CN111134401A - High-elasticity intelligent clothes based on liquid metal, and preparation method and application thereof - Google Patents
High-elasticity intelligent clothes based on liquid metal, and preparation method and application thereof Download PDFInfo
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- CN111134401A CN111134401A CN201811300760.9A CN201811300760A CN111134401A CN 111134401 A CN111134401 A CN 111134401A CN 201811300760 A CN201811300760 A CN 201811300760A CN 111134401 A CN111134401 A CN 111134401A
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- liquid metal
- printing
- clothes
- ink
- conductive
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- 238000010438 heat treatment Methods 0.000 claims abstract description 21
- 238000001514 detection method Methods 0.000 claims abstract description 18
- 238000000835 electrochemical detection Methods 0.000 claims abstract description 5
- 238000007650 screen-printing Methods 0.000 claims description 19
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- 238000012544 monitoring process Methods 0.000 claims description 11
- 239000006023 eutectic alloy Substances 0.000 claims description 10
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 10
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- WYTGDNHDOZPMIW-RCBQFDQVSA-N alstonine Natural products C1=CC2=C3C=CC=CC3=NC2=C2N1C[C@H]1[C@H](C)OC=C(C(=O)OC)[C@H]1C2 WYTGDNHDOZPMIW-RCBQFDQVSA-N 0.000 description 2
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- JHIVVAPYMSGYDF-UHFFFAOYSA-N cyclohexanone Chemical compound O=C1CCCCC1 JHIVVAPYMSGYDF-UHFFFAOYSA-N 0.000 description 2
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- MWKFXSUHUHTGQN-UHFFFAOYSA-N decan-1-ol Chemical compound CCCCCCCCCCO MWKFXSUHUHTGQN-UHFFFAOYSA-N 0.000 description 2
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- YZZNJYQZJKSEER-UHFFFAOYSA-N gallium tin Chemical compound [Ga].[Sn] YZZNJYQZJKSEER-UHFFFAOYSA-N 0.000 description 2
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- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
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- LOKCTEFSRHRXRJ-UHFFFAOYSA-I dipotassium trisodium dihydrogen phosphate hydrogen phosphate dichloride Chemical compound P(=O)(O)(O)[O-].[K+].P(=O)(O)([O-])[O-].[Na+].[Na+].[Cl-].[K+].[Cl-].[Na+] LOKCTEFSRHRXRJ-UHFFFAOYSA-I 0.000 description 1
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- 229920000435 poly(dimethylsiloxane) Polymers 0.000 description 1
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- 229920006254 polymer film Polymers 0.000 description 1
- 239000000256 polyoxyethylene sorbitan monolaurate Substances 0.000 description 1
- 235000010486 polyoxyethylene sorbitan monolaurate Nutrition 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000011897 real-time detection Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 1
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- KKEYFWRCBNTPAC-UHFFFAOYSA-L terephthalate(2-) Chemical compound [O-]C(=O)C1=CC=C(C([O-])=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-L 0.000 description 1
- 238000009210 therapy by ultrasound Methods 0.000 description 1
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- 231100000419 toxicity Toxicity 0.000 description 1
- FCFNRCROJUBPLU-DNDCDFAISA-N valinomycin Chemical compound CC(C)[C@@H]1NC(=O)[C@H](C)OC(=O)[C@@H](C(C)C)NC(=O)[C@@H](C(C)C)OC(=O)[C@H](C(C)C)NC(=O)[C@H](C)OC(=O)[C@@H](C(C)C)NC(=O)[C@@H](C(C)C)OC(=O)[C@H](C(C)C)NC(=O)[C@H](C)OC(=O)[C@@H](C(C)C)NC(=O)[C@@H](C(C)C)OC1=O FCFNRCROJUBPLU-DNDCDFAISA-N 0.000 description 1
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Images
Classifications
-
- A—HUMAN NECESSITIES
- A41—WEARING APPAREL
- A41D—OUTERWEAR; PROTECTIVE GARMENTS; ACCESSORIES
- A41D13/00—Professional, industrial or sporting protective garments, e.g. surgeons' gowns or garments protecting against blows or punches
- A41D13/12—Surgeons' or patients' gowns or dresses
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
- C09D11/00—Inks
- C09D11/02—Printing inks
- C09D11/03—Printing inks characterised by features other than the chemical nature of the binder
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Wood Science & Technology (AREA)
- Life Sciences & Earth Sciences (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Physical Education & Sports Medicine (AREA)
- Textile Engineering (AREA)
- Inks, Pencil-Leads, Or Crayons (AREA)
Abstract
The invention provides high-elasticity intelligent clothes based on liquid metal, and further provides a preparation method and application thereof. The intelligent garment of the present invention includes a controller part and a function part, the function part including: the device comprises an electrophysiological detection module, an electrochemical detection module and a heating and heat-preserving module. The invention realizes the printing of the flexible stretchable circuit on the clothes, and the clothes can not cause the interconnection lead and the electrode of the liquid metal to lose efficacy under various deformation conditions. The circuit manufactured by the method has excellent tensile stability and repeatability. The conductive ink disclosed by the invention is low in cost, high in utilization rate of liquid metal, small in liquid metal consumption, adjustable in line width of a circuit, extremely high in production efficiency, and very suitable for large-scale production of elastic circuits.
Description
Technical Field
The invention belongs to the field of wearable equipment, and particularly relates to high-elasticity intelligent clothes based on liquid metal, and a preparation method and application thereof.
