CN114589466A - Method for preparing three-dimensional microneedle blood glucose electrode based on dimensionality reduction screen printing - Google Patents

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

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CN114589466A
CN114589466A CN202210281003.1A CN202210281003A CN114589466A CN 114589466 A CN114589466 A CN 114589466A CN 202210281003 A CN202210281003 A CN 202210281003A CN 114589466 A CN114589466 A CN 114589466A
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layer
sheet
metal plane
metal
screen printing
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CN114589466B (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 invention discloses a method for preparing a three-dimensional microneedle blood glucose electrode based on dimensionality reduction screen printing, which comprises the following steps of: cutting the metal sheet to obtain a suspended metal plane micro-needle sheet; cleaning the metal plane micro-needle sheet, and preparing an electrode layer on the cleaned metal plane micro-needle sheet through magnetron sputtering; respectively and sequentially printing functional layers on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electronic medium layer, a glucose oxidase layer and an outer film layer; cutting the hanging part to demould the metal plane microneedle sheet plated with the functional layer; and assembling a plurality of demoulded metal plane micro-needle sheets through the substrate frame to obtain the three-dimensional micro-needle blood glucose electrode. The embodiment of the invention realizes batch repetitive coating modification, 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 glucose electrode based on dimensionality reduction screen printing
Technical Field
The invention relates to the technical field of microneedle preparation, in particular to a method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing.
Background
Diabetics need to take multiple blood glucose measurements and doses every day, and face the pain of pricking a finger when measuring blood glucose. Microneedle electrode arrays have been developed for continuous monitoring of diabetes, and implantable sensors based on microneedle electrodes have been developed to improve patient compliance by reducing pain, 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 glucose sensing electrode for detecting glucose in blood and tissue fluid are greatly improved.
At present, the scale processing difficulty of the three-dimensional microneedle electrode is high, the electrode processing technology is complex, the modification uniformity of the microneedle electrode surface coating prepared by adopting the conventional dip-coating method is poor, the batch repetitive modification is difficult, and the coating is not firmly modified and is easy to fall off.
Disclosure of Invention
In view of this, an object of the embodiments of the present invention is to provide a method for preparing a three-dimensional microneedle blood glucose electrode based on dimensionality reduction screen printing, which realizes batch repetitive modification of a coating, improves the firmness and uniformity of the coating, and optimizes a preparation process.
In a first aspect, an embodiment of the present invention 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 suspended metal plane micro-needle sheet;
cleaning the metal plane micro-needle sheet, and preparing an electrode layer on the cleaned metal plane micro-needle sheet through magnetron sputtering;
respectively and sequentially printing functional layers on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electronic medium layer, a glucose oxidase layer and an outer film layer;
cutting the hanging part to demould the metal plane microneedle sheet plated with the functional layer;
and assembling a plurality of demoulded metal plane micro-needle sheets through the substrate frame to obtain the three-dimensional micro-needle blood glucose electrode.
Optionally, the cutting of the metal sheet includes:
and cutting the metal sheet by using a laser marking machine or a laser cutting machine.
Optionally, when the laser marking machine is used to cut the metal sheet, the method specifically includes:
placing a metal sheet in a fixture tool of a laser marking machine for fixing, and setting the laser marking machine to perform reverse incomplete cutting on the metal sheet according to a first preset parameter; wherein, the cutting contour line extends for a plurality of times according to the preset distance.
Optionally, when the laser marking machine is used to cut the metal sheet, the marking times are positively correlated to the thickness of the metal sheet.
Optionally, the cleaning of the metal plane microneedle sheet specifically includes:
and respectively carrying out laser cleaning on the front side and the back side of the metal plane microneedle sheet by adopting a laser marking machine according to a second preset parameter.
Optionally, the material of the electronic medium layer comprises 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:
dissolving multi-wall carbon nanotube powder or reduced graphene oxide powder in isopropanol to prepare a solution with a preset concentration.
