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WO2018070433A1 - Composition de caoutchouc conducteur pour mesurer des bio-signaux, élément conducteur pour mesurer des bio-signaux, et vêtement pour mesurer des bio-signaux - Google Patents

Composition de caoutchouc conducteur pour mesurer des bio-signaux, élément conducteur pour mesurer des bio-signaux, et vêtement pour mesurer des bio-signaux Download PDF

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Publication number
WO2018070433A1
WO2018070433A1 PCT/JP2017/036843 JP2017036843W WO2018070433A1 WO 2018070433 A1 WO2018070433 A1 WO 2018070433A1 JP 2017036843 W JP2017036843 W JP 2017036843W WO 2018070433 A1 WO2018070433 A1 WO 2018070433A1
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WO
WIPO (PCT)
Prior art keywords
conductive
rubber composition
measurement
mass
rubber
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2017/036843
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English (en)
Japanese (ja)
Inventor
雅博 井上
泰徳 多田
祐作 天野
章郎 高橋
恒彦 寺田
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Gunma University NUC
Tatsuta Electric Wire and Cable Co Ltd
Original Assignee
Gunma University NUC
Tatsuta Electric Wire and Cable Co Ltd
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Filing date
Publication date
Application filed by Gunma University NUC, Tatsuta Electric Wire and Cable Co Ltd filed Critical Gunma University NUC
Publication of WO2018070433A1 publication Critical patent/WO2018070433A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/24—Detecting, measuring or recording bioelectric or biomagnetic signals of the body or parts thereof
    • A61B5/25—Bioelectric electrodes therefor
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/24—Detecting, measuring or recording bioelectric or biomagnetic signals of the body or parts thereof
    • A61B5/25—Bioelectric electrodes therefor
    • A61B5/251—Means for maintaining electrode contact with the body
    • A61B5/256—Wearable electrodes, e.g. having straps or bands
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/24—Detecting, measuring or recording bioelectric or biomagnetic signals of the body or parts thereof
    • A61B5/25—Bioelectric electrodes therefor
    • A61B5/263—Bioelectric electrodes therefor characterised by the electrode materials
    • A61B5/268—Bioelectric electrodes therefor characterised by the electrode materials containing conductive polymers, e.g. PEDOT:PSS polymers
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/24—Detecting, measuring or recording bioelectric or biomagnetic signals of the body or parts thereof
    • A61B5/25—Bioelectric electrodes therefor
    • A61B5/279—Bioelectric electrodes therefor specially adapted for particular uses
    • A61B5/28—Bioelectric electrodes therefor specially adapted for particular uses for electrocardiography [ECG]
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/24—Detecting, measuring or recording bioelectric or biomagnetic signals of the body or parts thereof
    • A61B5/25—Bioelectric electrodes therefor
    • A61B5/279—Bioelectric electrodes therefor specially adapted for particular uses
    • A61B5/291—Bioelectric electrodes therefor specially adapted for particular uses for electroencephalography [EEG]
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/24—Detecting, measuring or recording bioelectric or biomagnetic signals of the body or parts thereof
    • A61B5/316—Modalities, i.e. specific diagnostic methods
    • A61B5/318—Heart-related electrical modalities, e.g. electrocardiography [ECG]
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/02—Elements
    • C08K3/08—Metals
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L21/00—Compositions of unspecified rubbers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L33/00—Compositions of homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical, or of salts, anhydrides, esters, amides, imides or nitriles thereof; Compositions of derivatives of such polymers
    • C08L33/04—Homopolymers or copolymers of esters
    • C08L33/06—Homopolymers or copolymers of esters of esters containing only carbon, hydrogen and oxygen, which oxygen atoms are present only as part of the carboxyl radical
    • C08L33/08—Homopolymers or copolymers of acrylic acid esters
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L75/00—Compositions of polyureas or polyurethanes; Compositions of derivatives of such polymers
    • C08L75/04—Polyurethanes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/20—Conductive material dispersed in non-conductive organic material
    • H01B1/22—Conductive material dispersed in non-conductive organic material the conductive material comprising metals or alloys

Definitions

  • a clothing (sometimes referred to as a wearable electronic device) having a biological signal detection member has a conductive member disposed inside the clothing, i.e., at a location in contact with the human body, and the biological signal detected by the conductive member is detected. Transmitting to the transmitter and remotely detecting the electrical signal of the biological information transmitted from the transmitter to improve the efficiency of training based on the wearer's heart rate information, etc., and detect physical abnormalities Can be.
  • a method of transmitting data simply to a smartphone and transmitting data simply by synchronizing the smartphone with Bluetooth (registered trademark) used for short-distance wireless communication is also performed. Yes.
  • a hydrous conductive gel such as hydrogel is provided as an adhesive layer.
  • Electrode has been used.
  • a wearable electronic device having a recent biological signal measurement function a dry type electrode that does not use a conductive gel is required.
  • training wear is a stretchable garment that is in close contact with the body, and receives a biological signal by placing an electrode inside the garment.