Background
With the continuous improvement of the quality of life, people pay more and more attention to the health of the people. For athletes and some special patients, the real-time monitoring of the physiology in the body is very important, and the biochemical indexes such as electrocardio, myoelectricity, potassium ion concentration, sodium ion concentration, glucose concentration, lactic acid concentration and the like are very important. However, the acquisition of these physiological and biochemical indicators often requires trained personnel, expensive large instruments and long waiting times, and most tests are invasive and can cause pain and infection risks to the person being tested. Therefore, a wearable device capable of non-invasive detection and real-time monitoring of various indexes of the body is particularly necessary.
At present, the research on the real-time monitoring device for the physiological and biochemical indexes of the body surface is endless. Subject groups of professor JohnA. Rogers of northwest university in America develop several patches capable of being attached to the surface of skin and monitoring various indexes of body surface in real time, the patches adopt a snake-shaped lead structure and can resist certain tensile deformation (100% -150%), the patches can monitor indexes such as electrocardiosignals, electromyographic signals, temperature, pressure, acceleration and the like, but the processing technology of the patches is very complex, the components are very high, the area of the patches is limited by micro-processing technology, and the patches cannot simultaneously monitor multiple leads of electrophysiological signals distributed at various parts of the body.
The Ali Javey group developed a patch that could be attached to the skin surface for electrochemical signal detection. The patch can simultaneously monitor temperature, sodium ions, potassium ions, glucose and lactic acid in body surface sweat. Although the patch is highly integrated and can monitor signals of various chemical molecules at the same time, the patch has no tensile property, and the circuit part still adopts a traditional circuit board, so that the patch is inconvenient to wear.
To facilitate wearing, researchers consider integrating various sensors on clothing and garments. The clothes woven by conductive fibers are used for electrocardiographic detection, and the specific method is that the conductive fibers are used for weaving electrodes and interconnection leads on the clothes with elasticity. Because the electrocardio-detection does not need the electrode to have good conductive capability, the electrocardio-signal detection can be realized even if the conductive property of the conductive fiber is deficient. However, since the interconnection wire needs to have good conductivity at metal level, and the conductive fiber has insufficient conductivity, it is difficult to integrate electronic devices and various sensors on the interconnection wire of conductive fiber.
Recent literature reports of wearable devices for the detection of body surface electrophysiological and electrochemical signals are based on silica gel substrates, which are not suitable for contact with the skin. On the one hand, they are difficult to fix on the skin, and on the other hand, these substrates, especially silicone substrates, are prone to dirt and are difficult to reuse. Due to the limitation of processing technology lithography, the wearable devices are generally small in size, so that the detection of human body signals is limited to a small range, and the signals of all parts of the whole body are difficult to monitor simultaneously. The intelligent wearable preparation process is very complex, high in cost and only disposable, so that the practical application of the intelligent wearable preparation is fundamentally limited.
The intelligent clothes can be prepared by directly printing the upper electrodes and the interconnection wires on the clothes. Because the clothes have certain elasticity, and the conductive ink sold in the market has no elasticity, the requirement of the elasticity cannot be met, and the conductive ink can crack due to the stretching deformation of the clothes. The stretchable micro-nano silver sheet conductive ink reported in the literature is expensive in manufacturing cost and is not suitable for large-area circuit printing on clothes.
Disclosure of Invention
Therefore, the present invention aims to overcome the defects in the prior art and provide a high-elasticity intelligent clothing based on liquid metal, and a preparation method and application thereof.
To achieve the above object, a first aspect of the present invention provides a liquid metal-based high elasticity intelligent garment including a controller part and a function part, wherein:
the functional part includes: the device comprises an electrophysiological detection module, an electrochemical detection module and a heating and heat-preserving module; and is
The interconnection wire part, the heating part, the electrocardio-electrode part and the contact used for the electronic device and the sensor of the intelligent clothes are composed of liquid metal conducting layers.
The smart garment according to the first aspect of the invention, wherein the garment further comprises an interface for a sensor; preferably, the sensor is selected from one or more of: temperature sensors, stress-strain sensors, electrochemical sensors.
A second aspect of the present invention provides a method for preparing the smart garment of the first aspect, the method comprising the steps of:
(1) preparing liquid metal ink;
(2) printing a base layer;
(3) printing a liquid metal layer;
(4) printing an insulating layer;
(5) stretching;
(6) integration of intelligent clothing.
The production method according to the second aspect of the invention, wherein, in the step (1), the liquid metal ink is produced by: dissolving a macromolecule in a solvent, and fully stirring and dissolving to prepare a solution; adding liquid metal into the solution, and preparing the liquid metal into nano-sized or micro-sized particles by a physical method to prepare the liquid metal ink; wherein:
the polymer is preferably selected from one or more of the following: polyvinylpyrrolidone, polyvinyl alcohol, polyoxyethylene, polyacrylamide, polyurethane, polyacrylic acid, polylactic acid, polyglycolic acid, polylactic acid-glycolic acid copolymer, polycaprolactone;
the solvent is preferably selected from one or more of the following: water, alcohol solutions, acetone;
the mass fraction of the solution is preferably 0.5-20%;
the liquid metal is preferably a metal with a melting point below 200 degrees celsius, and further preferably the liquid metal is selected from one or more of the following: gallium, mercury, gallium-indium alloy, gallium-indium-tin alloy, bismuth-tin-lead-indium alloy; most preferably, the liquid metal is preferably a gallium indium eutectic alloy;
the concentration of the liquid metal in the liquid metal ink is preferably 0.1g/mL-5g/mL, and more preferably 3 g/mL; and/or
The physical method is preferably ultrasound and/or high speed rotational shear.
