WO2022220369A1

WO2022220369A1 - Skin attachment-type fluid collecting patch, and manufacturing method therefor

Info

Publication number: WO2022220369A1
Application number: PCT/KR2021/019373
Authority: WO
Inventors: 조길원; 손종현
Original assignee: 재단법인 나노기반소프트일렉트로닉스연구단; 포항공과대학교 산학협력단
Priority date: 2021-04-16
Filing date: 2021-12-20
Publication date: 2022-10-20
Also published as: KR102539836B1; KR20220143395A

Abstract

Disclosed are a skin attachment-type fluid collecting patch and a manufacturing method therefor. The skin attachment-type fluid collecting patch according to the present invention has a wedge pattern of hydrophobic/hydrophilic parts and thus enables faster collection of fluids than existing fluid collection devices and is not affected by changes in slope caused by body movements when attached to the skin, and can be used while coupled to various types of sensors.

Description

Skin-attachable fluid collection patch and manufacturing method thereof

The present invention relates to a skin-attached fluid collection patch and a method for manufacturing the same, and more particularly, by forming a water-repellent/hydrophilic wedge pattern, it enables the collection of fluid at a faster speed than that of a conventional fluid collection device, and prevents body movement when the skin is attached. It relates to a fluid collection patch that can be used in combination with various types of sensors and a method for manufacturing the same, regardless of the slope change.

Fluid collection technology using microfluidics channels is a technology that is being used throughout various industries, and it is a technology that makes it easy to analyze unknown fluids by collecting, preserving, and transporting a small amount of fluid. In particular, this fluid collection technology can also be effectively used for the analysis of bodily fluids present in the body, primarily used effectively to collect bodily fluids, and secondly as a device for analyzing bodily fluids in combination with an analysis device. is also used

Body fluids include blood, sweat, tears, and saliva, and these body fluids contain various substances (metabolites, electrolytes, amino acids, hormones, microchemicals, etc.) that indicate the health of our body. Therefore, we can obtain information on health status through bodily fluid analysis, and for this reason, various bodily fluid analysis sensors have been developed. In particular, in the case of sweat, tears, and saliva among various types of body fluids, unlike blood, they are non-invasive and can be continuously collected without pain. Therefore, the development of a wearable type sensor for body fluids capable of non-invasive collection is being actively conducted.

In the case of a wearable sensor, unlike existing fixed-type body fluid analysis devices, it must collect body fluid by itself while attached to the skin and then analyze it. An effective bodily fluid collection technique is very important for accurate analysis because if the collection is too slow, an error in the measurement value may occur. Therefore, for the effective use of wearable sensors, it is necessary to develop a fluid collection system capable of rapidly and efficiently collecting and transporting body fluids continuously secreted from the body. In addition, since body fluid must be collected on the body, it must be manufactured based on a flexible structure, and must be manufactured so that it can be collected and transported regardless of body movement.

Recently, attempts have been made to solve problems caused by sweat collection and contamination using microfluidics channels. However, in the case of the currently used microfluidics channel, it simply acts as a pipe for moving the fluid, and the sweat moves by the pressure of sweat. There is a problem in that it takes a lot of time to move the sweat to the part, and the sweat is wasted in filling the channel, thereby reducing the collection efficiency.

Therefore, there is a need for research on a fluid collection device that can quickly and efficiently collect and transport the body fluid secreted from the body, and can collect and transport it regardless of the body's movement on the body.

An object of the present invention is to solve the above problems, and to provide a fluid collecting patch capable of collecting fluid at a high speed, regardless of body movement when the skin is attached, and a method for manufacturing the same.

Another object of the present invention is to provide a fluid collection patch that can be used in combination with various types of sensors and a method for manufacturing the same.

According to an aspect of the present invention, a first flexible substrate 100; a channel part 200 formed on the first flexible substrate 100; a second flexible substrate 300 formed on the channel part 200; and a support portion 400 positioned between the first flexible substrate 100 and the second flexible substrate 300 and including a pillar 410 formed on the outside of the channel portion 200; The channel part 200 is formed on the first flexible substrate 100, and a first pattern layer including a first hydrophilic part 211 having a hydrophilic surface and a first water repellent part 212 having a water repellent surface ( 210); a second pattern layer 220 formed to be spaced apart from the first pattern layer 210 and including a second hydrophilic portion 221 having a hydrophilic surface and a second water repellent portion 222 having a water repellent surface; and a channel space 230 formed between the first pattern layer 210 and the second pattern layer 220 .

In addition, the hydrophilic surface may be a superhydrophilic surface, and the water repellent surface may be a superhydrophobic surface.

In addition, the hydrophilic surface may have a water contact angle of 0 to 20°, and the water-repellent surface may have a water contact angle of 120 to 180°.

In addition, the hydrophilic surface may have a water contact angle of 0 to 10°, and the water-repellent surface may have a water contact angle of 150 to 180°.

In addition, the hydrophilic surface may have a water contact angle of 0 to 5°, and the water-repellent surface may have a water contact angle of 160 to 180°.

In addition, the hydrophilic surface The hydrophilic surface and the water repellent surface may each have a fine concavo-convex shape.

Also, the first pattern layer 210 and the second pattern layer 220 may have patterns corresponding to each other.

In addition, the first hydrophilic part 211 and the second hydrophilic part 221 may have a pattern in which diameters decrease from the center of the patch to the edge in the horizontal direction.

Also, the pattern may be a wedge pattern.

In addition, the first water repellent part 212 includes a first 'water repellent part 2121 and a first "water repellent part 2122 spaced apart from the first water repellent part 2121, and the first hydrophilicity A portion 211 is positioned between the first 'water repellent part 2121 and the first" water repellent part 2122, and the second water repellent part 222 is a second 'water repellent part 2221 and the second' and a second "water repellent part 2222 positioned spaced apart from the water repellent part 2221, and the second hydrophilic part 221 is the second' water repellent part 2221 and the second" water repellent part 2222. can be located between

In addition, the first hydrophilic part 211 and the second hydrophilic part 221 may each independently be in contact with the pillar 410 .

In addition, the first hydrophilic part 211 and the second hydrophilic part 221 include first

hydrophilic layers

21101 and 22101, water repellent layers 21102 and 22102, and second hydrophilic layers 21103 and 22103, respectively. They may be sequentially stacked.

In addition, each of the first flexible substrate and the second flexible substrate is polydimethylsiloxane (PDMS), polyimide (PI), polyamide, polybutadiene, styrene-butadiene rubber ( Styrene-butadiene rubber), Styrene-Ethylene-butadiene-styrene rubber (SEBS), Ecoflex, poly(p-xylylene), parylene, Cytop, polystyrene (PS), poly(methyl methacrylate, PMMA), poly(vinyl pyrrolidone, PVP), polyurea, polyurethane, polyethylene terephthalate , polybutylene terephthalate, polyethylene naphthalate, may include one or more selected from the group consisting of polyethylene and polypropylene.

In addition, the first hydrophilic part or the second hydrophilic part may include a hydrophilic polymer and hydrophilic particles, respectively.

In addition, the hydrophilic particles are silica (Silica), aluminum oxide (Al ₂ O ₃ ), titanium oxide (TiO ₂ ), tin oxide (SnO ₂ ), iron oxide (Al ₂ O ₃ ), magnesium oxide (MgO), graphite ( Graphite) and may include one or more selected from the group consisting of cellulose (Cellulose).

In addition, the hydrophilic polymer is polyvinyl alcohol (PVA), polyacrylic acid (PAA), polyethylene glycol (PEG), polylactic acid (PLA), polyglycolide (PGA) and polylactate coglyclate (PLGA) It may include one or more selected from the group consisting of.

In addition, in the first water repellent part 212 and the second water repellent part 222 , first

hydrophilic layers

21211 , 21221 , 22211 , 22221 and

water repellent layers

21212 , 21222 , 22212 and 22222 are sequentially stacked. it may have been

In addition, each of the first water repellent part or the second water repellent part may include a water repellent material.

