CN114589466B - Method for preparing three-dimensional microneedle blood sugar electrode based on dimension reduction screen printing - Google Patents

Method for preparing three-dimensional microneedle blood sugar electrode based on dimension reduction screen printing Download PDF

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CN114589466B
CN114589466B CN202210281003.1A CN202210281003A CN114589466B CN 114589466 B CN114589466 B CN 114589466B CN 202210281003 A CN202210281003 A CN 202210281003A CN 114589466 B CN114589466 B CN 114589466B
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layer
needle
sheet
metal plane
metal
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CN114589466A (en
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谢曦
莫境山
黄新烁
陈惠琄
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Sun Yat Sen University
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B23MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
    • B23PMETAL-WORKING NOT OTHERWISE PROVIDED FOR; COMBINED OPERATIONS; UNIVERSAL MACHINE TOOLS
    • B23P15/00Making specific metal objects by operations not covered by a single other subclass or a group in this subclass
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00Measuring for diagnostic purposes; Identification of persons
    • A61B5/145Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue
    • A61B5/14503Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue invasive, e.g. introduced into the body by a catheter or needle or using implanted sensors
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00Measuring for diagnostic purposes; Identification of persons
    • A61B5/145Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue
    • A61B5/14532Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue for measuring glucose, e.g. by tissue impedance measurement
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61BDIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B2562/00Details of sensors; Constructional details of sensor housings or probes; Accessories for sensors
    • A61B2562/12Manufacturing methods specially adapted for producing sensors for in-vivo measurements
    • A61B2562/125Manufacturing methods specially adapted for producing sensors for in-vivo measurements characterised by the manufacture of electrodes
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00Technologies related to metal processing
    • Y02P10/25Process efficiency

Abstract

The application discloses a method for preparing a three-dimensional microneedle blood sugar electrode based on dimension reduction screen printing, which comprises the following steps: cutting the metal sheet to obtain a suspension type metal plane micro-needle sheet; cleaning the metal plane micro-needle, and preparing an electrode layer on the cleaned metal plane micro-needle by magnetron sputtering; sequentially printing functional layers on the front side and the back side of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electron mediator layer, a glucose oxidase layer and an outer membrane layer; cutting the hanging part to demould the metal plane micro-needle plated with the functional layer; and assembling a plurality of demoulded metal plane micro-needle sheets through the base frame to obtain the three-dimensional micro-needle blood sugar electrode. The embodiment of the application realizes the batch repeatability modification of the coating, improves the firmness and uniformity of the coating, optimizes the preparation process, and can be widely applied to the technical field of microneedle preparation.

Description

Method for preparing three-dimensional microneedle blood sugar electrode based on dimension reduction screen printing
Technical Field
The application relates to the technical field of microneedle preparation, in particular to a method for preparing a three-dimensional microneedle blood sugar electrode based on dimension reduction screen printing.
Background
Diabetes patients need to take blood glucose measurements and take medicine several times a day, and face the pain caused by puncturing the fingers when measuring blood glucose. Microneedle electrode arrays have been greatly developed in the continuous monitoring of diabetes, and implanted sensors based on microneedle electrodes improve patient compliance by reducing pain sensation, and strictly monitor blood glucose, reduce blood glucose and the risk of diabetic complications. With the continuous and deep research, the linear detection range, sensitivity, reaction time and storage time of the microneedle blood sugar sensing electrode for detecting glucose in blood and tissue fluid are greatly improved.
At present, the three-dimensional microneedle electrode has high mass processing difficulty, the electrode processing technology is complex, the coating modification uniformity of the surface of the microneedle electrode prepared by adopting a conventional dip-coating method is poor, the batch repeated modification is difficult, and the coating modification is not firm and easy to fall off.
Disclosure of Invention
In view of the above, the embodiment of the application aims to provide a method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing, which realizes batch repeatability modification of a coating, improves the firmness and uniformity of the coating and optimizes the preparation process.
