Binder for electrode, preparation method thereof, electrode and electrochemical element

Abstract

The invention particularly relates to a binder for an electrode, a preparation method of the binder, the electrode and an electrochemical element. The adhesive has the advantages that the adhesive can be used for electrodes, repeatability of detection results of electrochemical elements related to the electrodes can be improved, and reliability and stability of the detection results are further improved.

Description

Technical Field

[0001] The present disclosure specifically relates to an adhesive for electrodes, a preparation method thereof, and an electrode and an electrochemical element. Background Art

[0002] At present, electrochemical elements such as screen-printed electrode sheets, electrochemical sensors, and electrochemical chips have been widely used in point-of-care testing (POCT), such as home self-monitoring of blood glucose, uric acid, total cholesterol, etc. Electrochemical elements such as screen-printed electrode sheets, electrochemical sensors, and electrochemical chips all have electrodes, and the detection sensitivity of electrochemical elements such as screen-printed electrode sheets, electrochemical sensors, and electrochemical chips has a great relationship with the performance of the electrodes.

[0003] The electrode solution of the electrode often contains electrochemically active materials. General electrode solutions generate current through enzymatic catalysis with substrates, and often have poor repeatability, resulting in large measurement errors and affecting the reliability and stability of the detection results.

[0004] The adhesive is a polymer that plays a role in bonding, adhering, and supporting the structure in the electrode solution. When the adhesive is added to the electrode solution and dried and fixed in the reaction area of the screen-printed electrode sheet, the amount of the adhesive needs to be adjusted according to the size and pattern of the ink reaction area (i.e., the reaction area of the screen-printed electrode sheet) so that the electrode solution can be evenly adhered to the screen-printed electrode sheet after drying. If the diffusion is uneven or not in place, it will affect the final repeatability of the electrode.

[0005] The present disclosure aims to develop an adhesive for electrodes, a preparation method thereof, and an electrode and an electrochemical element, and the adhesive can improve the repeatability of the detection results of electrochemical elements related to the electrodes. Summary of the Invention

[0006] The technical problem to be solved by the present disclosure is that, aiming at the poor repeatability of the detection results of electrochemical elements such as screen-printed electrode sheets, electrochemical sensors, and electrochemical chips in the current market, an adhesive for electrodes, a preparation method thereof, and an electrode and an electrochemical element, and the adhesive can improve the repeatability of the detection results of electrochemical elements related to the electrodes, thereby further improving the reliability and stability of the detection results.

[0007] To achieve the above technical purpose, the technical solution adopted by the present disclosure is as follows:

[0008] On the one hand, the present disclosure provides an adhesive for electrodes, and the adhesive for electrodes includes the following components: cellulose derivatives, water-soluble polymer, electron mediators, and cellulose stabilizers.

[0009] In some embodiments of the present disclosure, the electrode adhesive comprises the following components by mass percentage: cellulose derivative 0.001% - 1.55%, water-soluble polymer 0.1% - 6.8%, electron mediator 0.1% - 15%, and cellulose stabilizer 0.001% - 5.55%.

[0010] In the present disclosure, the cellulose derivative, water-soluble polymer, electron mediator, and cellulose stabilizer cooperate with each other, which can improve the repeatability of the detection results of the electrochemical elements related to the electrode, thereby further improving the reliability and stability of the detection results.

[0011] The functions of the electrode adhesive in the electrode solution mainly include the following aspects: (1) uniform dispersion: the cellulose derivative can prevent the enzymes and electron mediators from being too concentrated and ensure the uniformity of the reaction sites; (2) improving the interfacial stability: reducing electrode polarization and optimizing the electron transfer path; (3) volume adaptability: the water-soluble polymer can buffer the swelling of the enzyme layer and maintain the integrity of the structure.

[0012] The technical advantages of the electrode adhesive: providing high adhesion to prevent the shedding of enzymes and electron mediators; plasticizing effect to reduce the brittleness of the cellulose derivative and optimize the low cutting performance; enhancing the wettability of the enzyme solution and accelerating glucose diffusion.

[0013] In some embodiments of the present disclosure, the cellulose derivative accounts for 0.1% - 1.3% of the total mass of the electrode adhesive.

[0014] In some embodiments of the present disclosure, the cellulose derivative accounts for 0.1% - 1.0% of the total mass of the electrode adhesive.

[0015] In some embodiments of the present disclosure, the cellulose derivative accounts for 0.2% - 0.90% of the total mass of the electrode adhesive.

[0016] In some embodiments of the present disclosure, the cellulose derivative accounts for 0.3% - 0.80% of the total mass of the electrode adhesive.

[0017] In some embodiments of the present disclosure, the water-soluble polymer accounts for 0.2% - 5.5% of the total mass of the electrode adhesive.

[0018] In some embodiments of the present disclosure, the water-soluble polymer accounts for 0.2% - 4% of the total mass of the electrode adhesive.

[0019] In some embodiments of the present disclosure, the water-soluble polymer accounts for 0.3% - 3% of the total mass of the electrode adhesive.

[0020] In some embodiments of the present disclosure, the water-soluble polymer accounts for 0.3% to 2% of the total mass of the binder for the electrode.

