WO2019059496A1

WO2019059496A1 - Glucose sensor

Info

Publication number: WO2019059496A1
Application number: PCT/KR2018/006341
Authority: WO
Inventors: 최봉진; 금중한; 김태균
Original assignee: 동우 화인켐 주식회사
Priority date: 2017-09-19
Filing date: 2018-06-04
Publication date: 2019-03-28
Also published as: KR102459679B1; KR20190031944A

Abstract

The present invention relates to a glucose sensor. The present invention comprises: an electrode part including a plurality of electrodes formed on a substrate; a glucose reaction part formed on the electrode part; a wire part including a plurality of electric wires extending from the electrodes constituting the electrode part; and a wire connection part electrically connecting the electric wires constituting the wire part. According to the present invention, the saturation time of a current sensed through the electrodes of the glucose sensor can be shortened to less than several seconds, and thus the measurement speed for a glucose concentration can be greatly increased.

Description

Glucose sensor

The present invention relates to a glucose sensor. More specifically, the present invention relates to a glucose sensor capable of greatly increasing the rate of measurement of glucose concentration.

Glucose is a broad nutrient source of most organisms and plays a fundamental role in energy supply, carbon storage, biosynthesis, and carbon skeleton and cell wall formation. Glucose sensor, which measures glucose concentration through potential difference or current measurement, Is being actively studied.

Most studies on glucose sensors are based on the fixation of enzymes such as glucose oxidase or glucose dehydrogenase, which catalyze the oxidation of glucose to gluconolactone.

These glucose sensors can be classified into Invasive, which mainly measures glucose contained in blood, and Non-invasive, which measures glucose contained mainly in saliva and sweat.

On the other hand, in the case of a noninvasive glucose sensor using saliva, sweat or the like as a sample, there is a problem that since the glucose contained in the sample is very small, the saturation time of the sensing current, which enables meaningful measurement, takes at least one minute .

[Prior Art Literature]

[Patent Literature]

(Patent Document 1) Korean Patent Laid-Open Publication No. 2001-0110272 (Disclosure Date: December 12, 2001, Name: Electrode for analyzing glucose containing Pt metal)

Disclosure of Invention Technical Problem [8] The present invention provides a glucose sensor capable of increasing the measurement speed with respect to the glucose concentration.

More specifically, the present invention provides a glucose sensor capable of greatly increasing the measurement speed with respect to glucose concentration by shortening the saturation time of the current sensed through the electrode of the non-invasive glucose sensor to less than several seconds As a technical task.

According to an aspect of the present invention, there is provided a glucose sensor comprising: an electrode unit including a plurality of electrodes formed on a substrate; a glucose reaction unit formed on the electrode unit; a plurality of electrons extended from electrodes constituting the electrode unit; And a wiring connection portion for electrically connecting the wiring portion made of wirings and the electric wirings constituting the wiring portion.

In the glucose sensor according to the present invention, the wiring connection part may reduce the initial potential difference between a plurality of electrodes constituting the electrode part, so that the saturation time of the current sensed through the electrode part by the glucose reaction of the glucose- Is shortened.

In the glucose sensor according to the present invention, the wiring connection part is provided in a pad area connected to an end of the wiring part.

In the glucose sensor according to the present invention, the wiring connection part may include a conductive tape or a conductive coating layer.

In the glucose sensor according to the present invention, a separation guide portion is formed between the electrode portion and the wiring connection portion.

In the glucose sensor according to the present invention, the electrode portion may be formed of at least one selected from the group consisting of Au, Ag, Cu, Pt, Ti, Ni, Ni, ), Cobalt (Co), and APC.

The glucose sensor according to the present invention may further include an electrode protection layer formed on the electrode unit and protecting electrodes constituting the electrode unit.

In the glucose sensor according to the present invention, the electrode protection layer may include carbon.

The glucose sensor according to the present invention further comprises an electron transport layer formed on the electrode portion.

In the glucose sensor according to the present invention, the electron transport layer may include prussian blue.

