阅读说明：本技术 一种柔性可拉伸的自粘附体表电极及其制备方法 (Flexible and stretchable self-adhesion body surface electrode and preparation method thereof ) 是由 胡本慧 陈士晟 唐文杰 周宇轩 尹思梦 于 2020-11-19 设计创作，主要内容包括：本发明涉及一种柔性可拉伸的自粘附体表电极及其制备方法,一种柔性可拉伸的自粘附体表电极,包括柔性可拉伸导电膜、电极引线以及导电银胶,将水喷涂在皮肤表面使其湿润,电极可以自主粘附在皮肤上,电极引线的一端连接导电银胶,另一端连接后级的检测设备；本发明还涉及一种柔性可拉伸的自粘附体表电极的制备方法,使用金属纳米线作为导电介质,混合在聚合物材料中形成导电膜,使其与形状不规则的皮肤接触,提高电极的界面导电能力,而且通过改变导电膜的尺寸,可以任意控制电极的贴附面积和电极形状,从而适应各种应用场合。本发明具有电极柔性和可拉伸性强,有利于与皮肤共形贴附,使用方便,信号质量好等优点。(The invention relates to a flexible stretchable self-adhesive body surface electrode and a preparation method thereof, the flexible stretchable self-adhesive body surface electrode comprises a flexible stretchable conductive film, an electrode lead and conductive silver colloid, water is sprayed on the surface of skin to moisten the skin surface, the electrode can be adhered to the skin automatically, one end of the electrode lead is connected with the conductive silver colloid, and the other end of the electrode lead is connected with a post-stage detection device; the invention also relates to a preparation method of the flexible and stretchable self-adhesion body surface electrode, which uses the metal nano-wire as a conductive medium to be mixed in a polymer material to form a conductive film so as to contact with the skin with irregular shape, thereby improving the interface conductive capability of the electrode, and the attachment area and the electrode shape of the electrode can be controlled at will by changing the size of the conductive film, thereby being suitable for various application occasions. The invention has the advantages of strong flexibility and stretchability of the electrode, convenient use, good signal quality and the like, and is beneficial to conformal attachment with skin.)

1. A flexible stretchable self-adhesive watch electrode consisting essentially of: flexible stretchable conductive film (1), electrode lead (2) and conductive silver adhesive (3), its characterized in that: the flexible stretchable conductive film (1) is directly contacted with the skin, the electrode lead (2) is covered on the flexible stretchable conductive film (1) through the conductive silver adhesive (3), one end of the electrode lead (2) is connected with the flexible stretchable conductive film (1), the other end of the electrode lead is connected with a rear-stage detection device, and the flexible stretchable conductive film (1), the electrode lead (2) and the conductive silver adhesive (3) jointly form an electrode plate.

2. A flexible stretchable self-adhesive watch electrode according to claim 1, characterised in that: the flexible stretchable conductive film (1) is formed by taking metal nanowires as a conductive material, dispersing the metal nanowires in a solution containing a polymer, evaporating and freely depositing the metal nanowires to form the conductive film, and is used for testing an electric signal of a target test position on the body surface of a tested person.

3. A flexible stretchable self-adhesive watch electrode according to claim 2, characterised in that: in the process of forming the conductive film, the polymer used comprises polyvinyl alcohol (PVA), polyvinylidene fluoride (PVDF) and polyurethane.

4. A flexible stretchable self-adhesive watch electrode according to claim 1, characterised in that: in the flexible stretchable conductive film (1), the metal nanowires are gold and silver nanowires.

5. A flexible stretchable self-adhesive watch electrode according to claim 1, characterised in that: the electrode lead (2) is made of conductive copper foil and an additional insulating layer.