In addition, the water repellent material is methyltrichlorosilane (methyltrichlorosilane), methyltrimethoxysilane (methyltrimethoxysilane), methyltriethoxysilane (methyltriethoxysilane), methylpropoxysilane (methyltri-n-propoxysilane), methyltrismethoxy Toxysilane (methyltrismethoxyethoxysilane), methyltriacetoxysilane (methyltriacetoxysilane), tris(dimethylamino)methylsilane, triscyclohexylaminomethylsilane (tris(cyclohexylamino)methylsilane), methyltrismethylethylketoxymino Silane (methyltris (methylethylketoximino)silane), ethyltrichlorosilane (ethyltrichlorosilane), ethyltrimethoxysilane (ethyltrimethoxysilane), ethyltriethoxysilane (ethyltriethoxysilane), ethyltriacetoxysilane (ethyltriacetoxysilane), propyltrichlorosilane ( propyltrichlorosilane, propyltrimethoxysilane, propyltriethoxysilane, n-butyltrichlorosilane, n-butyltrimethoxysilane, butyltriethoxysilane (n-) butyltriethoxysilane, phenyltrichlorosilane, phenyltriethoxysilane, hexyltrichlorosilane, hexyltrimethoxysilane, hexyltriethoxysilane, heptyltrichlorosilane (heptyltrichlorosilane), octyltrichlorosilane, octyltrimethoxysilane (octyltri) methoxysilane, octyltriethoxysilane, decyltrichlorosilane, decyltrimethoxysilane, decyltriethoxysilane, undecyltrichlorosilane, dodecyltrichlorosilane Dodecyltrichlorosilane, dodecyltrimethoxysilane, dodecyltriethoxysilane, tetradecyltrichlorosilane, hexadecyltrichlorosilane, hexadecyltrimethoxysilane (hexadecyltrimethoxysilane), hexadecyltriethoxysilane, octadecyltrichlorosilane, octadecyltrimethoxysilane, octadecyltriethoxysilane, octadecyltridimethylaminosilane (octadecyltris(dimethylamino)silane), trichloroperfluorooctylsilane (Trichloro(1H,1H,2H,2H-perfluorooctyl)silane), tridecafluorotetrahydrooctyltrimethoxysilane ((tridecafluoro-1,1,2) ,2-tetrahydrooctyl)trimethoxysilane), tridecafluorotetrahydrooctyltriethoxysilane ((tridecafluoro-1,1,2,2-tetrahydrooctyl)triethoxysilane), heptadecafluorotetrahydrodecyltrichlorosilane ((heptadecafluoro- 1,1,2,2-tetrahydrodecyl)trichlorosilane), heptadecafluorotetrahydrodecyltrimethoxysilane ((heptadecafluoro-1,1,2,2-tetrahydrodecyl) trimethoxysilane), heptadecafluoro-tetrahydrodecyltriethoxysilane (heptadecafluoro-1,1,2,2-tetrahydrodecyl)triethoxysilane), henecosyltetrahydrodecyltriethoxysilane 2-tetrahydrodecyltrichlorosilane), heptafluoroisopropoxypropyltrichlorosilane (heptafluoroisopropoxypropyltrichlorosilane), and heptafluoroisopropoxypropyltrimethoxysilane (heptafluoroisopropoxypropyltrimethoxysilane) may include at least one selected from the group consisting of.

In addition, the fluid collecting patch 10 is a collecting unit 500; and a collecting space 600 located on the collecting unit 500 and connected to the channel space 230 .

In addition, the fluid collecting patch 10 may include a plurality of channel parts 200 , and the plurality of channel parts 200 may be radially disposed around the collecting part 500 .

In addition, the fluid collection patch 10 further includes at least one sensor 700 selected from the group consisting of a blood glucose sensor, a lactic acid sensor, an alcohol sensor, and an electrolyte sensor, and the sensor 700 is disposed in the collection space 600 ) can be located on

In addition, the fluid collecting patch 10 includes a plurality of fluid inlet 800 passing through the first flexible substrate 100 and the first hydrophilic part 211 in a vertical direction; and an adhesive layer 900 positioned under the first flexible substrate 100 .

In another aspect of the present invention, (a) a first flexible substrate 100, and a support 400 including a pillar 410 formed on the first flexible substrate 100, and the first flexible Manufacturing a lower plate formed on the substrate 100 and including a first pattern layer 210 including a first hydrophilic portion 211 having a hydrophilic surface and a first water-repellent portion 212 having a water-repellent surface ; (b) a second pattern including a second flexible substrate 300 and a second hydrophilic portion 221 formed on the second flexible substrate and having a hydrophilic surface and a second water-repellent portion 222 having a water-repellent surface manufacturing a top plate including the layer 220; and (c) positioning the second flexible substrate 300 of the upper plate on the support part 400 of the lower plate to prepare the fluid collecting patch according to claim 1; do.

In addition, in step (a) (a-1) preparing a support 400 including a pillar 410 and a first flexible substrate 100 coupled to the support, and surface-treating the surface of the flexible substrate to be hydrophilic to do; (a-2) forming a first hydrophilic layer (21101, 21211, 21221) by coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated first flexible substrate 100; (a-3) coating a solution containing a water repellent material on the first

hydrophilic layers

21101, 21211, and 21221 of the first flexible substrate 100 on the first

hydrophilic layers

21101, 21211, 21221 forming a water repellent layer (21102, 21212, 21222); (a-4) surface-treating the surface of the water-repellent layer 21102 to be hydrophilic; and (a-5) coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated water-repellent layer 21102 to form a second hydrophilic layer 21103 to prepare the lower plate; can do.

In addition, in the step (a-5), the second hydrophilic layer may have a pattern as the coating progresses to a portion of the water repellent layer.

In addition, the step (a) comprises the steps of (a-1') preparing a support portion 400 including a pillar 410 and a first flexible substrate 100 coupled to the support portion; (a-2') coating a solution containing a water repellent material on the first flexible substrate 100 to form a first water repellent portion 212 on the first flexible substrate 100; and (a-3') treating a portion of the first water repellent portion 212 to be hydrophilic to form the first hydrophilic portion 211 .

In addition, in step (a-3'), as a part of the first water repellent part 212 is treated to be hydrophilic, the first hydrophilic part 211 may have a pattern.

In addition, the hydrophilic treatment in step (a-3') may be performed by any one selected from the group consisting of reactive ion etching (RIE) and UV plasma treatment.

In addition, the step (b) comprises the steps of (b-1) surface-treating the surface of the second flexible substrate 300 to be hydrophilic; (b-2) forming a second hydrophilic layer (22101, 22211, 22221) by coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated second flexible substrate 300; (b-3) coating a solution containing a water repellent material on the second

hydrophilic layers

22101, 22211, and 22221 of the second flexible substrate 300 on the second

hydrophilic layers

22101, 22211, 22221 forming a water repellent layer (22102, 22212, 22222); (b-4) treating the surface of the water repellent layer 22102 to be hydrophilic; and (b-5) coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated water-repellent layer 22102 to form a second hydrophilic layer 22103 to prepare the top plate; can do.

In addition, in the step (b-5), the second hydrophilic layer may have a pattern as the coating progresses to a portion of the water repellent layer.

In addition, the step (b) is (b-1') preparing a second flexible substrate (300); (b-2') coating a solution containing a water repellent material on the second flexible substrate 300 to form a second water repellent portion 222 on the second flexible substrate 300; and (b-3') treating a portion of the second water repellent portion 222 to be hydrophilic to form the second hydrophilic portion 221 .

In addition, in step (b-3'), as a part of the second water repellent part 222 is treated to be hydrophilic, the second hydrophilic part 221 may have a pattern.

In addition, the hydrophilic treatment in step (b-3') may be performed by any one selected from the group consisting of reactive ion etching (RIE) and UV plasma treatment.

The skin-attached fluid collection patch of the present invention can collect fluid at a high speed, and can collect fluid regardless of body movement when the skin is attached.

In addition, since the skin-attached fluid collection patch of the present invention can be used in combination with various types of sensors, it is possible to increase the overall utility value of using the sensor.

In addition, the skin-attached fluid collection patch of the present invention enables the spontaneous movement of the fluid entering the channel by using a phenomenon in which water droplets move on the super-hydrophobic/super-hydrophilic wedge pattern.