[0021] In some embodiments of the present disclosure, the water-soluble polymer accounts for 0.3% to 1.5% of the total mass of the binder for the electrode.

[0022] In some embodiments of the present disclosure, the water-soluble polymer accounts for 0.3% to 1.0% of the total mass of the binder for the electrode.

[0023] In some embodiments of the present disclosure, the electron mediator accounts for 0.3% to 12% of the total mass of the binder for the electrode.

[0024] In some embodiments of the present disclosure, the electron mediator accounts for 0.5% to 10% of the total mass of the binder for the electrode.

[0025] In some embodiments of the present disclosure, the electron mediator accounts for 0.5% to 6% of the total mass of the binder for the electrode.

[0026] In some embodiments of the present disclosure, the electron mediator accounts for 1.0% to 5.0% of the total mass of the binder for the electrode.

[0027] In some embodiments of the present disclosure, the electron mediator accounts for 1.0% to 4.0% of the total mass of the binder for the electrode.

[0028] In some embodiments of the present disclosure, the electron mediator accounts for 1.0% to 3.0% of the total mass of the binder for the electrode.

[0029] In some embodiments of the present disclosure, the cellulose stabilizer accounts for 0.01% to 5% of the total mass of the binder for the electrode.

[0030] In some embodiments of the present disclosure, the cellulose stabilizer accounts for 0.03% to 4% of the total mass of the binder for the electrode.

[0031] In some embodiments of the present disclosure, the cellulose stabilizer accounts for 0.05% to 2% of the total mass of the binder for the electrode.

[0032] In some embodiments of the present disclosure, the cellulose stabilizer accounts for 0.05% to 1% of the total mass of the binder for the electrode.

[0033] In some embodiments of the present disclosure, the cellulose stabilizer accounts for 0.05% to 0.8% of the total mass of the binder for the electrode.

[0034] In some embodiments of the present disclosure, the cellulose stabilizer accounts for 0.05% to 0.6% of the total mass of the binder for the electrode.

[0035] In some embodiments of the present disclosure, the cellulose derivative is selected from at least one of cellulose ethers, cellulose esters, cellulose carbamates, cellulose nitrates, cellulose sulfonates, and cellulose ether esters.

[0036] In some embodiments of the present disclosure, the cellulose derivative is selected from at least one of cellulose ethers.

[0037] In some embodiments of the present disclosure, the water-soluble polymer is selected from at least one of polyether polymers, polyvinylpyrrolidone, polyvinyl alcohol, and polyacrylamide.

[0038] In some embodiments of the present disclosure, the water-soluble polymer is selected from at least one of polyether polymers.

[0039] In some embodiments of the present disclosure, the binder for the electrode comprises the following components by mass percentage: 0.001% - 1.55% of cellulose ethers, 0.1% - 6.8% of polyether polymers, 0.1% - 15% of electron mediators, and 0.001% - 5.55% of cellulose stabilizers.

[0040] In the present disclosure, the cellulose ethers, polyether polymers, electron mediators, and cellulose stabilizers cooperate with each other, which can improve the repeatability of the detection results of the electrochemical elements related to the electrode, thereby further improving the reliability and stability of the detection results.

[0041] The functions of the binder for the electrode in the electrode solution are mainly as follows: (1) Uniform dispersion: Cellulose ethers can prevent the enzymes and electron mediators from being too concentrated and ensure the uniformity of the reaction sites; (2) Improving interface stability: Reducing electrode polarization and optimizing the electron transfer path; (3) Volume adaptability: Polyether polymers can buffer the swelling of the enzyme layer and maintain the integrity of the structure.

[0042] The technical advantages of the binder for the electrode: Providing high adhesion to prevent the shedding of enzymes and electron mediators; Plasticizing effect, reducing the brittleness of cellulose ethers and optimizing the low cutting performance; Improving the wettability of the enzyme solution and accelerating the diffusion of glucose.

[0043] In some embodiments of the present disclosure, the binder for the electrode further comprises water.

[0044] In some embodiments of the present disclosure, the water is deionized water.

[0045] In some embodiments of the present disclosure, the water accounts for 85% - 99.7% of the total mass of the binder for the electrode.

[0046] In some embodiments of the present disclosure, the water accounts for 90% - 99.5% of the total mass of the binder for the electrode.

[0047] In some embodiments of the present disclosure, the water accounts for 91% to 99% of the total mass of the electrode binder.

[0048] In some embodiments of the present disclosure, the cellulose ethers are selected from at least one of methyl cellulose, hydroxyethyl methyl cellulose, ethyl cellulose, benzyl cellulose, hydroxyethyl cellulose, hydroxypropyl methyl cellulose, carboxymethyl hydroxyethyl cellulose, and phenyl cellulose.

[0049] In some embodiments of the present disclosure, the cellulose ethers are selected from at least one of methyl cellulose, ethyl cellulose, and hydroxyethyl cellulose.

[0050] In some embodiments of the present disclosure, the cellulose ethers are selected from at least one of methyl cellulose and hydroxyethyl cellulose.

[0051] In some embodiments of the present disclosure, the cellulose ether is methyl cellulose.

[0052] In some embodiments of the present disclosure, the cellulose ether is hydroxyethyl cellulose.

