WO2019045232A1

WO2019045232A1 - Glucose sensor and method for manufacturing same

Info

Publication number: WO2019045232A1
Application number: PCT/KR2018/006340
Authority: WO
Inventors: 최봉진; 천승환; 금중한; 김태균
Original assignee: 동우 화인켐 주식회사
Priority date: 2017-09-01
Filing date: 2018-06-04
Publication date: 2019-03-07
Also published as: KR20190025354A; KR102499784B1

Abstract

The present invention relates to a method for manufacturing a glucose sensor. The present invention comprises: an electrode forming step of forming an electrode part composed of a plurality of electrodes on a substrate; an electrode protection/electron transport function layer forming step of forming an electrode protection/electron transport function layer including an electrode protector and an electron transporter on the electrode part; a glucose reaction part forming step of forming a glucose reaction part on the electrode protection/electron transport function layer; and an ion exchange membrane forming step of forming an ion exchange membrane on the glucose reaction part. According to the present invention, the number, time, and cost of the processes required to manufacture a glucose sensor can be reduced.

Description

Glucose sensor and manufacturing method thereof

The present invention relates to a glucose sensor and a manufacturing method thereof. More specifically, the present invention simplifies the process by forming the electrode protecting means for protecting the electrodes and the electrode transporting means for transporting the electrons to the electrodes through one printing process, thereby reducing the number, time and cost of the required processes And to a glucose sensor capable of realizing a thin film type and a method for manufacturing the same.

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.

According to the prior art related to the glucose sensor, a prussian blue layer is formed on the electrode by an electroplating method in order to increase the electrical sensitivity of the electrode. Since the prussian blue layer is highly oxidative, There is a problem that the sensitivity of the electrode is increased but the metal component constituting the electrode is oxidized and corroded by the Prussian blue layer.

According to the prior art, a step of further printing a carbon protective layer between the electrode and the Prussian blue layer is performed in order to prevent electrode corrosion by prussian blue.

As described above, according to the related art, since the process of electroplating the prussian blue layer on the carbon protective layer after printing the carbon protective layer on the electrode has been performed, there has been a problem that inefficiency occurs in terms of manufacturing time and cost.

Further, since the carbon protective layer and the Prussian blue layer are present as separate layers, there is a problem that the thinness of the glucose sensor is hindered.

[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)

SUMMARY OF THE INVENTION The present invention is directed to reducing the number, time, and cost of processes required to manufacture a glucose sensor.

It is another object of the present invention to provide a method of manufacturing a glucose sensor capable of simplifying a process by forming an electrode protecting means for protecting the electrode and an electrode transporting means for transporting electrons to the electrode through one printing process on the electrode. .

In addition, the present invention has a technical object to reduce the thickness of the glucose sensor by implementing electrode protection means for protecting the electrode and electrode transport means for transporting electrons to the electrode as one layer.

According to an aspect of the present invention, there is provided a method of fabricating a glucose sensor, including: forming an electrode portion having a plurality of electrodes on a substrate; forming an electrode protector on the electrode portion, Forming a glucose reaction part on the electrode protection / electron transporting function layer, and forming an ion exchange membrane on the glucose reaction part And an ion exchange membrane forming step.

In the method for manufacturing a glucose sensor according to the present invention, in the step of forming the electrode protection / electron transporting function layer, a paste mixed with the electrode protecting material and the electron transporting material is printed on the electrode part and dried, Thereby forming a transport function layer.

In the method for manufacturing a glucose sensor according to the present invention, the electrode protecting member includes carbon.

In the method of manufacturing a glucose sensor according to the present invention, the electron transporting body may include prussian blue.

In the method for manufacturing a glucose sensor according to the present invention, the electrode portion may be formed of gold (Au), silver (Ag), copper (Cu), platinum (Pt), titanium (Ti), nickel (Ni), tin (Mo), cobalt (Co), and APC.

