CN113907736A - Polymer-based flexible sensor structure design for human health monitoring and preparation method thereof - Google Patents

Polymer-based flexible sensor structure design for human health monitoring and preparation method thereof Download PDF

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Publication number
CN113907736A
CN113907736A CN202111169845.XA CN202111169845A CN113907736A CN 113907736 A CN113907736 A CN 113907736A CN 202111169845 A CN202111169845 A CN 202111169845A CN 113907736 A CN113907736 A CN 113907736A
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polymer
flexible
preparing
layer
flexible sensor
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孙靖尧
李东泰
冯宏宇
吴大鸣
许红
庄俭
刘颖
郑秀婷
盖晨辉
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Beijing University of Chemical Technology
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    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00Measuring for diagnostic purposes; Identification of persons
    • A61B5/02Detecting, measuring or recording pulse, heart rate, blood pressure or blood flow; Combined pulse/heart-rate/blood pressure determination; Evaluating a cardiovascular condition not otherwise provided for, e.g. using combinations of techniques provided for in this group with electrocardiography or electroauscultation; Heart catheters for measuring blood pressure
    • A61B5/024Detecting, measuring or recording pulse rate or heart rate
    • A61B5/02438Detecting, measuring or recording pulse rate or heart rate with portable devices, e.g. worn by the patient
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B2562/00Details of sensors; Constructional details of sensor housings or probes; Accessories for sensors
    • A61B2562/12Manufacturing methods specially adapted for producing sensors for in-vivo measurements
    • A61B2562/125Manufacturing methods specially adapted for producing sensors for in-vivo measurements characterised by the manufacture of electrodes
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B2562/00Details of sensors; Constructional details of sensor housings or probes; Accessories for sensors
    • A61B2562/16Details of sensor housings or probes; Details of structural supports for sensors
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B2562/00Details of sensors; Constructional details of sensor housings or probes; Accessories for sensors
    • A61B2562/16Details of sensor housings or probes; Details of structural supports for sensors
    • A61B2562/164Details of sensor housings or probes; Details of structural supports for sensors the sensor is mounted in or on a conformable substrate or carrier

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  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Cardiology (AREA)
  • Biomedical Technology (AREA)
  • Medical Informatics (AREA)
  • Biophysics (AREA)
  • Pathology (AREA)
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  • Heart & Thoracic Surgery (AREA)
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  • General Health & Medical Sciences (AREA)
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  • Measuring And Recording Apparatus For Diagnosis (AREA)
  • Force Measurement Appropriate To Specific Purposes (AREA)

Abstract

The invention discloses a polymer-based flexible sensor structure design for human health monitoring and a preparation method thereof. And for the flexible electrode with the microstructure, the preparation is carried out by adopting a mode of combining microstructure transfer printing and ink-jet printing. And then assembling and packaging according to the designed double-layer or multi-layer sensor structure form to obtain the double-layer and multi-layer polymer-based flexible sensors. The polymer-based flexible sensor prepared by the method is non-toxic and harmless, can be tightly attached to a human body, has the advantages of high sensitivity, good repeatability, good linearity, high response speed and the like, and has great application potential in the aspects of human health monitoring, motion detection, human-computer interaction and the like.

