CN107422016A - The preparation method of the minimally invasive glucose sensor of spiral shape implantable of PVA/PEG composite aquogel outer membrane structures - Google Patents
The preparation method of the minimally invasive glucose sensor of spiral shape implantable of PVA/PEG composite aquogel outer membrane structures Download PDFInfo
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- CN107422016A CN107422016A CN201710601489.1A CN201710601489A CN107422016A CN 107422016 A CN107422016 A CN 107422016A CN 201710601489 A CN201710601489 A CN 201710601489A CN 107422016 A CN107422016 A CN 107422016A
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/28—Electrolytic cell components
- G01N27/30—Electrodes, e.g. test electrodes; Half-cells
- G01N27/327—Biochemical electrodes, e.g. electrical or mechanical details for in vitro measurements
- G01N27/3271—Amperometric enzyme electrodes for analytes in body fluids, e.g. glucose in blood
- G01N27/3272—Test elements therefor, i.e. disposable laminated substrates with electrodes, reagent and channels
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N33/00—Investigating or analysing materials by specific methods not covered by groups G01N1/00 - G01N31/00
- G01N33/48—Biological material, e.g. blood, urine; Haemocytometers
- G01N33/50—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing
- G01N33/66—Chemical analysis of biological material, e.g. blood, urine; Testing involving biospecific ligand binding methods; Immunological testing involving blood sugars, e.g. galactose
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N2800/00—Detection or diagnosis of diseases
- G01N2800/04—Endocrine or metabolic disorders
- G01N2800/042—Disorders of carbohydrate metabolism, e.g. diabetes, glucose metabolism
Abstract
The invention provides the preparation method of the minimally invasive glucose sensor of spiral shape implantable of PVA/PEG composite aquogel outer membrane structures, the present invention selects screw type platinum iridium alloy electrode, implantable sensor biocompatibility and anti-interference are improved by coating Epoxy PU pellicles and hydrogel outer membrane, the influence of high spot reviews PVA/PEG different proportion to glucose sensor performance；In addition, the sensor has controllable sensitivity and good repeatability, stability and selectivity, laid a solid foundation for following the practical of continuous blood sugar monitoring sensor.
Description
Technical field
The present invention relates to the spiral in biosensor technology field, more particularly to PVA/PEG composite aquogels outer membrane structure
The preparation method of the minimally invasive glucose sensor of shape implantable.
Background technology
One of most important chronic disease of diabetic history current threat global human health, Etiological is responsible for secreting
The pancreatic beta cell of insulin breaks down, and leads to not the glucose level in strict control blood.Diabetes can induce high blood
The various disease conditions such as pressure, angiocarpy, kidney failure, brothers' necrosis, neurological disorders, have high risks to the life and health of people；According to state
Border diabetes alliance (IDF) counts, it is contemplated that and by 2030, the whole world nearly had 5.5 hundred million people to suffer from diabetes, wherein in China, I
Diabetes mellitus type sum is between 700-1000 ten thousand；In order to maintain close to normal blood sugar level (70-120mg/dL), mesh
Preceding diabetic is widely used that hand-held blood glucose meter, needs to puncture finger daily for several times to obtain blood sample, this
Mode can bring pain and inconvenience to patient, and can not continuously detect internal glucose level.