  • a material that can be used for a bioelectrode for example, a material in which a fine fiber surface is coated with poly (3,4-ethylenedioxythiophene) -poly (styrenesulfonic acid) (PEDOT-PSS) which is a conductive polymer has been proposed, and it is also described that it is applied to biological information measurement wear (see Non-Patent Document 1, for example).
  • This material can impart a certain degree of stretchability depending on the knitted state of the fiber, etc., and is said to have good adhesion to the body.
  • a stretchable conductive paste printing electrode produced by applying a stretchable conductive paste containing a urethane-based binder and silver particles to clothes by screen printing or the like (for example, see Non-Patent Document 2).
  • a conductive material having shape followability a rubber base material, at least one liquid material having one or both of a carboxyl group and a hydroxyl group as a terminal group, and a conductive material are kneaded.
  • a conductive putty has been proposed (see, for example, Patent Document 1).
  • Non-Patent Document 1 and Non-Patent Document 2 are also premised on measurement in a state where the skin during exercise has a high moisture content due to sweating, and is effective for receiving biological signals during exercise.
  • the skin surface is in a dry state, for example, in a quiet operation at rest or in daily life, signal reception may be reduced or noise may be generated in the signal. There was a tendency that the acquisition of was difficult.
  • the biological information measuring ware described in Non-Patent Document 1 and Non-Patent Document 2 It has proved difficult to effectively receive the signal.
  • Means for solving the above problems include the following embodiments.
  • Bioelectric signal measurement conductivity comprising at least one selected from the group consisting of synthetic rubbers and elastomers, and comprising a rubber component having a crosslinked structure, conductive metal particles, an adhesive, and a polar solvent.
  • Rubber composition ⁇ 2> The content of the rubber component is 10% by mass to 50% by mass with respect to the total amount of the composition, and the content of the conductive metal particles is 35% by mass to 70% by mass with respect to the total amount of the composition.
  • the content of the pressure-sensitive adhesive is 10% by mass to 40% by mass with respect to the total amount of the composition, and the content of the polar solvent is 0.1% by mass to 3% by mass with respect to the total amount of the composition.
  • conductive rubber composition for biosignal measurement according to ⁇ 1> % Of the conductive rubber composition for biosignal measurement according to ⁇ 1>.
  • conductive metal particles include silver particles having an average particle diameter of 2 ⁇ m to 10 ⁇ m.
  • a conductive member for measuring a biological signal comprising: a wiring for transmitting a biological signal obtained by an electrode.
  • a biological signal measurement clothing including the biological signal measurement conductive member according to ⁇ 4> on a surface of the clothing on the side in contact with the body.
  • the touch when touching the skin is good, and even when applied to a skin with a low water content such as when dry, the biosignal receiving ability is good.
  • a conductive rubber composition can be provided.
  • a biological signal measuring conductive member that can be used by being attached to clothing using a biological signal measuring conductive rubber composition, and a living body equipped with a biological signal measuring conductive member It is possible to provide clothing for signal measurement.
  • FIG. 2 is a schematic plan view of the biological signal measuring conductive member illustrated in FIG. 1.
  • An electrocardiographic waveform of a subject at rest obtained by a clothing provided with a conductive member for biosignal measurement having a layer made of the conductive rubber composition for biosignal measurement of Example 1 at a keratin water content of 26.6%. It is a graph to show. It is a graph which shows the electrocardiogram waveform of the test subject at the time of stationary acquired with the clothes for measurement of a living body signal provided with the printed electrode which is a control example in the amount of keratin moisture 26.6%.
  • a garment comprising a conductive member for measuring biosignals having a layer made of the conductive rubber composition for measuring biosignals of Example 1 at a keratin moisture content of 26.6%
  • FIG. It is a graph which shows the test subject's electrocardiogram waveform at the time of the acquisition acquired by the measurement location.
  • It is a graph which shows the electrocardiographic waveform of the test subject at the time of the walk acquired by the clothing for biosignal measurement provided with the printed electrode which is a control example in the amount of keratin moisture of 26.6%.
  • the amount of each component in the composition means the total amount of the plurality of substances present in the composition unless there is a specific notice when there are a plurality of substances corresponding to each component in the composition. To do.
  • normal temperature represents 25 ° C. unless otherwise specified.
  • the shape following property means that when the rubber composition is pressed against the solid surface, the shape follows the shape of the solid surface and is deformed and the surface of the rubber composition is in contact with the solid surface. It shows the property that the following deformation is maintained.
  • the solid surface includes a hard surface such as a metal plate and wood, and a soft surface such as human skin and leather.
  • the conductive rubber composition for biosignal measurement includes a rubber component having at least one selected from the group consisting of rubber and elastomer and having a crosslinked structure (hereinafter, sometimes referred to as “rubber component”).