Optionally, the functional layer is printed in proper order respectively on the positive and negative both sides of the metal plane micro-needle sheet plated with the electrode layer by screen printing, and the functional layer includes an electronic medium layer, a glucose oxidase layer and an outer film layer, and specifically includes:
printing an electronic medium layer on the front surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
printing an electronic medium 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 microneedle sheet printed with the electronic medium layer by adopting screen printing;
printing a glucose oxidase layer on the reverse side of the metal plane microneedle sheet printed with the electronic medium layer by adopting screen printing;
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;
and 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 implementation of the embodiment of the invention has the following beneficial effects: in the embodiment, firstly, a suspended metal plane micro-needle sheet is obtained by cutting a metal sheet; then preparing an electrode layer on the cleaned metal plane micro-needle sheet through magnetron sputtering, and respectively and sequentially printing functional layers on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; finally, assembling the demoulded metal plane microneedle sheet to obtain a three-dimensional microneedle blood glucose electrode; the functional layer with good firmness and uniformity is prepared in a batch and repetitive manner by adopting a screen printing process, and the two-dimensional plane microneedle sheet is prepared firstly 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 present invention;
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, provided by the embodiment of the invention;
FIG. 3 is a schematic diagram of a normal phase cutting and a reverse phase cutting according to an embodiment of the present invention;
FIG. 4 is an SEM image of a metal plane microneedle plate prepared by screen printing according to an embodiment of the present invention;
FIG. 5 is a graph comparing the blood glucose concentration of an electrode prepared by screen printing and a commercial electrode provided by an embodiment of the present invention;
fig. 6 is a graph showing the thickness results of carbon nanotubes prepared on a planar microneedle sheet by screen printing according to an embodiment of the present invention.
Detailed Description
The invention is described in further detail below with reference to the figures and the specific embodiments. For the step numbers in the following embodiments, they are set for convenience of illustration only, the order between the steps is not limited at all, and the execution order of each step in the embodiments can be adapted according to the understanding of those skilled in the art.
As shown in fig. 1, an embodiment of the present invention provides a method for preparing a three-dimensional microneedle blood glucose electrode based on dimension reduction screen printing, which includes the following steps:
and S100, cutting the metal sheet to obtain the suspended metal plane microneedle sheet.
It should be noted that the metal foil includes stainless steel sheet, such as stainless steel sheet of all grades such as 304H, and may be any other metal foil that can be etched by laser in 1064nm band, and the thickness of the foil is between 50um and 400 um. Suspended metal plane microneedle chips are understood to mean metal plane microneedle chips which are connected to the metal foil via connecting points.
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 of the metal sheet includes:
and S110, cutting the metal sheet by adopting a laser marking machine or a laser cutting machine.
Optionally, when the laser marking machine is used to cut the metal sheet, the method specifically includes:
s111, placing the metal sheet into a fixture tool of a laser marking machine for fixing, and setting the laser marking machine to perform reverse incomplete cutting on the metal sheet according to a first preset parameter; wherein, the cutting contour line extends for a plurality of times according to the preset distance.
Optionally, when the laser marking machine is used to cut the metal sheet, the marking times are positively correlated to the thickness of the metal sheet.
In one embodiment, a stainless steel sheet is placed in a laser marking machine fixture for fixing, reverse incomplete cutting is performed, 10 times of extension are performed on a contour line, and the distance is 1 um. The cutting parameters were as follows: marking speed is 700mm/s, skip 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.
S200, cleaning the metal plane micro-needle sheet, and preparing an electrode layer on the cleaned metal plane micro-needle sheet through magnetron sputtering.
It should be noted that, performing laser cleaning on the front and back sides of the metal plane microneedle 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 of the metal plane microneedle sheet specifically includes:
s210, respectively carrying out laser cleaning on the front side and the back side of the metal plane microneedle sheet by adopting a laser marking machine according to a second preset parameter.