[0053] In some embodiments of the present disclosure, the polyether polymers are selected from at least one of polyethylene glycol derivatives and polypropylene glycol derivatives.

[0054] In some embodiments of the present disclosure, the polyether polymer is polyethylene glycol.

[0055] In some embodiments of the present disclosure, the electron mediators are selected from at least one of hexammine ruthenium chloride, potassium ferricyanide, and ferrocene formic acid.

[0056] In some embodiments of the present disclosure, the electron mediators are selected from at least one of hexammine ruthenium chloride and potassium ferricyanide.

[0057] In some embodiments of the present disclosure, the electron mediator is hexammine ruthenium chloride.

[0058] In some embodiments of the present disclosure, the electron mediator is potassium ferricyanide.

[0059] In some embodiments of the present disclosure, the cellulose stabilizers are selected from at least one of sodium 2,6-dichloroindophenol, bovine serum albumin, glycerol, gelatin, DTT, glycine, gentamicin, EDTA, and cyclodextrin.

[0060] In some embodiments of the present disclosure, the cellulose stabilizer is sodium 2,6-dichloroindophenol. Compared with traditional cellulose stabilizers, sodium 2,6-dichloroindophenol has the following advantages when used as an electrode binder: it can participate in electron transfer, assist in the charge balance of the electrode, and reduce the polarization effect; it can promote conductivity, provide a weak electron conduction path, make up for the insulation defect of the cellulose binder, and reduce the interfacial impedance; it has little effect on enzyme activity and is not likely to cause protein denaturation. The stabilizing effect of sodium 2,6-dichloroindophenol on cellulose is better than that of traditional stabilizers. This innovative application brings new technical ideas to the field of electrode binders and has important technical value and practical application significance.

[0061] In some embodiments of the present disclosure, the electrode binder comprises the following components: cellulose ethers, polyether polymers, electron mediators, and cellulose stabilizers.

[0062] In some embodiments of the present disclosure, the electrode binder comprises the following components: cellulose ethers, polyether polymers, electron mediators, and sodium 2,6-dichloroindophenol.

[0063] In some embodiments of the present disclosure, the electrode binder comprises the following components: cellulose ethers, polyether polymers, hexaammine ruthenium chloride, and sodium 2,6-dichloroindophenol.

[0064] In some embodiments of the present disclosure, the electrode binder comprises the following components: cellulose ethers, polyether polymers, potassium ferricyanide, and sodium 2,6-dichloroindophenol.

[0065] In some embodiments of the present disclosure, the electrode binder comprises the following components: cellulose ethers, polyethylene glycol, electron mediators, and sodium 2,6-dichloroindophenol.

[0066] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: methylcellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, hexaammine ruthenium chloride 0.1% - 15%, and sodium 2,6-dichloroindophenol 0.001% - 5.55%.

[0067] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: methylcellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, hexaammine ruthenium chloride 0.1% - 15%, and sodium 2,6-dichloroindophenol 0.001% - 5.55%; the balance is water.

[0068] In some embodiments of the present disclosure, the components such as methylcellulose, polyethylene glycol, hexammine ruthenium chloride, sodium 2,6-dichloroindophenol, and water cooperate with each other, which can protect cellulose ethers from being easily oxidized; can improve the dispersibility of the conductive agent and reduce agglomeration; can simplify the reaction path and increase the electron transfer rate; and can be used as an internal reference to correct background interference.

[0069] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: methylcellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, potassium ferricyanide 0.1% - 15%, sodium 2,6-dichloroindophenol 0.001% - 5.55%.

[0070] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: methylcellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, potassium ferricyanide 0.1% - 15%, sodium 2,6-dichloroindophenol 0.001% - 5.55%; the balance is water.

[0071] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: hydroxyethyl cellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, hexammine ruthenium chloride 0.1% - 15%, sodium 2,6-dichloroindophenol 0.001% - 5.55%.

[0072] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: hydroxyethyl cellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, potassium ferricyanide 0.1% - 15%, sodium 2,6-dichloroindophenol 0.001% - 5.55%; the balance is water.

[0073] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: hydroxyethyl cellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, potassium ferricyanide 0.1% - 15%, sodium 2,6-dichloroindophenol 0.001% - 5.55%.

[0074] In some embodiments of the present disclosure, the electrode binder comprises the following components by mass percentage: hydroxyethyl cellulose 0.001% - 1.55%, polyethylene glycol 0.1% - 6.8%, potassium ferricyanide 0.1% - 15%, sodium 2,6-dichloroindophenol 0.001% - 5.55%; the balance is water.

[0075] In some embodiments of the present disclosure, the cellulose ethers account for 0.1% - 1.3% of the total mass of the electrode binder.

[0076] In some embodiments of the present disclosure, the cellulose ethers account for 0.1% to 1.0% of the total mass of the binder for the electrode.

[0077] In some embodiments of the present disclosure, the cellulose ethers account for 0.2% to 0.90% of the total mass of the binder for the electrode.

[0078] In some embodiments of the present disclosure, the cellulose ethers account for 0.3% to 0.80% of the total mass of the binder for the electrode.

[0079] In some embodiments of the present disclosure, the polyether polymers account for 0.2% to 5.5% of the total mass of the binder for the electrode.