  • rubber component having at least one selected from the group consisting of rubber and elastomer and having a crosslinked structure
  • a conductive rubber composition for biosignal measurement hereinafter referred to as “rubber composition”
  • metal particles hereinafter sometimes referred to as “metal particles”
  • the rubber composition in the present disclosure uses a rubber component having good shape followability as a base material, and includes metal particles, an adhesive, and a polar solvent in the rubber component as the base material. Therefore, when the rubber composition is brought into contact with the skin, the rubber composition is deformed according to the shape of the surface of the skin due to the function of the rubber component as the base material, and is in close contact with the skin. For this reason, the contact area to the skin of the rubber composition as an electrode increases.
  • the rubber composition contains an adhesive and adheres to the skin stably due to the self-adhesiveness of the surface. As a result, it is considered that the bioelectrical impedance is reduced and the biosignal can be received more accurately.
  • the rubber composition has a crosslinked structure, the shape retention of the composition itself is good, and the rubber composition has fine irregularities due to the metal particles on the surface of the rubber composition. Prevents the rubber composition from entering and adhering to fine gaps in accordance with the unevenness of the skin surface, and the adhesive force is moderately adjusted while stably adhering to the skin due to shape followability and self-adhesiveness.
  • the rubber composition contains a polar solvent in addition to the metal particles having excellent conductivity.
  • the polar solvent has better affinity with the metal particle surface, or the conductivity of the rubber composition as a whole becomes better by further including a polar solvent compared to a composition containing only metal particles as a conductive material. I found. Note that the present disclosure is not limited to the estimation mechanism.
  • the rubber composition in the present disclosure includes a rubber component.
  • the rubber component can be used without particular limitation as long as it is a material having a cross-linked structure and having a shape following property conforming to the body when it is in close contact with the body.
  • the rubber and elastomer as the main component of the rubber component examples include natural rubber; synthetic rubber such as butadiene rubber, styrene-butadiene rubber, isoprene rubber, isobutylene-isoprene rubber, acrylonitrile-butadiene rubber, butyl rubber, silicone rubber, urethane rubber; And natural resins such as chicle.
  • the rubber component preferably includes butyl rubber, silicone rubber, urethane rubber, and the like.
  • a rubber composition may contain only 1 type of rubber components, and may use 2 or more types together.
  • the crosslinked structure in the rubber component may be formed by vulcanization, for example, or may be formed by adding a crosslinking agent.
  • the degree of crosslinking is selected according to the purpose and can be appropriately adjusted by a known method.
  • the content of the rubber component contained in the rubber composition is preferably in the range of 10% by mass to 50% by mass and preferably in the range of 15% by mass to 40% by mass with respect to the total amount of the composition from the viewpoint of good moldability and electrical conductivity.
  • the range of mass% is more preferable, and the range of 15 mass% to 30 mass% is more preferable.
  • the rubber component may be used in combination with a softener or a plasticizer for imparting flexibility.
  • the softener and plasticizer include fatty acid esters such as oleic acid ester and palmitic acid ester, and hydrocarbon oils such as paraffin.
  • the rubber component may be used in combination with a filler for preventing stickiness.
  • the filler include inorganic fillers such as calcium carbonate powder and silica particles.
  • kneaded rubber (Artists' Eraser: trade name, Kusakabe Co., Ltd., vulcanized butyl rubber as a main ingredient, paraffin, oleate, and a mixture containing calcium carbonate as an inorganic filler),
  • Eraser Trade name, Thales Japan Co., Ltd., a mixture containing vulcanized butyl rubber and silicone rubber as main ingredients, paraffin, oleate ester, palmitate ester, calcium carbonate and silica particles as inorganic fillers
  • Faber-Castell Kentgumi Art Eraser 127020 Trade name, Faber Castel Co., Ltd., a mixture containing vulcanized butyl rubber as the main ingredient, paraffin, oleic acid ester, palmitic acid ester and calcium carbonate as inorganic filler
  • the rubber composition in the present disclosure contains conductive metal particles as a conductive material.
  • conductive metal particles There are no particular restrictions on the metal particles, but metal particles with good biocompatibility are preferred because they are used in close contact with living organisms. From such a viewpoint, silver particles, platinum particles, gold particles, silver / salt chlorides are preferred. Silver particles and the like are preferable, and silver particles are more preferable.
  • the average particle diameter of the metal particles is 0.1 ⁇ m as compared with particles having an average particle diameter of nanosize, which is feared for percutaneous absorption.
  • the above particles are preferred, more preferably 2 ⁇ m to 10 ⁇ m, and even more preferably 2 ⁇ m to 7 ⁇ m.
  • the average particle size of the metal particles is determined by measuring the particle size distribution using Nikkiso Co., Ltd. and Microtrac MT3300, and drawing a cumulative distribution based on the measured particle size range of the particle size distribution. Volume average particle diameter).
  • the silver particle which is a preferable example of a metal particle is demonstrated.
  • the silver particles may be silver particles or silver-containing alloy particles in which at least a part of the surface is oxidized as long as the main component is composed of silver.
  • that the main component is composed of silver means that 80% by mass or more of the silver particles are composed of silver.
