FIG. Figure 1 As shown, when the in situ conductive biogel obtained in this example is transferred from the oven to the environment, the in situ conductive biogel will solidify rapidly within 1 minute.

[0061] Example 2

[0062] This embodiment provides an in situ conductive biogel, which is prepared by the following raw materials: gelatin, conductive polymer, deep eutectic solvent, and deionized water. In this embodiment, the mass ratio of gelatin, conductive polymer, deep eutectic solvent, and deionized water is 2:0.02:0.87:3.5.

[0063] The conductive polymer in this embodiment is PEDOT:PSS, and the PEDOT:PSS in this embodiment is purchased from Sigma.

[0064] The deep eutectic solvent in this embodiment includes a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is glycerol and the hydrogen bond acceptor is choline chloride.

[0065] The gelatin and glycerol in this example were purchased from Sigma, and choline chloride was purchased from Macklin Inc.

[0066] The method for preparing the in situ conductive biogel in this embodiment comprises the following steps:

[0067] S1, mixing glycerol and deionized water evenly, and then mixing with PEDOT:PSS to obtain a first mixture;

[0068] S2, introducing gelatin into the first mixture, dissolving and mixing at high temperature to obtain a second mixture;

[0069] S3, adding choline chloride to the second mixture, putting it into a sealed bottle, and placing it in a high-temperature oven for 8 hours to eliminate residual bubbles, thereby obtaining a third mixture;

[0070] S4. Put the obtained third mixture into an oven, open the cap of the sealed bottle, and dry it for 4 hours to remove moisture, thereby obtaining an in-situ conductive biogel.

[0071] Example 3

[0072] This embodiment provides an in situ conductive biogel, which is prepared by the following raw materials: gelatin, conductive polymer, deep eutectic solvent, and deionized water. In this embodiment, the mass ratio of gelatin, conductive polymer, deep eutectic solvent, and deionized water is 2:0.02:2.62:2.5.

[0073] The conductive polymer in this embodiment is PEDOT:PSS, and the PEDOT:PSS in this embodiment is purchased from Sigma.

[0074] The deep eutectic solvent in this embodiment includes a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is glycerol and the hydrogen bond acceptor is choline chloride.

[0075] The gelatin and glycerol in this example were purchased from Sigma, and choline chloride was purchased from Macklin Inc.

[0076] The method for preparing the in situ conductive biogel in this embodiment comprises the following steps:

[0077] S1, mixing glycerol and deionized water evenly, and then mixing with PEDOT:PSS to obtain a first mixture;

[0078] S2, introducing gelatin into the first mixture, dissolving and mixing at high temperature to obtain a second mixture;

[0079] S3, adding choline chloride to the second mixture, putting it into a sealed bottle, and placing it in a high-temperature oven for 8 hours to eliminate residual bubbles, thereby obtaining a third mixture;

[0080] S4. Put the obtained third mixture into an oven, open the cap of the sealed bottle, and dry it for 4 hours to remove moisture, thereby obtaining an in-situ conductive biogel.

[0081] Example 4

[0082] This embodiment provides an in-situ conductive biogel, which is prepared from the following raw materials: gelatin, a conductive polymer, a deep eutectic solvent, and deionized water.

[0083] The conductive polymer in this embodiment is PEDOT:PSS, and the PEDOT:PSS in this embodiment is purchased from Sigma.

[0084] The deep eutectic solvent in this embodiment includes a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is glycerol and the hydrogen bond acceptor is choline chloride.

[0085] Wherein, the mass ratio of glycerol to water in this embodiment is 1:3.

[0086] Wherein, the mass ratio of glycerol to gelatin in this embodiment is 1:2.

[0087] Wherein, the mass ratio of gelatin to PEDOT:PSS in this embodiment is 10:1.

[0088] Wherein, the molar ratio of glycerol to choline chloride in this embodiment is 1:1.

[0089] The gelatin and glycerol in this example were purchased from Sigma, and choline chloride was purchased from Macklin Inc.

[0090] The method for preparing the in situ conductive biogel in this embodiment comprises the following steps:

[0091] S1, mixing glycerol and deionized water evenly, and then mixing with PEDOT:PSS to obtain a first mixture;

[0092] S2, introducing gelatin into the first mixture, dissolving and mixing at high temperature to obtain a second mixture;

[0093] S3, adding choline chloride to the second mixture, putting it into a sealed bottle, and placing it in a high-temperature oven for 8 hours to eliminate residual bubbles, thereby obtaining a third mixture;

[0094] S4. Put the obtained third mixture into an oven, open the cap of the sealed bottle, and dry it for 4 hours to remove moisture, thereby obtaining an in-situ conductive biogel.

[0095] Comparative Example 1

[0096] The commercial conductive hydrogel provided in this comparative example is a commercial biological gel, namely, Jinnot ECG conductive paste, and the utilization ratio is 0.75.

[0097] Experimental example

[0098] In this experimental example, the performance of the in situ conductive biogels obtained in Examples 1-3 and the commercial conductive hydrogel provided in Comparative Example 1 was tested.