The preparation method according to the second aspect of the present invention, wherein a surfactant is further included in the liquid metal ink; preferably, the surfactant is selected from one or more of the following: fluorocarbon surfactant, disodium lauryl sulfosuccinate, span, tween, sodium dodecyl benzene sulfonate and potassium dodecyl phosphate; more preferably, the mass fraction of the added surfactant is 0.05% -1%; and/or
The liquid metal ink also comprises a viscosity regulator; preferably, the viscosity modifier is selected from one or more of: chitin, polyethylene wax, alkyl diethanolamide, polyethylene glycol distearate and hydroxyethyl cellulose; more preferably, the viscosity modifier is added in a mass fraction of 0.05% to 1%.
The preparation method according to the second aspect of the present invention, wherein, in the step (2), commercial elastic printing paste for clothes is printed on the inner side of the clothes according to a specific pattern;
preferably, the printing method is selected from one or more of the following: screen printing, thermal transfer printing, digital direct injection printing process and ink-jet printing;
more preferably, after printing, the adhesive cement is cured for 5-120 minutes in an environment at 25-200 ℃.
The preparation method according to the second aspect of the present invention, wherein, in the step (3), the liquid metal ink prepared in the step (1) is printed on the substrate layer according to a specific pattern;
preferably, the printing method is selected from one or more of the following: screen printing, ink jet printing;
more preferably, after printing, the clothes are dried for 10-30 minutes in an environment of drying for 6-12 hours at room temperature or 80 ℃.
The manufacturing method according to the second aspect of the present invention, wherein, in the step (4), a commercial elastic printing paste for clothes is printed on the liquid metal layer, the liquid metal interconnection lead part is encapsulated in an insulating paste, and the electrode part and the contact part are not encapsulated by the insulating paste;
preferably, the printing method is selected from one or more of the following: screen printing, thermal transfer printing, digital direct injection printing process and ink-jet printing;
more preferably, after printing, the adhesive cement is placed in an environment with the temperature of 25-200 ℃ for curing for 5-120 minutes; and/or
In the step (5), after printing is finished, the clothes are stretched, and the clothes are made to conduct electricity by applying 20% -200% strain.
According to the preparation method of the second aspect of the invention, in the step (6), the intelligent clothes are integrated, and the controller is connected with each sensor through the contact of the liquid metal interconnection lead;
preferably, the step (6) further comprises covering the liquid metal electrode with a conductive material, wherein the conductive material is selected from one or more of the following materials: conductive hydrogel, conductive polymer, silver foil, copper foil and gold foil.
A third aspect of the invention provides the use of the smart garment of the first aspect or the smart garment made according to the method of the second aspect in health monitoring and disease treatment.
The invention combines the liquid metal patterning technology, the electrode circuits are printed on different positions on the surface of the clothes, and then various sensors are integrated on the clothes to manufacture the intelligent clothes with low price and super high elasticity, thereby realizing the real-time detection of various signals of body surface electrophysiology, electrochemistry and the like.
The invention realizes the printing of electrodes and interconnection leads on the surface of clothes by utilizing a liquid metal patterning technology, and then further integrates various sensors on the clothes, thereby realizing the non-invasive real-time health monitoring. Compared with the prior art, the method provided by the invention adopts a quick and efficient printing method, and can print the cheap liquid metal conductive ink with excellent tensile property on clothes in a large scale and large area. Through the sensor of integrated different functions, can realize the preparation of multi-functional intelligent clothing, monitor the signal of whole body surface.
The invention provides a method for manufacturing intelligent clothes based on a liquid metal patterning technology. The whole process mainly comprises the steps of preparing liquid metal ink, printing a base layer, printing a liquid metal layer, printing an insulating layer, stretching clothes, integrating intelligent clothes and the like. The intelligent clothes functional part comprises three modules, namely an electrophysiological detection module, an electrochemical detection module and a heating and heat-preserving module. The electrophysiological detection module is used for detecting electrophysiological signals such as electrocardiosignals, electromyographic signals and the like; the electrochemical detection module is used for detecting various molecular signals on the body surface, such as potassium ion concentration, sodium ion concentration, glucose concentration, lactic acid concentration and the like; the heating constant temperature module comprises a coil and a temperature sensor which are composed of liquid metal and is used for monitoring the body temperature, actively heating when the body temperature is too low and keeping the body constant temperature. The intelligent clothes are cheap and simple to prepare, and are particularly suitable for large-scale application. The main process of the process comprises the following steps:
1. and preparing liquid metal ink. The high-elasticity liquid metal conductive ink is prepared by adopting a formula which is low in toxicity or harmless to human bodies because clothes need to be in direct contact with the human bodies, and the preparation method is as follows. The invention dissolves one or more polymers of polyvinylpyrrolidone (PVP), polyvinyl alcohol (PVA), Polyoxyethylene (PEO), Polyacrylamide (PAM), Polyurethane (PU), polyacrylic acid (PAA), polylactic acid (PLA), polyglycolic acid (PGA), polylactic-glycolic acid copolymer (PLGA) and Polycaprolactone (PCL) in one or more common organic solvents such as water, alcohol solution, acetone and the like, fully stirs and dissolves the polymers to prepare the solution with the mass fraction of 0.5 to 20 percent.