  • flaky silver particles are preferable from the viewpoints of low cost compared to platinum and gold, easy availability, and good conductivity.
  • the flaky silver particles preferably have a maximum particle size of 2 ⁇ m to 10 ⁇ m, more preferably 3 ⁇ m to 7 ⁇ m, from the viewpoint of conductivity.
  • the aspect ratio of the flaky silver particles is preferably 1 to 10, and more preferably 2 to 5.
  • spherical silver particles include, for example, Ag-HWQ (trade name, Fukuda Metal Foil Powder Industry Co., Ltd .: average particle diameter 5 ⁇ m), Ag-HWQ (trade name, Fukuda Metal Foil Powder Industry Co., Ltd.): Average particle size 2.5 ⁇ m), Ag-HWQ (trade name, Fukuda Metal Foil Powder Co., Ltd .: average particle size 1.5 ⁇ m) and the like.
  • Ag flake AgC-A (trade name, Fukuda Metal Foil Powder Co., Ltd .: average particle diameter 3 ⁇ m to 10 ⁇ m: Ag-XF301 (trade name, Fukuda Metal Foil) Powder Industry Co., Ltd.), AgC-224 (trade name, Fukuda Metal Foil Powder Industry Co., Ltd.) and the like.
  • amorphous silver particles include, for example, AgC-156I (trade name, Fukuda Metal Foil Powder Industry Co., Ltd.), AgC-132 (trade name, Fukuda Metal Foil Powder Industry Co., Ltd.), AgC-143. (Fukuda Metal Foil Powder Industry Co., Ltd.).
  • Silver particles that have been subjected to surface treatment for the purpose of improving dispersibility may be used.
  • the surface treatment agent include monocarboxylic acids such as hexanoic acid and oleic acid, and dicarboxylic acids such as adipic acid and malonic acid.
  • the rubber composition may contain only one type of metal particle or two or more types.
  • particles having different metal types may be used in combination
  • particles having different shapes may be used in combination
  • particles having different average particle diameters may be used in combination. Examples of the combined use of particles having different shapes include a combination of spherical silver particles and tabular silver particles, a combination of tabular silver particles and irregularly shaped silver particles, and the like.
  • the content of metal particles with respect to the total amount of the rubber composition is preferably in the range of 35% by mass to 70% by mass, more preferably in the range of 40% by mass to 70% by mass, and in the range of 50% by mass to 65% by mass.
  • the content of the metal particles with respect to the total amount of the rubber composition is 35% by mass or more, the conductivity of the rubber composition becomes favorable, and when it is 70% by mass or less, the rubber composition is uniform and has good shape followability. A composition is obtained, and the obtained rubber composition has good adhesion to the skin.
  • the rubber composition in the present disclosure contains an adhesive.
  • the rubber composition contains the pressure-sensitive adhesive, the adhesion to the skin becomes good when the rubber composition is applied to a living body.
  • a well-known adhesive can be suitably selected and used as a urethane type adhesive and an acrylic adhesive. Among these, from the viewpoint of biocompatibility, urethane adhesives used for medical patches and the like are preferable.
  • urethane pressure-sensitive adhesive examples include a polyester polyurethane pressure-sensitive adhesive and a polycarbonate polyurethane pressure-sensitive adhesive.
  • a polyester polyurethane pressure-sensitive adhesive which is a reaction product obtained by reacting adipic acid and polypropylene glycol with tolylene-2,4-diisocyanate (TDI) as a curing agent, can be mentioned.
  • TDI tolylene-2,4-diisocyanate
  • a commercially available product may be used as the adhesive.
  • Examples of commercially available products include Polybond (registered trademark) AY-651A (trade name: Sanyo Chemical Industries, Ltd.), Polymedica (registered trademark) A-801 (trade name: Sanyo Chemical Industries, Ltd.), and the like. It is done.
  • the rubber composition may contain only one type of pressure-sensitive adhesive or two or more types.
  • the content of the adhesive with respect to the total amount of the rubber composition is preferably in the range of 10% by mass to 40% by mass, more preferably in the range of 10% by mass to 35% by mass, and still more preferably in the range of 10% by mass to 30% by mass. A range of 15% by mass to 30% by mass is most preferable.
  • the content of the pressure-sensitive adhesive is 10% by mass or more with respect to the total amount of the rubber composition, the adhesion of the rubber composition to the skin is improved, and when it is 40% by mass or less, skin irritation is suppressed and peeling is performed. The property becomes better.
  • the rubber composition in the present disclosure contains a polar solvent.
  • the conductivity of the rubber composition becomes good.
  • the polar solvent examples include water and polyhydric alcohol.
  • water ion-exchanged water, distilled water, pure water, ultrapure water and the like are preferable from the viewpoint of few impurities.
  • the polyhydric alcohol preferably includes, for example, at least one selected from the group consisting of glycerin, polyethylene glycol, propylene glycol, and 1,3-butylene glycol, and among them, glycerin, polyethylene glycol, and the like are preferable.
