CN210871604U

CN210871604U - Microneedle electrode for glucose sensor and microneedle glucose sensor

Info

Publication number: CN210871604U
Application number: CN201921133518.7U
Authority: CN
Inventors: 沈永健; 王强; 陈毅豪
Original assignee: Zhejiang Heqing Flexible Electronic Technology Co ltd
Current assignee: Zhejiang Heqing Flexible Electronic Technology Co ltd
Priority date: 2019-07-18
Filing date: 2019-07-18
Publication date: 2020-06-30
Anticipated expiration: 2029-07-18

Abstract

A microneedle type electrode for a glucose sensor comprises a working electrode and a sheet-shaped substrate, wherein the working electrode comprises a current collecting layer, a medium layer, an enzyme layer and a first permeable membrane layer, the current collecting layer, the medium layer, the enzyme layer and the first permeable membrane layer are sequentially stacked from the direction close to the substrate to the direction far away from the substrate, and the extending directions of the current collecting layer, the medium layer, the enzyme layer and the first permeable membrane layer are all parallel to the substrate. The micro-needle type electrode for the glucose sensor has the advantages of large effective sensing area and high sensitivity.

Description

Microneedle electrode for glucose sensor and microneedle glucose sensor

Technical Field

The utility model belongs to the technical field of the sensor technique and specifically relates to a micropin formula electrode that glucose sensor used and have its micropin formula glucose sensor.

Background

Glucose sensors are a core device in blood glucose monitoring systems. According to the detection method, common glucose sensors can be classified into three categories: blood type, non-invasive type (including interstitial fluid glucose sensor and glucose optical sensor) and micro-needle type. The micro-needle type can go deep into the human body for measurement, so that the measurement result is accurate.

The needle body of the micro-needle type electrode for the prior glucose sensor is generally in a conical shape, and all working film layers of the sensor are sequentially arranged on a conical substrate. The sensor in the form has a large volume, the pain in the puncturing process is strong, and the effective sensing area of the sensor is very limited, so that the sensitivity is low, the signal-to-noise ratio is high, and the stability after implantation is poor.

SUMMERY OF THE UTILITY MODEL

In view of this, the utility model provides a micropin formula electrode and have its micropin formula glucose sensor that glucose sensor used, this effective sensing area of micropin formula electrode that glucose sensor used is great, and sensitivity is higher.

The utility model provides a micropin formula electrode that glucose sensor used, including working electrode and flaky base plate, working electrode sets up in basic one side, working electrode includes current collector layer, medium layer, enzyme layer and first infiltration rete, the current collector layer the medium layer the enzyme layer reaches first infiltration rete is from being close to the base plate direction is to keeping away from the base plate direction is range upon range of the setting in proper order, the current collector layer the medium layer the enzyme layer reaches first infiltration rete all with the base plate is parallel.

Further, the microneedle type electrode for the glucose sensor further comprises a reference electrode, the reference electrode is arranged on the other side of the substrate, back to the working electrode, and comprises a first electrode layer and a second permeation film layer, the first electrode layer is arranged on one side, away from the current collector layer, of the substrate, and the second permeation film layer covers the first electrode layer.

Further, the reference electrode is multiplexed as a counter electrode.

Further, the substrate includes a needle body portion, in the needle body portion region, the current collecting layer, the mediator layer, the enzyme layer, and the first permeation film layer are disposed on one side of the needle body portion, and the first electrode layer and the second permeation film layer are disposed on the other side of the needle body portion.

The substrate further comprises a base body portion, pins corresponding to the working electrode and the reference electrode are arranged on the base body portion, and the working electrode and the reference electrode are respectively and electrically connected with the corresponding pins.

Further, the width of the needle body part is not more than 0.3mm, the length is not more than 6mm, and the thickness is not more than 0.2 mm.

Further, the substrate is a substrate formed of an inorganic non-metallic ceramic, a silica glass, or an organic polymer.