In the glucose sensor according to the present invention, the glucose reaction unit may include a glucose oxidase or a glucose dehydrogenase.

The glucose sensor according to the present invention further comprises an ion exchange membrane formed on the glucose reaction unit.

In the glucose sensor according to the present invention, the ion exchange membrane is characterized by protecting the glucose oxidase or the glucose dehydrogenase constituting the glucose reaction unit by preventing penetration of the impurity ion component.

In the glucose sensor according to the present invention, the ion exchange membrane may include Nafion.

The glucose sensor according to the present invention further includes a temperature sensor formed on the substrate.

According to the present invention, it is possible to provide a glucose sensor capable of increasing the measuring speed with respect to the glucose concentration.

Particularly, there is an effect that a saturation time of a current sensed through an electrode of a non-invasive glucose sensor is shortened to a few seconds, and thus a glucose sensor capable of greatly increasing a measurement speed with respect to glucose concentration is provided .

1 is a cross-sectional view of a glucose sensor according to an embodiment of the present invention,

Figure 2 is an exemplary top view of a glucose sensor made in accordance with one embodiment of the present invention,

FIG. 3 is a graph illustrating a comparison of a sensing current saturation time of a glucose sensor according to an embodiment of the present invention with a conventional one.

It is to be understood that the specific structural or functional description of embodiments of the present invention disclosed herein is for illustrative purposes only and is not intended to limit the scope of the inventive concept But may be embodied in many different forms and is not limited to the embodiments set forth herein.

The embodiments according to the concept of the present invention can make various changes and can take various forms, so that the embodiments are illustrated in the drawings and described in detail herein. It should be understood, however, that it is not intended to limit the embodiments according to the concepts of the present invention to the particular forms disclosed, but includes all modifications, equivalents, or alternatives falling within the spirit and scope of the invention.

The terms first, second, etc. may be used to describe various elements, but the elements should not be limited by the terms. The terms may be named for the purpose of distinguishing one element from another, for example, without departing from the scope of the right according to the concept of the present invention, the first element may be referred to as a second element, The component may also be referred to as a first component.

It is to be understood that when an element is referred to as being "connected" or "connected" to another element, it may be directly connected or connected to the other element, . On the other hand, when an element is referred to as being "directly connected" or "directly connected" to another element, it should be understood that there are no other elements in between. Other expressions that describe the relationship between components, such as "between" and "between" or "neighboring to" and "directly adjacent to" should be interpreted as well.

The terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. The singular expressions include plural expressions unless the context clearly dictates otherwise. In this specification, the terms "comprises" or "having" and the like are used to specify that there are features, numbers, steps, operations, elements, parts or combinations thereof described herein, But do not preclude the presence or addition of one or more other features, integers, steps, operations, components, parts, or combinations thereof.

Unless otherwise defined, all terms used herein, including technical or scientific terms, have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. Terms such as those defined in commonly used dictionaries are to be interpreted as having a meaning consistent with the meaning of the context in the relevant art and, unless explicitly defined herein, are to be interpreted as ideal or overly formal Do not.

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

FIG. 1 is a cross-sectional view of a glucose sensor according to an embodiment of the present invention, and FIG. 2 is an exemplary plan view of a glucose sensor manufactured according to an embodiment of the present invention.

1 and 2, a glucose sensor according to an embodiment of the present invention includes a substrate 10, an electrode unit 20, an electrode protection layer 30, an electron transport layer 40, a glucose reaction unit 50, An ion exchange membrane 60, a wiring section 70, a wiring connection section 80, a separation guide section 90, and a temperature sensor 100.

The substrate 10 serves to provide a structural base of the components making up the glucose sensor.