Since these drawings are for reference in describing an exemplary embodiment of the present invention, the technical spirit of the present invention should not be construed as being limited to the accompanying drawings.

1A is a cross-sectional view showing a first flexible substrate, a channel portion, and a second flexible substrate of the fluid collecting patch according to an embodiment of the present invention.

Figure 1b shows the structure of the fluid collection patch according to an embodiment of the present invention.

1c is a cross-sectional view of a first flexible substrate, a channel portion, and a second flexible substrate of the fluid collecting patch according to an embodiment of the present invention.

1D is a schematic view illustrating a structure and a cross-sectional view of a fluid collecting patch according to an embodiment of the present invention, and a fluid movement phenomenon in a channel portion.

Figure 1e shows the chemical structure and water contact angle (surface energy) of the surface of the patterned layer when manufacturing a fluid trap patch according to an embodiment of the present invention.

FIG. 1f illustrates the role of a key process for making the wedge pattern surface to be stably maintained in the pattern layer of the fluid collection patch manufactured according to Example 1, and 1,000 cycles of tensioning the upper plate manufactured according to Preparation Example 2-1 The state of the surface after the test is shown with an optical microscope (OM) image.

1g is an observation graph showing the change in contact angle with time of each surface of the water repellent part/hydrophilic part in the upper plate prepared according to Preparation Example 2-1.

1H is a schematic diagram of a method for manufacturing a fluid collection patch according to an embodiment of the present invention.

1I is a schematic diagram of a method for manufacturing a fluid collection patch according to an embodiment of the present invention.

Figure 2a is a simplified representation of the force due to the surface tension applied to the sweat drop on the wedge pattern in the pattern layer of the fluid collection patch according to an embodiment of the present invention.

Figure 2b is a simplified representation of the force due to the surface tension applied to the sweat drop on the wedge pattern in the pattern layer of the fluid collection patch according to an embodiment of the present invention.

FIG. 2c is a graph showing the change in laplace pressure and the change in speed according to the wedge angle of the pattern layer in the upper plate manufactured according to Preparation Example 2-1.

FIG. 2d shows that fluid (sweat) is present on each wedge pattern when only the lower plate manufactured according to Preparation Example 2-1 is used (open structure) and when the fluid collection patch manufactured according to Example 1 is used (closed structure) It is shown by comparing the difference in volume and area.

FIG. 2e shows a comparison of the volume and length of the fluid located in the channel space according to the change in the height of the channel space in the fluid collecting patch manufactured according to Example 1. FIG.

FIG. 2f shows a comparison of the fluid movement speed between the channel part (right figure) of the fluid collecting patch manufactured according to Example 1 and the channel part (left figure) of the fluid collecting patch manufactured according to Comparative Example 1. FIG.

3a is a graph showing the change in the movement speed of the fluid according to the change in gravity while changing the gradient of the fluid collecting patch prepared according to Example 1, by observing and measuring the change.

FIG. 3b is a photograph of actually observing the movement of a fluid with a high-speed camera when measuring FIG. 3a.

FIG. 4A is a diagram illustrating that, when a fluid is collected using a plurality of channel units in a fluid collecting patch according to an embodiment of the present invention, the fluid can be quickly collected.

4B shows an actual skin adhesion image of the fluid collection patch prepared according to Example 2. FIG.

FIG. 4c shows a comparison of the speed at which the fluid is collected in the collecting unit where each fluid is collected when the fluid collecting patch prepared according to Example 1 and the fluid collecting patch prepared according to Comparative Example 1 are used.

FIG. 4d shows a case in which a microfluidics channel is not used (No micro-channel), a case in which an existing microfluidics channel is used (Micro-channel), and a fluid trapping patch prepared according to Example 2 (Wedge patterned channel) is used. In this case, the sampling time required to fill the collection unit is predicted using a computational model and displayed as a graph.

FIG. 4e shows the phenomenon in which sweat is collected in the fluid collection patch prepared according to Example 2 when sweat is injected at a rate of 2 μL/min-cm ² using an artificial sweat secretion system to prove the prediction result of FIG. 4D. The results of observations over time are shown.

FIG. 4f is a measurement of the time the sweat is filled in the collecting part of the fluid collecting patch prepared according to Example 2 under the same conditions as in FIG. 4e to prove the prediction result of FIG. 4d.

FIG. 4G shows the results of the experiment performed in FIG. 4F on actual skin.

5A is a diagram illustrating a form in which a fluid collecting patch and a wearable sweat sensor are combined according to an embodiment of the present invention.

5B is a diagram illustrating the measurement of the glucose concentration in sweat by combining the fluid collection patch prepared according to Example 2 and the wearable glucose sensor with reference to FIG. 5A and comparing it with the blood glucose concentration.

Hereinafter, embodiments of the present invention will be described in detail with reference to the accompanying drawings so that those of ordinary skill in the art can easily carry out the present invention.

However, the following description is not intended to limit the present invention to specific embodiments, and when it is determined that a detailed description of a related known technology may obscure the gist of the present invention in describing the present invention, the detailed description thereof will be omitted. .

The terminology used herein is used only to describe specific embodiments, and is not intended to limit the present invention. The singular expression includes the plural expression unless the context clearly dictates otherwise. In the present application, terms such as "comprise" or "have" are intended to designate that a feature, number, step, operation, element, or combination thereof described in the specification exists, but is one or more other features or It should be understood that the possibility of the presence or addition of numbers, steps, acts, elements, or combinations thereof is not precluded in advance.

In addition, terms including ordinal numbers such as first, second, etc. to be used hereinafter may be used to describe various elements, but the elements are not limited by the terms. The above terms are used only for the purpose of distinguishing one component from another. For example, without departing from the scope of the present invention, a first component may be referred to as a second component, and similarly, a second component may also be referred to as a first component.

In addition, when it is said that a component is "formed" or "stacked" on another component, it may be formed or laminated directly attached to the front surface or one surface on the surface of the other component. It should be understood that there may be other components in the .

Hereinafter, the skin-attachable fluid collection patch of the present invention and a manufacturing method thereof will be described in detail. However, this is provided as an example, and the present invention is not limited thereto, and the present invention is only defined by the scope of the claims to be described later.

1A and 1C are cross-sectional views of a first flexible substrate, a channel portion, and a second flexible substrate of a fluid collection patch according to an embodiment of the present invention, and FIG. 1B is a fluid collection patch according to an embodiment of the present invention. structure is shown. 1D is a schematic view illustrating a structure and a cross-sectional view of a fluid collecting patch according to an embodiment of the present invention, and a fluid movement phenomenon in a channel portion.

1a to 1d, the present invention is a first flexible substrate 100; a channel part 200 formed on the first flexible substrate 100; a second flexible substrate 300 formed on the channel part 200; and a support portion 400 positioned between the first flexible substrate 100 and the second flexible substrate 300 and including a pillar 410 formed on the outside of the channel portion 200; The channel part 200 is formed on the first flexible substrate 100, and a first pattern layer including a first hydrophilic part 211 having a hydrophilic surface and a first water repellent part 212 having a water repellent surface ( 210); a second pattern layer 220 formed to be spaced apart from the first pattern layer 210 and including a second hydrophilic portion 221 having a hydrophilic surface and a second water repellent portion 222 having a water repellent surface; and a channel space 230 formed between the first pattern layer 210 and the second pattern layer 220 .

In addition, the water contact angle of the hydrophilic surface is 0 to 20˚, the water contact angle of the water repellent surface may be 120 to 180˚, preferably, the water contact angle of the hydrophilic surface is 0 to 10˚, the water repellent surface may have a water contact angle of 150 to 180°.

When the water contact angle of the hydrophilic surface exceeds 20˚, it is not preferable because water is not sufficiently attracted to the surface, and when the water contact angle of the water-repellent surface is less than 120˚, water cannot be pushed out from the surface, and It is undesirable as it interferes with movement.

In addition, the hydrophilic surface and the water-repellent surface may each have a fine concavo-convex shape.