Further, the organic polymer includes polytetrafluoroethylene, polyethylene, polyvinyl chloride, acrylonitrile-butadiene-styrene copolymer, polymethyl methacrylate, polycarbonate, or polyimide.

Further, the current collector layer is a current collector layer formed of gold, silver, platinum, or a conductive polymer.

Further, the medium layer is a medium layer formed of gold, silver, platinum, or prussian blue.

Further, the enzyme layer is an enzyme layer formed of glucose oxidase or glucose dehydrogenase.

To sum up, in the utility model discloses in, through the range upon range of setting of the diaphragm layer with working electrode, the extending direction that makes the diaphragm layer all is parallel with the base plate, becomes the flaky base plate in this embodiment with the toper of base member from prior art, makes conical needle body become the platykurtic of present each rete parallel range upon range of setting then, can increase effective sensing area like this, improves the sensitivity of sensor.

The foregoing description is only an overview of the technical solutions of the present invention, and in order to make the technical means of the present invention more clearly understood, the present invention may be implemented according to the content of the description, and in order to make the above and other objects, features, and advantages of the present invention more obvious and understandable, the following preferred embodiments are described in detail with reference to the accompanying drawings.

Drawings

Fig. 1 is a schematic structural diagram of a microneedle electrode for a glucose sensor according to an embodiment of the present invention.

Fig. 2 is a schematic cross-sectional view of the various layers in the needle body of fig. 1.

Detailed Description

To further illustrate the technical means and effects of the present invention adopted to achieve the intended purpose of the invention, the following detailed description is given with reference to the accompanying drawings and preferred embodiments.

The utility model provides a micropin formula electrode that glucose sensor used and have its micropin formula glucose sensor, the effective sensing area of the micropin formula electrode that this glucose sensor used is great, and sensitivity is higher.

Fig. 1 is a schematic view showing a structure of a microneedle type electrode for a glucose sensor, fig. 2 is a schematic view showing a cross-sectional structure of each membrane layer in a needle body of fig. 1, as shown in fig. 1 and fig. 2, in this embodiment, the microneedle type electrode for the glucose sensor includes a working electrode 10 and a sheet-shaped substrate 20, the working electrode 10 is disposed on one side of the substrate 20, the working electrode 10 includes a current collecting layer 11, a mediator layer 12, an enzyme layer 13 and a first permeable membrane layer 14, the current collecting layer 11, the mediator layer 12, the enzyme layer 13 and the first permeable membrane layer 14 are sequentially stacked from a direction close to the substrate 20 to a direction far away from the substrate 20, and each membrane layer is parallel to the substrate 20.

In this embodiment, the diaphragm layers of the working electrode 10 are stacked on the substrate 20, and all the diaphragm layers are parallel to the substrate 20, so that the tapered base body in the prior art is changed into the sheet-shaped substrate 20 in this embodiment, and then the tapered needle body is changed into the flat needle body in which the current film layers are stacked in parallel, which can increase the effective sensing area and improve the sensitivity of the sensor.

In the fabrication of the microneedle type electrode for glucose sensor, the current collector layer 11 may be formed on the substrate 20 by a deposition process such as electron beam evaporation, magnetron sputtering, or thermal evaporation, and the medium layer 12 may be formed on the current collector layer 11 by a deposition process. The forming process can realize the uniform distribution of the current collector layer 11 and the medium layer 12 on one hand; on the other hand, the interaction among the working layers can be increased, the high-strength adhesion among the working layers is realized, and the electronic transmission is facilitated, so that the sensitivity and the stability of the sensor are improved; on the other hand, the current collector layer 11 and the medium layer 12 formed by the deposition process do not need to be dried, so that the forming time is shortened, and the processes of other film layers can be performed faster after the current collector layer 11 and the medium layer 12 are formed.