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

In the method for manufacturing a glucose sensor according to the present invention, the ion exchange membrane prevents permeation of an impurity ion component, thereby protecting a glucose oxidase or a glucose dehydrogenase constituting the glucose reaction unit.

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

The glucose sensor according to the present invention includes an electrode protection electrode / electron transport function layer including an electrode portion formed of a plurality of electrodes formed on a substrate, an electrode protector formed on the electrode portion and an electron transporter, A glucose reaction part formed on the functional layer and an ion exchange membrane formed on the glucose reaction part.

In the glucose sensor according to the present invention, the electrode protecting / electron transporting function layer is formed of one layer in which the electrode protecting body and the electron transporting body are mixed.

According to the present invention, it is possible to reduce the number, time, and cost of a process required for manufacturing a glucose sensor.

In addition, the electrode protecting means for protecting the electrodes and the electrode transporting means for transporting the electrons to the electrodes are formed on the electrodes through one printing step, thereby simplifying the process.

In addition, by implementing electrode protection means for protecting the electrodes and electrode transport means for transporting electrons to the electrodes, the glucose sensor can be made thinner.

FIG. 1 is a process flow chart of a method of manufacturing a glucose sensor according to an embodiment of the present invention,

FIGS. 2 to 5 are cross-sectional views illustrating a method of manufacturing a glucose sensor according to an embodiment of the present invention,

Figure 6 is an exemplary top view of a glucose sensor made in accordance with one embodiment of the present invention.

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 process flow diagram of a method of manufacturing a glucose sensor according to an embodiment of the present invention, FIGS. 2 to 5 are sectional views of a process for manufacturing a glucose sensor according to an embodiment of the present invention, 1 is an exemplary top view of a glucose sensor made according to an embodiment.

Referring to FIGS. 1 to 6, a method for fabricating a glucose sensor according to an embodiment of the present invention includes forming an electrode (S10), forming an electrode protection / electron transport layer (S20), forming a glucose reaction part (S30) And an ion exchange membrane forming step (S40).

First, referring to FIGS. 1 and 2, in an electrode forming step (S10), a process of forming an electrode unit 20 including a plurality of electrodes on a substrate 10 is performed.

The electrode unit 20 senses an electrical signal generated by a reaction between a substance included in the glucose reaction unit 40 described later and glucose contained in the measurement target substance. For example, the substance to be measured may be, but not limited to, sweat, body fluids, blood, etc. of the human body.

For example, as illustrated in FIG. 6, the electrodes constituting the electrode unit 20 correspond to the sensing electrodes 21-1 and 22-1 and the sensing electrodes 21-1 and 22-1, respectively. 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.

Reference numeral 60 in FIG. 6 denotes electric wiring, and reference numeral 70 denotes a temperature sensor. This temperature sensor can be used as a means for correcting the measurement deviation according to the temperature.

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.

1 and 3, in the electrode protection / electron transport function layer formation step S20, an electrode protection / electron transport function layer 30 including an electrode protection body and an electron transporter is formed on the electrode portion 20, Are formed.

For example, the electrode protector may include carbon, and the electron transport material may include prussian blue.

The Prussian blue, which is an electron transport included in the electrode protection / electron transport function layer 30, functions to increase the electrical sensitivity of the electrode unit 20. [

Such prussian blue is a blue pigment mainly composed of potassium hexacyanoferrate (II) iron (III) oxide, and has a high oxidizing property. Although the sensitivity of the electrode unit 20 can be improved by forming Prussian blue between the electrode unit 20 and the glucose reaction unit 40, the metallic electrode unit 20 located at the lower portion of Prussian blue It can be oxidized and corroded. In an embodiment of the present invention, Prussian blue, which is an electron transporting material, and an electrode protection carbon are mixed to form an electrode protection / electron transport function layer 30 on the electrode portion 20, (20) corrosion can be prevented, and the sensitivity of the electrode portion (20) can be improved.