  • the rubber composition may contain only one type of polar solvent or two or more types of polar solvents.
  • the content of the polar solvent with respect to the total amount of the rubber composition is preferably in the range of 0.1% by mass to 3% by mass, more preferably in the range of 0.5% by mass to 2% by mass, and 1% by mass to 1.5% by mass. % Range is preferred.
  • the content of the polar solvent with respect to the total amount of the rubber composition is 0.1% by mass or more, the conductivity of the rubber composition is improved, and when the content is 3% by mass or less, the shape followability of the rubber composition, The shape retaining property is maintained at a good level, and a decrease in feel due to the inclusion of the liquid component is suppressed.
  • the rubber composition of this embodiment can be prepared by a conventional method.
  • a silicone rubber sheet is used as a base material when mixing the components contained in the rubber composition, and a predetermined amount of pressure-sensitive adhesive is provided on the surface of the silicone rubber sheet. Apply and heat to remove at least a portion of the solvent contained in the adhesive. The heating can be performed, for example, at 60 ° C. to 90 ° C. for 10 minutes to 60 minutes. Thereafter, a rubber component, metal particles, and a polar solvent are added to the silicone rubber sheet coated with the pressure-sensitive adhesive from which at least a part of the solvent has been removed, and the pressure-sensitive adhesive and each added component are kneaded.
  • the kneading is sufficiently performed until the metallic luster due to the metal particles contained in the rubber composition is not confirmed when the mixture is visually observed.
  • the order of addition of the rubber component, metal particles, and polar solvent added to the adhesive is arbitrary.
  • the metal luster is no longer observed visually, so that kneading is sufficiently performed and the metal particles are uniformly dispersed in the base material containing the rubber component. It can be used as a guideline.
  • the adhesive, the rubber component, the metal particles, and the polar solvent, the solvent content of which has been reduced in advance by heat treatment are added to the mixing device, and shear force is applied.
  • shear force is applied.
  • a known apparatus can be used as the mixing apparatus.
  • the mixing apparatus include a mixing apparatus that applies a high shearing force such as a roll mill, a pressure kneader, a single or twin screw extruder, and the like.
  • a three-roll mill mixing device is preferable from the viewpoint that it can be uniformly mixed.
  • mixing may be performed by heating, it is preferable to carry out at normal temperature (25 degreeC).
  • the resulting rubber composition has a low content of liquid components such as water and water-soluble solvents, and thus has a good feel when it comes into contact with the skin.
  • liquid components such as water and water-soluble solvents
  • the biosignal reception is good, and it is suitably used for various members for biosignal measurement.
  • the conductive member for biosignal measurement in the present disclosure includes an electrode having a layer made of the conductive rubber composition for biosignal measurement in the present disclosure described above on the surface of the conductive substrate, and the conductive substrate. And a wiring for transmitting a biological signal obtained by the electrode.
  • FIG. 1 is a schematic cross-sectional view showing an electrode 12 portion of a biological signal measuring conductive member 10 according to an embodiment of the present invention.
  • the biological signal measuring conductive member 10 includes an electrode 12 made of the rubber composition described above on a conductive base material 14.
  • a nickel metal plate is used as the conductive substrate 14. 1 has a pair of conductive surface adhesive tapes 16A and 16B between a conductive substrate 14 having electrodes 12 and a printed electrode 18 provided on a surface of the clothing 20 in contact with the body. Is provided.
  • One of the conductive surface adhesive tapes 16 ⁇ / b> A is fixed to the conductive base material 14, and the other of the conductive surface adhesive tapes 16 ⁇ / b> B is fixed to the printed electrode 18 provided on the garment 20.
  • the laminated body of the electrode 12 and the conductive base material 14 can be detachably fixed to the printed electrode 18 provided in advance on the surface of the clothing 20 that is in contact with the body via the adhesive tapes 16A and 16B.
  • the electrode 12 By wearing the clothing 20 provided with the member 10, the electrode 12 provided on the surface of the clothing 20 in contact with the living body is brought into close contact with the skin.
  • the electrode 12 is made of the conductive rubber composition for biological signal measurement according to the present disclosure described above, and has shape followability and self-adhesiveness, so that the electrode 12 is closely adhered to the surface shape of the skin and efficiently receives the biological signal. be able to.
  • FIG. 2 is a schematic plan view of the biological signal measuring conductive member 10 shown in FIG.
  • the member 10 further includes a wiring 22 that transmits a biological signal received from the electrode 12 provided on the surface of the conductive base material 14.
  • the surface of the wiring 22 on the side in contact with the skin is covered with an insulating film 24 to prevent a short circuit.
  • the biological signal measurement conductive member may include, for example, a connector that is located at the end of the wiring and enables connection between the measurement terminal that receives the biological signal and the wiring.
  • the conductive substrate used for the member is not particularly limited as long as the electrode can be stably held and the electrode has conductivity capable of transmitting the detected biological signal to the wiring.