Description

Polymer-based flexible sensor structure design for human health monitoring and preparation method thereof
Technical Field
The invention relates to a double-layer and multi-layer flexible sensor, in particular to a structural design, preparation, packaging and data transmission method of a double-layer and multi-layer polymer-based flexible sensor taking human health monitoring as a main application scene.
Background
A flexible sensor refers to a flexible device that is capable of converting a physical or environmental stimulus into a detectable signal. In recent years, polymer-based flexible sensors have received increasing attention due to their great potential for applications in electronics and electricians, industrial engineering facilities, health care, military safety facilities, and the like. The wearable human body monitoring device can be used for preparing scientific exploration equipment, preparing wearable human body monitoring equipment to monitor physiological information of a human body, preparing combat uniforms for detecting toxic and harmful substances, and the like.
Traditional flexible sensor has the shortcoming such as sensitivity is low, the cyclic characteristic is poor, and this patent is through preparing high sensitive electrode on the flexible polymer base of inkjet printing method leveling and having the microstructure, assists with multiple bilayer and multilayer sensor structural design, further promotes sensitivity, stability etc. of sensing device. The inkjet printing technology overcomes the limitations of the conventional microelectronic manufacturing process and can obtain the required electrode shape by designing the printed pattern. The polymer-based flexible sensor prepared by the ink-jet printing technology has the characteristics of high sensitivity, strong stability and the like, has good flexibility, ductility, comfort and air permeability by selecting and designing a proper substrate shape, has good application prospect in the field of medical health, can be attached to skin to monitor physiological and physical signals, and can also be implanted into a human body to monitor vital signs. Besides the structural design of the sensor, the polymer-based flexible sensor is prepared by selecting proper conductive ink, a substrate surface micro-processing method and a connection and packaging mode. The technology of the patent provides a new idea and method for the structural design and preparation of the flexible sensor.
Disclosure of Invention
In order to overcome the defects of the traditional flexible sensor, the invention provides a polymer-based flexible sensor structure design for human health monitoring and a preparation method thereof. The conductive ink is coated on the flexible polymer substrate by an efficient, environment-friendly and pattern-customizable ink-jet printing method, and the conductive layer structure is obtained on the flexible polymer substrate by heating, ultraviolet curing and other modes. And for the flexible electrode with the microstructure, the preparation is carried out by adopting a mode of combining microstructure transfer printing and ink-jet printing. And then assembling and packaging according to the designed double-layer or multi-layer sensor structure form to obtain the double-layer and multi-layer polymer-based flexible sensors.
The technical scheme adopted by the invention comprises the following steps:
s1, determining a flexible polymer substrate and a conductive ink material;
s2, determining a microstructure form and preparing a flexible polymer substrate with a surface microstructure by using modes such as mould turnover and the like;
s3, preparing a sensitive electrode layer on a flat flexible polymer substrate with a surface microstructure by using an ink-jet printing method;
s4, assembling, connecting and packaging the flat flexible electrode with the surface microstructure according to the designed sensor structure form;
and S5, carrying out application verification on the flexible sensing device in a proper application scene.
The invention aims to overcome the defects of the prior art and provides a method for efficiently preparing a polymer-based flexible sensor by an ink-jet printing film compounding technology. The method has the advantages of high efficiency, environmental protection, close fit with human bodies, no toxicity, no harm and the like, and the patterns can be customized and have more application scenes through different designs. Many flexible sensors reported to date do not respond sensitively to minute pressure, and sensing in a minute stress range is difficult to achieve. The polymer-based flexible sensor prepared by the method has high sensitivity and linearity. By adding the microstructure in the sensor element, the sensitivity of the sensor can be more effectively improved, and the response time of sensing can be reduced. The sensor has good comfort and air permeability, can be perfectly attached to the surface of a human body in a shape designed by drawing, and has great application potential in the directions of medical health care, human health monitoring, implantable biochemical sensing and the like.
Drawings
FIG. 1 is a schematic diagram of the preparation process of a PUA silver electrode composite film, in which for a PUA film with a microstructure, the microstructure of PDMS is firstly transferred to a sand paper and then transferred to the PUA film.
FIG. 2 shows a two-layer polymer-based flexible sensor composed of a flat electrode layer and a microstructure-containing electrode layer.
FIG. 3 is a two-layer polymer-based flexible sensor composed of two layers of micro-structured electrode layers.
FIG. 4 is a multi-layer polymer-based capacitive flexible sensor composed of a two-layer electrode layer with a microstructure and a middle flat insulating dielectric layer.
