KR200297594Y1 - Patch for glucose extraction apparatus - Google Patents

Abstract

Patches for glucose extraction are provided for ease of manufacture and ease of use. The patch is provided with two hydrophilic gel discs each containing an enzyme capable of reacting with glucose to produce hydrogen peroxide, a frame with two holes for accommodating the gel disc, and a position facing the gel disc. And an electrode, a terminal for connection with the measuring device, and circuit means for electrically connecting the electrode and the terminal to each other, and having a flexible circuit board attached to the upper portion of the frame. For the support of the gel disk, a film having a diameter smaller than the diameter of the mold hole and having two cutouts provided corresponding to the two holes of the mold may be attached to the bottom of the mold. Alternatively, a wing projecting into the hole may be formed in the lower part of the two holes of the mold to support the hydrophilic gel disc. The electrodes are formed on the flexible circuit board using the silkscreen method. The electrode may be pretreated for improved performance.

Description

Patch for glucose extraction apparatus

The present invention relates to a patch for glucose extracting apparatus, and more particularly to a patch for glucose extracting apparatus which is simple to manufacture and easy to use.

Conventional blood glucose meters collect blood by using a needle to cut blood from a finger, and measure the blood glucose level by absorbing blood into a sensor site where an enzyme is fixed to an electrode surface using a polymer. These blood glucose meters have considerable pain and fear of blood collection. Particularly in diabetics who require periodic blood glucose measurement, the use of blood glucose meters may be avoided due to significant discomfort. In addition, since the blood sugar may be momentarily high, the patient may be in a dangerous state, and thus, continuous blood glucose monitoring is often required. However, the conventional blood glucose measurement method has a disadvantage in that continuous monitoring is difficult.

In view of these problems, various methods for measuring the concentration of analytes in blood without blood collection have been developed. For example, US Pat. No. 5,267,152 to Yang et al. Describes a non-invasive technique for measuring blood glucose concentrations using near infrared radiation diffusion-reflection laser spectroscopy. Similar near infrared spectroscopy devices are described in US Pat. No. 5,086,229 to Rosenthal et al. And US Pat. No. 4,975,581 to Robinson et al. However, these methods have not been put to practical use due to technical problems.

Stanley, U.S. Pat. Is described. Sembrowich, US Pat. No. 5,036,861, describes a passive glucose monitor that collects sweat through a skin patch where cholinergic agents are used to stimulate sweat secretion from the extrasecretory line. Similarly, a sweat collection device is described in Schöndorfer, U.S. Patent No. 5,076,273 and Schroeder, U.S. Patent No. 5,140,985.

In addition, US Pat. No. 5,279,543 to Glikfeld describes the use of iontophoresis (electroosmotic pressure) for noninvasive sampling of materials through the skin into a reservoir on the skin surface. Glickfeld suggests that this sampling method can be combined with glucose specific biosensors or glucose specific electrodes to monitor blood glucose. In addition, Tamada International Publication No. WO 96/00110 discloses ions for transdermal monitoring of target substances in which iontophoretic electrodes are used to transfer analytes to a collection reservoir and biosensors are used to detect target analytes in the reservoir. The device for moving is described.

However, these devices do not present a configuration that can be easily used by patients, and also has a disadvantage in that it is difficult to continuously monitor blood glucose levels.

In view of this point, the Korean Patent Publication No. 1997-7003790 has been proposed a device using two patches, but it is difficult to work with patients attached as well. In order to solve this problem, Korean Patent Publication No. 1999-0077833 discloses a device using one patch. However, this apparatus also has a disadvantage in that its configuration is complicated, making assembly difficult and expensive. In addition, there is a disadvantage in that the measurement performance is insufficient to be practical.

The present invention has been made in view of this point, and an object of the present invention is to provide a patch for a glucose extracting device having a simple configuration and an electrode used therefor, and a method of manufacturing the same, in which a patient can be attached to work.

Another object of the present invention is to provide a simple and inexpensive patch for a glucose extracting device, an electrode used therein, and a manufacturing method thereof.

Another object of the present invention is to provide a composition of an electrode capable of improving measurement performance and a pretreatment method thereof.

1A and 1B are views showing the appearance of a glucose monitoring apparatus.

Figure 2a is an exploded perspective view showing the configuration of a patch according to an embodiment of the present invention.

Figure 2b is an exploded perspective view showing the configuration of a patch according to another embodiment of the present invention.