For example, the substrate 10 may be implemented in the form of a substrate film having a hard material, such as glass, or having flexible characteristics. Examples of specific materials that can be applied to the substrate film when the substrate 10 is flexibly embodied include polyester resins such as polyethylene terephthalate, polyethylene isophthalate, polyethylene naphthalate and polybutylene terephthalate; Cellulose-based resins such as diacetylcellulose and triacetylcellulose; Polycarbonate resin; Acrylic resins such as polymethyl (meth) acrylate and polyethyl (meth) acrylate; Styrene resins such as polystyrene and acrylonitrile-styrene copolymer; Polyolefin resins such as polyethylene, polypropylene, cyclo- or norbornene-structured polyolefins, ethylene-propylene copolymers; Vinyl chloride resin; Amide resins such as nylon and aromatic polyamide; Imide resin; Polyether sulfone type resin; Sulfone based resin; Polyether ether ketone resin; A sulfided polyphenylene resin; Vinyl alcohol-based resin; Vinylidene chloride resins; Vinyl butyral resin; Allylate series resin; Polyoxymethylene type resin; Epoxy resin, and the like, and a film composed of the blend of the thermoplastic resin may also be used. Further, a film made of a thermosetting resin such as (meth) acrylic, urethane, acrylic urethane, epoxy, or silicone or a film made of an ultraviolet curable resin may be used. The thickness of such a transparent optical film can be suitably determined, but in general, it can be determined to be 1 to 500 占 퐉 in consideration of workability such as strength and handling property, thin layer property, and the like. Particularly preferably 1 to 300 mu m, and more preferably 5 to 200 mu m.

Such a base film may contain one or more suitable additives. Examples of the additive include an ultraviolet absorber, an antioxidant, a lubricant, a plasticizer, a release agent, a coloring inhibitor, a flame retardant, a nucleating agent, an antistatic agent, a pigment and a colorant. The base film may be a structure including various functional layers such as a hard coating layer, an antireflection layer, and a gas barrier layer on one side or both sides of the film. The functional layer is not limited to the above, and may include various functional layers can do.

Further, if necessary, the base film may be surface-treated. Examples of the surface treatment include a chemical treatment such as a plasma treatment, a corona treatment, a dry treatment such as a primer treatment, and an alkali treatment including a saponification treatment.

The electrode portion 20 is formed of a plurality of electrodes formed on the substrate 10. The electrode unit 20 senses an electrical signal generated by a reaction between a substance included in the glucose reaction unit 50 described later and glucose contained in the measurement target substance. For example, the substance to be measured may be, but is not limited to, saliva, sweat, body fluids, blood, etc. of the human body.

For example, as illustrated in FIG. 2, the electrodes constituting the electrode unit 20 correspond to the working electrodes 21-1 and 22-1 and the working electrodes 21-1 and 22-1 And the reference electrode 21-2 or 22-2 may be formed of gold (Au), silver (Ag), copper (Cu), platinum (Pt), titanium (Ti ), Nickel (Ni), tin (Ni), molybdenum (Mo), cobalt (Co), and APC. APC is an Ag-Pd-Cu alloy.

The electrode protection layer 30 is formed on the electrode portion 20 to protect the electrodes constituting the electrode portion 20.

For example, the electrode protection layer 30 may include carbon.

The electron transport layer 40 is formed on the electrode protection layer 30 and functions to increase the electrical sensitivity of the electrode unit 20 through electron transport.

For example, the electron transport layer 40 may include prussian blue. Such prussian blue is a blue pigment mainly composed of potassium hexacyanoferrate (II) iron (III) oxide, and has a high oxidizing property. The sensitivity of the electrode can be improved by forming the electron transport layer 40 including prussian blue between the electrode unit 20 and the glucose reaction unit 50. However, (20) may be oxidized and corroded. According to an embodiment of the present invention, since the electrode protecting layer 30 is formed between the electron transporting layer 40 including prussian blue and the electrode portion 20, Corrosion of the electrode part 20 due to blue can be prevented.

The glucose reaction unit 50 is formed on the electron transport layer 40 and is a component that reacts with glucose contained in the measurement target substance.

For example, the glucose reaction unit 50 may include a glucose oxidase or a glucose dehydrogenase.