In a first aspect, an embodiment of the present application provides a method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing, including the following steps:
cutting the metal sheet to obtain a suspension type metal plane micro-needle sheet;
cleaning the metal plane micro-needle, and preparing an electrode layer from the cleaned metal plane micro-needle by magnetron sputtering;
sequentially printing functional layers on the front side and the back side of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electron mediator layer, a glucose oxidase layer and an outer membrane layer;
cutting the hanging part to demould the metal plane micro-needle plated with the functional layer;
and assembling a plurality of demoulded metal plane micro-needle sheets through the base frame to obtain the three-dimensional micro-needle blood sugar electrode.
Optionally, the cutting the metal sheet includes:
and cutting the metal sheet by using a laser marking machine or a laser cutting machine.
Optionally, when the metal sheet is cut by a laser marking machine, the method specifically comprises the following steps:
placing a metal sheet into a fixture tool of a laser marking machine for fixation, and setting the laser marking machine to execute reverse incomplete cutting on the metal sheet according to a first preset parameter; the cut contour lines extend for a plurality of times according to the preset interval.
Alternatively, when the metal sheet is cut using a laser marking machine, the number of marking times is positively correlated with the thickness of the metal sheet.
Optionally, the cleaning the metal plane microneedle sheet specifically includes:
and respectively performing laser cleaning on the front side and the back side of the metal plane micro-needle by adopting a laser marking machine according to a second preset parameter.
Optionally, the material of the electron mediator layer includes carbon nanotubes or reduced graphene oxide, and the screen printing material of the carbon nanotubes or reduced graphene oxide is prepared by the following method:
the multi-wall carbon nano tube powder or the reduced graphene oxide powder is dissolved in isopropanol to prepare a solution with preset concentration.
Optionally, the front and back sides of the metal plane microneedle sheet plated with the electrode layer are respectively printed with functional layers in sequence by adopting screen printing, wherein the functional layers comprise an electron mediator layer, a glucose oxidase layer and an outer membrane layer, and specifically comprise:
printing an electron mediator layer on the front surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
printing an electronic mediator layer on the reverse side of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
printing a glucose oxidase layer on the front surface of the metal plane micro-needle sheet printed with the electron mediator layer by adopting screen printing;
printing a glucose oxidase layer on the reverse side of the metal plane micro-needle sheet printed with the electron mediator layer by adopting screen printing;
adopting screen printing to print an outer film layer on the front surface of the metal plane microneedle sheet printed with the glucose oxidase layer;
and (3) printing an outer film layer on the reverse side of the metal plane microneedle sheet printed with the glucose oxidase layer by adopting screen printing.
Optionally, the method comprises:
and detecting the thicknesses of the electrode layer and the functional layer by using a film thickness meter.
The embodiment of the application has the following beneficial effects: in the embodiment, firstly, a metal sheet is cut to obtain a suspension type metal plane micro-needle sheet; preparing an electrode layer on the cleaned metal plane micro-needle through magnetron sputtering, and sequentially printing functional layers on the front side and the back side of the metal plane micro-needle plated with the electrode layer through screen printing; finally, assembling the demoulded metal plane microneedle sheet to obtain a three-dimensional microneedle blood sugar electrode; the functional layers with good firmness and uniformity are prepared in batches and repeatedly by adopting a screen printing process, and the two-dimensional plane microneedle sheets are prepared first and then assembled into the three-dimensional microneedle electrode, so that the preparation process is optimized, and the production and processing cost is reduced.
Drawings
Fig. 1 is a schematic flow chart of steps of a method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing according to an embodiment of the application;
FIG. 2 is a schematic flow chart of steps of another method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing according to an embodiment of the present application;
FIG. 3 is a schematic diagram of a normal phase cutting and reverse phase cutting structure according to an embodiment of the present application;
FIG. 4 is an SEM image of a metal planar microneedle sheet prepared by screen printing according to an embodiment of the present application;
FIG. 5 is a graph showing a comparison of blood glucose concentrations for electrodes prepared by screen printing and commercial electrodes according to an embodiment of the present application;
fig. 6 is a graph showing the thickness results of a carbon nanotube prepared on a planar microneedle sheet using screen printing according to an embodiment of the present application.