Referring to fig. 1 and fig. 2, in the present embodiment, the microneedle type electrode for a glucose sensor further includes a reference electrode 30, the reference electrode 30 is disposed on the other side of the substrate 20 opposite to the working electrode 10, the reference electrode 30 includes a first electrode layer 31 and a second permeation membrane layer 32, the first electrode layer 31 is disposed on one side of the substrate 20 away from the current collector layer 11, and the second permeation membrane layer 32 covers the first electrode layer 31. That is, the film layers of the reference electrode 30 are disposed on the side of the substrate 20 away from the film layers of the working electrode 10.

In other embodiments, the reference electrode 30 can also be used as a counter electrode at the same time, that is, the reference electrode 30 and the counter electrode are combined into one to improve the accuracy of the signal. The first electrode layer 31 may be formed of a silver/silver chloride electrode, a calomel electrode, or the like.

Further, the base plate 20 includes a base portion 21 and a needle portion 22 connected to the base portion 21, and the needle portion 22 is used for being inserted into the skin of a human body. The current collector layer 11, the mediator layer 12, the enzyme layer 13, and the first permeable membrane layer 14 are stacked on one side of the needle body portion 22, and one side of the first electrode layer 31 and the second permeable membrane layer 32 is disposed on the other side of the needle body portion 22. In addition, the current collector layer 11 and the first electrode layer 31 extend from the needle body 22 to the base portion 21 to extract signals of the working electrode 10 and the reference electrode 30. That is, the medium layer 12, the enzyme layer 13, the first permeable membrane layer 14, the first electrode layer 31, and the second permeable membrane layer 32 are all disposed on the needle portion 22, and the current collector layer 11 and the first electrode layer 31 are all disposed on both the needle portion 22 and the base portion 21.

In this embodiment, the material of the substrate 20 may be made of inorganic non-metallic ceramic, silica glass, organic polymer, or the like. The organic polymer may include one or a combination of more of Polytetrafluoroethylene (PTFE), Polyethylene (PE), Polyvinyl chloride (PVC), Acrylonitrile butadiene Styrene copolymer (ABS), polymethyl methacrylate (PMMA), Polycarbonate (PC), Polyimide (PI), and the like.

The current collector layer 11 and the first electrode layer 31 may extract an electrical signal generated by the sensor, and the current collector layer 11 and the first electrode layer 31 may be formed of a metal material such as gold, silver, or platinum, or a conductive polymer, and preferably, are formed of a gold material, and have a thickness of 50 to 300 nm.

The medium layer 12 can promote the reaction between glucose and the enzyme layer 13, and the medium layer 12 can be formed of metal such as gold, silver, platinum, or the like, or Prussian blue analog, preferably platinum, and has a thickness of 50-300 nm.

The enzyme layer 13 is used for reacting with glucose and generating a corresponding electric signal, and the enzyme layer 13 may be formed by solidifying a laminate of glucose oxidase or glucose dehydrogenase, and preferably, the enzyme layer 13 may be formed by solidifying the cross-linked glucose oxidase layer 13.

The first and second

permeable membrane layers

14 and 32 can isolate the enzyme layer 13 and the first electrode layer 31 from interfering substances other than glucose in the human body, and the first and second

permeable membrane layers

14 and 32 can be formed of polyvinyl acetate (PVA), Polyethylene glycol (PEG), Polyacrylamide (PAM), acetate (acetate), a first permeable membrane 15 made of one or more materials selected from polyethylene oxide (PEO), polyvinylpyrrolidone (PVP), and a copolymer of polytetrafluoroethylene and perfluoro-3, 6-diepoxy-4-methyl-7-decene-sulfuric acid (Nafion), preferably a copolymer of polytetrafluoroethylene and perfluoro-3, 6-diepoxy-4-methyl-7-decene-sulfuric acid (Nafion).

In the area of the needle portion 22 of the base plate 20, the width of the microneedle electrode needle portion 22 for the glucose sensor is not more than 0.3mm, the length is not more than 6mm, and the thickness is not more than 0.2mm, so as to ensure that the microneedle electrode for the glucose sensor can be smoothly inserted into the human body.