6. A preparation method of a flexible and stretchable self-adhesion body surface electrode is characterized by comprising the following steps:

step 1, adding 200-400 mg of polyvinylpyrrolidone (PVP) and 100-200 mL of ethylene glycol into a round-bottom flask, and heating the mixture to 175 ℃; after PVP is completely dispersed, 500-1000 mu L of 4mM CuCl is added₂·2H₂O solution; after 10 minutes, dropwise adding 10-50 mL of 0.095M AgNO₃A solution; after the reaction is kept for 30 minutes, washing the synthesized Ag nanowire for many times to remove redundant PVP; preparing Ag nanowires;

step 2, mixing 100-200 mL of deionized water, 5-10 mL of NaOH (0.2M) solution and 1-2 mL of HAuCl₄(0.25M) solution and 100-150 mL of Na₂SO₃The (0.01M) solution is sequentially added into a 500mL flat-bottom beaker and uniformly mixed to be used as an Au growth solution; in a beaker, adding 300-400 mL of H₂O, 100mg Ag nanowire, 50-100 mL PVP (5 wt%, MW 54000) solution, 10-20 mL L-Ascorbic acid (L-AA) (0.5M) solution, 10-20 mL NaOH (0.5M), 3-5 mL Na₂SO₃Mixing the (0.1M) solution and the prepared Au growth solution to prepare a reaction solution; the mixture solution was allowed to react at 30 ℃ for 12 hours; finally, the Au @ Ag nanowires are collected through centrifugation and washed by deionized water and ethanol;

step 3, as shown in FIG. 4, manufacturing a mold (6), adding 20mL of deionized water, 300-500 mg of PVA and 10 mu L of Hexamethylene Diisocyanate (HDI) into a flat-bottom beaker, and magnetically stirring for 4h at 60 ℃ to obtain a cross-linked PVA solution; mixing the Au @ Ag nanowire with a PVA solution according to a certain proportion to obtain conductive paste (5); pouring 40 mu L of prepared conductive slurry (5) into a mould (6); the conductive film (7) is removed after the solvent has completely evaporated.

7. A method of making a flexible stretchable self-adherent body surface electrode according to claim 6, further comprising: PVP molecular weight 360k was used when PVP and ethylene glycol were added to the round bottom flask.

8. A method of making a flexible stretchable self-adherent body surface electrode according to claim 6, further comprising: the dimensions of the produced mold were 10mm × 10mm × 0.5 mm.

Technical Field

The invention relates to the technical field of medical equipment, in particular to a flexible and stretchable self-adhesion body surface electrode and a preparation method thereof.

Background

With the development and progress of society, the related biomedical disciplines are rapidly developed, and the requirements of scientific researchers and medical workers on the acquisition technology of bioelectricity signals are more and more strong. Typically, the in vivo electrical potentials of a human or other animal are measured and recorded. In addition, electrical skin stimulation is also a frequently used method of adjuvant therapy in clinical practice. In the above methods, both measurement and stimulation need to be performed by contacting the living body with an appropriate electrode to transmit an electric signal. The body surface electrode has the advantages of no wound, convenient use and the like, and is widely used in clinic and scientific research, such as: measuring myoelectric and electrocardio signals; functional electrical stimulation assists in treating hemiplegia patients; collecting brain electricity to identify emotion.

Currently, body surface electrodes are mainly classified into dry electrodes and wet electrodes. The wet electrode generally uses conductive paste or hydrogel materials, and has obviously poor performance after water loss and is airtight. The dry electrode is an electrode which does not need to be matched with conductive paste for use, is mainly used for measuring biopotential signals such as electrocardio signals, electroencephalogram signals and myoelectric signals, generally needs external force to enable the skin of the dry electrode to be tightly attached, and is easy to cause dislocation in the using process to influence the signal quality. And the two materials can not be stretched, and the requirement of changeable body surface structures of human bodies can not be completely met. Therefore, there is a need for a flexible stretchable self-adherent surface electrode having good flexibility and elasticity and a method for making the same.

Disclosure of Invention

In order to overcome the defects of the prior art, the invention designs a flexible and stretchable self-adhesion body surface electrode and a preparation method thereof. The metal nanowires are used as a conductive medium and mixed in a polymer material to form a conductive film, so that the conductive film is in contact with skin with irregular shapes, the interface conductivity of the electrode is improved, and the attaching area and the shape of the electrode can be controlled at will by changing the size of the conductive film, thereby being suitable for various application occasions.