The product that research at present and in the market are sold is mainly aciculiform glucose electrode, because its is easily fabricated and is adapted to plant
The characteristic that enters and receive significant attention, such as the aciculiform implanted grape of Ahyeon Koh et al. ultramicropore polyurethane-coateds designed
Sugared sensor, but its shortcoming is also more apparent：GOD loadings are too low to cause its service life shorter；In order to solve problems, spiral shell
Rotating glucose sensor is reported successively；For example, the coil type sensor made by Y μ et al., in vitro constant polarization 3
Remain to play preferable function after month, but just start after implanting to lose its sensitiveness；Because glucose sensor is implanted into
The biological pollution and rejection for damaging and triggering eventually result in sensor failure, and sensor gradually loses work(after the implantation
Can, be primarily due to implantation after body foreign body reaction (FBR) caused by wound surrounding tissue, including fibrous capsule and inflammation it is anti-
Should；In order to improve the life-span of implantable glucose sensor, there is the material of biocompatible coating, such as：Based on silica
Composite, sol-gel process coating, diamond-like carbon film, nanoporous anode aluminium film etc. studied as coating, institute
There are some researches show these materials have the potentiality as sensor outer membrane and the external skin of glucose sensor must be in biology
The deposition for ensure transport of the glucose in sensor, reducing protein and other chaff interferences is stabilized in body and is subtracted as far as possible
Few fibrous capsule.Some new materials be attempted successively for as far as possible reduces these influences, including hydrogel, collagen or
It is PLA as protective coating, uses corticosteroid to suppress immune response；And in numerous materials, hydrogel is a species
The material of vital tissues is similar to, its surface is not easy attachment proteins matter and cell, when being contacted with blood of human body, cell and tissue,
Good biocompatibility can be shown, wherein the hydrogel of three-dimensional cross-linked converging network structure can meet requirements above and in water
It is middle swelling and do not dissolve；Service life of the sensor in human body can be greatly improved by these methods.
The content of the invention
The technical problem to be solved in the present invention is to provide a kind of spiral shape based on PVA/PEG composite aquogel outer membrane structures
The preparation method of the minimally invasive glucose sensor of implantable.
To reach above-mentioned purpose, technical scheme is as follows：
The preparation method of the minimally invasive glucose sensor of spiral shape implantable of PVA/PEG composite aquogel outer membrane structures,
The preparation method comprises the following steps：
(1) preparation of screw electrode；
Long 4-7cm medical grade platinoiridita silk is taken, peels off the teflon coating for removing end 1-2cm, it is ultrasonic in ultra-pure water
Handle 5-10min；Above-mentioned platinoiridita silk is closely spiraled along hypodermic needle with the tweezers that absolute ethyl alcohol wipes and winds 5 circles -8
Circle, obtain Pt-Ir coils；
(2) in the above-mentioned spiral winding for preparing the insertion of a small gangs of porous fibrous material, to improve GOD loadings；
(3) preparation of GOD solution；
0.001-0.5g bovine serum albumins and 0.001-0.1g glucose oxidases are dissolved in 100-500 μ L deionized waters
In, shaking table stirs, and instills 1-10 μ L glutaraldehyde, continues to stir；
(4) take 2-15 μ L stir after GOD solution drop coating to electrode surface, after natural drying at room temperature, take 2-15 μ L again
GOD solution drop coating after stirring dries at least 1h to electrode surface under room temperature environment；
(5) by 0.01-1g polyurethane, 0.001-0.5g epoxy adhesive A and 0.001-0.5g epoxy adhesive
B is dissolved in 1-10mL tetrahydrofurans and 1-5 μ L dodecyl polytetroxide vinethene, makes it well mixed on shaking table；
(6) 1-10 μ LEpoxy-PU solution drop coatings are taken to enzyme electrode, the enzyme electrode for coating Epoxy-PU is placed on room
Temperature is lower to dry 30min；
(7) it is the epoxy adhesive B of 0.05-1g polyurethane, 0.01-0.5g epoxy adhesive A and 0.01-0.5g is molten
In 1-10mL tetrahydrofurans, make it well mixed on shaking table；
(8) the above-mentioned configuration solution drop coatings of 1-10 μ L are taken to be placed on the enzyme electrode for coating Epoxy-PU to enzyme electrode both ends
10-60min is dried at room temperature, is then placed within 10-100 DEG C of thermostatic drying chamber and is solidified 5-30min；
(9) polyvinyl alcohol of 2-15g polyethylene glycol and 2-15g is dissolved in 100-500mL deionized water, temperature control
50-200 DEG C of heating stirring 2-5h；
(10) after the cooling of hydrogel solution room temperature, hydrogel solution is sucked using injector for medical purpose, makes needle lumen
Full of hydrogel, and above-mentioned screw electrode is filled in the inner chamber for filling up water-setting needle head, be then placed in cold in -4-20 DEG C of refrigerator
Freeze 5-30h；
(11) electrode taking-up juxtaposition 1 hour of thawing at room temperature can be tested.