[0080] In some embodiments of the present disclosure, the polyether polymers account for 0.2% to 4% of the total mass of the binder for the electrode.

[0081] In some embodiments of the present disclosure, the polyether polymers account for 0.3% to 3% of the total mass of the binder for the electrode.

[0082] In some embodiments of the present disclosure, the polyether polymers account for 0.3% to 2% of the total mass of the binder for the electrode.

[0083] In some embodiments of the present disclosure, the polyether polymers account for 0.3% to 1.5% of the total mass of the binder for the electrode.

[0084] In some embodiments of the present disclosure, the polyether polymers account for 0.3% to 1.0% of the total mass of the binder for the electrode.

[0085] In some embodiments of the present disclosure, the hexammine ruthenium chloride accounts for 0.3% to 12% of the total mass of the binder for the electrode.

[0086] In some embodiments of the present disclosure, the hexammine ruthenium chloride accounts for 0.5% to 10% of the total mass of the binder for the electrode.

[0087] In some embodiments of the present disclosure, the hexammine ruthenium chloride accounts for 0.5% to 6% of the total mass of the binder for the electrode.

[0088] In some embodiments of the present disclosure, the hexammine ruthenium chloride accounts for 1.0% to 5.0% of the total mass of the binder for the electrode.

[0089] In some embodiments of the present disclosure, the hexammine ruthenium chloride accounts for 1.0% to 4.0% of the total mass of the binder for the electrode.

[0090] In some embodiments of the present disclosure, the hexammine ruthenium chloride accounts for 1.0% to 3.0% of the total mass of the binder for the electrode.

[0091] In some embodiments of the present disclosure, the sodium 2,6-dichloroindophenol accounts for 0.01% to 5% of the total mass of the binder for the electrode.

[0092] In some embodiments of the present disclosure, the sodium 2,6-dichloroindophenol accounts for 0.03% to 4% of the total mass of the binder for the electrode.

[0093] In some embodiments of the present disclosure, the sodium 2,6-dichloroindophenol accounts for 0.05% to 2% of the total mass of the binder for the electrode.

[0094] In some embodiments of the present disclosure, the sodium 2,6-dichloroindophenol accounts for 0.05% to 1% of the total mass of the binder for the electrode.

[0095] In some embodiments of the present disclosure, the sodium 2,6-dichloroindophenol accounts for 0.05% to 0.8% of the total mass of the binder for the electrode.

[0096] In some embodiments of the present disclosure, the sodium 2,6-dichloroindophenol accounts for 0.05% to 0.6% of the total mass of the binder for the electrode.

[0097] On the other hand, the present disclosure provides a method for preparing the binder for the electrode as described above, which includes the following steps: adding a formulated amount of a cellulose derivative to a part of the formulated amount of water, then adding a formulated amount of a water-soluble polymer, adding the remaining formulated amount of water, filtering and taking the filtrate, adding a formulated amount of an electron mediator and a cellulose stabilizer to the filtrate, and mixing evenly to obtain the binder for the electrode.

[0098] On the other hand, the present disclosure provides a method for preparing the binder for the electrode as described above, which includes the following steps: adding a formulated amount of a cellulose ether to a part of the formulated amount of water, then adding a formulated amount of a polyether polymer, adding the remaining formulated amount of water, filtering and taking the filtrate, adding a formulated amount of an electron mediator and a cellulose stabilizer to the filtrate, and mixing evenly to obtain the binder for the electrode.

[0099] On the other hand, the present disclosure provides a method for preparing the binder for the electrode as described above, which includes the following steps: adding a formulated amount of a cellulose ether to a part of the formulated amount of water, then adding a formulated amount of a polyether polymer, adding the remaining formulated amount of water, filtering and taking the filtrate, adding a formulated amount of hexammine ruthenium chloride and sodium 2,6-dichloroindophenol to the filtrate, and mixing evenly to obtain the binder for the electrode.

[0100] On the other hand, the present disclosure provides a method for preparing an electrode binder as described above, which comprises the following steps: adding a formulated amount of methyl cellulose to a part of the formulated amount of water, then adding a formulated amount of polyethylene glycol, adding the remaining formulated amount of water, filtering and taking the filtrate, and adding a formulated amount of hexammine ruthenium chloride and sodium 2,6-dichloroindophenol to the filtrate, and mixing evenly to obtain the electrode binder.

[0101] The electrode binder of the present disclosure can be applied to electrode liquids, electrodes, screen-printed electrode sheets, test strips, electrochemical sensors, electrochemical chips, blood glucose detection chips, blood lipid detection chips, and other electrochemical components containing the electrode binder.

[0102] On the other hand, the present disclosure provides an electrode liquid, which comprises the electrode binder as described above.

[0103] On the other hand, the present disclosure provides an electrode, which comprises the electrode binder as described above or the electrode liquid as described above.

[0104] On the other hand, the present disclosure provides an electrochemical component, which comprises the electrode as described above.

[0105] On the other hand, the present disclosure provides an electrochemical component, which comprises the electrode as described above; the electrochemical component is selected from one or more of a screen-printed electrode sheet, a test strip, an electrochemical sensor, an electrochemical chip, a blood glucose detection chip, and a blood lipid detection chip.