Figure 2c is a cross-sectional view showing the form of the frame according to another embodiment of the present invention.

3 is an exploded perspective view showing the configuration of a printed circuit.

4 is a view for explaining an electrode forming process by the silk screen method.

5A to 5C are views illustrating various forms of electrodes.

The patch for glucose extracting apparatus according to the present invention comprises two hydrophilic gel discs each containing an enzyme capable of reacting with glucose to produce hydrogen peroxide, and a frame in which two holes for accommodating the gel disc are formed; An electrode provided at a position facing the gel disc, a terminal for connection with a measuring device, and circuit means for electrically connecting the electrode and the terminal to each other, the flexible circuit board being attached to the upper portion of the frame. Equipped.

In addition, for supporting the gel disk, a film having a diameter smaller than the diameter of the mold hole and having two cutouts corresponding to the two holes of the mold may be attached to the bottom of the mold. Alternatively, a wing projecting into the hole may be formed in the lower part of the two holes of the mold to support the hydrophilic gel disc.

The electrode is formed using an ink containing platinum metal and carbon or an ink containing Ag / AgCl, and includes first and second extraction electrodes for extracting glucose from the skin, and containing platinum metal and carbon. It is formed using an ink, and is formed using a working electrode applying a voltage for measuring a current generated by the reaction of the hydrophilic gel and the extracted glucose, and an ink containing Ag / AgCl, and the hydrophilic gel and extraction It is formed by using a reference electrode used as a reference potential when measuring the current generated by the reaction with glucose and an ink containing platinum metal and carbon, and is produced by the reaction between the hydrophilic gel and the extracted glucose. There is a counter electrode for measuring the current. At this time, the weight ratio of platinum to carbon of the working electrode is preferably 95: 5.

The first extraction electrode is located at a position corresponding to one of the hydrophilic gel disks in a ring shape, and the second extraction electrode is located at a position corresponding to the other one of the hydrophilic gel disks in a partially cut ring shape, and the working electrode is The second extraction electrode may have a circular shape located inside the annular shape, and the reference electrode and the counter electrode may be arranged in a line at the cutout portion of the second extraction electrode. Alternatively, the reference electrode and the counter electrode may be arranged in parallel to the cutout portion of the second extraction electrode.

Alternatively, the first extraction electrode is located in a ring corresponding to one of the hydrophilic gel disks, the second extraction electrode is located in a ring corresponding to the other of the hydrophilic gel disks, and the working electrode is a second It is also possible to have a shape of a circle located inside the ring shape of the extraction electrode of the reference electrode, the reference electrode and the counter electrode may be configured to be positioned so as to surround each of the outer half of the ring shape of the second extraction electrode.

On the other hand, it is preferable that the electrode, the terminal, and the circuit means are formed on the same surface on the flexible circuit board, and the portion of the substrate where the terminals are formed is cut off so that the terminals are exposed to the opposite side of the substrate.

Such a patch may include a first step of placing a hydrophilic gel disc in a frame configured to receive a hydrophilic gel disc, a second step of forming terminals and circuit patterns on a flexible circuit board film by copper wire, and the circuit pattern. A third step of aligning the mask having the electrode pattern of the first material on the formed surface, applying and curing the ink of the first material, and a fourth step of repeating the third step for each electrode material And a fifth step of curing the film on which the electrode is formed for a predetermined time, and a sixth step of applying an adhesive to a portion other than the electrode of the cured film and attaching the hydrophilic gel disk to the mold containing the hydrophilic gel disk. do.

In this case, after the fifth step, the electrode is immersed in a sulfuric acid solution of 0.01 ~ 10M, and then subjected to an oxidation reaction in the range of 0.0 ~ 1.2V using cyclic voltammetry to improve the performance The effect can be obtained. In addition, the curing time in the fifth step is preferably 3 hours.

The method may further include attaching a film having a hole smaller than the diameter of the hydrophilic gel disk to a corresponding portion of the hydrophilic gel disk on the opposite side of the surface to which the flexible circuit board is attached.

Hereinafter, exemplary embodiments of the present invention will be described in detail with reference to the accompanying drawings.

The patch of the present invention is used mounted on the glucose monitoring device. The glucose monitoring device may take the form of an wrist watch as shown in FIG. 1A. The front of the device is arranged a display such as an LCD for displaying the measured glucose value, and a button for the user's device operation.