In one embodiment of the invention, the polyethylene glycol is selected from polyethylene glycol (1000), polyethylene glycol (6000)
In one or more.
In one embodiment of the invention, the mass ratio of polyvinyl alcohol and polyethylene glycol is 4 in step (9):1、2:1 or
5:1。
In one embodiment of the invention, the temperature control in step (9) is 150 DEG C or 200 DEG C.
In one embodiment of the invention, the cooling time in step (10) is 12 or 24 hours.
Pass through above-mentioned technical proposal, the beneficial effects of the invention are as follows：
The present invention has obtained PVA/PEG composite aquogels using simple heating stirring, and the material is coated into electrode table
Face, prepare a kind of glucose sensor；Wherein PVA (polyvinyl alcohol) is that a kind of quite extensive water soluble polymer of purposes gathers
Compound, there is good film forming and tensile strength, wear-resisting, good insulating；It is PEG (polyethylene glycol) good water solubility, nontoxic, raw
Thing compatibility is good；Polyethylene glycol (PEG) is grafted on polyvinyl alcohol (PVA), prepares the hydrogel of combination property better performances；
The sensitivity of sensor can be controlled in 10nA/mM；In addition, the electrode of coating best complex hydrogel has good repeatability
And long-time stability, show that prepared sensor meets the requirement being chronically implanted.
Brief description of the drawings
In order to illustrate more clearly about the embodiment of the present invention or technical scheme of the prior art, below will be to embodiment or existing
There is the required accompanying drawing used in technology description to be briefly described, it should be apparent that, drawings in the following description are only this
Some embodiments of invention, for those of ordinary skill in the art, on the premise of not paying creative work, can be with
Other accompanying drawings are obtained according to these accompanying drawings.
Fig. 1 is the minimally invasive Portugal of spiral shape implantable based on PVA/PEG composite aquogel outer membrane structures made from embodiment 1
Grape sugar sensor construction schematic diagram；
Fig. 2 prepares ESEM (SEM) photo for PVA/PEG composite aquogels made from embodiment 1；
Fig. 3 is the timing Ampere currents sound that PVA/PEG composite aquogels made from embodiment 1 coat screw electrode before and after water
Answer curve map；
Fig. 4 is the timing Ampere currents sound that PVA/PEG composite aquogels made from embodiment 2 coat screw electrode before and after water
Answer curve map；
Fig. 5 is the anti-interference test for the electrode that PVA/PEG composite aquogels made from embodiment 1 coat water rear screw electrode
Figure；
Fig. 6 is the long-time stability that PVA/PEG composite aquogels made from embodiment 1 coat water rear screw electrode；
Fig. 7 is the minimally invasive glucose sensor bag of spiral shape implantable based on PVA/PEG composite aquogel outer membrane structures
Cover test chart after gel；
Fig. 8 is the anti-interference test chart of the sensor of cladding hydrogel；
Fig. 9 is the long term stability tests figure of the sensor of cladding hydrogel.
Embodiment
In order that the technical means, the inventive features, the objects and the advantages of the present invention are easy to understand, tie below
Conjunction is specifically illustrating, and the present invention is expanded on further.