In order to make the conductive ink easier to pattern, increase the wettability of the conductive ink with a substrate, reduce a contact angle and stabilize liquid metal particles, the inventor adds one or more surfactants such as fluorocarbon surfactant, disodium lauryl sulfosuccinate, span, tween, sodium dodecyl benzene sulfonate, potassium dodecyl phosphate and the like into the conductive ink, and the mass fraction of the added surfactant is 0.05-1%.
To adjust the viscosity of the ink, the conductive ink is allowed to match the viscosity requirements of various patterning techniques. The inventor adds a viscosity regulator such as one or more substances of chitin, polyethylene wax, alkyl diethanolamide, polyethylene glycol distearate, hydroxyethyl cellulose and the like into the ink, wherein the added mass fraction is between 0.1 and 5 percent.
The liquid metal is added into the polymer solution, the liquid metal comprises gallium, mercury, gallium-indium alloy, gallium-indium-tin alloy, bismuth-tin-lead-indium alloy and other metals with the melting point lower than 200 ℃, the concentration of the liquid metal is 0.1g/mL-5g/mL, and optimally, the concentration of the liquid metal gallium-indium eutectic alloy (the mass fraction of gallium is 75.5%, and the mass fraction of indium is 24.5%) is 3 g/mL. After adding the liquid metal into the aqueous polymer solution, the present inventors prepared the liquid metal into nano-or micro-sized particles using physical methods such as ultrasound and high-speed rotational shearing, the size of the particles depending on the amplitude and time of the physical action. When the ultrasonic amplitude is 30% and the ultrasonic time is 1min, 30min, 60min, 90min and 120min, the average diameters of the obtained gallium-indium eutectic alloy particles are 4700nm, 800nm, 520nm, 315nm and 274nm respectively. Optimally, the inventor uses an ultrasonic cell disruptor to carry out ultrasonic treatment on 3g/mL liquid gallium-indium eutectic alloy for 1min at the amplitude of 30% to obtain a gray liquid metal suspension, the metal is dispersed into countless micro-nano-sized small particles, and the average particle size of the small particles is 3700 nm. The inner core of the small particles is liquid metal, and the outer part of the small particles is coated by a thin oxide film. Thereby, the gallium-indium alloy liquid metal ink is obtained.
2. And printing the base layer. The invention uses the technologies of silk screen printing, thermal transfer printing, digital direct injection printing technology, ink-jet printing and the like to print the commercial elastic printing adhesive cement of the clothes on the inner side of the clothes according to a specific pattern (figure 1). And curing the mucilage for 5-120 minutes in an environment at 25-200 ℃. To this end, an upper substrate layer is prepared on the garment.
3. And printing the liquid metal layer. The liquid metal ink is printed on a substrate layer according to a specific pattern by using a screen printing method and an ink-jet printing method. And after printing, drying the clothes for 10-30 minutes in an environment of drying for 6-12 hours at room temperature or 80 ℃. The pattern is not conductive between the metal particles due to the insulation of the insulating oxide film and the polymer film.
4. And printing an insulating layer. In order to avoid the problems of direct contact between the liquid metal interconnection lead and the outside, short circuit and the like, the invention prints the elastic printing adhesive paste on the liquid metal layer according to the method 2, and partially encapsulates the liquid metal interconnection lead in the insulating adhesive paste.
5. And (5) stretching. After printing, the pattern of liquid metal particles is not conductive due to the isolation of the oxide films on the surface of the particles. At this time, the present inventors stretched the garment, giving the garment a strain of 20% -200%. The strain can cause the insulating oxide film of the liquid metal particles to break, releasing the conductive core, and enabling the liquid metal layer on the clothes to have the conductive capability.
6. Integration of intelligent clothing. Through the five steps, the inventor manufactures the pattern on the inner side of the clothes. The liquid metal conducting layer forms an interconnected wire part, a heating part, an electrocardio-electrode part and a contact for electronic devices and sensors of the intelligent clothes. The electrode portion and the contact portion are not encapsulated by the insulating paste.
The electrocardio-electrode lead number is designed according to the actual requirement, and the position of the clothing corresponds to the specific part of the body. In order to avoid the pollution of the skin caused by the direct contact of the liquid metal and the skin, the liquid metal electrode is covered with a layer of conductive material, such as conductive hydrogel, conductive polymer, silver foil, copper foil, gold foil and other materials.
According to the invention, the flexible and stretchable conductive ink is directly printed on the clothes by adopting a printing method to serve as a complex conductive circuit and an electrode, and various sensors are integrated on the flexible and stretchable conductive ink, so that the intelligent clothes with various functions can be conveniently and rapidly manufactured in a large scale.
The material used in the invention has no toxicity and is harmless to human body. The athlete can monitor the changes of various physical and chemical signals such as electrocardio and myoelectric signals, the concentration of potassium and sodium ions in sweat and the like in real time during the exercise process, so that the athlete can be guided to train, and the physical injury caused by excessive exercise can be prevented. The invention can be used for patients with special diseases such as diabetes. After glucose, lactic acid and other sensors are integrated, the concentration of special indexes in a human body can be monitored in real time, and a patient is guided to take medicine. The invention also has important significance for the battle of soldiers. The body temperature of the soldier can be kept constant under the extremely cold condition, and the body state of the soldier can be monitored in real time.