[0106] On the other hand, the present disclosure provides a screen-printed electrode sheet, which comprises the electrode binder as described above or the electrode as described above.

[0107] Screen-printed electrode sheet: Printing an enzyme solution (electrode liquid) containing a binder on a carbon electrode to fix the enzyme and the electron mediator, and form a stable enzyme reaction layer.

[0108] On the other hand, the present disclosure provides a test strip, which comprises the electrode binder as described above or the electrode as described above.

[0109] On the other hand, the present disclosure provides an electrochemical sensor, which comprises the electrode binder as described above or the electrode as described above.

[0110] Electrochemical sensor: Adapted to different oxidases or dehydrogenases, and the viscosity can be adjusted.

[0111] On the other hand, the present disclosure provides an electrochemical chip, which comprises the electrode binder as described above or the electrode as described above.

[0112] On the other hand, the present disclosure provides a blood glucose detection chip, which comprises the electrode binder as described above or the electrode as described above.

[0113] In some embodiments of the present disclosure, the blood glucose detection chip is preferably a continuous glucose monitoring (CGM) chip.

[0114] Continuous glucose monitoring (CGM) chip: The adhesive enhances the durability of the enzyme membrane, adapts to the body fluid environment, reduces protein adsorption, and lowers the risk of biological contamination.

[0115] On the other hand, the present disclosure provides a blood lipid detection chip, which includes the adhesive for electrodes as described above or the electrodes as described above.

[0116] The present disclosure has the following advantages:

[0117] (1) The adhesive of the present disclosure can be used for electrodes, which can improve the repeatability of the detection results of the electrochemical components related to the electrodes, thereby further improving the reliability and stability of the detection results.

[0118] (2) The adhesive of the present disclosure can be used for electrodes, which can change the linear performance of electrochemical components such as screen-printed electrode sheets, electrochemical sensors, and electrochemical chips.

[0119] (3) The adhesive of the present disclosure can be used for electrochemical components such as screen-printed electrode sheets, electrochemical sensors, and electrochemical chips, which can improve the repeatability of the detection results of the electrochemical components related to the electrodes, thereby further improving the reliability and stability of the detection results. BRIEF DESCRIPTION OF THE DRAWINGS

[0120] In order to more clearly illustrate the specific embodiments of the present disclosure or the technical solutions in the prior art, the following will briefly introduce the drawings required for the description of the specific embodiments or the prior art. Obviously, the following drawings are some embodiments of the present disclosure. For those of ordinary skill in the art, without creative efforts, other drawings can also be obtained based on these drawings. The drawings here are incorporated into the specification and constitute a part of this specification, showing the embodiments consistent with this specification, and are used together with the specification to explain the principles of this specification.

[0121] Figure 1 Shows the screen-printed electrode sheet containing the adhesive in Example 5.

[0122] Figure 2 Shows the linear effect of the adhesive on the test strip detection in Example 7; wherein, the horizontal axis is the signal value (current value) detected by electrochemistry; the vertical axis is the biochemical value (i.e., the biochemical detection concentration value, the sample concentration, the concentration measured by a commercial biochemical instrument). DETAILED DESCRIPTION OF THE EMBODIMENTS

[0123] Definitions and Explanations

[0124] To facilitate a better understanding of the present disclosure, certain technical and scientific terms are specifically defined below. In the present disclosure, unless otherwise specified, the scientific and technical terms used herein have the meanings commonly understood by those skilled in the art. Moreover, the terms related to cell and tissue culture, microbiology, and laboratory operation procedures used herein are all widely used terms and conventional procedures in their respective fields. Meanwhile, to better understand the present disclosure, the definitions and explanations of relevant terms are provided below. It should be understood that the present disclosure is not limited to specific methods, reagents, compounds, compositions, or biological systems, and of course, changes can be made thereto. It should also be understood that the terms used in this application are only for describing specific embodiments and are not intended to be limiting.

[0125] Unless the content is otherwise clearly stated, the terms "a", "an", and "the" as used in this specification and the appended claims cover one or more.

[0126] As used herein, the terms "comprising" and "having" and any variations thereof are intended to cover non-exclusive inclusion. For example, a process, method, device, product, or equipment that includes a series of steps is not limited to the listed steps or modules, but optionally further includes steps not listed, or optionally further includes other steps inherent to these processes, methods, products, or equipment.

[0127] In the description herein, reference is made to "some embodiments", "some implementations", or "some embodiments", which describe subsets of all possible embodiments. However, it can be understood that "some embodiments" can be the same subset or different subsets of all possible embodiments and can be combined with each other without conflict.

[0128] Examples

[0129] To make the objectives, technical solutions, and advantages of the embodiments of the present disclosure clearer, the technical solutions in the embodiments of the present disclosure will be clearly and completely described below in conjunction with the accompanying drawings in the embodiments of the present disclosure. Obviously, the described embodiments are part of the embodiments of the present disclosure, rather than all of the embodiments. The following is only a further description of the present disclosure, and the protection scope of the present disclosure is not limited thereto.

[0130] The symbols and explanations used in the following examples or comparative examples are as follows:

[0131] 1. CV (Coefficient of Variation)

[0132] (1) Definition of CV: The coefficient of variation is the ratio of the standard deviation to the mean and is used to measure the relative dispersion of data (i.e., the volatility of the unit mean). Its advantage lies in eliminating the influence of dimension and is applicable to comparing datasets with different units or magnitudes.