Also, each of the first hydrophilic part 211 and the second hydrophilic part 221 may have a pattern in which the diameter decreases from the center of the patch to the edge in the horizontal direction, and in detail, the pattern is a wedge pattern. can be

hydrophilic layers

In addition, each of the first flexible substrate and the second flexible substrate is polydimethylsiloxane (PDMS), polyimide (PI), polyamide, polybutadiene, styrene-butadiene rubber ( Styrene-butadiene rubber, Styrene-Ethylene-butadiene-styrene rubber, Ecoflex, poly(p-xylylene, parylene), Cytop ( Cytop), polystyrene (PS), poly(methyl methacrylate, PMMA), polyvinyl pyrrolidone (poly(vinyl pyrrolidone), PVP), polyurea, polyurethane, polyethylene terephthalate, poly It may include at least one selected from the group consisting of butylene terephthalate, polyethylene naphthalate, polyethylene and polypropylene, and preferably include polydimethylsiloxane (PDMS).

The hydrophilic particles are silica (Silica), aluminum oxide (Al ₂ O ₃ ), titanium oxide (TiO ₂ ), tin oxide (SnO ₂ ) iron oxide (Al ₂ O ₃ ), magnesium oxide (MgO), graphite (Graphite) and It may include one or more selected from the group consisting of cellulose, preferably silica.

The hydrophilic polymer is made of polyvinyl alcohol (PVA), polyacrylic acid (PAA), polyethylene glycol (PEG), polylactic acid (PLA), polyglycolide (PGA) and polylactate coglyclate (PLGA). It may include one or more selected from the group, preferably polyvinyl alcohol.

hydrophilic layers

21211 , 21221 , 22211 , 22221 and water repellent layers 21212 , 21222 , 22212 and 22222 are sequentially stacked. it may have been

In addition, the first water repellent part 212 and the second water repellent part 222 may each include a water repellent material, and the water repellent material may include methyltrichlorosilane, methyltrimethoxysilane, Methyltriethoxysilane, methyltri-n-propoxysilane, methyltrismethoxyethoxysilane, methyltriacetoxysilane, trisdimethylaminomethylsilane (tris) (dimethylamino)methylsilane), triscyclohexylaminomethylsilane (tris(cyclohexylamino)methylsilane), methyltrismethylethylketoximinosilane (methyltris(methylethylketoximino)silane), ethyltrichlorosilane, ethyltrimethoxysilane (ethyltrimethoxysilane), ethyltriethoxysilane, ethyltriacetoxysilane, propyltrichlorosilane, propyltrimethoxysilane, propyltriethoxysilane, butyltrichlorosilane Losilane (n-butyltrichlorosilane), butyltrimethoxysilane (n-butyltrimethoxysilane), butyltriethoxysilane (n-butyltriethoxysilane), phenyltrichlorosilane (pentyltrichlorosilane), phenyltriethoxysilane (pentyltriethoxysilane), hexyltrichlorosilane Silane (hexyltrichlorosilane), hexyltrimethoxysilane (hexyltrimethoxysilane), hexyltriethoxysilane (hexyltriethoxysilane), heptyltrichlorosilane (heptyltrichlorosila) ne), octyltrichlorosilane, octyltrimethoxysilane, octyltriethoxysilane, decyltrichlorosilane, decyltrimethoxysilane, decyltriethoxysilane Silane (decyltriethoxysilane), undecyltrichlorosilane (undecyltrichlorosilane), dodecyltrichlorosilane (dodecyltrichlorosilane), dodecyltrimethoxysilane (dodecyltrimethoxysilane), dodecyltriethoxysilane (dodecyltriethoxysilane), tetradecyltrichlorosilane (tetradecyltrichlorosilane) ), hexadecyltrichlorosilane, hexadecyltrimethoxysilane, hexadecyltriethoxysilane, octadecyltrichlorosilane, octadecyltrimethoxysilane, Octadecyltriethoxysilane, octadecyltris(dimethylamino)silane, trichloroperfluorooctylsilane (Trichloro(1H,1H,2H,2H-perfluorooctyl)silane), tridecafluoro Rotetrahydrooctyltrimethoxysilane ((tridecafluoro-1,1,2,2-tetrahydrooctyl)trimethoxysilane), tridecafluorotetrahydrooctyltriethoxysilane ((tridecafluoro-1,1,2,2-tetrahydrooctyl) triethoxysilane), heptadecafluorotetrahydrodecyltrichlorosilane ((heptadecafluoro-1,1,2,2-tetrahydrodecyl)trichlorosilane), heptadecafluorotetra Lahydrodecyltrimethoxysilane ((heptadecafluoro-1,1,2,2-tetrahydrodecyl)trimethoxysilane), heptadecafluorotetrahydrodecyltriethoxysilane ((heptadecafluoro-1,1,2,2-tetrahydrodecyl)triethoxysilane ), henecocyl tetrahydrodecyltriethoxysilane (heneicocyl-1,1,2,2-tetrahydrodecyltrichlorosilane), heptafluoroisopropoxypropyltrichlorosilane and heptafluoroisopropoxypropyltrimethoxysilane It may include at least one selected from the group consisting of (heptafluoroisopropoxypropyltrimethoxysilane), preferably octadecyltrichlorosilane.

1C is a cross-sectional view of a fluid collection patch according to an embodiment of the present invention.

Referring to FIG. 1C , the first hydrophilic layer 21101 of the first hydrophilic part 211 may be the same material as the first hydrophilic layers 21211 and 21221 of the first water repellent part 212 , in detail may be on the same layer. In addition, the first hydrophilic layer 22101 of the second hydrophilic part 221 may be the same material as the first

hydrophilic layers

22211 and 22221 of the second water repellent part 212, and in detail, it may be the same layer. have.

Referring to FIG. 1C , the water repellent layer 21102 of the first hydrophilic part 211 may be the same material as the

water repellent layers

21212 and 21222 of the first water repellent part 212, and specifically may be the same layer. have. In addition, the water repellent layer 22102 of the second hydrophilic part 221 may be the same material as the water repellent layers 22212 and 22222 of the second water repellent part 212 , and in detail, it may be the same layer.

FIG. 4A illustrates that when fluid is collected using a plurality of channel units in the fluid collecting patch according to an embodiment of the present invention, sweat can be collected from a large area of skin and collected in one place to increase the collection speed.

Referring to FIG. 4A , the fluid collecting patch 10 may include a plurality of channel parts 200 , and a plurality of the channel parts 200 may be radially arranged around the collecting part 500 . .

Also, referring to FIG. 4A , the size of the fluid collecting patch may be 3 cm in diameter and 1 mm in thickness.

In addition, the fluid collection patch 10 has a blood glucose sensor that detects glucose, a lactate sensor that detects lactate, an alcohol sensor that detects ethanol, and sodium ions (Na ⁺ ), potassium ions ( K ⁺ ), magnesium ions (Mg ²⁺ ) and calcium ions (Ca ²⁺ ) may further include one or more sensors 700 selected from the group consisting of an electrolyte sensor for detecting, preferably a blood glucose sensor may additionally include.

In addition, the sensor 700 may be a chemical sensor or a biological sensor (biosensor).

Also, the sensor 700 may be located on the collection space 600 .

Referring to FIG. 1D , the fluid collecting patch 10 includes a plurality of fluid inlets 800 passing through the first flexible substrate 100 and the first hydrophilic part 211 in a vertical direction; and an adhesive layer 900 positioned under the first flexible substrate 100 .

In addition, the thickness of the adhesive layer may be 0.1 mm.

Figure 1e shows the chemical structure and water contact angle (surface energy) of the surface of the patterned layer when manufacturing the fluid collection patch according to one embodiment of the present invention, and Figure 1F is the one manufactured according to one embodiment of the present invention. It explains the role of a key process that allows the wedge pattern surface to be stably maintained in the pattern layer of the fluid trapping patch.

In the case of a super water-repellent surface, since a flexible polymer is generally made of carbon and has hydrophobic properties, the surface of the flexible substrate can be made into a super water-repellent surface by making the surface of the flexible substrate in the form of micro/nano-sized irregularities.