[0099] Among them, it should be noted that Figure 2 A. Figure 2 B. Figure 2 C. Figure 2 D. Figure 4 A. Figure 4 B. Figure 4 C. Figure 4 In D, In-situ0.37DE gela / P:P refers to the in situ conductive biogel prepared in Example 2, In-situ 0.75DE gela / P:P refers to the in situ conductive biogel prepared in Example 1, and In-situ1.12DE gela / P:P refers to the in situ conductive biogel prepared in Example 3. Figure 4 A. Figure 4 B. Figure 4 C. Figure 4 D. Figure 6 In A and 6B, the commercial biogel refers to the in situ gel in Comparative Example 1. Figure 5 The commercial biogel electrode in A refers to the commercial biogel electrode prepared from the biogel in the comparative example. Figure 5 The in-situ gel electrode in B refers to the in-situ gel electrode prepared by the in-situ conductive biogel prepared in Example 1.

[0100] Mechanical property test: The test method is as follows: clamp the prepared biogel on the two end clamps of the mechanical testing machine and stretch it axially to obtain the mechanical property results of the biogel. Figure 2 Figure 2 is the test result of mechanical properties of biogel; Figure 2 A is a graph of tensile strength of in-situ conductive biogels (Example 1, Example 2, Example 3) with different contents of deep eutectic solvent (0.37, 0.75, 1.12), Figure 2 B is the toughness diagram of the in-situ conductive biogel (Example 1, Example 2, Example 3), Figure 2 C is the tensile modulus diagram of the in situ conductive biogel (Example 1, Example 2, Example 3), Figure 2 D is the stress-strain curve of the in-situ conductive biogel (Example 1, Example 2, Example 3), Figure 2 E is a diagram of using the in-situ biogel in Example 1 to pull a one-kilogram weight; Figure 2 A shows that the biogels prepared in Examples 1, 2, and 3 all have high tensile strength; Figure 2 B shows that the biogels prepared in Examples 1, 2, and 3 all have good toughness; Figure 2 C shows that the elastic modulus of the biogels prepared in Examples 1, 2, and 3 are all less than 1 MPa, which is close to the elastic modulus of the skin. Figure 2 D shows that the biogels prepared in Examples 1, 2, and 3 all have good strain properties; Figure 2E It can be seen that the biogel prepared in Example 1 has good tensile properties. As mentioned above, the in situ conductive biogels provided in Examples 1-3 have higher tensile strengths. In contrast, the tensile strength of the common commercial conductive hydrogels provided in the comparative example is less than 1 MPa. The biogels provided in Examples 1-3 also exhibit a modulus similar to that of the skin (approximately <1 MPa), allowing deformation with the deformation of the skin.

[0101] In-situ adhesion performance test, the test method is as follows: the gel material is coated between two pieces of pig skin (electrodes). After adhesion, force is applied from both ends to stretch until the pig skin is separated from the material, and the required force is recorded to determine the adhesion strength. Figure 3 This is a graph showing the in-situ adhesion performance test results of the biogel in Example 1. Due to the characteristics of the in-situ gel, the surface of the gel prepared in Example 1 presents the same texture as the skin, highlighting the excellent interface between the biogel and the skin.

[0102] Figure 4 The graphs are the adhesion test results of the biogels, pig skin and electrodes in Examples 1-3 and Comparative Examples, wherein: Figure 4 A is the adhesion strength diagram of in-situ biogels with different contents of deep eutectic solvent on pig skin. Figure 4 B is the adhesion strength diagram with the electrode, Figure 4 C is the adhesion strength diagram with pig skin in the case of sodium chloride solution, Figure 4 D is the adhesion strength diagram with the electrode in the case of sodium chloride solution; Figure 4 A shows that the biogels prepared in Examples 1-3 have much higher adhesion strength than commercial biogels, exceeding 35-140 times; Figure 4 B shows that the adhesion strength of the biogels prepared in Examples 1-3 to the electrodes is 20-150 times that of the commercial biogels. Figure 4 C shows that the biogels prepared in Examples 1-3 still have a high adhesion strength to the skin even in a sodium chloride solution; Figure 4 D It can be seen that the biogel prepared in Examples 1-3 still has a high adhesion strength to the electrode even in a sodium chloride solution; In summary, the adhesion strength of the in-situ conductive biogel prepared in Examples 1-3 on the skin and the electrode is better than that of the commercial biogel (Comparative Example 1). The adhesion strength of the in-situ conductive biogel provided in Examples 1-3 on the skin and the electrode exceeds that of the commercial biogel (Comparative Example 1).