[0133] The coefficient of variation (CV) quantifies the data dispersion through the ratio of the standard deviation to the mean.

[0134] (2) Calculation formula:

[0135] CV = (Standard Deviation (SD) / Mean) × 100% or CV = (Mean / Standard Deviation (SD)) × 100%

[0136] Wherein, SD and Mean are defined as follows:

[0137] Standard Deviation (SD): Reflects the dispersion degree of data distribution, and the calculation formula is:

[0138]

[0139] Wherein, SD represents the sample standard deviation;

[0140] n represents the number of sample data;

[0141] xi represents the i-th sample data point;

[0142] represents the mean (Mean).

[0143] Mean (Mean): The average value of the data set:

[0144]

[0145] Wherein, represents the mean (Mean);

[0146] n represents the number of sample data;

[0147] x i represents the i-th sample data point.

[0148] 2. A (Slope) and B (Intercept)

[0149] A (Slope) and B (Intercept): Estimate the regression parameters through the least squares method, and respectively describe the action intensity between the baseline value and the variable.

[0150] 3. R 2 (Coefficient of Determination)

[0151] R 2 (Coefficient of Determination) is the "gold standard" for evaluating the linear performance in electrochemical detection, and directly reflects the reliability of the concentration-signal relationship. A high R 2 value (close to 1) indicates that the detection system has the ability of accurate quantification, but it needs to be comprehensively verified by combining the slope, residual analysis and experimental design. In practical applications, R 2The reasonable threshold depends on the detection scenario (e.g., clinical diagnosis requires strictness, and scientific research exploration can be appropriately relaxed), which is the core basis for optimizing sensor design and validating detection methods.

[0152] R 2 : Together with B (intercept), it reflects the explanatory power of the model, while CV (coefficient of variation) indicates the impact of data quality on the reliability of the model.

[0153] 4. Theoretical value

[0154] The theoretical value is the concentration value calculated by the main blood glucose curve equation. In Example 6, Comparative Example 1, Comparative Example 2, and Comparative Example 3, the theoretical values are the concentration values in mmol units calculated by using the linear formula (Y = AX + B) for the current values in Example 6, Comparative Example 1, Comparative Example 2, and Comparative Example 3, that is, the electrochemically calculated concentration or the electrochemically determined concentration; where X is the current value; Y is the electrochemically determined concentration calculated, that is, the electrochemically calculated concentration; A is the slope; B is the intercept.

[0155] 5. Biochemical value

[0156] The biochemical value usually refers to the actual concentration of the analyte measured by standard biochemical analysis methods (such as mass spectrometry, enzyme-linked immunosorbent assay, or laboratory biochemical analyzer), usually expressed in mmol / L or other concentration units.

[0157] The determination of the biochemical value is usually carried out according to the common general knowledge in the art, and reference can be made to the methods for blood glucose determination in Section 1, Chapter 2 of "National Clinical Laboratory Operating Procedures (Fourth Edition)", the detection methods of conventional biochemical analyzers in "Liu Hanbo. Value Analysis of Rapid Blood Glucose Meters and Conventional Biochemical Analyzers in Clinical Blood Glucose Detection [J]. Chinese Journal of Modern Drug Application, 2022, 16(14): 108 - 110", the detection methods of fully automatic biochemical analyzers in "Aizuramu·Supi, Yusifu·Keyoum, Zulumila·Abulimiti, etc. Comparative Analysis of Blood Glucose Detection Results between Portable Blood Glucose Meters and Fully Automatic Biochemical Analyzers [J]. China Medical Device Information, 2022, 28(15): 92 - 94", etc.

[0158] In the present disclosure, in Example 6, Comparative Example 1, Comparative Example 2, and Comparative Example 3, after the whole blood experiment is completed, the whole blood sample is centrifuged, and then plasma is taken, and the blood glucose concentration value in the plasma is detected by using a biochemical analyzer.

[0159] The comparison between the theoretical value and the biochemical value is an index for measuring the accuracy of the test strip.

[0160] Compared with the biochemical value detection method, the advantage of the method for detecting concentration by using the electrode adhesive in the present application is that the result can be detected in a short time, the blood volume used for testing is small, it is more convenient to carry than a biochemical analyzer, and dynamic monitoring can be carried out.

[0161] Example 1-1. Preparation of Adhesive 1

[0162] The formulation of Adhesive 1 is as follows: Taking 100 ml of Adhesive 1 as an example, 0.24 g of hydroxyethyl cellulose, 0.4 g of polyethylene glycol, 4 g of hexammine ruthenium(III) chloride, and 0.5 g of sodium 2,6-dichloroindophenol; the balance is deionized water.

[0163] Taking the preparation of 100 mL of Adhesive 1 as an example, the preparation method of Adhesive 1 is as follows: Taking 100 ml as an example

[0164] ① Calculate and weigh 0.24 g of the required hydroxyethyl cellulose.

[0165] ② Slowly pour the cellulose ether into a beaker containing about 80 mL of deionized water, and magnetically stir for at least 30 minutes until the solution is transparent and free of particles to obtain Mixture 1.