The base body 21 has pins corresponding to the working electrode, the counter electrode, and the reference electrode, and each electrode is electrically connected to its corresponding pin through a wire.

In summary, in the present invention, the diaphragm layer of the working electrode 10 is stacked, the extending direction of the diaphragm layer is parallel to the substrate 20, the substrate is changed into the sheet-shaped substrate 20 in the present embodiment from the taper in the prior art, and then the tapered needle body is changed into the flat shape of the parallel stacked arrangement of the current films, so that the effective sensing area can be increased, and the sensitivity of the sensor can be improved.

The utility model also provides a micropin formula glucose sensor, this micropin formula glucose sensor include the micropin formula electrode that foretell glucose sensor used, about other technical characteristics of this micropin formula glucose sensor, please see prior art, no longer give consideration to here.

The above description is only a preferred embodiment of the present invention, and the present invention is not limited to the above embodiments, and although the present invention has been disclosed with the preferred embodiments, it is not limited to the present invention, and any skilled person in the art can make some modifications or equivalent changes without departing from the technical scope of the present invention.

Claims

1. A microneedle electrode for a glucose sensor, comprising: the electrode comprises a working electrode and a flaky substrate, wherein the working electrode is arranged on one side of the substrate, the working electrode comprises a current collecting layer, a medium layer, an enzyme layer and a first permeable membrane layer, the current collecting layer, the medium layer, the enzyme layer and the first permeable membrane layer are sequentially stacked from the direction close to the substrate to the direction far away from the substrate, and the current collecting layer, the medium layer, the enzyme layer and the first permeable membrane layer are all parallel to the substrate.

2. A microneedle electrode for a glucose sensor according to claim 1, wherein: the micro-needle type electrode for the glucose sensor further comprises a reference electrode, the reference electrode is arranged on the other side of the substrate, back to the working electrode, and comprises a first electrode layer and a second permeation film layer, the first electrode layer is arranged on one side, away from the substrate, of the current collector layer, and the second permeation film layer covers the first electrode layer.

3. A microneedle electrode for a glucose sensor according to claim 2, characterized in that: the reference electrode is reused as a counter electrode.

4. A microneedle electrode for a glucose sensor according to claim 2, characterized in that: the substrate includes a needle body portion, the current collecting layer, the mediator layer, the enzyme layer, and the first permeation film layer are disposed on one side of the needle body portion in the needle body portion region, and the first electrode layer and the second permeation film layer are disposed on the other side of the needle body portion.

5. A microneedle electrode for a glucose sensor according to claim 4, wherein: the base plate further comprises a base body part, pins corresponding to the working electrode and the reference electrode are arranged on the base body part, and the working electrode and the reference electrode are respectively and electrically connected with the corresponding pins.

6. A microneedle electrode for a glucose sensor according to claim 4, wherein: the width of the needle body part is not more than 0.3mm, the length is not more than 6mm, and the thickness is not more than 0.2 mm.

7. A microneedle electrode for a glucose sensor according to claim 1, wherein: the substrate is formed by inorganic non-metallic ceramic, silica glass or organic polymer.

8. A microneedle electrode for a glucose sensor according to claim 7, wherein: the organic polymer comprises polytetrafluoroethylene, polyethylene, polyvinyl chloride, acrylonitrile-butadiene-styrene copolymer, polymethyl methacrylate, polycarbonate or polyimide.

9. A microneedle electrode for a glucose sensor according to claim 1, wherein: the current collector layer is a current collector layer formed of gold, silver, platinum, or a conductive polymer.

10. A microneedle electrode for a glucose sensor according to claim 1, wherein: the medium layer is formed by gold, silver, platinum or Prussian blue.

11. A microneedle electrode for a glucose sensor according to claim 1, wherein: the enzyme layer is formed by glucose oxidase or glucose dehydrogenase.

12. A microneedle glucose sensor, comprising: a microneedle electrode for a glucose sensor comprising any one of claims 1-11.