[0103] Electrocardiogram (ECG) signal test, the test steps are as follows: Figure 5 As shown, two electrodes are placed on the left and right wrists, and the reference electrode is placed on the right ankle. After connecting to the ECG device, the measurement can be done; Figure 5 This is a data graph of an electrocardiogram (ECG) signal test performed using the in situ conductive biogel provided in Example 1, wherein: Figure 5 A is a test diagram of a commercial electrode sheet and an electrode prepared by in-situ biogel provided in Example 1, Figure 5 B is the measured signal-to-noise ratio using the commercial patch and the in situ biogel provided in Example 1, as well as the signal-to-noise ratio after long-term application. Figure 5 From the electrocardiogram test of B, it can be seen that the in situ conductive biogel provided in Example 1 shows a higher signal-to-noise ratio (SNR) than the commercial biogel (comparative example). In addition, even after 48 hours of use, the SNR of the in situ conductive biogel still remains at a high level, surpassing the performance of the commercial gel after 24 hours of use.

[0104] Electromyography (EMG) signal test, the test steps are as follows: During the test, stick the patch on the forearm, connect the patch and the electromyography device, and make a fist once to generate a signal. Figure 6 The commercial patch here refers to the incentive Figure 1 Disposable ECG electrodes; Figure 6 This is a data graph of electrocardiogram and electromyogram (EMG) testing using the in situ conductive biogel provided in Example 1, wherein: Figure 6 A is a graph showing the electromyographic signal of the electrode arm prepared by the commercial patch and the in situ biogel provided in Example 1 under multiple grasping conditions, as well as the electromyographic signal graph in the presence of sodium chloride solution. Figure 6 B is the corresponding myoelectric noise ratio diagram. Figure 6 It can be seen that the in situ conductive biogel provided in Example 1 exhibits superior signal quality and higher signal-to-noise ratio (SNR) than commercial gel in electromyography (EMG) signal testing, even after being soaked in a NaCl solution simulating sweat conditions. This highlights its great application potential in EMG testing.

[0105] The above describes the specific embodiments of the present invention. It should be understood that the present invention is not limited to the above specific embodiments, and those skilled in the art can make various changes or modifications within the scope of the claims, which does not affect the essence of the present invention. In the absence of conflict, the embodiments of the present application and the features in the embodiments can be combined with each other arbitrarily.

Claims

1. An in situ conductive biogel, characterized in that: The invention is prepared from the following raw materials: gelatin, conductive polymer, deep eutectic solvent, and deionized water; the mass ratio of the gelatin, conductive polymer, deep eutectic solvent, and deionized water is (1-100):1:(0.5-100):(1-300).

2. The in situ conductive biogel according to claim 1, characterized in that: The conductive polymer is at least one of PEDOT:PSS, PANI and PPy.

3. The in situ conductive biogel according to claim 2, characterized in that: The conductive polymer is PEDOT:PSS.

4. The in situ conductive biogel according to claim 1, characterized in that: The deep eutectic solvent comprises a hydrogen bond donor and a hydrogen bond acceptor, wherein the hydrogen bond donor is at least one of glycerol, urea, ethylene glycol, vanillic acid, sebacic acid, acetamide, phenol, benzamide, benzoic acid, malonic acid, thiourea, succinic acid, 1,3-dimethylurea, oxalic acid, lactic acid, citric acid, glucose, 1-methylurea, 1,1-dimethylurea, 1,4-butanediol, capric acid, fructose, triethylene glycol, dodecanoic acid, menthol, thymol, and 1-naphthol; The hydrogen bond acceptor is at least one of choline chloride, lactic acid, choline carbonate, 2-(chlorocarbonyloxy)-N,N,N-trimethylethyleneamine chloride, benzyltriphenylphosphonium chloride, lidocaine, proline, histidine, nicotinic acid, betaine and tetramethylammonium chloride.

5. The in situ conductive biogel according to claim 4, characterized in that: The deep eutectic solvent consists of glycerol and choline chloride.

6. The in situ conductive biogel according to claim 5, characterized in that: The mass ratio of the gelatin to the conductive polymer is (1-100):

1.

7. The in situ conductive biogel according to claim 6, characterized in that: The mass ratio of the glycerol to the gelatin is 1:(0.1-10).

8. The in situ conductive biogel according to claim 7, characterized in that: The mass ratio of the glycerol to the choline chloride is 1:(0.1-10).

9. The method for preparing the in situ conductive biogel according to any one of claims 1 to 8, characterized in that: The following steps are involved: S1, mixing a hydrogen bond donor, a conductive polymer and deionized water in a deep eutectic solvent to obtain a first mixture; S2, introducing gelatin into the first mixture, dissolving and mixing at high temperature to obtain a second mixture; S3, adding the hydrogen bond acceptor in the deep eutectic solvent to the second mixture, placing it in a high temperature oven for 4-8 hours to eliminate residual bubbles, and obtaining a third mixture; S4. The obtained third mixture is placed in an oven for drying for 4-8 hours to remove moisture and obtain an in-situ biogel.

10. The method for preparing the in situ conductive biogel according to claim 9, characterized in that: Step S1 specifically comprises: mixing the hydrogen bond donor in the deep eutectic solvent with deionized water, and then adding the hydrogen bond donor in the deep eutectic solvent to mix, to obtain a first mixture; or, Step S1 specifically includes: mixing a conductive polymer with deionized water, and then adding a hydrogen bond donor in a deep eutectic solvent to mix, so as to obtain a first mixture.

Images