For example, in the electrode protection / electron transport function layer formation step S20, a paste in which carbon, which is electrode protection, and Prussian blue, which is an electron transport, is mixed and printed on the electrode portion 20, And may be configured to form the functional layer 30. According to this configuration, since the electrode protecting means for protecting the electrodes and the electrode transporting means for transporting the electrons to the electrodes can be formed on the electrodes through one printing process, the process can be simplified and the manufacturing time and cost can be reduced .

Referring to FIGS. 1 and 4, a glucose reaction unit 40 is formed on the electrode protection / electron transport function layer 30 in the glucose reaction unit formation step S30.

The glucose reaction unit 40 is a component that reacts with glucose contained in the measurement target substance.

For example, the glucose reaction unit 40 may include a glucose oxidase or a glucose dehydrogenase.

The reaction in the glucose reaction unit 40 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.

1 and 5, in the ion exchange membrane forming step S40, a process of forming the ion exchange membrane 50 on the glucose reaction unit 40 is performed.

Since the ion exchange membrane 50 passes only the component to be measured out of the substances contained in the sample, it prevents the penetration of the external impurity ion component and protects the glucose oxidase or glucose dehydrogenase constituting the glucose reaction unit 40 do. For example, the ion exchange membrane 50 may include Nafion, but this is only one example, and the ion exchange membrane 50 is not limited thereto.

When the above-described manufacturing process is performed, since the electrode protecting / electron transporting function layer 30 is formed as a single layer in which the electrode protecting member and the electron transporting material are mixed, a thin film glucose sensor can be obtained in comparison with the conventional one.

That is, according to the related art, the electrode protection function layer and the electron transport function layer exist as separate layers and the thickness of the glucose sensor is thick, but according to the present invention, the electrode protection / It is possible to make the glucose sensor thinner.

As described above in detail, according to the present invention, it is possible to reduce the number, time, and cost of a process required for manufacturing a glucose sensor.

[Description of Symbols]

10: substrate

20:

30: electrode protection / electron transport function layer

40: glucose reaction part

50: ion exchange membrane

S10: Electrode formation step

S20: Electrode protection / electron transport function layer formation step

S30: Glucose reaction part formation step

S40: ion exchange membrane forming step

Claims

An electrode forming step of forming an electrode part composed of a plurality of electrodes on a substrate;

An electrode protection / electron transport function layer forming step of forming an electrode protection / electron transport function layer including an electrode protector and an electron transporter on the electrode part;

A glucose reaction part forming step of forming a glucose reaction part on the electrode protection / electron transport function layer; And

And forming an ion exchange membrane on the glucose reaction unit.
The method according to claim 1,

In the electrode protecting / electron transporting function layer forming step,

Wherein the electrode protecting / electron transporting function layer is formed by printing and drying a paste in which the electrode protecting material and the electron transporting material are mixed on the electrode portion.
The method according to claim 1,

Wherein the electrode protector comprises carbon. &Lt; RTI ID = 0.0 > 8. < / RTI >
The method according to claim 1,

Wherein the electron transporter comprises prussian blue. &Lt; RTI ID = 0.0 > 11. < / RTI >
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:
The method according to claim 1,

Wherein the glucose reaction unit comprises a glucose oxidase or a glucose dehydrogenase.
The method according to claim 6,

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.
The method according to claim 1,

Wherein the ion exchange membrane comprises Nafion. &Lt; RTI ID = 0.0 > 8. < / RTI >
An electrode unit including a plurality of electrodes formed on a substrate;

An electrode protecting / electron transporting function layer including an electrode protecting body formed on the electrode portion and an electron transporter;

A glucose reaction unit formed on the electrode protection / electron transport function layer; And

And an ion exchange membrane formed on the glucose reaction unit.
10. The method of claim 9,

The electrode protective /

And the glucose sensor is formed of one layer in which the electrode protecting member and the electron transporting member are mixed.