The reaction in the glucose reaction unit 50 and the signal detection principle of the electrode unit 20 will be described below as an example.

When a sample to be measured is injected into a glucose sensor, the glucose contained in the sample is oxidized by a glucose oxidase or a glucose dehydrogenase, and a glucose oxidase or a glucose dehydrogenase is reduced. At this time, the electron transfer mediator oxidizes glucose oxidase or glucose dehydrogenase and itself is reduced. The reduced electron transfer mediator loses electrons at the surface of the electrode to which a constant voltage is applied and is electrochemically reoxidized. The glucose concentration in the sample is proportional to the amount of current generated in the course of the oxidation of the electron transport mediator. Thus, the glucose concentration can be measured by measuring this amount of current.

Since the ion exchange membrane 60 is formed on the glucose reaction unit 50 and only the measurement target component is passed among the substances contained in the sample, the ion exchange membrane 60 prevents penetration of the external impurity ion component, Which protects glucose oxidase or glucose dehydrogenase. For example, the ion exchange membrane 60 may include Nafion, but this is only one example, and the ion exchange membrane 60 is not limited thereto.

The wiring portion 70 is composed of electrodes constituting the electrode portion 20 and a plurality of electric wirings extended from the temperature sensor 100. The wiring portion 70 may be connected to a sensing analysis means that performs a current analysis function via an electrically connecting medium such as an FPCB (Flexible Printed Circuit Board) (not shown). Although not shown in the figure, a pad region may be provided at the end of the wiring portion 70, and the FPCB may be electrically connected to the pad region.

The wiring connection portion 80 is a component for electrically connecting the electric wiring constituting the wiring portion 70. [ For example, the wiring connection portion 80 may be provided in a pad region connected to the end of the wiring portion 70, and may be configured to include a conductive tape or a conductive coating layer.

The separation guide unit 90 is provided near the wiring connection unit 80 and is a component for guiding the user to disconnect the wiring connection unit 80.

The principle that the sensing current saturation time is shortened by the wiring connection part 80 will be described as follows.

When the plurality of electric wires constituting the wiring portion 70 are electrically connected by using the wiring connection portion 80, the reference electrode and the working electrode are electrically shorted, and the voltage is previously applied to the working electrode And the measurement time of the sensor is shortened as the potential difference level between the electrodes is adjusted to be similar to each other.

This will be described in more detail as follows.

A plurality of electric wirings constituting the wiring portion 70 are connected to a plurality of electrodes constituting the electrode portion. A pad region is provided at the end of the wiring portion 70, that is, at the end of the electric wiring.

If a plurality of electric wires constituting the wiring portion 70 are not electrically connected by using the wire connecting portion 80 in a state where the glucose sensor is not used, the electrodes connected to the electric wires are not floating ) State, resulting in a minute potential difference between the electrodes. When the glucose concentration is to be measured using the glucose sensor in such a state, the potential difference acts as an error component, and therefore, a time for removing the glucose concentration is required.

In contrast, according to the embodiment of the present invention, the wiring connection portion 80 for electrically connecting the electric wires constituting the wiring portion 70 can prevent the initial electric potential difference between the plurality of electrodes constituting the electrode portion 20 from being substantially The saturation time of the current sensed through the electrode part by the glucose reaction in the glucose reaction part 50 is shortened to less than several seconds.

That is, according to an embodiment of the present invention, in a state in which the glucose sensor is not used, a plurality of electric wires constituting the wiring part 70 are electrically connected by using the wiring connection part 80, When the glucose concentration is measured by the user using the glucose sensor, it is possible to reduce the initial electric potential difference between the plurality of electrodes constituting the electrode by the operation of the detection and analysis means after removing the wiring connection portion 80 The saturation time of the current sensed through the electrode unit 20 is shortened to a few seconds or less.