In order to achieve the purpose, the technical scheme adopted by the invention is as follows:

a flexible stretchable self-adhesive watch electrode consisting essentially of: flexible stretchable conductive film, electrode lead and conductive silver adhesive, which is characterized in that: the flexible stretchable conductive film is directly contacted with the skin, the electrode lead is covered on the flexible stretchable conductive film through conductive silver colloid, one end of the electrode wire is connected with the flexible stretchable conductive film, the other end of the electrode wire is connected with a post-stage detection device, and the flexible stretchable conductive film, the electrode lead and the conductive silver colloid jointly form an electrode plate;

preferably, the flexible stretchable conductive film is formed by taking metal nanowires as a conductive material, dispersing the metal nanowires in a solution containing a polymer, evaporating and freely depositing to form the conductive film, and is used for testing an electric signal of a target test position on the body surface of a human subject;

preferably, the polymers used include polyvinyl alcohol (PVA), polyvinylidene fluoride (PVDF), polyurethane; the metal nano-wire is a gold-silver nano-wire;

preferably, the electrode lead uses a conductive copper foil with an additional insulating layer.

A preparation method of a flexible and stretchable self-adhesion body surface electrode is characterized by comprising the following steps:

step 1, adding 200-400 mg of polyvinylpyrrolidone (PVP) and 100-200 mL of ethylene glycol into a round-bottom flask, and heating the mixture to 175 ℃. After PVP is completely dispersed, 500-1000 mu L of 4mM CuCl is added₂·2H₂And (4) O solution. After 10 minutes, dropwise adding 10-50 mL of 0.095M AgNO₃And (3) solution. After the reaction is kept for 30 minutes, the synthesized Ag nanowire is washed for multiple times to remove the redundant PVP. Preparing Ag nanowires;

step 2, mixing 100-200 mL of deionized water, 5-10 mL of NaOH (0.2M) solution and 1-2 mL of HAuCl₄(0.25M) solution and 100-150 mL of Na₂SO₃The (0.01M) solutions were sequentially added to a 500mL flat bottom beaker and mixed well as an Au growth solution. In a beaker, adding 300-400 mL of H₂O, 100mg of Ag nanowire, 50-100 mL of PVP (5 wt%, MW 54000) solution, 10-20 mL of L-ascorbic acid (L-AA) (0.5M) solution, 10-20 mL of NaOH (0.5M) and 3-5 mL of Na₂SO₃The (0.1M) solution was mixed with the prepared Au growth solution to prepare a reaction solution. The mixture solution was allowed to react at 30 ℃ for 12 hours. Finally, the Au @ Ag nanowires are collected through centrifugation and washed by deionized water and ethanol;

and 3, as shown in FIG. 4, manufacturing a mold 6, adding 20mL of deionized water, 300-500 mg of PVA and 10 mu L of Hexamethylene Diisocyanate (HDI) into a flat-bottom beaker, and magnetically stirring for 4 hours at 60 ℃ to obtain a cross-linked PVA solution. And mixing the Au @ Ag nanowire with a PVA solution according to a certain proportion to obtain the conductive paste 5. 40 μ L of the prepared conductive paste 5 was poured into a mold 6. The conductive film 7 is taken down after the solvent is completely evaporated;

in the step 3, the molecular weight of PVP used when PVP and ethylene glycol are added into the round-bottom flask is 360 k;

in the step 3, the size of the manufactured mold is 10mm × 10mm × 0.5 m.

The flexible stretchable self-adhesion body surface electrode is simple in overall structure and easy to prepare; the electrode has good flexibility and stretchability, can be attached to skin in a good conformal manner, and can be used for joints; the use method is simple and convenient, the electrode can be adhered to the skin only by dropping water, and the electrode can be removed by washing with clear water after use; the test shows that the invention has good signal quality, and the signal-to-noise ratio, the signal intensity and the skin interface impedance have no obvious difference with the Ag/AgCl commercial electrode (as shown in figure 5).