The backside of the device is attached with a disposable patch 200 as shown in FIG. 1B. The device is equipped with a locker 102 for this purpose. In addition, spaces 101a and 101b may be provided to accommodate the batteries.

When the patient places the device on the wrist, the back side of the patch contacts the patient's skin. When the device applies a current to the patch 200, glucose is extracted from the patient's skin into the patch by electroosmotic pressure. The extracted glucose causes an electrochemical reaction with the hydrophilic gel provided in the patch, thus generating a current. The device monitors blood glucose levels by measuring the current generated.

The patch 200 is provided with a terminal 211 for electrical connection with the device. When the patch 200 is attached to the device, the terminal 211 is in electrical connection with the terminal 103 provided on the back of the device. The device applies current through these terminals and measures the current according to the electrochemical reaction.

Next, the configuration of the patch will be described in detail with reference to FIGS. 2A and 2B.

Figure 2a is an exploded view showing the configuration of a patch according to an embodiment of the present invention.

The patch 200 has two gel disks 220a and 220b, a mold 230 for accommodating these gel disks, a film 240 for supporting the gel disks, and a printed circuit 210. Electrodes for contact with the gel disks 220a and 220b are formed in the printed circuit 210, and the electrodes are connected to the terminal 211 by a conductive circuit such as a copper wire.

Gel discs 220a and 220b are hydrophilic gels containing an enzyme. This is referred to US Patent No. 5,139,023, Korean Patent Publication No. 1999-028884, Korean Patent Publication No. 1999-0077833, etc. The present invention is not limited to a gel of a specific composition.

In the mold 230, a hole having the same size as the gel discs 220a and 220b is formed to accommodate the gel discs 220a and 220b. The material of the mold 230 may be used as long as it is a material harmless to the human body, such as Teflon.

The film 240 serves to support the gel disks 220a and 220b so as not to escape from the mold 230. The film 240 is provided with a hole 241 for contact between the body and the gel disks 220a and 220b. The size of the holes 241 should be smaller than the gel discs 220a and 220b in order to prevent the gel discs 220a and 220b from falling out.

2B shows an embodiment in which the film 240 is not used. In FIG. 2B, instead of using the film 240, the gel discs 220a and 220b have the shape of the bottom surface smaller than the area of the top surface, and the shape of the hole of the mold corresponds to that of the gel discs 220a, 220b. 220b) is prevented from falling out of the frame 240.

Alternatively, the gel discs 220a and 220b may be shaped as shown in FIG. 2A, but the gel discs 220a and 220b may not be removed from the holes by forming the holes of the mold 230 as shown in FIG. 2C. That is, it is possible to prevent the gel disks 220a and 220b from falling out by providing the wing 231 for supporting the gel disk 220 at the bottom of the hole of the mold 230. At this time, the thickness of the wing 231 is preferably to be as thin as possible so that the gel disk can be in close contact with the skin.

The printed circuit 210 is made of a polyimide film 212, a copper wire 214, and an electrode 215. 3 is an exploded perspective view showing the configuration of the printed circuit 210.

The film 212 may be used as long as it is a substrate material used for a flexible printed circuit. Holes 213 are formed in the film 212 so that the terminals 216 formed by copper wires can be exposed above the patch 200. The copper wire 214 may be formed on the film 212 by a general flexible circuit board manufacturing method.

The electrode 215 is formed on the film 212 on which the copper wire 214 is formed. The electrode 215 may be formed on the film in a silk screen manner. 4 is a view for explaining an electrode forming process by the silk screen method.

The electrodes may have different materials depending on their purpose. First, a mask 311 in the form of electrodes having a material is placed on the film 212 (a). Then, the ink 321 of the material is applied on the mask 311 (b). The mask 311 is removed and then cured at a high temperature, for example, 130 ° C. (c). Curing conditions at this time are similar to the curing conditions between printing of one chromaticity and printing of another chromaticity in a general silkscreen method. Experiments have shown that curing for 10 minutes at 130 ° C. is sufficient, but the invention is not limited thereto.

After curing, the steps (a) to (c) are repeated for other materials. As such, the steps (a) to (c) were performed for all materials, followed by curing at 130 ° C. for 3 hours. Then, as shown in (d), electrodes made of inks 321, 322, and 323 of various materials are formed on the film 212.

Table 1 shows how the current change due to glucose changes with the final curing time. As can be seen from this table, the most current change occurred when curing for 3 hours. Therefore, it can be seen that when the final curing time is 3 hours, the most sensitive reaction can be obtained.