Detailed Description
The application will now be described in further detail with reference to the drawings and to specific examples. The step numbers in the following embodiments are set for convenience of illustration only, and the order between the steps is not limited in any way, and the execution order of the steps in the embodiments may be adaptively adjusted according to the understanding of those skilled in the art.
As shown in fig. 1, the embodiment of the application provides a method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing, which comprises the following steps:
s100, cutting the metal sheet to obtain the suspension type metal plane microneedle sheet.
It should be noted that the metal sheet includes stainless steel sheets, such as 304H, all the brands of stainless steel sheets, and any other metal sheet that can be etched by laser in 1064nm band, and the thickness of the metal sheet is between 50um and 400um. A suspended metal planar microneedle can be understood as a metal planar microneedle which is connected to a metal foil by a connection site.
It should be noted that, the cutting device may be a laser marking machine, or any device capable of precisely cutting a planar metal sheet, such as a laser cutting machine or a precision machining center.
Optionally, the cutting the metal sheet includes:
s110, cutting the metal sheet by using a laser marking machine or a laser cutting machine.
Optionally, when the metal sheet is cut by a laser marking machine, the method specifically comprises the following steps:
s111, placing a metal sheet into a fixture tool of a laser marking machine for fixation, and setting the laser marking machine to execute reverse incomplete cutting on the metal sheet according to a first preset parameter; the cut contour lines extend for a plurality of times according to the preset interval.
Alternatively, when the metal sheet is cut using a laser marking machine, the number of marking times is positively correlated with the thickness of the metal sheet.
In one embodiment, stainless steel sheets are placed in a fixture tool of a laser marking machine for fixation, inverted incomplete cutting is performed, and the contour lines are subjected to 10 extensions with a spacing of 1um. The cutting parameters were as follows: marking speed is 700mm/s, space jump speed is 2000mm/s, Q frequency is 40kHz, Q release: 1us, power 6W, laser pulse width 30us, marking times/steel sheet thickness: 1200 times/150 um, 1400 times/200 um, 2500 times/400 um.
And S200, cleaning the metal plane micro-needle, and preparing an electrode layer on the cleaned metal plane micro-needle by magnetron sputtering.
It should be noted that, performing laser cleaning on the front and back sides of the metal planar micro-needle sheet can further improve the firmness of the electrode layer and the metal sheet.
The material of the electrode layer includes, but is not limited to, carbon, gold, platinum, or the like.
Optionally, the cleaning the metal plane microneedle sheet specifically includes:
and S210, respectively performing laser cleaning on the front side and the back side of the metal plane micro-needle by adopting a laser marking machine according to a second preset parameter.
In one embodiment, the steel sheet with the microneedle pattern is obtained by removing the inverted pattern from the cut steel sheet, and laser cleaning is performed on the front and back surfaces of the steel sheet once respectively, wherein the cleaning parameters are as follows: marking speed is 2000mm/s, air-jumping speed is 3000mm/s, Q frequency is 50kHz, Q release: 1us, power 4W, laser pulse width 8us.
S300, adopting screen printing to print functional layers on the front side and the back side of the metal plane micro-needle sheet plated with the electrode layer respectively in sequence; the functional layer comprises an electron mediator layer, a glucose oxidase layer and an outer membrane layer.
Those skilled in the art will appreciate that the outer film layer may improve wear resistance and prevent the functional coating from falling off, and may also improve the rate of passage of the test object.
In one specific embodiment, the glucose oxidase solution is formulated as follows: 500mg of glucose oxidase was accurately weighed and dissolved in a 10mL of buffer solution of LPBS to prepare a glucose oxidase solution having a concentration of 50 mg/mL. The adventitia fluid is prepared as follows: the 6% PEG/THF solution and the 4% PU/THF solution were mixed and stirred well in a 4:1 ratio.
The material of the electron mediator layer includes, but is not limited to, CNT (carbon nanotube), reduced graphene oxide, mxene, hydrogel electron mediator, and the like.
MXene materials are a class of metal carbo/nitrides (transition metal carbide/nitride) having a two-dimensional layered structure of the general chemical formula Mn+1XnTx, where (n=1-3), M represents early transition metals such as Ti, zr, V, mo, etc., X represents C or N element, tx is a surface group, typically-OH, -O, -F and-Cl.