FIG. 5 is a multi-layer polymer-based flexible sensor composed of a two-layer microstructure-bearing electrode layer and a middle flat conductive layer.
FIG. 6 is a multi-layer polymer-based flexible sensor composed of a two-layer flat electrode layer and a conductive layer with a microstructure in the middle.
FIG. 7 shows a physical diagram of the PUA/Ag flexible sensor fixed on the finger sleeve, applied to human health monitoring for testing human pulse. The PUA/Ag flexible sensor is proved by experiments to have the capability of monitoring fine deformation in real time.
FIG. 8 is a response curve of the multi-layer polymer-based flexible sensor under 2000 times of 1kpa pressure/release cycles, and the image is stable as a whole, which proves that PUA/Ag has good binding capacity and the flexible pressure sensor has good repeatability capacity.
Detailed Description
The present invention will be described in further detail with reference to specific embodiments.
The invention adopts the technical scheme that a method for preparing a polymer-based flexible sensor structure for monitoring human health comprises the following steps,
s1, determining a flexible polymer substrate and a conductive ink material, wherein the flexible polymer substrate and the conductive ink material are nontoxic and harmless and can be in close contact with a human body;
s2, determining the structural form of the flexible sensor and preparing a flexible polymer substrate with a surface microstructure by using modes such as mould overturning and the like;
s3, preparing a sensitive electrode layer on a flat flexible polymer substrate with a surface microstructure by using an ink-jet printing method;
s4, connecting, assembling and packaging the flat flexible electrode with the surface microstructure according to the designed sensor structure form;
and S5, carrying out application verification on the flexible sensing device in a proper application scene.
Example one
This example is a method for preparing a two-layer polymer-based flexible sensor, comprising the following steps, as shown in fig. 1:
(1) determination of flexible polymer substrate material and selection of conductive ink: the substrate for the sensor was selected to be a PUA film that was prepared to be non-toxic and to conform closely to the surface of the human body. Silver ink was selected as the conductive ink.
(2) Determining the structural form and preparing the flexible polymer substrate: the structure form is a double-layer polymer-based flexible sensor, wherein one layer is a flat-sheet PUA polymer substrate, and the other layer is a PUA polymer substrate with a microstructure. The flat-sheet PUA polymer substrate is prepared by first uniformly coating a PUA precursor on an FEP film, and then forming the PUA/FEP film into a 0.5mm film with a high-precision doctor blade. Finally, the film is placed under ultraviolet light for curing for 5min to obtain a PUA film, and then the PUA film is cut into a rectangle with the size of 20mm multiplied by 10mm to meet the requirements of ink-jet printing, and the process is carried out in a ten thousand clean rooms. The preparation method of the PUA polymer substrate with the microstructure comprises the following steps of firstly, mixing PDMS prepolymer and curing agent according to the weight ratio of 10: 1, then vacuumizing for 2 minutes, coating on 400-mesh sand paper, and putting the sand paper into a 120 ℃ oven to heat for 10 minutes to obtain a completely cured PDMS film with a microstructure. Uniformly coating the PUA precursor on a PDMS film with a microstructure, covering the FEP film on the PDMS film, preparing the PUA/FEP film into a 0.5mm film by using a high-precision scraper, and then placing the film under ultraviolet light for curing for 5min to obtain the PUA film with the microstructure.
(3) Preparing a flexible electrode layer: and respectively printing silver ink on the prepared flat piece PUA film and the PUA film with the microstructure by ink-jet printing, and preparing by controlling related parameters, wherein the temperature of a substrate is 30 ℃, the temperature of a spray head is 35 ℃, the distance between ink-jet points is 20 mu m, the number of printing layers is 3, and the shape of an electrode layer is a rectangle of 15mm multiplied by 5 mm. Different post-treatment temperatures and times resulted in different conductivity properties, where post-treatment was done by oven heating at 230 ℃ for 60 min.
(4) Connecting, assembling and packaging according to the designed structural form of the sensor: silver wire is selected here to connect the polymer-based flexible sensor to a data acquisition device. And connecting the silver wire with one end of the flexible electrode layer by a conductive silver paste bonding method, wherein the drying temperature of the silver paste is 150 ℃, and the drying time is 30 min. The structural form of the sensor is schematically assembled as shown in fig. 2, and the packaging mode is to use two 0.1mm nontoxic PDMS films which can perfectly adhere to the surface of a human body to package the polymer-based flexible sensor.
(5) And (3) carrying out performance test on the double-layer polymer-based flexible sensor: the obtained sensor has high sensitivity and linearity and can sense tiny pressure. The sensor has good air permeability and comfortableness, and obvious stable pulse periodic pulsation data can be acquired by attaching the sensor to human body pulse, so that the prepared PUA/Ag flexible sensor is proved to have the capability of monitoring micro deformation in real time and is expected to be widely applied to the fields of human body health monitoring, medical diagnosis and the like.
Example two
This example is a method for preparing a two-layer polymer-based flexible sensor, comprising the steps of:
(1) determination of flexible polymer substrate material and selection of conductive ink: the PU film which is nontoxic and can be closely attached to the surface of a human body is selected as the substrate of the sensor. The CNT dispersion was selected as a conductive ink. (2) Determining the structural form and preparing the flexible polymer substrate: the structure is in a double-layer polymer-based flexible sensor, and the upper layer and the lower layer of the structure are PU polymer substrates with microstructures. The preparation method of the PU polymer substrate with the microstructure comprises the following steps of firstly, mixing PDMS prepolymer and curing agent according to the weight ratio of 10: 1, then vacuumizing for 2 minutes, coating on 400-mesh sand paper, and putting the sand paper into a 120 ℃ oven to heat for 10 minutes to obtain a completely cured PDMS film with a microstructure. Uniformly coating a PU precursor on a PDMS film with a microstructure, covering an FEP film on the PDMS film, preparing the PU/FEP film into a film with the thickness of 0.5mm by using a high-precision scraper, and then placing the film under ultraviolet light for curing for 5min to obtain the PU film with the microstructure.
(3) Preparing a flexible electrode layer: the CNT dispersion liquid is respectively printed on two prepared PU films with microstructures by ink-jet printing, the preparation is carried out by controlling relevant parameters, the temperature of a substrate is 30 ℃, the temperature of a spray head is 35 ℃, the distance between ink-jet points is 20 mu m, the number of printing layers is 5, and the shape of an electrode layer is a rectangle of 15mm multiplied by 5 mm. Here, the post-treatment was carried out by heating in an oven at 100 ℃ for 30 min.
(4) Connecting, assembling and packaging according to the designed structural form of the sensor: silver wire is selected here to connect the polymer-based flexible sensor to a data acquisition device. And connecting the silver wire with one end of the flexible electrode layer by a silver paste bonding method, wherein the drying temperature of the silver paste is 150 ℃, and the drying time is 30 min. The structural form assembly of the sensor is schematically shown in fig. 3, and the packaging mode is to use two 0.1mm non-toxic PI films which can be closely attached to a human body to package the polymer-based flexible sensor.
(5) And (3) carrying out performance test on the double-layer polymer-based flexible sensor: the obtained sensor has high sensitivity and linearity, can feel tiny pressure, has good instantaneous response capability and cycle characteristic, can be closely attached to the surface of a human body through a figure, has good comfort and air permeability, and can play a good monitoring effect by connecting the sensor with a manipulator and human body pulse.
EXAMPLE III
This example is a method for making a multilayer polymer-based flexible sensor comprising the steps of:
(1) determination of flexible polymer substrate material and selection of conductive ink: the PDMS film which is nontoxic and can be closely attached to a human body is selected as a substrate of the sensor, a PEDOT (Polytetrafluoroethylene)/PSS system is selected as a conductive material, and a PDMS/SCF composite film is selected as an intermediate conductive layer.
(2) Determining the structural form and preparing the flexible polymer substrate and the intermediate conductive layer: the structure form is a multi-layer polymer-based flexible sensor, wherein the upper layer and the lower layer are flat-sheet PDMS polymer substrates, the middle conducting layer is a PDMS/SCF composite film, and the structure form is shown in figure 5. The preparation method of the flat PDMS polymer substrate comprises the following steps of firstly, mixing PDMS prepolymer and curing agent according to the ratio of 10: 1, then coating the FEP film after vacuumizing for 2 minutes, and then putting the PDMS/FEP film into a 0.6mm film by a high-precision scraper, and heating the film in an oven at 120 ℃ for 10 minutes to completely cure the film. The preparation method of the PDMS/SCF composite film with the intermediate conductive layer comprises the steps of uniformly mixing 70 mass percent of uncured PDMS and 30 mass percent of SCF, and preparing the mixture into a film with the thickness of 0.5mm by a hot stamping method, wherein the heating temperature is 120 ℃. The PDMS/SCF film was cut into a 15mm by 5mm rectangle.
(3) Preparing a flexible electrode layer: uniformly spin-coating a PEDOT/PSS dispersion solution on the prepared flat PDMS film by a spin-coating method, preparing by controlling related parameters, heating to 70 ℃ by using an oven after each spin-coating, heating for 20min, drying for 5 times, and repeating the operation to complete the post-treatment.
(4) Connecting, assembling and packaging according to the designed structural form of the sensor: silver wire is selected here to connect the polymer-based flexible sensor to a data acquisition device. And connecting the silver wire with one end of the flexible electrode layer by a silver paste bonding method, wherein the drying temperature of the silver paste is 150 ℃, and the drying time is 30 min. The structural form of the sensor is schematically assembled as shown in fig. 5, and the packaging mode is to use two 0.1mm PUA films which are nontoxic and can be closely attached to a human body to package the polymer-based flexible sensor.
(5) The multilayer polymer-based flexible sensor was subjected to performance testing: the obtained sensor has high sensitivity and linearity and can sense tiny pressure. The sensor has good cycle characteristic, short sensing response time, excellent comfort and air permeability, and good application prospect in the medical health care field and the human health monitoring direction, and the flexible sensor which can be designed according to the graph can be closely attached to the human body.