  • a metal plate such as a nickel plate, a silver plate, and a stainless plate, a conductive resin film, a conductive resin plate, and the like can be given.
  • a well-known thing can be used arbitrarily as a conductive resin.
  • the metal plate and the conductive resin plate are plates formed of a hard material and can stably hold the electrode.
  • a stainless steel plate or a silver plate is preferable from the viewpoint of conductivity and biocompatibility.
  • the electrode can be stably held by setting the thickness to 0.1 mm to 1 mm.
  • the size is not particularly limited, but from the viewpoint of handling properties, for example, a square with an area in a plan view of 1 cm 2 to 10 cm 2 or a circle with a diameter of 1 cm to 3 cm is used. It is preferable.
  • a conductive film, a flexible wiring board, etc. can be used as a conductive base material.
  • a conductive film or a flexible wiring board is used as a base material, since the conductive base material has flexibility, an electrode having a larger area can be formed, and the electrode can be adhered to a wider area of the skin.
  • the thickness of the electrode formed on the conductive film can be 0.1 mm to 1 mm, preferably 0.1 mm to 0.5 mm, from the viewpoint of adhesion to the skin.
  • the area of the electrode in plan view can be in the range of 1 cm 2 to 20 cm 2 .
  • the shape in plan view can be a square, a rectangle, or the like.
  • the electrode can be formed by disposing the above-described rubber composition according to the present disclosure on a conductive substrate.
  • the rubber composition may be formed into a sheet in advance, cut into a predetermined shape, and placed on a conductive base material to form an electrode.
  • the rubber composition may be applied to the conductive base material. You may form an electrode by shape
  • a conductive surface adhesive tape for fixing the electrode to the garment can be fixed on the surface of the conductive substrate opposite to the surface on which the electrode is formed.
  • a commercial item can be used as an electroconductive surface adhesive tape. Examples of the commercially available products include conductive magic tape (registered trademark) SWITCHSCIENCE ADA-1324: trade name.
  • the method for fixing the electrode to the clothing is not limited to the embodiment shown in FIG. 1.
  • the conductive base material provided with the electrode on the printed electrode provided on the surface of the clothing that contacts the body. May be fixed.
  • the member 10 including the electrode 12 and the like is detachably attached to the clothing 20 as shown in FIG.
  • a well-known method is applicable.
  • a well-known coating method is applicable.
  • a printing method such as a screen printing method, a relief printing method, and an offset printing method can be applied.
  • a screen printing method is preferable as the printing method.
  • the thickness of the printed electrode formed of the conductive ink can be set in the range of 10 ⁇ m to 50 ⁇ m, for example, and is appropriately selected according to the usage mode. For example, by using a conductive ink containing a urethane-based elastomer as the conductive ink, stretchability can be imparted to the formed printed electrode.
  • the wiring and insulating film attached to the electrode and the conductive substrate There is no particular limitation on the wiring and insulating film attached to the electrode and the conductive substrate. Known materials can be used as appropriate.
  • the connector can be appropriately provided with an aspect suitable for a device that receives a biological signal connected to a biological signal measuring conductive member.
  • the connector may be connected to a biological signal receiving device by wire, for example, connected to a portable amplifier that is attached to clothing and wirelessly transmits data to the biological signal receiving device. It may be possible.
  • the biological signal measurement conductive member in the present disclosure includes an electrode made of the rubber composition in the present disclosure described above. For this reason, since the electrode is deformed following the shape of the skin and has self-adhesiveness, the adhesion between the electrode and the skin is good, and the biological signal is efficient even when the amount of moisture in the skin is small. I can visit a doctor well. Further, since the adhesion is good, for example, even when there is a movement of the body due to walking or the like, it is difficult for the electrode to be detached from the skin, so that a good biological signal can be continuously received.
  • the biological signal measurement clothing in the present disclosure includes the biological signal measurement conductive member in the present disclosure described above on the surface of the clothing in contact with the body.
  • the electrode made of the rubber composition of the present disclosure described above fixed to the garment is in close contact with the skin, and a biosignal can be received efficiently.
  • the attachment position of the biological signal measuring conductive member in the clothing is appropriately selected depending on the measurement object.
  • electrocardiogram measurement is often performed, it is possible to efficiently measure a biological signal by attaching three to six conductive members for measuring a biological signal at predetermined positions around the heart. .
  • Example 1 (Preparation of conductive rubber composition 1) -Composition of conductive rubber composition 1- -Kneaded rubber (Artists' Eraser: trade name, Kusakabe Co., Ltd.) (Including vulcanized butyl rubber: rubber component) 28.89% Silver particles (Ag flakes AgC-A, Fukuda Metal Foil Powder Co., Ltd.) (Average particle diameter: 3 ⁇ m to 10 ⁇ m: flat metal particles) 35.18% ⁇ Adhesive (Polybond (registered trademark) AY-651A (Sanyo Chemical Industries, Ltd.) Solid content concentration 60%) 34.89% ⁇ Glycerin (Wako Pure Chemical Industries, Ltd .: Polar solvent) 1.09%
  • An adhesive was applied on a silicone rubber sheet washed with ethanol and heated at 80 ° C. for 10 minutes to remove at least a part of the solvent. Then, kneaded rubber, Ag flakes, and glycerin were added onto the silicone rubber sheet, and the pressure-sensitive adhesive and each added component were kneaded. The kneading was sufficiently performed until the metallic luster due to the metal particles contained in the rubber composition was not observed when visually observed, and the conductive rubber composition 1 was obtained. The content of Ag flakes in the obtained rubber composition is about 40%.