Embodiment 1：The minimally invasive glucose sensor of spiral shape implantable based on PVA/PEG composite aquogel outer membrane structures
Preparation method, comprise the following steps
(1) the medical grade platinoiridita silk for being about 5cm is taken, peels off the teflon coating for removing end 0.5cm, is surpassed in ultra-pure water
Sonication 5min；The tweezers wiped with absolute ethyl alcohol closely spiral above-mentioned platinoiridita silk along hypodermic needle (30gauge)
The circle of winding 8, obtains Pt-Ir coils；
(2) a small gangs of porous fibrous material is embedded in the above-mentioned spiral winding prepared；
(3) 0.012g bovine serum albumins and 0.0025g glucose oxidases are dissolved in 300 μ L deionized waters, shaking table stirs
The glutaraldehyde for uniformly instilling 4.8 μ L is mixed, continues to stir；
(4) take 8 μ L stir after GOD solution drop coating arrive electrode surface, after natural drying at room temperature, after taking 8 μ L stirrings again
GOD solution drop coating to electrode surface, 1h is dried under room temperature environment；
(5) the epoxy adhesive B of 0.0267g polyurethane and 0.0089g epoxy adhesive A and 0.0089g is dissolved in 4mL
In tetrahydrofuran and 1.15 μ L dodecyl polytetroxide vinethene, make it well mixed on shaking table；
(6) the epoxy adhesive B of 0.0267g polyurethane, 0.0089g epoxy adhesive A and 0.0089g is dissolved in
In 4mL tetrahydrofurans and 1.15 μ L dodecyl polytetroxide vinethene, make it well mixed on shaking table；
(7) the epoxy adhesive B of 0.092g polyurethane and 0.046g epoxy adhesive A and 0.0465g is dissolved in 4mL tetra-
In hydrogen furans, make it well mixed on shaking table；
(8) take the above-mentioned configuration solution drop coatings of 0.5 μ L that the enzyme electrode for coating Epoxy-PU is placed on into room to enzyme electrode both ends
Temperature is lower to dry 30min, is then placed within 80 DEG C of thermostatic drying chambers and solidifies 20min；
(9) polyvinyl alcohol of 3g polyethylene glycol (PEG1000) and 12g is dissolved in 100mL deionized water；
(10) by heating stirring 3h of the mixed solution at 150 DEG C；
(11) after the cooling of solution room temperature, hydrogel solution is sucked using injector for medical purpose (syringe needle (15G)), makes syringe needle
The inner chamber that inner chamber fills up water-setting needle head full of hydrogel and fill in screw electrode is then placed in (- 20 DEG C) refrigerator freezing 12h；
(12) electrode taking-up juxtaposition is thawed one hour at room temperature, based on PVA/PEG composite aquogel outer membrane structures
Its structural representation of spiral shape glucose sensor, is shown in Fig. 1.
Embodiment 2, the preparation of PVA/PEG composite aquogels：
Embodiment 1 the step of in (9), mass ratio is polyvinyl alcohol：Polyethylene glycol=4:1, polyvinyl alcohol can be changed to：It is poly-
Ethylene glycol=2:1, other steps and condition are all same as Example 1, and actual conditions makees phase in the range of content of the invention restriction
The variation and adjustment answered, can obtain composite aquogel, and composite aquogel prepares ESEM (SEM) photo, sees Fig. 2；Not
Coat pair of the sensor of hydrogel and the sensor of coating polyvinyl alcohol/polyethylene glycol hydrogel to different concentration of glucose
Than figure, Fig. 3 is seen, 4.
Embodiment 3, the preparation of PVA/PEG composite aquogels；
Embodiment 1 the step of in (9), mass ratio is polyvinyl alcohol：Polyethylene glycol=4:1, polyvinyl alcohol can be changed to：It is poly-
Ethylene glycol=5:1, other steps and condition are all same as Example 1, and actual conditions makees phase in the range of content of the invention restriction
The variation and adjustment answered, can obtain composite aquogel.The sensor and coating polyvinyl alcohol/polyethylene glycol of uncoated hydrogel
The sensor of hydrogel is shown in Fig. 5 to the comparison diagram of different concentration of glucose.
Embodiment 4, the preparation of PVA/PEG composite aquogels：
Embodiment 1 the step of in (10), 150 DEG C of heating-up temperature can be replaced by 200 DEG C of heating-up temperature, other steps
All same as Example 1 with condition, actual conditions makees corresponding variation and adjustment in the range of content of the invention restriction, can obtain
To composite aquogel.
Embodiment 5, the preparation of PVA/PEG composite aquogels：
Embodiment 1 the step of in (9), polyethylene glycol (PEG 1000) can be replaced by polyethylene glycol (PEG 6000), its
His step and condition are all same as Example 1, actual conditions make in the range of content of the invention restriction it is corresponding change and adjustment,
Composite aquogel can be obtained.The sensor and cladding polyethylene of coating polyvinyl alcohol/polyethylene glycol (PEG 1000) hydrogel
The sensor of alcohol/polyethylene glycol (PEG 6000) hydrogel is shown in Fig. 6 to the comparison diagram of different concentration of glucose.