In a specific embodiment, the reverse phase pattern of the cut steel sheet is removed to obtain a steel sheet with a microneedle pattern, laser cleaning is performed on the front side and the back side of the steel sheet respectively, and the cleaning parameters are as follows: marking speed is 2000mm/s, blank jump speed is 3000mm/s, Q frequency is 50kHz, and Q release: 1us, power 4W, laser pulse width 8 us.
S300, respectively and sequentially printing functional layers on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electronic medium layer, a glucose oxidase layer and an outer film layer.
As can be understood by those skilled in the art, the outer film layer can improve the wear resistance and prevent the functional coating from falling off, and can also improve the passing rate of the object to be detected.
In one particular embodiment, the glucose oxidase solution is formulated as follows: 500mg of glucose oxidase is accurately weighed and dissolved in 10mL of PBS buffer solution to prepare a glucose oxidase solution with the concentration of 50 mg/mL. The external membrane liquid is prepared as follows: the 6% PEG/THF solution and the 4% PU/THF solution were mixed at a ratio of 4:1 and stirred well.
The material of the electron mediator layer includes, but is not limited to, CNT (carbon nanotube), reduced graphene oxide, Mxene, a hydrogel electron mediator, and the like.
MXene materials are a class of metal carbon/nitrides with two-dimensional layered structure, and the chemical formula is Mn +1XnTx, wherein (N ═ 1-3), M represents early transition metal such as Ti, Zr, V, Mo, etc., X represents C or N element, Tx is surface group, usually-OH, -O, -F and-Cl.
Optionally, the material of the electronic medium layer comprises 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 the multi-walled carbon nanotube powder or the reduced graphene oxide powder in isopropanol to prepare a solution with a preset concentration.
In one embodiment, the nanoelectron mediator solution is formulated as follows: 500mg of multi-walled 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 functional layer is printed in proper order respectively on the positive and negative both sides of the metal plane micro-needle sheet plated with the electrode layer by screen printing, and the functional layer includes an electronic medium layer, a glucose oxidase layer and an outer film layer, and specifically includes:
s321, printing an electronic medium 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 medium 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 microneedle sheet printed with the electronic medium 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 electronic medium 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;
and S326, 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.
In one embodiment, a whole plate of stainless steel sheet with microneedle patterns is taken, and the front and back surfaces of the stainless steel sheet are sequentially modified with a functional layer by a screen printing method, wherein the functional layer modification sequence is as follows:
step 1: placing SS-Au (steel sheet with a gold protective layer) in a tooling position of an automatic screen printing machine, taking a clean material groove with a mask pattern, pouring a carbon nano tube solution, installing the material groove and brushing a plate, and performing one-time printing; and taking down the stainless steel sheet after printing, turning over, putting the stainless steel sheet on a tool position again, performing second printing, taking out the stainless steel sheet (marked as SS-Au-CNT), naturally drying, and entering the next procedure.
And a step 2: placing SS-Au-CNT at a tooling position of an automatic screen printing machine, taking a clean material groove with a mask pattern, pouring a glucose oxidase solution, installing the material groove and brushing a plate, and performing one-time printing; and taking down the stainless steel sheet after printing, turning over, putting the stainless steel sheet on a tool position again, performing second printing, taking out the stainless steel sheet (marked as SS-Au-CNT-GOx), naturally drying, and entering the next procedure.
Step 3: placing SS-Au-CNT-GOx in a tooling position of an automatic screen printing machine, taking a clean material groove with a mask pattern, pouring an outer membrane solution, installing the material groove and brushing a plate, and performing one-time printing; and (4) taking down the stainless steel sheet after printing is finished, turning over the stainless steel sheet, putting the stainless steel sheet on a tool position again, performing second printing, taking out the stainless steel sheet (marked as SS-Au-CNT-Gox-PU), and naturally drying.
S400, cutting the hanging part to enable the metal plane microneedle sheet plated with the functional layer to be demoulded.