However, in the case of super-hydrophilic surfaces, unlike super _- repellent surface production, the surface properties of flexible polymers must be made hydrophilic. However, in the case of flexible polymers, hydrophobicity is recovered in half a day due to chain-entanglement. Therefore, in order to produce a surface that can fundamentally maintain hydrophilic properties, it is necessary to make the surface with a material that does not cause chain-entanglement. However, in general, polymers that do not undergo chain-entanglement have weak tensile properties. Therefore, in order to fabricate an ideal surface structure, it was necessary to devise a structure with the characteristics of being able to maintain the surface energy stably while being flexible throughout the substrate.

1e and 1f, the present invention devised a surface structure in which island-shaped hard hydrophilic particles are coated on a flexible polymer in order to satisfy the characteristics that the entire substrate is flexible but the surface is not.

By chemically bonding hydrophilic particles having hydrophilic properties and not having a large change in surface energy on a flexible substrate, a super-hydrophilic layer with irregularities was formed. It is possible to stably form a superhydrophobic layer in the form of

Figure 2a is a simplified representation of the force due to the surface tension received by sweat droplets on the wedge pattern in the channel portion of the fluid collection patch according to an embodiment of the present invention, Figure 2b is a fluid collection patch according to an embodiment of the present invention It is a simplified expression of the force caused by the surface tension applied to the sweat drop on the wedge pattern in the channel part of the

Referring to FIGS. 2A and 2B , the fundamental force that moves the fluid on the wedge pattern is generated by the attraction between the particles constituting the fluid, and the intermolecular attraction between the particles located on the surface of the fluid and the intermolecular force acting on the inside of the fluid It is caused by differences in the intermolecular forces acting between the particles. The force generated by the difference in surface tension is called Laplace pressure, and this force increases as the surface tension of the fluid is strong and the curvature of the fluid droplet increases (Fig. 2a). Therefore, in the case of a fluid on the wedge pattern, the Laplace pressure generated at the oblique interface of the wedge pattern is received, and the force received at this time is in the vertical direction of the interface where the superhydrophobic/superhydrophilic surface is divided, and opposite to the plane containing the convex curved surface of the fluid droplet. direction, in the case of a fluid drop whose diameter is larger than the width of the wedge pattern, it moves in the super-hydrophilic direction by the resultant force of Laplace pressure (Fig. 2b).

The present invention is (a) a first flexible substrate 100, a support portion 400 including a pillar 410 formed on the first flexible substrate 100, and formed on the first flexible substrate (100) and manufacturing a lower plate including a first pattern layer 210 including a first hydrophilic portion 211 having a hydrophilic surface and a first water-repellent portion 212 having a water-repellent surface; (b) a second pattern including a second flexible substrate 300 and a second hydrophilic portion 221 formed on the second flexible substrate and having a hydrophilic surface and a second water-repellent portion 222 having a water-repellent surface manufacturing a top plate including the layer 220; and (c) positioning the second flexible substrate 300 of the upper plate on the support part 400 of the lower plate to manufacture the fluid collecting patch; provides a method of manufacturing a fluid collecting patch comprising.

Referring to Figure 1h, the step (a) is (a-1) to prepare the support portion 400 including the pillar 410 and the first flexible substrate 100 coupled to the support portion, and the surface of the flexible substrate surface treatment with hydrophilicity; (a-2) forming a first hydrophilic layer (21101, 21211, 21221) by coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated first flexible substrate 100; (a-3) coating a solution containing a water repellent material on the first

hydrophilic layers

21101, 21211, and 21221 of the first flexible substrate 100 on the first

hydrophilic layers

22101, 22211, and 22221 of the second flexible substrate 300 on the second

hydrophilic layers

22101, 22211, 22221 forming a water repellent layer (22102, 22212, 22222); (b-4) surface-treating the surface of the water-repellent layer 22102 to be hydrophilic; and (b-5) coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated water-repellent layer 22102 to form a second hydrophilic layer 22103 to prepare the top plate; can do.

Referring to FIG. 1I, the step (a) is (a-1') preparing a support portion 400 including a pillar 410 and a first flexible substrate 100 coupled to the support portion; (a-2') coating a solution containing a water repellent material on the first flexible substrate 100 to form a first water repellent portion 212 on the first flexible substrate 100; and (a-3') treating a portion of the first water repellent portion 212 to be hydrophilic to form the first hydrophilic portion 211 .

In addition, in step (a-3'), as a part of the first water-repellent part 212 is treated to be hydrophilic, the first hydrophilic part may have a pattern.

In addition, in step (b-3'), as a part of the second water repellent part 222 is treated to be hydrophilic, the second hydrophilic part 212 may have a pattern.

The water-repellent material is a hydrophilic particle coated with a water-repellent silane coupling agent. By treating the hydrophilic particles coated with the silane coupling agent with any one selected from the group consisting of reactive ion etching (RIE) and UV plasma treatment in step (a-3') or (b-3'), the silane coupling agent is It is oxidized and, at the same time, forms a hydroxyl group on the surface to form a hydrophilic moiety.

Hereinafter, the present invention will be described in more detail through examples. However, this is for illustrative purposes and the scope of the present invention is not limited thereby.

[Example]

Preparation Example 1: Preparation of lower plate

Preparation Example 1-1: Preparation of a lower plate having a first pattern layer of a first hydrophilic layer/water repellent layer/second hydrophilic layer

1H is a schematic diagram of a method for manufacturing a fluid collection patch according to an embodiment of the present invention. The lower plate of Preparation Example 1-1 was manufactured with reference to the preparation of the lower plate of FIG. 1H.

After pouring the liquid polydimethylsiloxane (Poly(dimethylsiloxane), PDMS) solution (prepared with a ratio of PDMS base to curing agent of 10:1) on the aluminum mold, it was cured in an oven at 120°C for 30 minutes to form the column 410. The support 400 including the support part and the PDMS first flexible substrate 100 combined with the support part were manufactured. At this time, a plurality of fluid inlet (diameter: 0.5 mm) passing through the channel portion of the first flexible substrate (PDMS) was created using an aluminum mold. The surface of the PDMS flexible substrate was surface-treated to be hydrophilic. Specifically, a hydroxyl group was made on the surface of the PDMS flexible substrate by using reactive ion plasma (RIE).

The first hydrophilic layer ( 21101, 21211, 21221) were formed. The spraying coating was made in a state where the PDMS flexible substrate having a hydroxyl functional group on the surface was placed on a hot plate at a high temperature of 140° C., and was patterned using a shadow mask during spray coating. By using the 'PVA/Silica/ADC' mixture, the hydroxyl group on the PDMS flexible substrate and the hydroxyl group on the PVA and silica particles were initiated by ADC and chemically combined, so that the coating state could be stably maintained even on the surface of the PDMS flexible substrate.

The PDMS flexible substrate on which the first hydrophilic layer was formed was put into an Octadecyltrichlorosilane (ODTS) in toluene solution and chemically reacted to form water repellent layers 21102, 21212, 21222 with a contact angle of 160° or more on the first hydrophilic layer.

The surface of the water-repellent layer was treated to be hydrophilic using RIE (Reactive ion plasma). At this time, a very short RIE treatment was performed in a state where only the portion to be raised on the second hydrophilic layer was exposed using a shadow mask to make a hydroxyl group on a part of the surface of the water repellent layer.

After transferring the PDMS flexible substrate including the super water-repellent layer having a hydroxyl group on some surface to a hot plate at 140° C. Spray coating was carried out, and a second hydrophilic layer 21103 of a wedge pattern was formed on the superhydrophobic layer along the pattern of the shadow mask to form the first

hydrophilic layer

21101, 21211, 21221 /

water repellent layer

21102, 21212 and 21222)/a lower plate having the first patterned layer 210 of the second hydrophilic layer 21103 was manufactured.

Preparation Example 1-2: Preparation of a lower plate having a first pattern layer of a first hydrophilic part/a first water-repellent part

1I is a schematic diagram of a method for manufacturing a fluid collection patch according to an embodiment of the present invention. The lower plate of Preparation Example 1-2 was manufactured with reference to the preparation of the lower plate of FIG. 1I.

After pouring a polydimethylsiloxane (PDMS) solution in a liquid state on an aluminum mold, it was cured in an oven at 120° C. for 30 minutes. 1 A flexible substrate 100 was manufactured. At this time, the PDMS solution was prepared in a ratio of PDMS base and curing agent of 10: 1.