Optionally, the material of the electron mediator layer includes carbon nanotubes or reduced graphene oxide, and the screen printing material of the carbon nanotubes or reduced graphene oxide is prepared by the following method:
s310, dissolving multi-wall carbon nano tube powder or reduced graphene oxide powder in isopropanol to prepare a solution with preset concentration.
In one embodiment, the nanoelectrode mediator solution is formulated as follows: 500mg of multiwall carbon nanotube powder (reduced graphene powder) was accurately weighed and dissolved in 10mL of isopropanol to prepare a carbon nanotube solution (reduced graphene solution) having a concentration of 50 mg/mL.
Optionally, the front and back sides of the metal plane microneedle sheet plated with the electrode layer are respectively printed with functional layers in sequence by adopting screen printing, wherein the functional layers comprise an electron mediator layer, a glucose oxidase layer and an outer membrane layer, and specifically comprise:
s321, printing an electron mediator layer on the front surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
s322, printing an electronic mediator layer on the reverse side of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
s323, printing a glucose oxidase layer on the front surface of the metal plane micro-needle sheet printed with the electron mediator layer by adopting screen printing;
s324, printing a glucose oxidase layer on the reverse side of the metal plane micro-needle sheet printed with the electron mediator layer by adopting screen printing;
s325, printing an outer film layer on the front surface of the metal plane microneedle sheet printed with the glucose oxidase layer by adopting screen printing;
s326, printing an outer film layer on the reverse side of the metal plane micro-needle sheet printed with the glucose oxidase layer by adopting screen printing.
In a specific embodiment, a full-page stainless steel sheet with microneedle patterns is taken, and the front and back surfaces of the stainless steel sheet are sequentially decorated with functional layers by adopting a screen printing method, wherein the order of the functional layer decoration is as follows:
step 1: placing SS-Au (steel sheet with gold protective layer) in a tooling position of an automatic screen printer, taking a clean trough with mask patterning, pouring carbon nanotube solution, installing the trough and a brush plate, and executing primary printing; and after printing, taking down the stainless steel sheet, turning over, then placing in a tooling position again, performing secondary printing, taking out the stainless steel sheet (marked as SS-Au-CNT), naturally airing, and then entering the next working procedure.
Step 2: placing SS-Au-CNT in a tooling position of an automatic screen printer, taking a clean trough which is patterned by a mask, pouring glucose oxidase solution, installing the trough and a brush plate, and executing primary printing; and after printing, taking down the stainless steel sheet, turning over, then placing the stainless steel sheet in a tooling position again, performing secondary printing, taking out the stainless steel sheet (marked as SS-Au-CNT-GOx), naturally airing, and then entering the next working procedure.
And step 3: placing SS-Au-CNT-GOx in a tooling position of an automatic screen printer, taking a clean trough subjected to mask patterning, pouring an outer film solution, installing the trough and a brush plate, and executing primary printing; and after printing, taking down the stainless steel sheet, turning over, then placing the stainless steel sheet in a tooling position again, performing secondary printing, taking out the stainless steel sheet (marked as SS-Au-CNT-Gox-PU), and naturally airing.
S400, cutting the hanging part to demould the metal plane microneedle sheet plated with the functional layer.
In one embodiment, laser cutting is performed on the stainless steel sheet finished with the functional layer modification, and the microneedle pattern is bonded to the base plate to release the mold.
S500, assembling a plurality of demoulded metal plane micro-needle sheets through a base frame to obtain the three-dimensional micro-needle blood sugar electrode.
In one embodiment, the released microneedle sheets are assembled by a three-dimensional frame and three-dimensionally arrayed to form an electrode array.
Referring to fig. 2, taking a stainless steel sheet as an example, a laser reverse phase cutting is adopted to prepare a suspended planar microneedle sheet, magnetron sputtering is adopted to prepare a gold protection layer on the surface of the suspended planar microneedle sheet, screen printing is adopted to prepare functional layers on the front side and the back side of the gold protection layer, finally the suspended planar microneedle sheet printed with the functional layers is subjected to laser cutting and demoulding, and three-dimensional assembly is carried out to prepare the three-dimensional microneedle electrode. Referring to fig. 3, a schematic diagram of normal phase cutting and reverse phase cutting of a planar microneedle sheet is shown. An SEM image of a planar microneedle sheet prepared by the above method is shown in fig. 4.