In one embodiment, laser cutting is performed on the bonding position of the microneedle pattern and the base plate for demolding on the stainless steel sheet subjected to functional layer modification.
S500, assembling a plurality of demoulded metal plane micro-needle sheets through a substrate frame to obtain the three-dimensional micro-needle blood glucose electrode.
In one embodiment, the released microneedle array is 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 suspended planar microneedle sheet is prepared by cutting the stainless steel sheet in a reverse laser phase manner, a gold protective layer is prepared on the surface of the suspended planar microneedle sheet by magnetron sputtering, then functional layers are prepared on the front and back sides plated with the gold protective layer by screen printing, finally, the suspended planar microneedle sheet printed with the functional layers is subjected to laser cutting demolding, and three-dimensional assembly is performed to prepare a three-dimensional microneedle electrode. Referring to fig. 3, a schematic diagram of normal phase cutting and reverse phase cutting of a planar microneedle array is shown. An SEM image of the flat 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: taking one 10mL beaker, taking the modified working electrode as a working electrode, taking a commercial platinum electrode as a counter electrode, taking an Ag/AgCl electrode as a reference electrode, putting the counter electrode into the beaker, adding 10mL of PBS buffer solution into the beaker, and immersing the electrode into the solution. The electrochemical workstation software was turned on and the Cyclic-volt measurement option was selected. Setting parameters: init E: -0.2V, High E: 0.8V, Low E: -0.2V, Final E: -0.2V, Initial Scan policy: the peak values were observed at Negative Scan Rate of 0.1V/s, at sweet Segments of 10 and Sample Interval of 0.001V.
Performance of microneedle electrodes the process of characterizing the glucose response is as follows: taking one 10mL beaker, taking the modified working electrode as a working electrode, taking a commercial platinum electrode as a counter electrode, taking an Ag/AgCl electrode as a reference electrode, putting the counter electrode into the beaker, adding 10mL of PBS buffer solution into the beaker, and immersing the electrode into the solution. And opening the Shanghai Chenghua electrochemical workstation software and selecting an Amperometric i-t Curve option. Setting parameters: init E:0.5V, Sample Interval:0.1s, Run Time: glucose solutions of different concentrations were added to the solution at 300s, Sensitivity:0.00001A/V, so that the concentration of the solution changed to 2mM/4mM/6mM/8mM/10mM/12mM/14mM/16mM/18mM/20mM, and glucose responses at different concentrations were measured.
The microneedle blood sugar electrode prepared above is tested in vivo, the experimental result is shown in figure 5, blood sugar is continuously and stably tested for 3 days, and the testing range is 0-22 mM. The electrode surface is flat, the linear range is doubled, the range of detecting glucose is 0-25mM, the blood glucose fluctuation can be detected in a living body, and the in-vivo detection range is 0-22 mM.
Optionally, the method comprises:
and 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 functional layer is detected by a film thickness meter, so that the problems of rough electrode surface, thickness difference of batch functional layers and the like in the conventional dip coating method are solved, and the consistency of the electrode is improved.
The implementation of the embodiment of the invention has the following beneficial effects: in the embodiment, firstly, a suspended metal plane micro-needle sheet is obtained by cutting a metal sheet; then preparing an electrode layer on the cleaned metal plane micro-needle sheet through magnetron sputtering, and respectively and sequentially printing functional layers on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; finally, assembling the demoulded metal plane microneedle sheet to obtain a three-dimensional microneedle blood glucose electrode; the functional layer with good firmness and uniformity is prepared in a batch and repetitive manner by adopting a screen printing process, and the two-dimensional plane microneedle sheet is prepared firstly 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 carried out in the following examples.
Example 1: and preparing the carbon nano tube electronic mediator three-dimensional microneedle array blood glucose electrode in a modeling manner by a dimension reduction screen printing method.