Hydrophilic particles Silica particles and water-repellent substance Octadecyltrichlorosilane (ODTS) were chemically reacted, and then the water-repellent particles were extracted using a centrifuge. The extracted water-repellent particles were dispersed in a trace amount of a water-repellent polymer solution Poly(dimethylsiloxane)/Hexane solution 1wt% to prepare a water-repellent silica-polymer dispersion. The water-repellent silica-polymer dispersion was spray-coated on a flexible substrate to form a first water-repellent portion.

After attaching a shadow mask to the surface of the first water-repellent portion, reactive ion plasma (RIE) treatment was performed in a state where only a portion to be formed of the first hydrophilic portion was exposed. The water-repellent polymer on the surface of the water-repellent silica was oxidized and removed by the RIE treatment, and a hydroxyl group was generated on the surface to form a first hydrophilic portion of a wedge pattern. Accordingly, a lower plate having the first pattern layer 210 of the first hydrophilic part 211/first water repellent part 212 was manufactured.

Preparation Example 2: Preparation of top plate

Preparation Example 2-1: Preparation of a top plate having a second pattern layer of a first hydrophilic layer/water repellent layer/second hydrophilic layer

1H is a schematic diagram of a method for manufacturing a fluid collection patch according to an embodiment of the present invention. The top plate of Preparation Example 2-1 was manufactured with reference to the preparation of the top plate of FIG. 1H.

Instead of producing and using the support portion 400 including the pillar 410 and the PDMS first flexible substrate 100 coupled to the support portion, the PDMS second flexible substrate 300 having a flat structure was manufactured and used except that and having a second pattern layer 220 of the first hydrophilic layer (22101, 22211, 22221)/water-repellent layer (22102, 22212, 22222)/second hydrophilic layer (22103) in the same manner as in Preparation Example 1-1 A top plate was prepared.

Preparation Example 2-2: Preparation of a top plate having a second pattern layer of the second hydrophilic part/the second water-repellent part

1I is a schematic diagram of a method for manufacturing a fluid collection patch according to an embodiment of the present invention. The top plate of Preparation Example 2-2 was manufactured with reference to the preparation of the top plate of FIG. 1I.

Instead of producing and using the support portion 400 including the pillar 410 and the PDMS first flexible substrate 100 coupled to the support portion, the PDMS second flexible substrate 300 having a flat structure was manufactured and used except that Then, an upper plate having the second pattern layer 220 of the second hydrophilic part 221 / second water repellent part 222 was manufactured in the same manner as in Preparation Example 1-2.

Preparation Comparative Example 1: Lower plate manufacturing

The first flexible substrate 100 in the same manner as in Preparation Example 1-1, except that a second hydrophilic layer of a stripe pattern was formed instead of a second hydrophilic layer of a wedge pattern was formed. )/first hydrophilic layer (21101, 21211, 21221)/water-repellent layer (21102, 21212, 21222)/second hydrophilic layer (21103) were prepared.

Preparation Comparative Example 2: Preparation of top plate

The second flexible substrate 300 was formed in the same manner as in Preparation Example 2-1, except that a second hydrophilic layer of a stripe pattern was formed instead of a second hydrophilic layer of a wedge pattern was formed. )/first hydrophilic layers (22101, 22211, 22221)/water repellent layers (22102, 22212, 22222)/second hydrophilic layer (22103) were prepared.

Example 1: Preparation of a fluid entrapment patch

Figure 1b shows a cross-sectional view of a fluid collection patch according to an embodiment of the present invention, Figure 1c is a cross-sectional view of the first flexible substrate, the channel portion and the second flexible substrate of the fluid collection patch according to an embodiment of the present invention it has been shown 1D is a schematic view showing the structure and cross-sectional view of a fluid collection patch according to an embodiment of the present invention, and a fluid movement phenomenon in a channel part, and FIG. 1H is a method for manufacturing a fluid collection patch according to an embodiment of the present invention. It is a schematic diagram about 1b to 1d, the fluid collection patch of Example 1 was prepared with reference to the upper-lower plate bonding of 1h.

After thinly coating polydimethylsiloxane (PDMS) with high viscosity on the support part of the lower plate prepared according to Preparation Example 1-1, the upper plate prepared according to Preparation Example 2-1 was attached. At this time, the pattern of the second hydrophilic layer 22103 of the upper plate and the pattern of the second hydrophilic layer 21103 of the lower plate were made to have the same shape while facing each other. Thereafter, after removing air bubbles through a vacuum, the reaction was carried out in an oven at 120° C. for 30 minutes to form a channel space 230 formed between the pattern of the second hydrophilic layer 22103 of the upper plate and the pattern of the second hydrophilic layer 21103 of the lower plate. ) was prepared including a channel portion 200.

A fluid collecting patch including a collecting part 500 positioned on the second hydrophilic layer 21103 of the lower plate and including a collecting space 510 connected to the channel space 230 was manufactured.

Example 2: Fabrication of a fluid entrapment patch comprising a plurality of channel portions

Referring to FIG. 4A , the seven channel parts manufactured according to Example 1 were radially arranged around the collecting unit, and a fluid collecting patch having a diameter of 3 cm and a thickness of 1 mm was prepared. The fluid collection patch includes an adhesive layer having a thickness of 0.1 mm at the bottom, and an actual skin attachment image is shown in FIG. 4B .

Example 3: Preparation of Fluid Entrapment Patches

1A is a cross-sectional view of a first flexible substrate, a channel portion, and a second flexible substrate of a fluid collecting patch according to an embodiment of the present invention, and FIG. 1B is a cross-sectional view of a fluid collecting patch according to an embodiment of the present invention it has been shown 1D is a schematic view showing the structure and cross-sectional view of a fluid collection patch according to an embodiment of the present invention, and a fluid movement phenomenon in a channel part, and FIG. 1H is a method for manufacturing a fluid collection patch according to an embodiment of the present invention. It is a schematic diagram about The fluid collection patch of Example 3 was prepared with reference to the upper-lower plate bonding of FIGS. 1A, 1B, 1D and 1H.

Instead of using the lower plate prepared according to Preparation Example 1-1 and the upper plate prepared according to Preparation Example 2-1, the lower plate prepared according to Preparation Example 1-2 and the upper plate prepared according to Preparation Example 2-2 were used. A fluid collection patch was prepared in the same manner as in Example 1, except that.

Comparative Example 1: Preparation of a fluid collection patch

Except for using the lower plate prepared according to Comparative Preparation Example 1 instead of the lower plate prepared according to Preparation Example 1-1, and using the upper plate prepared according to Comparative Preparation Example 2 instead of the upper plate prepared according to Preparation Example 2-1 Then, a fluid collection patch was prepared in the same manner as in Example 1.

[Test Example]

Test Example 1: Preparation of super water-repellent/super-hydrophilic surface on flexible substrate

Figure 1e shows the chemical structure and water contact angle (surface energy) of the surface of the water repellent part/hydrophilic part in the upper plate prepared according to Preparation Example 2-1, and FIG. 1f is the pattern of the fluid collection patch prepared according to Example 1 The role of the core process for making the wedge pattern surface can be stably maintained in the layer is described, and the surface state of the upper plate prepared according to Preparation Example 2-1 after 1,000 cycles of tensile testing is shown as an optical microscope (OM) image. 1g is an observation graph showing the change in contact angle with time of each surface of the water repellent part/hydrophilic part in the upper plate prepared according to Preparation Example 2-1.

In the case of the surface of the water-repellent part, in general, the flexible polymer is carbon-based and has hydrophobic properties. However, in the case of the surface of the hydrophilic part, unlike the production of super water _- repellent surface, the surface properties of the flexible polymer must be made hydrophilic. However, in the case of flexible polymers, hydrophobicity is recovered in half a day due to chain-entanglement. Therefore, in order to produce a surface that can fundamentally maintain hydrophilic properties, it is necessary to make the surface with a material that does not cause chain-entanglement. However, in general, polymers that do not undergo chain-entanglement have weak tensile properties. Therefore, in order to fabricate an ideal surface structure, it was necessary to devise a structure with the characteristics of being able to maintain the surface energy stably while being flexible throughout the substrate.