The smart garment of the present invention may have, but is not limited to, the following beneficial effects:
1. the invention realizes the printing of the flexible stretchable circuit on the clothes, and the clothes can not cause the interconnection lead and the electrode of the liquid metal to lose efficacy under various deformation conditions. When the tensile strain reaches 200%, the resistivity changes by less than 10%. The circuit manufactured by the method has excellent tensile stability and repeatability.
2. The conductive ink disclosed by the invention is low in cost, high in utilization rate of liquid metal (close to 100%), small in liquid metal consumption (only 2-10 mg of liquid metal is needed for any pattern per square centimeter), adjustable in line width of a circuit, extremely high in production efficiency, and very suitable for large-scale production of an elastic circuit.
3. The invention can realize large-area, high-speed and low-cost printing of liquid metal interconnection conduction and electrodes on clothes.
4. The conductive ink has no toxicity and no harm to human body due to the main components of liquid metal (generally gallium-indium alloy) and common medical polymers (such as polyvinylpyrrolidone and polyvinyl alcohol), can be attached to the human body without causing adverse reaction, and further can be used for research and development of implanted devices and health monitoring and disease treatment in the body.
Drawings
Embodiments of the invention are described in detail below with reference to the attached drawing figures, wherein:
FIG. 1 shows a schematic diagram of the interconnection wiring, electrodes and sensor distribution of the smart garment of the present invention.
FIG. 2a shows potential versus time for a smart garment for multi-lead electrocardiographic signal detection; FIG. 2b shows the concentration of smart clothing for potassium ion concentration detection versus time and potential versus potassium ion concentration; fig. 2c shows the resistance of the smart garment for strain detection versus strain at different times.
Fig. 3 shows the temperature distribution of the intelligent clothes heating area under the infrared thermal imager.
Description of reference numerals:
1. an electrocardio-electrode; 2. a controller interface; 3. a potassium ion sensor interface; 4. a temperature sensor interface; 5. a strain sensor interface; 6. and a heating coil.
Detailed Description
The invention is further illustrated by the following specific examples, which, however, are to be construed as merely illustrative, and not limitative of the remainder of the disclosure in any way whatsoever.
This section generally describes the materials used in the testing of the present invention, as well as the testing methods. Although many materials and methods of operation are known in the art for the purpose of carrying out the invention, the invention is nevertheless described herein in as detail as possible. It will be apparent to those skilled in the art that the materials and methods of operation used in the present invention are well within the skill of the art, provided that they are not specifically illustrated.
The reagents and instrumentation used in the following examples are as follows:
reagent:
liquid indium gallium eutectic alloy (Ga 75.5 wt% In 24.5 wt%), liquid indium gallium tin alloy (In22 wt% Ga68 wt% Sn 10 wt%) from Beijing Haoke technology Inc., polyvinylpyrrolidone (average molecular weight 1300000), polylactic acid PLA, Tween 20, paraffin oil, N- (2-hydroxyethyl) dodecylamide, ethanol, chitosan from Shanghai Michelin Biochemical technology Inc.;
phosphate buffered saline (PBS, PH 7.2), Tris-HCl buffered saline (Tris-HCl, PH 7.5) was purchased from semer feishel, usa;
fluorocarbon surfactant (FS-30) was purchased from Shanghai warpont industries, Inc.;
indium gallium eutectic alloy was purchased from Sigma Aldrich;
t-shirt screen printing ink (Geliya WG-NY102) was purchased from Miao ink coatings, Inc.;
polydimethylsiloxane prepolymers and their curatives (Sylgard 184) were purchased from Dow Corning corporation;
ecoflex 0030 silica gel was purchased from Smooth-On, USA;
waterborne polyurethane (Archsol 8560) was purchased from wanghua chemical group, inc;
thermoplastic polyurethane (TPU 65A) was purchased from Xinxin Plastic materials, Inc., Dongguan;
the elastic long-sleeve swimsuit is purchased from a Tianmao Fang Hua sports outdoor special shop, and the brand shark bate;
the heat transfer ink and the heat transfer paper are purchased from new materials of Zhuhai Tianwei GmbH, brand Tianwei;
the medical conductive hydrogel is purchased from a tianmao flag ship store, model Top-Touch, open to the sea.
The conductive fiber is purchased from Beijing GaoZhi Gaomei Komao Co Ltd, model 3D-76-KC575
The instrument comprises the following steps:
oven, purchased from Shanghai Pudong Rongfeng scientific instruments, Inc., model number DHG-9030A;
an ultrasonic cell disruptor, available from BINEUTINOIN ULTRASONIC CORPORATION, model S-450D;
scanning electron microscope, available from Hitachi, model S4800;
a small-sized manual printing and screen printing machine which is purchased from hardware tool special shops at Kyoto-Yuan-Port and has the model of Guanxing 0C;
the precision multimeter is purchased from Fuluke electronic instruments, model 8846A;
dynamic mechanical analyzer, model DMA Q800;
spray gun, model S-120, bore 0.5mm, purchased from Taiwan Shanben pneumatic equipment company;
a thermal transfer printer, purchased from tianmachang print service flagship shop, model number high pressure flat panel pyrograph machine;
centrifuge, purchased from semer feishale, model Pico 17;
electric grinder, available from cut, model DREMEL 3000.
Printer available from Epson, model EPSON4400
Infrared thermal imagers are available from FLIR corporation, model E40.