[0166] ③ Calculate and weigh 0.4 g of the required polyethylene glycol and pour it into Mixture 1, and magnetically stir for about 30 minutes until the solution is transparent and free of particles to obtain Mixture 2.

[0167] ④ Transfer Mixture 2 to a 100 mL volumetric flask, rinse the beaker 3 times with deionized water, pour the rinsing solution into the volumetric flask, and use deionized water to make up the solution to the 100 mL graduation mark and mix well to obtain Mixture 3.

[0168] ⑤ Long-term storage: After filtering Mixture 3 with a 0.22 μm filter membrane, take the filtrate to obtain Mixture 4 and store it.

[0169] ⑥ Calculate and weigh 4 g of hexammine ruthenium(III) chloride, slowly add it to Mixture 4, and magnetically stir for at least 1 hour until the solution is transparent and free of particles to obtain Mixture 5.

[0170] ⑦ Calculate and weigh 0.5 g of sodium 2,6-dichloroindophenol, slowly add it to Mixture 5, and magnetically stir for at least 1 hour until the solution is transparent and free of particles to obtain Adhesive 1.

[0171] Example 1-2. Preparation of Adhesive 2

[0172] The formulation of Adhesive 2 is as follows: Taking 100 ml of Adhesive 2 as an example, 0.50 g of hydroxyethyl cellulose, 0.6 g of polyethylene glycol, 0.5 g of potassium ferricyanide, and 0.8 g of sodium 2,6-dichloroindophenol; the balance is deionized water.

[0173] According to the preparation method of Adhesive 1 in Example 1-1, Adhesive 2 is prepared using the formulation of Adhesive 2.

[0174] Example 1-3. Preparation of Adhesive 3

[0175] The formulation of Adhesive 3 is as follows: Taking 100 ml of Adhesive 3 as an example, methylcellulose 0.90 g, polyethylene glycol 2.0 g, hexammine ruthenium(III) chloride 3.0 g, 2,6-dichlorophenolindophenol sodium 3.0 g; the balance is deionized water.

[0176] According to the preparation method of Adhesive 1 in Example 1-1, Adhesive 3 was prepared using the formulation of Adhesive 3.

[0177] Example 1-4. Preparation of Adhesive 4

[0178] The formulation of Adhesive 4 is as follows: Taking 100 ml of Adhesive 4 as an example, hydroxyethyl cellulose 1.0 g, polyethylene glycol 3.0 g, hexammine ruthenium(III) chloride 4.0 g, 2,6-dichlorophenolindophenol sodium 4.0 g; the balance is deionized water.

[0179] According to the preparation method of Adhesive 1 in Example 1-1, Adhesive 4 was prepared using the formulation of Adhesive 4.

[0180] Example 1-5. Preparation of Adhesive 5

[0181] The formulation of Adhesive 5 is as follows: Taking 100 ml of Adhesive 5 as an example, methylcellulose 1.5 g, polyethylene glycol 5.0 g, potassium ferricyanide 5.0 g, 2,6-dichlorophenolindophenol sodium 5.0 g; the balance is deionized water.

[0182] According to the preparation method of Adhesive 1 in Example 1-1, Adhesive 5 was prepared using the formulation of Adhesive 5.

[0183] Example 2. Viscosity Test of Adhesives

[0184] Experimental instrument: JBN2010A rotational viscometer (Shanghai Runxinsen Electronic Technology)

[0185] Experimental steps:

[0186] ① Pour the adhesives of Example 1-1, 1-2, 1-3, 1-4, and 1-5 into a beaker or straight cylindrical container with a diameter of not less than 70 mm, and use a rotational viscometer to measure their viscosities.

[0187] ② Repeat the test 3 times and take the average value.

[0188] Result analysis: The viscosity test results are qualified within the range of 260-340 mPa·s. The viscosity tests of the adhesives in Example 1-1, 1-2, 1-3, 1-4, and 1-5 are all qualified.

[0189] Example 3. Verification of Anti-Stripping Ability

[0190] Verification of anti-stripping ability: Test the adhesion firmness of the enzyme layer in the test paper reaction area to avoid detachment during cutting or use.

[0191] Experimental procedures:

[0192] ① Prepare enzyme solutions using the adhesives of Examples 1-1, 1-2, 1-3, 1-4, and 1-5 respectively. Spray the prepared enzyme solutions onto the reaction areas of the screen-printed electrode sheets and dry them at 50 °C for 10 minutes;

[0193] ② Prepare a 1-mm-wide tape, attach it to the enzyme layer in the reaction area, and use a universal material testing machine to peel it off at an angle of 90° and a speed of 30 mm / min. Observe the size of the range of the enzyme layer remaining in the reaction area;

[0194] ③ Immerse the test strips in PBS (37 °C) and oscillate for 1 hour, and repeat the peeling test.

[0195] Result analysis: Observe the size of the range of the enzyme layer remaining in the reaction area. If the peeled area is less than 1 / 10 of the overall area, it is qualified. The anti-peeling ability verifications of the adhesives of Examples 1-1, 1-2, 1-3, 1-4, and 1-5 are all qualified.