Embodiment 6, the minimally invasive glucose sensor of spiral shape implantable based on PVA/PEG composite aquogel outer membrane structures
Preparation：
Embodiment 1 the step of in (11), 12h cooling time can be replaced by 24h cooling time, other steps and bar
Part is all same as Example 1, and actual conditions makees corresponding variation and adjustment in the range of content of the invention restriction, can obtain base
In the minimally invasive glucose sensor of spiral shape implantable of PVA/PEG composite aquogel outer membrane structures, test chart after gel is coated,
See Fig. 7.
Embodiment 7：The inspection of the sensor of uncoated hydrogel and the sensor of cladding hydrogel to different concentration of glucose
Survey：
Different concentration of glucose are detected using TBR4100 test systems, in homemade polytetrafluoroethylene (PTFE) electrochemistry
In reaction tank, using PBS as supporting electrolyte, appropriate glucose solution is added, sensor is entered using chronoamperometry
Row test, its test chart are shown in Fig. 3, Fig. 4, Fig. 5.
Embodiment 8：Coat the anti-interference test of the sensor of hydrogel：
Different concentration of glucose are detected using TBR4100 test systems, in homemade polytetrafluoroethylene (PTFE) electrochemistry
In reaction tank, using PBS as supporting electrolyte, the operating potential of sensor is 0.7V, and interference--free experiments are arranged to point
Not Zhu Ru 5mM glucose, 0.5mMAA, 0.5mMMA, 0.5mMDA and 0.5mM fructose (Fr μ ctose), respectively detecting electrode
Curent change after above-mentioned contact material, the results showed that, show to have wrapped up detection of the sensor of hydrogel to grape have compared with
Good anti-interference, its test chart, is shown in Fig. 8.
Embodiment 9：Coat the long term stability tests of the sensor of hydrogel：
Different concentration of glucose are detected using TBR4100 test systems, in homemade polytetrafluoroethylene (PTFE) electrochemistry
In reaction tank, using PBS as supporting electrolyte, the operating potential of sensor is 0.7V；After 31 days, response current
It still can reach more than the 90% of initial signal；Show that the hydrogel of cladding is smaller to the performance impact of sensor, the weight of sensor
Renaturation is preferable, can meet the requirement being chronically implanted, its test chart, see Fig. 9.
The general principle and principal character and advantages of the present invention of the present invention has been shown and described above.The technology of the industry
Personnel are it should be appreciated that the present invention is not limited to the above embodiments, and the simply explanation described in above-described embodiment and specification is originally
The principle of invention, without departing from the spirit and scope of the present invention, various changes and modifications of the present invention are possible, these changes
Change and improvement all fall within the protetion scope of the claimed invention.The claimed scope of the invention by appended claims and its
Equivalent thereof.
Claims (5)
- The preparation method of the minimally invasive glucose sensor of spiral shape implantable of 1.PVA/PEG composite aquogel outer membrane structures, its It is characterised by, the preparation method comprises the following steps：(1) preparation of screw electrode；Long 4-7cm medical grade platinoiridita silk is taken, the teflon coating for removing end 1-2cm is peeled off, is ultrasonically treated in ultra-pure water 5-10min；Closely spiraled above-mentioned platinoiridita silk along hypodermic needle with the tweezers that absolute ethyl alcohol wipes the circle of the circle of winding 5-8, Obtain Pt-Ir coils；(2) in the above-mentioned spiral winding for preparing the insertion of a small gangs of porous fibrous material, to improve GOD loadings；(3) preparation of GOD solution；0.001-0.5g bovine serum albumins and 0.001-0.1g glucose oxidases are dissolved in 100-500 μ L deionized waters, shaken Bed stirs, and instills 1-10 μ L glutaraldehyde, continues to stir；(4) take 2-15 μ L stir after GOD solution drop coating arrive electrode surface, after natural drying at room temperature, take 