Example 1
This example illustrates the preparation of a liquid metal conductive ink.
0.3g of polyethylene oxide and 5uL of fluorocarbon surfactant were added to 10mL of distilled water, and stirred for 24 hours to dissolve sufficiently. After the polyethylene oxide was sufficiently dissolved, 3 ml of ethanol was placed In a plastic tube, and 5g of liquid indium gallium tin alloy (In 22% wt Ga 68% wt Sn 10% wt) was added at the same time. Sonication was carried out with an ultrasonic cell disruptor at a range of 30% for 60s, resulting in a grey dispersion of the liquid metal in ethanol. The dispersion was centrifuged at 2000 rpm for 2 minutes, the supernatant removed and sealed for long term storage. Before use, 2mL of polyoxyethylene aqueous solution is added into the precipitate of the liquid metal particles, and the mixture is stirred uniformly for use.
Example 2
This example illustrates the preparation of a liquid metal conductive ink.
5g of polyvinylpyrrolidone is added into 100mL of n-decanol, and the mixture is stirred for 24 hours to be fully dissolved to prepare an alcoholic solution of the polyvinylpyrrolidone. After the polyvinylpyrrolidone (PVP) was fully dissolved, 35 ml of the solution was placed In a beaker and 100g of liquid indium gallium eutectic alloy (Ga 75.5% wt In 24.5% wt) was added at the same time. Stirring the liquid metal by an electric grinder at the speed of 20000 revolutions per minute for 20 minutes, dispersing the metal into small particles in the solution, thus obtaining the gray liquid metal ink, and stirring the ink uniformly for use.
Example 3
This example is used to illustrate the preparation of flexible stretchable conductive traces on the surface of a smart garment.
The T-shirt silk-screen printing ink is printed on the inner side of the elastic long-sleeve swimsuit as a base layer according to the pattern of a figure 1 in a silk-screen printing mode by using a silk-screen printing table, and is dried for 20 minutes at the temperature of 80 ℃. The liquid metal ink of example 1 or 2 was then printed on the substrate layer using a screen pad and dried at 80 degrees celsius for 30 minutes or at room temperature for 24 hours. And finally, printing the T-shirt silk-screen printing ink on the liquid metal ink layer by using a silk-screen printing table for packaging the liquid metal layer. And drying the mixture for 20 minutes in an environment of 80 ℃. After curing, the elastic long-sleeve swimsuit is stretched by 30% so that the liquid metal ink is conductive.
Example 4
This example is used to illustrate the preparation of flexible stretchable conductive traces on the surface of a smart garment.
The invention uses a commercial thermal transfer printing method, commercial thermal transfer printing ink is printed on transfer paper by a printer according to the pattern shown in figure 1, then the temperature of the thermal transfer printing machine is set to be 180 ℃, the time is set to be 100 seconds, and the pattern on the transfer paper is transferred to the inner side of the elastic long-sleeve swimming suit to be used as a substrate layer. Adding the prepared conductive ink into a piezoelectric type spray head, wherein the diameter of the spray head is 40 micrometers, printing liquid metal ink on a substrate layer, and drying for 30 minutes at 80 ℃. And finally, printing the T-shirt silk-screen printing ink on the liquid metal ink layer by using a silk-screen printing table for packaging the liquid metal layer. And after curing for 20 minutes at the temperature of 80 ℃, stretching the elastic long-sleeve swimsuit by 30% to enable the liquid metal ink to be conductive.
Example 5
This embodiment is used to illustrate the integration of sensors on conductive traces on the surface of a smart garment.
(1) An electrocardio-electrode.
The electrocardio-electrode adopts medical conductive hydrogel or conductive fiber, the conductive hydrogel is cut into a round shape with the diameter of 25mm, the conductive fiber is made into conductive cloth with the diameter of 25mm, and the conductive cloth is fixed at the corresponding position of the electrocardio-electrode by silica gel. As shown in fig. 1.
The electrocardio-electrode lead is designed according to actual requirements, the position of clothes corresponds to a specific part of a body, R is 1/3 parts outside a right clavicle, R is 1/3 parts outside the left clavicle, F is arranged on the left clavicle, N is arranged on the costal surface at the intersection of a left axillary anterior line and a costal arch, and v1 is arranged on the costal surface at the intersection of the right axillary anterior line and the costal arch: fourth intercostal space at the right sternal margin v 2: sternal left edge fourth intercostal v 3: midpoint v4 of the line connecting v2 and v 4: v5 at the intersection of the left mid-clavicular line and the 5 th intercostal: left anterior axillary line at level v6 with v 4: the left axillary midline is at the same level as v 4. Fig. 1 includes 6 electrocardio-electrodes, i.e. R, L, F, N, v1 and v 5. In order to avoid the pollution of the skin caused by the direct contact of the liquid metal and the skin, the invention covers a layer of conductive material, such as conductive hydrogel, conductive fiber and the like, on the liquid metal electrode, and the covering mode of the conductive hydrogel is to directly paste a medical conductive hydrogel sheet on the liquid metal electrode and fix the sheet by buttons. The covering mode of the conductive fiber is that the conductive fiber is directly woven into conductive cloth to cover the liquid metal electrode.
The heating constant temperature module comprises a heating coil and a temperature sensor which are made of liquid metal. The heating coil of the liquid metal is serpentine and generates joule heat when current passes through it. Temperature sensors are integrated around the heating coil for monitoring body temperature and the temperature of the coil. When the body temperature is lower than the specified value, the heating coil works to generate heat, and stops working after reaching the specified temperature, thereby realizing the function of constant temperature.