Claims (8)

1. A preparation method of a polymer-based flexible sensor structure for monitoring human health is characterized by comprising the following steps: the method comprises the following steps of,
s1, determining a flexible polymer substrate and a conductive ink material, wherein the flexible polymer substrate and the conductive ink material are nontoxic and harmless and can be in close contact with a human body;
s2, determining the structural form of the flexible sensor and preparing a flexible polymer substrate with a surface microstructure by using modes such as mould overturning and the like;
s3, preparing a sensitive electrode layer on a flat flexible polymer substrate with a surface microstructure by using an ink-jet printing method;
s4, connecting, assembling and packaging the flat flexible electrode with the surface microstructure according to the designed sensor structure form;
and S5, carrying out application verification on the flexible sensing device.
2. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: the structural form of the polymer-based flexible sensor comprises a double-layer structure and a multi-layer structure which are composed of a flat flexible electrode, a flexible electrode with a surface microstructure, a conductive layer and a dielectric layer.
3. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: the sensitive materials used include carbon-based conductive materials, metal conductive materials, MXene, conductive polymer materials.
4. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: the flexible polymer substrate used includes Polydimethylsiloxane (PDMS), polyethylene terephthalate (PET), Polyimide (PI), Polyethylene (PE), Polyurethane (PU), polyurethane acrylate (PUA), styrene- (ethylene-butadiene copolymer) -styrene block copolymer (SEBS).
5. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: the substrate surface microstructure forms used include rectangular, cylindrical, triangular pyramidal, spherical, and combinations thereof.
6. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: sensing mechanisms used include resistive, capacitive, triboelectric, piezoelectric.
7. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: the packaging methods of the high polymer film package include Polydimethylsiloxane (PDMS) film package, polyethylene terephthalate (PET) film package, Polyimide (PI) film package, Polyethylene (PE) film package and Polyurethane (PU) film package.
8. The method of claim 1, wherein the step of preparing a polymer-based flexible sensor structure comprises: the data transmission modes used include Bluetooth transmission, radio frequency signals, PCI connection and USB connection.
CN202111169845.XA 2021-10-08 2021-10-08 Polymer-based flexible sensor structure design for human health monitoring and preparation method thereof Pending CN113907736A (en)

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