The temperature sensor 100 is a component that is formed on the substrate 10 and measures the temperature of the environment in which the glucose concentration is measured. That is, the temperature sensor 100 transmits the current corresponding to the temperature to the IC having the current analysis function, and the IC converts the current value received from the temperature sensor 100 according to the set conversion algorithm. Since the measured glucose concentration may vary depending on the temperature, it is possible to measure the temperature together with the concentration of glucose, correct the concentration of glucose according to this temperature, or use it by matching the measured concentration and temperature .

Table 1 below is experimental data showing the comparison of the sensed current saturation time measured when the electrical wires constituting the wiring portion are electrically connected to each other and when the electrical wires are electrically connected to each other.

샘플Sample	연결전 포화시간(sec)Saturation time before connection (sec)	연결후 포화시간(sec)Saturation time after connection (sec)
1One	7070	1515
22	7373	1515
33	6969	1515

Referring to Table 1, since the sensing current of most of the samples prior to the electrical connection is saturated at about 70 seconds, the user measuring the glucose concentration must wait at least 70 to 80 seconds for the current to saturate for reliable measurement .

On the other hand, according to one embodiment of the present invention, when the electric wires constituting the wiring portion are electrically connected using the wiring connection portion, the saturation time of the sensing current is shortened to about 15 sec. It can be increased to a level corresponding to shortening of the sensing current saturation time.

It can be seen from FIG. 3A that the conventional sensing current graph is saturated at about 70 sec. On the other hand, FIG. 3B is a graph of the sensing current according to an embodiment of the present invention, which is saturated at about 15 seconds, and is shortened by about 55 seconds compared to the conventional art.

As described above, according to the present invention, a glucose sensor capable of increasing the measurement speed with respect to the glucose concentration is provided.

[Description of Symbols]

10: substrate

20:

21-1, 22-1: Working electrode

21-2, 22-2: reference electrode

30: electrode protection layer

40: electron transport layer

50: glucose reaction part

60: ion exchange membrane

70:

80:

90: separation guide

100: Temperature sensor

Claims

An electrode unit including a plurality of electrodes formed on a substrate;

A glucose reaction unit formed on the electrode unit;

A wiring portion formed of a plurality of electric wirings extending from the electrodes constituting the electrode portion; And

And a wiring connection portion for electrically connecting the electric wires constituting the wiring portion.
The method according to claim 1,

Wherein the wiring connection portion reduces the initial potential difference between the plurality of electrodes constituting the electrode portion to shorten the saturation time of the current sensed through the electrode portion by the glucose reaction in the glucose reaction portion, sensor.
The method according to claim 1,

Wherein the wiring connection portion is provided in a pad region connected to an end of the wiring portion.
The method according to claim 1,

Wherein the wiring connection part comprises a conductive tape or a conductive coating layer.
The method according to claim 1,

And a separation guide portion is formed between the electrode portion and the wiring connection portion.
The method according to claim 1,

The electrode part may be formed of at least one of Au, Ag, Cu, Pt, Ti, Ni, Ni, Mo, &Lt; / RTI > wherein the glucose sensor comprises at least one selected from the group consisting of glucose.
The method according to claim 1,

Further comprising an electrode protection layer formed on the electrode portion to protect the electrodes constituting the electrode portion.
8. The method of claim 7,

Characterized in that the electrode protection layer comprises carbon.
The method according to claim 1,

And an electron transport layer formed on the electrode portion.
10. The method of claim 9,

Wherein the electron transport layer comprises prussian blue.
The method according to claim 1,

Wherein the glucose reaction unit comprises a glucose oxidase or a glucose dehydrogenase.
The method according to claim 1,

Wherein the glucose sensor further comprises an ion exchange membrane formed on the glucose reaction unit.
13. The method of claim 12,

Wherein the ion exchange membrane prevents penetration of an impurity ion component to protect the glucose oxidase or the glucose dehydrogenase constituting the glucose reaction unit.
13. The method of claim 12,

Characterized in that the ion exchange membrane comprises Nafion.
The method according to claim 1,

And a temperature sensor formed on the substrate.