Example 2: and preparing the carbon reduction graphene oxide electronic mediator three-dimensional microneedle array blood glucose electrode in a modeling manner by a dimension reduction screen printing method.
Comparative example 1: the carbon nano tube electron mediator three-dimensional microneedle blood sugar electrode is prepared 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 sensing electrodes prepared in example 1 and example 2, comparative example 1 and comparative example 2 were subjected to a glucose solution concentration test, and the obtained data are shown in table 1.
TABLE 1 Ampere response test data for glucose 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 the probe 120nA/mM 40nA/mM 16nA/mM 8nA/mM
Test results show that the screen printing three-dimensional microneedle electrode has the same effect as that of a conventional dip coating method in the prior art. As shown in fig. 6, the CNT layer material of example 1 has a uniformity of <87um, an electrode sensitivity difference of less than 23%, and the highest limit of the linear range is 18-19 mM. The microneedle electrode prepared by adopting the conventional dip coating modification method in the comparative example 1 has the uniformity of less than 30um, the electrode sensitivity difference of less than 263 percent and the linear range of 8-20 mM.
While the preferred embodiments of the present invention have been illustrated and described, it will be understood by those skilled in the art that various changes in form and details may be made therein without departing from the spirit and scope of the invention as defined by the appended claims.

Claims (8)

1. A method for preparing a three-dimensional microneedle blood glucose electrode based on dimensionality reduction screen printing is characterized by comprising the following steps:
cutting the metal sheet to obtain a suspended metal plane micro-needle sheet;
cleaning the metal plane micro-needle sheet, and preparing an electrode layer on the cleaned metal plane micro-needle sheet through magnetron sputtering;
respectively and sequentially printing functional layers on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing; the functional layer comprises an electronic medium layer, a glucose oxidase layer and an outer film layer;
cutting the hanging part to demould the metal plane microneedle sheet plated with the functional layer;
and assembling a plurality of demoulded metal plane micro-needle sheets through the substrate frame to obtain the three-dimensional micro-needle blood glucose electrode.
2. The method of claim 1, wherein said cutting of 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, wherein when the laser marking machine is used to cut the metal sheet, the method comprises:
placing a metal sheet in a fixture tool of a laser marking machine for fixing, and setting the laser marking machine to perform reverse incomplete cutting on the metal sheet according to a first preset parameter; wherein the cut contour lines are extended for a plurality of times according to the preset distance.
4. The method of claim 2, wherein the number of markings is positively correlated to the thickness of the foil when the foil is cut using a laser marking machine.
5. The method according to claim 1, wherein the cleaning of the metal planar microneedle sheet comprises:
and respectively carrying out laser cleaning on the front side and the back side of the metal plane microneedle sheet by adopting a laser marking machine according to a second preset parameter.
6. 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 carbon nanotubes or reduced graphene oxide is prepared by:
dissolving multi-wall carbon nanotube powder or reduced graphene oxide powder in isopropanol to prepare a solution with a preset concentration.
7. The method according to claim 1, wherein the functional layers are respectively printed on the front surface and the back surface of the metal plane micro-needle sheet plated with the electrode layer in sequence by screen printing, and the functional layers comprise an electronic medium layer, a glucose oxidase layer and an outer film layer, and specifically comprise:
printing an electronic medium layer on the front surface of the metal plane micro-needle sheet plated with the electrode layer by adopting screen printing;
printing an electronic medium 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 electronic medium layer by adopting screen printing;
printing a glucose oxidase layer on the reverse side of the metal plane microneedle sheet printed with the electronic medium layer by adopting screen printing;
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;
and 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.
8. The method according to claim 1, characterized in that it comprises:
and detecting the thicknesses of the electrode layer and the functional layer by using a film thickness meter.
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Cited By (1)

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Publication number Priority date Publication date Assignee Title
CN115184421A (en) * 2022-06-21 2022-10-14 中山大学 Microneedle blood glucose sensor, preparation method thereof and differential pulse voltammetry test method

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