The electrochemical test method of the three-dimensional microneedle electrode array comprises the following steps: one 10mL beaker is taken, a modified working electrode is taken as a working electrode, a commercial platinum electrode is taken as a counter electrode, an Ag/AgCl electrode is taken as a reference electrode, the mixture is put into a beaker, 10mL PBS buffer solution is added into the beaker, and the electrode is immersed into the solution. The electrochemical workstation software is opened and the Cyclic-Voltammery option is selected. Setting parameters: init E, -0.2v, high E:0.8V, low E, -0.2V, final E: -0.2V,Initial Scan Polarity: negative Scan Rate A.0.1V/s, sweep Segments 10,Sample Interval:0.001V, the peak values measured were observed.
The process of characterizing glucose response for the microneedle electrode is as follows: one 10mL beaker is taken, a modified working electrode is taken as a working electrode, a commercial platinum electrode is taken as a counter electrode, an Ag/AgCl electrode is taken as a reference electrode, the mixture is put into a beaker, 10mL PBS buffer solution is added into the beaker, and the electrode is immersed into the solution. Open Shanghai Chenhua electrochemical workstation software, select the Amperetric i-t Curve option. Setting parameters: init E0.5V,Sample Interval:0.1s,Run Time:300s, sensitivity:0.00001A/V, glucose solutions of different concentrations were added to the solution so that the concentration of the solution was changed to 2mM/4mM/6mM/8mM/10mM/12mM/14mM/16mM/18mM/20mM, and glucose responses at different concentrations were measured.
The microneedle blood glucose electrode prepared above was tested in vivo, and the test results were shown in FIG. 5, and blood glucose was continuously and stably tested for 3 days, with a test range of 0-22mM. The electrode surface is smooth, the linear range is doubled, the range of 0-25mM of glucose detection is achieved, the blood sugar fluctuation can be detected in a living body, and the in-vivo detection range also reaches 0-22mM.
Optionally, the method comprises:
s600, detecting the thicknesses of the electrode layer and the functional layer by using a film thickness meter.
The thickness of the electrode layer and the thickness of the functional layer are detected through the film thickness meter, so that the problems of rough electrode surface, thickness difference of batch of functional layers and the like of a conventional dip coating method are solved, and the consistency of the electrode is improved.
The embodiment of the application has the following beneficial effects: in the embodiment, firstly, a metal sheet is cut to obtain a suspension type metal plane micro-needle sheet; preparing an electrode layer on the cleaned metal plane micro-needle through magnetron sputtering, and sequentially printing functional layers on the front side and the back side of the metal plane micro-needle plated with the electrode layer through screen printing; finally, assembling the demoulded metal plane microneedle sheet to obtain a three-dimensional microneedle blood sugar electrode; the functional layers with good firmness and uniformity are prepared in batches and repeatedly by adopting a screen printing process, and the two-dimensional plane microneedle sheets are prepared first and then assembled into the three-dimensional microneedle electrode, so that the preparation process is optimized, and the production and processing cost is reduced.
Comparative experiments are performed in several examples below.
Example 1: and preparing the carbon nanotube electron mediator three-dimensional microneedle array blood glucose electrode in a large scale by a dimension-reducing screen printing method.
Example 2: and preparing the carbon reduction graphene oxide electron mediator three-dimensional microneedle array blood sugar electrode on a large scale by a dimension reduction screen printing method.
Comparative example 1: and preparing the three-dimensional microneedle blood sugar electrode of the carbon nanotube electron mediator by adopting a conventional dip coating method.
Comparative example 2: and preparing the reduced graphene mediator three-dimensional microneedle blood glucose electrode by adopting a conventional dip coating method.
The three-dimensional microneedle sensor electrodes prepared in example 1, example 2, comparative example 1, and comparative example 2 were subjected to glucose solution concentration test, and the data obtained are shown in table 1.