Referring to Figure 1e, the present invention produced a hydrophilic surface with irregularities by chemically bonding silica particles having hydrophilic properties and not having a large change in surface energy over time on a PDMS substrate, and as a result, a surface with super-hydrophilic properties It was confirmed that it could be produced.

Referring to FIG. 1f , the upper plate prepared according to Preparation Example 2-1 was strongly bonded to both the water-repellent part/hydrophilic part surface through the PVA polymer and maintained its shape stably regardless of the strength of the droplet, and silica particles during tension. Although the gap between them is widened, it can be confirmed that the surface energy is stably maintained by strongly bonding with the PDMS.

Referring to Figure 1g, in the top plate prepared according to Preparation Example 2-1, the superhydrophobic property showed a tendency to be maintained regardless of time, and it can be confirmed that the superhydrophilic property is stably maintained for about 2 weeks or more. .

Test Example 2: Speed change according to the wedge angle of the wedge pattern

The movement of water droplets on the water repellent/hydrophilic wedge pattern is caused by the difference in curvature according to the location of the interface of the water drop on the pattern and the laplace pressure generated by the surface tension of the fluid. Therefore, in order to move water droplets effectively, the Laplace pressure must be maximized. (3) The width of the left and right of the droplet is larger than the width of the wedge pattern so that it protrudes convexly to the super-repellent surface centering on the super-hydrophobic/super-hydrophilic interface, so that Laplace pressure due to curvature can exist. We need to design a wedge pattern. At this time, first, in the case of condition (1), the contact angle of the super water-repellent surface was manufactured to be 160° or more, and the super-hydrophilic surface was manufactured to 0°, and the difference was maximized and fixed. However, conditions (2) and (3) tend to be inversely proportional, so a conditional experiment was conducted to find an experimentally appropriate value.

Referring to Figure 2c, the force that moves the droplet by the surface energy shows a characteristic that increases as the wedge angle increases according to condition (2) (by changing the tilting angle and controlling the strength of gravity acting on the droplet, The force due to the acting surface energy was calculated). However, in the case of the moving speed of the droplet on the plane, it was observed that the moving droplet moved the fastest when the wedge angle was 3.4°. This phenomenon is related to condition (3). If the wedge angle is too large, the width of the moving droplet is This is because the time to become smaller than the width of the wedge pattern becomes faster, and the shape of the water droplet quickly changes from a convex shape to a concave shape at the super-hydrophobic/super-hydrophilic interface. could be inferred that

Therefore, as a result, it can be confirmed that the wedge pattern that can move the fluid the fastest is the case where the wedge angle is 3.4°.

Test Example 3: Comparison of open and closed structures of laminates including wedge patterns

Referring to FIG. 2D , it can be seen that the water droplets on the open structure of the water-repellent/hydrophilic wedge pattern are greatly affected by gravity, and the movement speed of the fluid is greatly affected by the slope of the surface. Therefore, it can be confirmed that, in the case of an open wedge pattern channel, water droplets cannot stably move regardless of body movement when the body is attached.

In order to overcome this phenomenon, it is necessary to reduce the force due to gravity acting on the fluid and maximize the force due to surface energy. A structure that can receive less is required, and a structure (sealing structure) in which the laminate is facing each other is devised using two laminates manufactured according to an embodiment of the present invention.

Referring to FIG. 2E , by controlling the height of the channel space, by limiting the height of the fluid located in the channel space, the area of the surface area relative to the volume of the fluid is increased, thereby maximizing the force due to the surface energy received by the fluid.

Test Example 4: Comparison of fluid movement speed between wedge pattern and stripe pattern

FIG. 2f shows a comparison of the fluid movement speed of the channel part (right figure) of the fluid collecting patch manufactured according to Example 1 and the channel part of the fluid collecting patch manufactured according to Comparative Example 1 (left figure).

Referring to FIG. 2F , it can be seen that the fluid collection patch (picture on the right) prepared according to Example 1 including a wedge pattern moves fluid (sweat) at a much faster rate.

Test Example 5: Check whether sweat can be collected regardless of body movement when actually attaching to the skin

Figure 3a is changing the inclination of the fluid collecting patch (wedge pattern) prepared according to Example 1 to 30 °, 60 °, 90 °, 120 °, 150 °, 180 °, the movement speed of the fluid according to the change in gravity The change is observed and measured and shown as a graph, and FIG. 3B is a photograph of actually observing the movement of the fluid with a high-speed camera when measuring FIG. 3A.

Referring to FIGS. 3A and 3B , as a result of observing the moving speed of the fluid while changing the slope, it can be confirmed that the fluid can move at a very high speed regardless of gravity.

Therefore, as a result, it can be confirmed that fast fluid collection is possible not only in a 90 degree tilted state but also in an inverted state.

Test Example 6: Comparison of the rate at which sweat is collected in the collecting unit

FIG. 4c shows a comparison of the speed at which the fluid is collected by the sensing unit where each fluid is collected when the fluid collecting patch prepared according to Example 1 and the fluid collecting patch prepared according to Comparative Example 1 are used.

Referring to FIG. 4C , in the case of the fluid collection patch (Comparative Example 1) including a stripe pattern similar to that of the existing microfluidics channel, it can be seen that it takes more than 100 seconds to fill the channel because the fluid moves while filling the channel.

On the other hand, in the case of the fluid collection patch (Example 1) including the wedge pattern, the fluid flowing into the channel moves directly to the collection unit and is collected, so it can be confirmed that much faster and more efficient collection is possible as a result of observation and recording with a high-speed camera. have.

Test Example 7: Confirmation of superiority of wedge pattern in fluid collection patch when using a plurality of channel parts

Test Example 7-1: Comparison of prediction of time taken to fill the collecting unit with a fluid using a calculation model

FIG. 4d shows a case in which a microfluidics channel is not used (No micro-channel), a case in which an existing microfluidics channel is used (Micro-channel), and a fluid trapping patch prepared according to Example 2 (Wedge patterned channel) is used. In this case, the sampling time required to fill the collection unit is predicted using a computational model and displayed as a graph. In detail, the calculation model predicted by limiting the 7 channel units to the collection unit.

The existing microfluidics channel has the shape of a tube having a rectangular structure in cut, and includes a channel portion in which the upper and lower surfaces are coated with a hydrophilic material (the bottom surface is coated on the entire surface, there is no super water-repellent surface). The existing microfluidics channel does not have a stripe pattern, but since there is no change in the area of the coated hydrophilic surface, it has a structure similar to that of the fluid collection patch having the stripe pattern of Comparative Example 1, and the phenomenon of fluid movement is also similar to that of the fluid collection patch of Comparative Example 1. Almost identical.

Referring to FIG. 4D , when the collecting unit without the channel unit is attached to the skin (No micro-channel), the overall collecting speed is reduced due to the small area that can collect the fluid, and it takes relatively the most time to fill the collecting unit with the fluid. that can be checked

In the case of using the existing microfluidics channel, it can be seen that the collection area is wider than when the channel is not used, so that the total collection speed is increased, and the time taken to fill the collection unit is reduced. However, when the existing microfluidics channel is used, not only the sensing unit but also the microfluidics channel must be filled with a fluid to collect it. You can see that it takes more time to do it.

In the case of using the fluid collecting patch (Wedge patterned channel) prepared according to Example 2, the collecting area was also enlarged and the total collecting speed was increased. It can be seen that the time taken is relatively short.

Test Example 7-2: Experiment to prove the prediction result

FIG. 4e shows the phenomenon in which sweat is collected in the fluid collection patch prepared according to Example 2 when sweat is injected at a rate of 2 μL/min-cm ² using an artificial sweat secretion system to prove the prediction result of FIG. 4D. It shows the results observed over time, and Fig. 4f is a measurement of the time the sweat is filled in the collecting part of the fluid collecting patch prepared according to Example 2 under the same conditions as in Fig. 4e to prove the predicted result of Fig. 4d. did it

In detail, FIG. 4f shows a total of three attempts to measure the time that sweat is filled in the collecting part of the fluid collecting patch, and is displayed in black (primary), red (secondary), and blue (tertiary), respectively. and the time for the sweat to be filled is measured using a phenomenon in which the impedance between the separated electrodes changes when the sweat contacts the electrodes.