Besides the electrocardio-electrode and the heating coil which can be directly printed, the intelligent clothing reserves the interfaces of the sensors and is used for various sensors such as a temperature sensor, a stress strain sensor, an electrochemical sensor and the like.
A controller section. The controller is connected with each sensor through the contact of the liquid metal interconnection wire. The controller is an integrated circuit responsible for providing voltage, collecting and processing signals of the sensors, and sending the signals of the sensors to a user terminal.
(2) A temperature sensor.
The invention connects a commercial temperature sensor on a reserved interface, the interface is connected by liquid indium gallium eutectic alloy, and is packaged by silica gel.
(3) A strain sensor.
The invention adopts a screen printing technology, liquid metal ink is printed on a silica gel substrate according to the shape of a serpentine, and the silica gel substrate is dried for 20 minutes at the temperature of 80 ℃. And then stretching the silica gel substrate, giving 100% strain, and recovering the deformation to be used as a strain sensor. And connecting the strain sensor to the corresponding position on the clothes. The interface is connected by liquid indium gallium eutectic alloy and is packaged by silica gel.
(4) An electrochemical electrode.
The invention integrates a potassium ion electrode as an electrochemical electrode. The invention adopts a screen printing method to print carbon working electrode ink and silver/silver chloride reference electrode ink on a polyethylene glycol terephthalate film respectively to prepare a working electrode and a reference electrode, wherein the electrodes are rectangles with 2 mm x 2 mm, the electrodes are led out by leads printed by the carbon working electrode ink with the line width of 1 mm, and the leads are partially encapsulated by silica gel. 2 mg of valinomycin, 0.5 mg of sodium tetraphenylborate, 32.7 mg of polyvinyl chloride, and 64.7 mg of bis (2-ethylhexyl) sebacate were added to 350. mu.l of cyclohexanone to be sufficiently dissolved. 20 microliters of the above mixed solution was dropped on the working electrode and dried overnight. Then, 79.1 mg of polyvinyl butyral and 50 mg of sodium chloride were added to 1 ml of methanol to prepare a mixed solution, and 20. mu.l of the mixed solution was dropped onto a reference electrode, and dried overnight, to thereby prepare a potassium ion electrode. And connecting the electrode to a reserved interface on the clothes for monitoring the concentration of potassium ions in sweat.
Test example 1
This test example is used to illustrate the smart garment detection electrocardiosignal (8 lead) of the present invention.
The invention the electrocardio-electrode of example 5 was prepared on a garment. The experimenter wears the garment so that the electrodes are in close contact with the skin. An electrocardiogram signal as in fig. 2A can be obtained.
Test example 2
This test example is used to illustrate the detection of potassium ion signals using the smart clothing of the present invention.
The present invention prepares the potassium ion electrode of example 5 on clothes. The electrodes on the smart clothes were treated with potassium chloride solutions at concentrations of 0mmol/L, 3.125mmol/L, 6.25mmol/L, 12.5mmol/L, 25mmol/L, 50mmol/L, and 100mmol/L, respectively. To demonstrate that the detection of potassium ions is not affected by the tensile deformation of the laundry, 30% strain was applied to the laundry when 12.5mmol/L potassium chloride solution was added. After the potassium chloride solution with different concentrations is treated, the intelligent clothes can output different potential values, as shown in fig. 2B.
Test example 3
This test example is used to illustrate the use of the smart garment of the present invention for motion monitoring.
The invention prepares the strain sensor of example 5 on a garment. The experimenter does the chest expanding movement after wearing the clothes, the strain sensor is stretched, the resistance of the strain sensor changes, and therefore the movement state of the experimenter is detected, and the experimenter is shown in figure 2C.
Test example 4
This test example is used to illustrate the effect of the heating thermostat module using the smart clothes of the present invention.
Example 5 heating thermostat module was prepared on laundry. The temperature of the incubation was preset to 42 degrees celsius. The test was started at normal temperature. The temperature change of the heating coil of the intelligent clothes is monitored in real time by using an infrared thermal imager. The temperature of the heating coil area can reach 42 degrees celsius within 10 minutes and can be maintained at this temperature at all times. As shown in fig. 3.
Although the present invention has been described to a certain extent, it is apparent that appropriate changes in the respective conditions may be made without departing from the spirit and scope of the present invention. It is to be understood that the invention is not limited to the described embodiments, but is to be accorded the scope consistent with the claims, including equivalents of each element described.
Claims (10)
1. An intelligent liquid metal-based high elasticity garment, comprising a controller portion and a functional portion, wherein:
the functional part includes: the device comprises an electrophysiological detection module, an electrochemical detection module and a heating and heat-preserving module; and is
The interconnection wire part, the heating part, the electrocardio-electrode part and the contact used for the electronic device and the sensor of the intelligent clothes are composed of liquid metal conducting layers.
2. The smart garment of claim 1, wherein the garment further comprises an interface for a sensor; preferably, the sensor is selected from one or more of: temperature sensors, stress-strain sensors, electrochemical sensors.
3. Method for preparing a smart garment according to claim 1 or 2, characterized in that it comprises the following steps:
(1) preparing liquid metal ink;
(2) printing a base layer;
(3) printing a liquid metal layer;
(4) printing an insulating layer;
(5) stretching;
(6) integration of intelligent clothing.