Table 1, table of glucose amperometric response test data in PBS buffer solution
Performance of Example 1 Example 2 Comparative example 1 Comparative example 2
Detection interval 0-20mM 0-20mM 1-10mM 0-16mM
Detection limit 200uM 200uM 200uM 200uM
Sensitivity of 120nA/mM 40nA/mM 16nA/mM 8nA/mM
Test results show that the screen-printed three-dimensional microneedle electrode can achieve the same effect as that achieved by adopting a conventional dip-coating method in the prior art. As shown in FIG. 6, the uniformity of the CNT layer material of example 1 is <87um, the difference in electrode sensitivity is less than 23%, and the highest limit of the linear range is 18-19mM. The conventional dip-coating modification method is adopted in comparative example 1, the uniformity of the prepared microneedle electrode is less than 30um, the electrode sensitivity difference is less than 263 percent, and the linear range is 8-20mM.
While the preferred embodiment of the present application has been described in detail, the application is not limited to the embodiment, and various equivalent modifications and substitutions can be made by those skilled in the art without departing from the spirit of the application, and these equivalent modifications and substitutions are intended to be included in the scope of the present application as defined in the appended claims.

Claims (7)

1. The method for preparing the three-dimensional microneedle blood sugar electrode based on the dimension reduction screen printing is characterized by comprising the following steps of:
cutting the metal sheet to obtain a suspension type metal plane micro-needle sheet; the suspension type metal plane micro-needle characterizes that the metal plane micro-needle is connected with the metal sheet through a connecting part;
cleaning the metal plane micro-needle, and preparing an electrode layer from the cleaned metal plane micro-needle by magnetron sputtering; wherein, wash metal plane microneedle slice, specifically include: respectively performing laser cleaning on the front and back sides of the metal plane micro-needle by adopting a laser marking machine according to second preset parameters;
sequentially printing functional layers on the front side and the back side of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electron mediator layer, a glucose oxidase layer and an outer membrane layer;
cutting the hanging part to demould the metal plane micro-needle plated with the functional layer;
and assembling a plurality of demoulded metal plane micro-needle sheets through the base frame to obtain the three-dimensional micro-needle blood sugar electrode.
2. The method of claim 1, wherein the cutting the metal sheet comprises:
and cutting the metal sheet by using a laser marking machine or a laser cutting machine.
3. The method according to claim 2, characterized in that when the metal sheet is cut with a laser marking machine, it comprises in particular:
placing a metal sheet into a fixture tool of a laser marking machine for fixation, and setting the laser marking machine to execute reverse incomplete cutting on the metal sheet according to a first preset parameter; the cut contour lines extend for a plurality of times according to the preset interval.
4. The method of claim 2, wherein when the metal sheet is cut using a laser marking machine, the number of markings is positively correlated with the thickness of the metal sheet.
5. The method according to claim 1, wherein the material of the electron mediator layer comprises carbon nanotubes or reduced graphene oxide, and the screen printed material of the carbon nanotubes or reduced graphene oxide is prepared by:
the multi-wall carbon nano tube powder or the reduced graphene oxide powder is dissolved in isopropanol to prepare a solution with preset concentration.
6. The method according to claim 1, wherein the functional layers are sequentially printed on the front and back sides of the metal planar microneedle sheet coated with the electrode layer by screen printing, respectively, and the functional layers comprise an electron mediator layer, a glucose oxidase layer and an outer membrane layer, and specifically comprise:
printing an electron mediator layer on the front surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
printing an electronic mediator layer on the reverse side of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
printing a glucose oxidase layer on the front surface of the metal plane micro-needle sheet printed with the electron mediator layer by adopting screen printing;
printing a glucose oxidase layer on the reverse side of the metal plane micro-needle sheet printed with the electron mediator layer by adopting screen printing;
adopting screen printing to print an outer film layer on the front surface of the metal plane microneedle sheet printed with the glucose oxidase layer;
and (3) printing an outer film layer on the reverse side of the metal plane microneedle sheet printed with the glucose oxidase layer by adopting screen printing.
7. The method according to claim 1, wherein the method further comprises:
and detecting the thicknesses of the electrode layer and the functional layer by using a film thickness meter.
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