Referring to FIG. 4E, the time it takes to fill the collecting unit is set as the sampling time, and the sampling time at which the collecting unit is filled according to the sweat injection rate is observed through the camera. As a result, the collecting unit is filled in a time similar to the predicted result. can be visually confirmed.

Referring to FIG. 4f, as a result of measuring the impedance change with time by attaching a humidity sensor to the collection unit, it was confirmed that the change in the impedance value occurred after the sampling time consistent with the predicted result, so that the predicted and experimental results were significantly improved. It can be seen that similar results are shown. In addition, it can be seen that the first (black line), the second (red line), and the third (blue line) attempts all fill the sweat collection unit within a similar time.

Test Example 7-3: Experiment to prove the predicted result on real skin

FIG. 4G shows the results of the experiment performed in FIG. 4F on the actual skin, and the time it takes for the impedance value to change is measured when riding a cycle with the sensor and the patch attached to the actual skin.

Referring to FIG. 4G , after attaching the patch on the actual skin and combining the humidity sensor to measure the sampling time, it was confirmed that the impedance value changed between about 1 minute and 2 minutes, and through this, it was also sampled on the actual skin. You can see that this happens quickly.

Test Example 8: Combination of fluid collection patch and chemical sensor

5A is a diagram illustrating a form in which a fluid collecting patch and a wearable sweat sensor are combined according to an embodiment of the present invention. 5B is a diagram illustrating the measurement of the glucose concentration in sweat by combining the fluid collection patch prepared according to Example 2 and the wearable glucose sensor with reference to FIG. 5A and comparing it with the blood glucose concentration.

Referring to FIG. 5B , after attaching the patch to the actual skin, a wearable glucose sensor was combined to collect and measure sweat during exercise, and as a result, it was confirmed that there is a correlation with the concentration of glucose in the blood. It is possible to continuously measure changes in blood sugar and sweat concentration with a time difference of about 15 minutes, and it can be confirmed that the patch is practically usable.

The scope of the present invention is indicated by the following claims rather than the above detailed description, and all changes or modifications derived from the meaning and scope of the claims and their equivalent concepts should be interpreted as being included in the scope of the present invention. do.

Claims

a first flexible substrate;

a channel portion formed on the first flexible substrate;

a second flexible substrate formed on the channel part; and

and a support part positioned between the first flexible substrate and the second flexible substrate and including a column formed outside the channel part; and

the channel part

a first pattern layer formed on the first flexible substrate and including a first hydrophilic part having a hydrophilic surface and a first water repellent part having a water repellent surface;

a second pattern layer spaced apart from the first pattern layer and including a second hydrophilic part having a hydrophilic surface and a second water repellent part having a water repellent surface; and

The fluid collection patch comprising a; channel space formed between the first pattern layer and the second pattern layer.
According to claim 1,

wherein the hydrophilic surface is a superhydrophilic surface, and the water repellent surface is a superhydrophobic surface.
According to claim 1,

The hydrophilic surface has a water contact angle of 0 to 20˚, and the water repellent surface has a water contact angle of 120 to 180˚.
The method of claim 1,

The fluid collection patch, characterized in that the hydrophilic surface and the water-repellent surface each have a fine concavo-convex shape.
The method of claim 1,

The fluid collection patch, characterized in that the first patterned layer and the second patterned layer have patterns corresponding to each other.
6. The method of claim 5,

The fluid collection patch, characterized in that the first hydrophilic portion and the second hydrophilic portion each has a pattern in which the diameter decreases from the center of the patch to the edge in the horizontal direction.
7. The method of claim 6,

The fluid collection patch, characterized in that the pattern is a wedge pattern.
According to claim 1,

The first water-repellent portion includes a first 'water-repellent portion and a first "water-repellent portion located spaced apart from the first water-repellent portion,

The first hydrophilic portion is located between the first 'water-repellent portion and the first" water-repellent portion,

The second water-repellent portion includes a second 'water-repellent portion and a second" water-repellent portion positioned spaced apart from the second water-repellent portion,

The second hydrophilic portion is located between the second' water-repellent portion and the second"water-repellent portion.
The method of claim 1,

The first hydrophilic part and the second hydrophilic part are each independently fluid collection patch, characterized in that not in contact with the pillar.
The method of claim 1,

The first hydrophilic part or the second hydrophilic part comprises a hydrophilic polymer and hydrophilic particles, respectively.
The method of claim 1,

The fluid collection patch, characterized in that the first water repellent portion or the second water repellent portion each comprises a water repellent material.
According to claim 1,

The fluid collecting patch is a collecting unit; and a collection space located on the collection unit and connected to the channel space.
13. The method of claim 12,

the fluid collection patch

including a plurality of channel units,

A fluid collection patch, characterized in that the plurality of channel portions are radially disposed around the collection portion.
13. The method of claim 12,

The fluid collection patch, characterized in that the fluid collection patch further comprises at least one sensor selected from the group consisting of a blood glucose sensor, a lactic acid sensor, an alcohol sensor, and an electrolyte sensor, wherein the sensor is located on the collection space.
The method of claim 1,

the fluid collection patch

a plurality of fluid inlets penetrating the first flexible substrate and the first hydrophilic part in a vertical direction; and

The fluid collection patch, characterized in that it further comprises; an adhesive layer located under the first flexible substrate.
(a) a first flexible substrate, a support portion including a pillar formed on the first flexible substrate, and a first water repellent portion formed on the first flexible substrate and having a hydrophilic surface and a water repellent surface manufacturing a lower plate including a first pattern layer including a portion;

(b) manufacturing an upper plate comprising a second flexible substrate and a second pattern layer formed on the second flexible substrate and including a second hydrophilic part having a hydrophilic surface and a second water repellent part having a water repellent surface;

(c) positioning the second flexible substrate of the upper plate on the support part of the lower plate to prepare the fluid collection patch according to claim 1;

A method of manufacturing a fluid collection patch comprising a.
17. The method of claim 16,

The step (a) is

(a-1) preparing a support portion including a pillar and a first flexible substrate coupled to the support portion, and surface-treating the surface of the flexible substrate to be hydrophilic;

(a-2) forming a first hydrophilic layer by coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated first flexible substrate;

(a-3) forming a water repellent layer on the first hydrophilic layer by coating a solution containing a water repellent material on the first hydrophilic layer;

(a-4) surface-treating the surface of the water-repellent layer to be hydrophilic; and

(a-5) coating the hydrophilic surface of the surface-treated water-repellent layer with a solution containing hydrophilic particles and a hydrophilic polymer to form a second hydrophilic layer to prepare the lower plate; Fluid collection comprising a A method for manufacturing a patch.
17. The method of claim 16,

The step (a) is

(a-1') preparing a support portion including a pillar and a first flexible substrate coupled to the support portion;

(a-2') forming a first water repellent part on the first flexible substrate by coating a solution containing a water repellent material on the first flexible substrate; and

(a-3') forming a first hydrophilic part by treating a part of the first water-repellent part to be hydrophilic;
17. The method of claim 16,

The step (b) is

(b-1) surface-treating the surface of the second flexible substrate to be hydrophilic;

(b-2) forming a second hydrophilic layer by coating a solution containing hydrophilic particles and a hydrophilic polymer on the hydrophilic surface of the surface-treated second flexible substrate;

(b-3) forming a water repellent layer on the second hydrophilic layer by coating a solution containing a water repellent material on the second hydrophilic layer of the second flexible substrate;

(b-4) surface-treating the surface of the water-repellent layer to be hydrophilic; and

(b-5) coating the hydrophilic surface of the surface-treated water-repellent layer with a solution containing hydrophilic particles and a hydrophilic polymer to form a second hydrophilic layer to prepare the top plate; Fluid collection comprising a A method for manufacturing a patch.
17. The method of claim 16,

The step (b) is

(b-1') preparing a second flexible substrate;

(b-2') forming a second water repellent part on the second flexible substrate by coating a solution containing a water repellent material on the second flexible substrate; and

(b-3') forming a second hydrophilic part by treating a part of the second water-repellent part to be hydrophilic.