  • the rubber composition was taken out from the opening of the jig, and the size and cross-sectional area of the rubber composition were measured with a caliper (manufactured by Mitutoyo Corporation, DIGIMATIC CALIPER). The dimension was measured for each nickel plate, and a value obtained by removing the thickness of the nickel plate from the measured value was adopted. The cross-sectional area was measured at three locations and the average value was adopted. The electric resistivity of the rubber composition was calculated from the resistance value measured as described above and the size of the rubber composition. The rubber composition after measurement was kneaded again, and the resistivity was measured three times in the same procedure, and the average of the three times was defined as the electrical resistivity. The electrical resistivity of the rubber composition 1 was 0.0220 ⁇ cm, and it was confirmed that the rubber composition 1 of Example 1 has conductivity.
  • the rubber compositions of the examples all exhibited electrical conductivity.
  • the electrical resistivity preferable for biosignal measurement is 1 ⁇ cm or less, and all the examples described above are preferable electrical resistivity for biosignal measurement.
  • the comparison between Examples 2 to 5 shows that as the content of Ag flakes, which are metal particles, increases, the electrical resistivity decreases and the conductivity becomes better.
  • Examples 6 to 8, Comparative Example 1 In addition to the components used in Example 1, rubber compositions of Examples 6 to 8 and Comparative Example 1 were prepared in the same manner as Example 1 according to the compositions described in Table 2 below. About the obtained rubber composition, it carried out similarly to Example 1, and measured the electrical resistivity. The results are shown in Table 2 below. In addition, since the value of the electrical resistivity of the rubber composition of Comparative Example 1 exceeded the measurement range of the digital multimeter used in the evaluation of Example 1 or the like, it was replaced with the digital multimeter under the condition of an applied voltage of 1V. Electrometer 340A: trade name, manufactured by ADC Co., Ltd.) was used to measure the current, and the result was calculated. The components described in Example 1 are as described above. Details of other components are as described below.
  • Example 9 (Production of biological signal measurement clothing) 1. Formation of Printed Electrode A compression shirt (Under Armor) was used as a clothing substrate used for electrocardiogram measurement.
  • the composition of the conductive ink for printing formed on the side of the clothing that contacts the body is as follows. -Composition of conductive ink- -Urethane elastomer (Matsui Dye Industry Co., Ltd .: Ink binder) 35.0% Silver particles (Ag flakes AgC-A, Fukuda Metal Foil Powder Co., Ltd.) (Average particle size 3 ⁇ m ⁇ 10 ⁇ m) 65.0%
  • the ink binder and silver particles were mixed to obtain a paste-like conductive ink.
  • the obtained conductive ink was screen-printed on a compression shirt to form a printed electrode.
  • the printed electrodes were formed at six locations corresponding to the positions of Wilson's monopolar chest dielectric used in the standard 12-lead ECG (see Naoto Yamamoto et al., “Bioelectric Measurement”, pp. 86-87, Corona, 2011, see ). That is, the sternum right edge (first measurement point) between the fourth ribs, the sternum left edge (second measurement point) between the fourth ribs, and the third measurement point are the second measurement point and the fourth measurement point described later.
  • Example 2 Production of Conductive Member for Biological Signal Measurement Using a nickel plate as a conductive base material, the conductive rubber composition obtained in Example 1 is placed on the nickel plate, and a circular electrode having a thickness of 3 mm and a diameter of 15 mm Formed. The nickel plate is used for the purpose of facilitating attachment / detachment when holding the electrode. Wiring was connected to a nickel plate, and the side of the wiring that was in contact with the body was covered with a resin sheet, which was an insulating film, to obtain a conductive member for biosignal measurement as shown in FIG.
  • conductive surface adhesive tape conductive Magic Tape (registered trademark) ADA-1324: trade name, manufactured by SWITCHCIENCE, Inc.
  • ADA-1324 trade name, manufactured by SWITCHCIENCE, Inc.
  • ECG measurement (at rest) The electrocardiogram is measured using 3 points, with 2 points, + point and -point, so that the heart is sandwiched from the 6 electrodes attached to the clothes as described above, and the other one as the ground. went. In this evaluation, the measurement was performed using three points of the first measurement location, the second measurement location, and the fifth measurement location. The measurement is performed by connecting the connector of the conductive member for biosignal measurement to a portable amplifier (Biosignal Co., Ltd.) attached to the clothing, and receiving information transmitted wirelessly from the portable amplifier on the personal computer side. Measurement data was obtained. An electrocardiogram measured by wearing the clothes of Example 9 is shown in FIG. As apparent from FIG.