Drawings

Fig. 1 is a schematic view showing a structure of a flexible and stretchable self-adhesive watch electrode of the invention.

FIG. 2 is a schematic diagram of a second structure of the flexible and stretchable self-adhesive body surface electrode of the present invention.

FIG. 3 is a diagram of the use of the flexible stretchable self-adherent surface electrode of the invention on a human body surface.

FIG. 4 is a method of making a flexible stretchable self-adherent body surface electrode of the invention.

FIG. 5 is a graph of the impedance profile of a flexible, stretchable, self-adhesive body surface of the present invention on human skin.

In the figure: 1. a flexible stretchable conductive film; 2. an electrode lead; 3. conductive silver paste; 4. a body surface schematic structure; 5. conductive paste; 6. a mold; 7. and a conductive film.

Detailed Description

As shown in fig. 1, 2 and 3, the present invention is embodied and embodied in a flexible stretchable self-adhesive watch electrode, mainly comprising: flexible stretchable conductive film 1, electrode lead 2 and conductive silver adhesive 3, its characterized in that: the flexible stretchable conductive film 1 is directly contacted with the skin 4, the electrode lead 2 is covered on the flexible stretchable conductive film 1 through the conductive silver colloid 3, one end of the electrode wire 2 is connected with the flexible stretchable conductive film 1, the other end of the electrode wire is connected with a rear-stage detection device, and the flexible stretchable conductive film 1, the electrode lead 2 and the conductive silver colloid 3 jointly form an electrode plate.

The invention relates to a preparation method of a flexible and stretchable self-adhesion body surface electrode, which is characterized by comprising the following steps:

step 1, adding 200-400 mg of PVP and 100-200 mL of ethylene glycol into a round-bottom flask, and heating the mixture to 175 ℃. After PVP is completely dispersed, 500-1000 mu L of 4mM CuCl is added₂·2H₂And (4) O solution. After 10 minutes, dropwise adding 10-50 mL of 0.095M AgNO₃And (3) solution. After the reaction is kept for 30 minutes, the synthesized Ag nanowire is washed for multiple times to remove the redundant PVP. And preparing the Ag nanowire.

Step 2, mixing 100-200 mL of deionized water, 5-10 mL of NaOH (0.2M) solution and 1-2 mL of HAuCl₄(0.25M) solution and 100-150 mL of Na₂SO₃The (0.01M) solutions were sequentially added to a 500mL flat bottom beaker and mixed well as an Au growth solution. In a beaker, adding 300-400 mL of H₂O, 100mg of Ag nanowire, 50-100 mL of PVP (5 wt%, MW 54000) solution, 10-20 mL of L-AA (0.5M) solution, 10-20 mL of NaOH (0.5M) and 3-5 mL of Na₂SO₃The (0.1M) solution was mixed with the prepared Au growth solution to prepare a reaction solution. The mixture solution was allowed to react at 30 ℃ for 12 hours. Finally, the Au @ Ag nanowires were collected by centrifugation and washed with deionized water and ethanol.

And 3, manufacturing a mold 6 as shown in FIG. 4, adding 20mL of deionized water, 300-500 mg of PVA and 10 mu L of HDI into a flat-bottom beaker, and magnetically stirring for 4 hours at 60 ℃ to obtain a cross-linked PVA solution. And mixing the Au @ Ag nanowire with a PVA solution according to a certain proportion to obtain the conductive paste 5. 40 μ L of the prepared conductive paste 5 was dropped into the mold 6. The conductive film 7 is removed after the solvent is completely evaporated.

The molecular weight of PVP used when PVP and ethylene glycol were added to the round bottom flask was 360 k.

The dimensions of the mold produced therein were 10mm by 0.5 mm.

The use process of the invention is as follows: as shown in fig. 3, an appropriate amount of water is first sprayed on the skin surface 4, and the electrode 1 is naturally attached to the wet skin surface.