Examples of electrode shapes are shown in FIGS. 5A-5C. The patch 200 includes five electrodes, that is, two extraction electrodes 215a and 215b, a working electrode 215c, a reference electrode 215d, and a counter electrode. ) 215e is formed.

The extraction electrodes 215a and 215b are electrodes for extracting glucose from the skin and are formed using a platinum ink containing carbon or an ink containing Ag / AgCl.

The working electrode 215c is an electrode for applying a voltage for measuring a current generated by the reaction between the hydrophilic gel and the extracted glucose, and is formed using an ink in which platinum metal and carbon are mixed in an appropriate ratio. Table 2 shows the results of measuring the change in current according to the weight ratio of platinum and carbon. The electrode manufactured for the measurement was subjected to the pretreatment described below.

As can be seen from this table, the case where the weight ratio of platinum to carbon is 95: 5 is the most sensitive.

The reference electrode 215d is used as a reference potential when measuring the current generated by the reaction between the hydrophilic gel and the extracted glucose, and is formed using an ink containing Ag / AgCl.

The counter electrode 215e is an electrode for measuring the electric current generated by the reaction between the hydrophilic gel and the extracted glucose, and is formed using a platinum metal ink containing carbon.

At this time, when the electrode is pretreated, its performance may be further improved. The pretreatment process is performed by first immersing an electrode in 0.01 to 10 M sulfuric acid solution, and then performing an oxidation reaction in a range of 0.0 to 1.2 V using cyclic voltammetry.

Table 3 shows the current change values with and without pretreatment with 0.5M sulfuric acid solution. Here, 3 ml of physiological saline solution in which glucose oxidase is dissolved in a predetermined amount is put in a constant temperature cell at a constant temperature (38 ° C.), and then a portion of a strip-shaped electrode is dipped. 0.4V was applied to the pretreated electrode through a potentiostat to examine the current change according to the reaction of glucose and glucose oxidase at a concentration of 500 μM.

As shown in Table 3, the pre-treatment showed the best analytical performance when the weight ratio of platinum was 95%, and the overall pretreatment was able to detect the current change due to glucose more effectively than it did otherwise. .

The flexible circuit board 210 having the electrode formed thereon is attached to the mold 230 by an adhesive or the like. When the substrate 210 is adhered to the mold 230 by an adhesive, the substrate 210 is adhered after the adhesive is applied to a portion of the substrate except for a portion where the electrode is formed, that is, a portion where the electrode is in contact with the hydrophilic gel.

As mentioned above, although some Example was given and demonstrated this invention, this invention is not limited to this. Those skilled in the art will appreciate that many modifications and variations can be made without departing from the spirit of the invention.

As described above, according to the present invention, since the electrode and the hydrophilic gel are composed of one patch, the glucose extracting device can be easily attached and detached. In addition, since the electrode, terminal, and the circuit line can be manufactured using a method applying a silk screen method and a printed circuit board manufacturing method, there is an effect that the production is easy. In addition, the measurement performance is excellent by using a material of a special composition for the electrode and undergoing a pretreatment process.

Claims (6)

Two hydrophilic gel discs each containing an enzyme capable of reacting with glucose to produce hydrogen peroxide, A frame in which two holes are formed to accommodate the gel disc, An electrode provided at a position facing the gel disc, a terminal for connection with a measuring device, and circuit means for electrically connecting the electrode and the terminal are formed, and a flexible circuit attached to an upper portion of the frame. Board Glucose extraction patch having a. The method of claim 1, A film attached to the lower part of the mold and having two cutouts having a diameter smaller than the diameter of the two holes provided corresponding to the two holes of the mold; Patch for extracting glucose further comprising a. The method of claim 1, The lower portion of the two holes of the frame is a patch for extracting glucose, characterized in that the wing protruding into the hole is formed to support the hydrophilic gel disk. The method of claim 1, The gel disc has an area of the bottom surface smaller than that of the top surface, And said two holes of said frame have a shape corresponding to said gel disc. 2. The substrate according to claim 1, wherein the electrode, the terminal, and the circuit means are formed on the same surface on the flexible circuit board, and the portion of the substrate where the terminal is formed is cut out so that the terminal is exposed to the opposite side of the substrate. Glucose extraction patch, characterized in that. The patch for extracting glucose according to claim 5, wherein the flexible circuit board is attached to the mold by an insulating adhesive, and the adhesive is applied to a portion except the electrode.