2-15 μ L stirrings again GOD solution drop coating afterwards dries at least 1h to electrode surface under room temperature environment；(5) the epoxy adhesive B of 0.01-1g polyurethane, 0.001-0.5g epoxy adhesive A and 0.001-0.5g is dissolved in In 1-10mL tetrahydrofurans and 1-5 μ L dodecyl polytetroxide vinethene, make it well mixed on shaking table；(6) 1-10 μ LEpoxy-PU solution drop coatings are taken to enzyme electrode, the enzyme electrode for coating Epoxy-PU is placed at room temperature Dry 30min；(7) the epoxy adhesive B of 0.05-1g polyurethane, 0.01-0.5g epoxy adhesive A and 0.01-0.5g is dissolved in 1- In 10mL tetrahydrofurans, make it well mixed on shaking table；(8) take the above-mentioned configuration solution drop coatings of 1-10 μ L that the enzyme electrode for coating Epoxy-PU is placed on into room temperature to enzyme electrode both ends Lower dry 10-60min, is then placed within 10-100 DEG C of thermostatic drying chamber and solidifies 5-30min；(9) polyvinyl alcohol of 2-15g polyethylene glycol and 2-15g is dissolved in 100-500mL deionized water, temperature control 50-200 DEG C heating stirring 2-5h；(10) after the cooling of hydrogel solution room temperature, hydrogel solution is sucked using injector for medical purpose, is full of needle lumen Hydrogel, and above-mentioned screw electrode is filled in the inner chamber for filling up water-setting needle head, it is then placed in freezing 5- in -4-20 DEG C of refrigerator 30h；(11) electrode taking-up juxtaposition 1 hour of thawing at room temperature can be tested.
- 2. the minimally invasive glucose of spiral shape implantable of PVA/PEG composite aquogels outer membrane structure according to claim 1 The preparation method of sensor, it is characterised in that the polyethylene glycol is selected from polyethylene glycol (1000), polyethylene glycol (6000) It is one or more of.
- 3. the minimally invasive glucose of spiral shape implantable of PVA/PEG composite aquogels outer membrane structure according to claim 1 The preparation method of sensor, it is characterised in that the mass ratio of polyvinyl alcohol and polyethylene glycol is 4 in step (9):1、2:1 or 5: 1。
- 4. the minimally invasive glucose of spiral shape implantable of PVA/PEG composite aquogels outer membrane structure according to claim 1 The preparation method of sensor, it is characterised in that the temperature control in step (9) is 150 DEG C or 200 DEG C.
- 5. the minimally invasive glucose of spiral shape implantable of PVA/PEG composite aquogels outer membrane structure according to claim 1 The preparation method of sensor, it is characterised in that the cooling time in step (10) is 12 or 24 hours.
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| CN110448308A (en) * | 2019-07-19 | 2019-11-15 | 杭州微策生物技术有限公司 | A kind of implantable sensor and preparation method thereof |
| CN110806438A (en) * | 2019-10-21 | 2020-02-18 | 中国地质大学（武汉） | Electrochemical aptamer biosensor based on hydrogel protection and preparation method and application thereof |
| CN111307906A (en) * | 2017-12-29 | 2020-06-19 | 深圳硅基传感科技有限公司 | Analyte monitoring probe |
| CN112505121A (en) * | 2020-12-11 | 2021-03-16 | 江苏知至生物科技有限公司 | Anti-interference photoelectrochemical disease marker sensor and preparation method and application thereof |
| CN115266865A (en) * | 2022-07-29 | 2022-11-01 | 北京大学 | Method for improving stability of electrochemical sensor |
| CN115266865B (en) * | 2022-07-29 | 2024-04-16 | 北京大学 | Method for improving stability of electrochemical sensor |
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| CN110806438A (en) * | 2019-10-21 | 2020-02-18 | 中国地质大学（武汉） | Electrochemical aptamer biosensor based on hydrogel protection and preparation method and application thereof |
| CN112505121A (en) * | 2020-12-11 | 2021-03-16 | 江苏知至生物科技有限公司 | Anti-interference photoelectrochemical disease marker sensor and preparation method and application thereof |
| CN115266865A (en) * | 2022-07-29 | 2022-11-01 | 北京大学 | Method for improving stability of electrochemical sensor |
| CN115266865B (en) * | 2022-07-29 | 2024-04-16 | 北京大学 | Method for improving stability of electrochemical sensor |
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