4. The method according to claim 3, wherein in step (1), the liquid metal ink is prepared by: dissolving a macromolecule in a solvent, and fully stirring and dissolving to prepare a solution; adding liquid metal into the solution, and preparing the liquid metal into nano-sized or micro-sized particles by a physical method to prepare the liquid metal ink; wherein:
the polymer is preferably selected from one or more of the following: polyvinylpyrrolidone, polyvinyl alcohol, polyoxyethylene, polyacrylamide, polyurethane, polyacrylic acid, polylactic acid, polyglycolic acid, polylactic acid-glycolic acid copolymer, polycaprolactone;
the solvent is preferably selected from one or more of the following: water, alcohol solutions, acetone;
the mass fraction of the solution is preferably 0.5-20%;
the liquid metal is preferably a metal with a melting point below 200 degrees celsius, and further preferably the liquid metal is selected from one or more of the following: gallium, mercury, gallium-indium alloy, gallium-indium-tin alloy, bismuth-tin-lead-indium alloy; most preferably, the liquid metal is preferably a gallium indium eutectic alloy;
the concentration of the liquid metal in the liquid metal ink is preferably 0.1g/mL-5g/mL, and more preferably 3 g/mL; and/or
The physical method is preferably ultrasound and/or high speed rotational shear.
5. The method according to claim 3 or 4, wherein in step (1):
the liquid metal ink also comprises a surfactant; preferably, the surfactant is selected from one or more of the following: fluorocarbon surfactant, disodium lauryl sulfosuccinate, span, tween, sodium dodecyl benzene sulfonate and potassium dodecyl phosphate; more preferably, the mass fraction of the added surfactant is 0.05% -1%; and/or
The liquid metal ink also comprises a viscosity regulator; preferably, the viscosity modifier is selected from one or more of: chitin, polyethylene wax, alkyl diethanolamide, polyethylene glycol distearate and hydroxyethyl cellulose; more preferably, the viscosity modifier is added in a mass fraction of 0.05% to 1%.
6. The method according to any one of claims 3 to 5, wherein in the step (2), commercial elastic printing paste for clothes is printed on the inner side of the clothes according to a specific pattern;
preferably, the printing method is selected from one or more of the following: screen printing, thermal transfer printing, digital direct injection printing process and ink-jet printing;
more preferably, after printing, the adhesive cement is cured for 5-120 minutes in an environment at 25-200 ℃.
7. The method according to any one of claims 3 to 6, wherein in the step (3), the liquid metal ink prepared in the step (1) is printed on a substrate layer according to a specific pattern;
preferably, the printing method is selected from one or more of the following: screen printing, ink jet printing;
more preferably, after printing, the clothes are dried for 10-30 minutes in an environment of drying for 6-12 hours at room temperature or 80 ℃.
8. The method according to any one of claims 3 to 7, wherein in the step (4), commercial clothing elastic printing paste is printed on the liquid metal layer, the liquid metal interconnection lead part is encapsulated in the insulating paste, and the electrode part and the contact part are not encapsulated by the insulating paste;
preferably, the printing method is selected from one or more of the following: screen printing, thermal transfer printing, digital direct injection printing process and ink-jet printing;
more preferably, after printing, the adhesive cement is placed in an environment with the temperature of 25-200 ℃ for curing for 5-120 minutes; and/or
In the step (5), after printing is finished, the clothes are stretched, and the clothes are made to conduct electricity by applying 20% -200% strain.
9. The method according to any one of claims 3 to 8, wherein in the step (6), the intelligent clothes are integrated, and a controller is connected with each sensor through a contact of a liquid metal interconnection wire;
preferably, the step (6) further comprises covering the liquid metal electrode with a conductive material, wherein the conductive material is selected from one or more of the following materials: conductive hydrogel, conductive polymer, silver foil, copper foil and gold foil.
10. Use of smart clothing according to claim 1 or 2 or made according to the method of any one of claims 3 to 9 for health monitoring and disease treatment.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201811300760.9A CN111134401A (en) | 2018-11-02 | 2018-11-02 | High-elasticity intelligent clothes based on liquid metal, and preparation method and application thereof |
Applications Claiming Priority (1)
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| CN112137191A (en) * | 2020-09-27 | 2020-12-29 | 西安邮电大学 | Work clothes for cleaning |
| CN112801257A (en) * | 2021-01-29 | 2021-05-14 | 南方科技大学 | RFID electronic tag and manufacturing method and system thereof |
| CN112924495A (en) * | 2021-01-29 | 2021-06-08 | 南方科技大学 | Sensing device and manufacturing method thereof |
| CN113397255A (en) * | 2021-07-01 | 2021-09-17 | 云南迈特力医疗技术有限公司 | Multifunctional dress |
| CN113521524A (en) * | 2021-07-19 | 2021-10-22 | 南方科技大学 | Electronic skin tattoo with heating function and preparation method and application thereof |
| CN113768496A (en) * | 2021-09-09 | 2021-12-10 | 清华大学 | Device for monitoring motion state of biological body surface or bionic body inner surface |
| CN114869271A (en) * | 2022-04-01 | 2022-08-09 | 国家纳米科学中心 | Electronic external nervous system for motion detection and preparation method thereof |
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| CN112801257A (en) * | 2021-01-29 | 2021-05-14 | 南方科技大学 | RFID electronic tag and manufacturing method and system thereof |
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