  • Example 3 the electrocardiogram measured by wearing the clothes of Example 9 to which the electrode made of the rubber composition obtained in Example 1 was attached was confirmed to be able to measure the electrocardiogram with almost no noise. It was.
  • the electrocardiogram was measured in an environment of 20 ° C. to 25 ° C. and 40% to 60% RH.
  • ECG measurement (when walking) Next, the electrocardiogram during walking was performed using the clothes of Example 9. The electrocardiogram is measured using 3 points, with 2 points, + point and -point, so that the heart is sandwiched from the 6 electrodes attached to the above-mentioned clothes, and the other one as the ground. went. In this evaluation, the measurement was performed using the three points of the third measurement point, the fourth measurement point, and the sixth measurement point. First, the electrocardiogram at rest was measured under these conditions. The results are shown in FIG. From the graph of FIG. 5, as in FIG. 3, the electrocardiogram measured by wearing the clothing of Example 9 to which the electrode made of the rubber composition obtained in Example 1 was attached was almost free from noise, and the electrocardiogram was measured. It was confirmed that it was possible.
  • the biological signal measurement conductive member and the biological signal measurement clothing in the present disclosure are useful for measurement of biological signals in daily life, and measurement of biological signals for elderly people with low mobility, care recipients, sick people, and the like. Yes, it can be expected to be applied to biological signal measurement in many environments.
  • Conductive member for biosignal measurement member
  • Electrode Electrode made of conductive rubber composition for biological signal measurement
  • Conductive substrate conductive plate
  • Conductive surface adhesive tape 18
  • Print electrode 20
  • Clothing 22
  • Wiring 24 Insulating film

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Abstract

L'invention concerne une composition de caoutchouc conducteur pour mesurer des bio-signaux, un élément conducteur pour mesurer des bio-signaux, et un vêtement pour mesurer des bio-signaux, qui est agréable lorsqu'elle est en contact avec la peau et qui présente une bonne aptitude à la réception de bio-signal, même lorsqu'elle est appliquée à une peau ayant un faible taux d'humidité. L'invention concerne : une composition de caoutchouc conducteur pour mesurer des bio-signaux, la composition de caoutchouc conducteur contenant un composant de caoutchouc ayant une structure réticulée, des particules métalliques conductrices, un adhésif, un solvant polaire, et au moins un élément choisi dans le groupe constitué de caoutchoucs synthétiques et d'élastomères ; et des applications de la composition de caoutchouc conducteur.
PCT/JP2017/036843 2016-10-14 2017-10-11 Composition de caoutchouc conducteur pour mesurer des bio-signaux, élément conducteur pour mesurer des bio-signaux, et vêtement pour mesurer des bio-signaux Ceased WO2018070433A1 (fr)

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WO2019240147A1 (fr) * 2018-06-14 2019-12-19 Nok株式会社 Électrode en chlorure d'argent-argent et circuit électrique
CN111511280A (zh) * 2018-10-17 2020-08-07 Nok株式会社 生物电极以及生物电极的制造方法
WO2020245908A1 (fr) * 2019-06-04 2020-12-10 日本電信電話株式会社 Biocapteur
SE543602C2 (en) * 2018-10-03 2021-04-13 Azadeh Soroudi Use of contact paste comprising conductive or semi-conductive particles for contact between skin and electrode
JPWO2022059608A1 (fr) * 2020-09-18 2022-03-24
JP2022083344A (ja) * 2020-11-24 2022-06-03 東和株式会社 ウェアラブルデバイス用電極パッド

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EP3977925A4 (fr) * 2019-05-31 2023-10-25 Seiren Co., Ltd. Bioélectrode et appareil équipé d'une bioélectrode
WO2022070726A1 (fr) * 2020-09-30 2022-04-07 リンテック株式会社 Capteur et dispositif de détection
JP7536299B2 (ja) * 2021-02-03 2024-08-20 プラスコート株式会社 導電性ペーストおよび導電膜
WO2025173769A1 (fr) * 2024-02-16 2025-08-21 株式会社村田製作所 Électrode de détection de signal biométrique
JP7706604B1 (ja) 2024-05-29 2025-07-11 ペルノックス株式会社 医療用デバイス

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JPWO2019240147A1 (ja) * 2018-06-14 2021-02-18 Nok株式会社 銀−塩化銀電極および電気回路
SE543602C2 (en) * 2018-10-03 2021-04-13 Azadeh Soroudi Use of contact paste comprising conductive or semi-conductive particles for contact between skin and electrode
CN111511280A (zh) * 2018-10-17 2020-08-07 Nok株式会社 生物电极以及生物电极的制造方法
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JP2022083344A (ja) * 2020-11-24 2022-06-03 東和株式会社 ウェアラブルデバイス用電極パッド

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