[0196] Example 4. Aging verification

[0197] Experimental instruments: drying oven, electrochemistry workstation (Shanghai Chenhua)

[0198] Experimental procedures:

[0199] ① After preparing enzyme solutions using the adhesives of Examples 1-1, 1-2, 1-3, 1-4, and 1-5 respectively, prepare test strips respectively. Take out the prepared test strips after storing them at 60 °C for 7 days.

[0200] ② Use the same samples to test the test strips stored at room temperature and the test strips stored at 60 °C, and record the current values.

[0201] ③ Calculate the current values as concentration values and compare the aged test strips with the room-temperature control group

[0202] Result analysis: If the deviation of the result from the result of the room-temperature test strip is within 10%, it meets the requirements. The aging verifications of the adhesives of Examples 1-1, 1-2, 1-3, 1-4, and 1-5 are all qualified.

[0203] Example 5. Screen-printed electrode sheet containing adhesive

[0204] The preparation steps of the screen-printed electrode sheet containing adhesive are as follows:

[0205] Prepare the adhesive according to the preparation method of Example 1-1.

[0206] Dissolve the adhesive and glucose dehydrogenase in phosphate buffer (pH = 7.4), mix well, spray it on the reaction area of the screen-printed electrode sheet, dry it at 50 °C for 10 minutes, cut it into strips to obtain a screen-printed electrode sheet containing the adhesive, see the attached Figure 1 of the specification. Test the electrochemical performance of the screen-printed electrode sheet containing the adhesive.

[0207] The response time of the screen-printed electrode sheet containing the adhesive is 5 seconds, the linear range is 0.6 - 33.3 mmol / L, R2 > 0.99, and the cutting qualification rate is 98%.

[0208] Example 6. Adhesive 0828

[0209] (1) Detect blood glucose using a screen-printed electrode sheet containing adhesive 0828

[0210] Experimental materials: self-prepared electrode solution, screen-printed electrode sheet (Xinde), hydrophilic upper cover sheet (Funa)

[0211] Experimental instruments: dispensing machine, electrochemical workstation (Shanghai Chenhua)

[0212] Experimental operation steps:

[0213] ① The formula of adhesive 0828 is 0.5% methyl cellulose, 0.6% polyethylene glycol, 2% hexammine ruthenium chloride, 0.1% 2,6-dichlorophenol indophenol sodium, and the balance is deionized water; prepare adhesive 0828 according to the preparation method of Example 1-1.

[0214] ② Prepare an enzyme solution (electrode solution) using the adhesive in ① above, and use a dispensing machine to spray the enzyme solution on the reaction area of the screen-printed electrode sheet to produce test strips with different formulas.

[0215] ③ Prepare 5 concentration gradients of samples with blood glucose concentrations of about 1.80 mmol / L, 3.50 mmol / L, 5.00 mmol / L, 12.00 mmol / L, and 23.5 mmol / L respectively.

[0216] ④ Use an electrochemical workstation to test the current signal values of the test strips, test about 5 times at the same horizontal concentration, and calculate the current mean and CV at different horizontal concentrations. The theoretical value is the concentration value in mmol units calculated by the current value using the linear formula (Y = AX + B), that is, the electrochemical calculation concentration or electrochemical determination concentration; where X is the current value; Y is the calculated electrochemical determination concentration, that is, the electrochemical calculation concentration; A is the slope; B is the intercept.

[0217] (2) Biochemical value detection method

[0218] Experimental steps:

[0219] (i) Use a heparin - anticoagulated whole - blood sample to test the test strip and obtain the theoretical concentration value.

[0220] (ii) Set the DLAB high - speed refrigerated centrifuge to 3000 rpm for 5 minutes. Immediately centrifuge the whole blood and take out the plasma.

[0221] (iii) Immediately use the biochemical analyzer BECKMAN - AU680 to test the blood - glucose concentration of the plasma and obtain the biochemical values (1.96 mmol / L, 3.75 mmol / L, 6.15 mmol / L, 17.46 mmol / L, 27.37 mmol / L).

[0222] Compare the theoretical value in (1) with the biochemical value in (2) to obtain the relative deviation and the absolute deviation. The requirements are met within the following ranges: when the blood - glucose concentration < 5.55 mmol / L, the absolute deviation < 0.83 mmol / L; when ≥ 5.55 mmol / L, the relative deviation < 15%.

[0223] The mean current and CV, the theoretical value, and the comparison with the biochemical value are shown in the following table.

[0224] Table 1. Mean current and CV at different concentration levels

[0225]

[0226] Table 2. Theoretical values at different concentration levels

[0227]

[0228] Table 3. Comparison with the biochemical value

[0229]

[0230] Experimental data analysis:

[0231] ① Repeatability: Calculate the CV of the test results at the same concentration level. If the current CV exceeds 4.5%, the repeatability is judged to be poor.

[0232] ② Linearity: Compare the mean value of the test results with the biochemical value and fit a linear equation. If its R 2 < 0.92, the linearity is judged to be poor.

[0233] The comparison between the theoretical value and the biochemical value is an index to measure the accuracy of the test strip.

[0234] Compared with the biochemical value detection method, the advantages of the method for detecting the concentration using the electrode adhesive in this application are short result - detection time, less blood volume for testing, more convenient to carry than the biochemical analyzer, and can perform dynamic monitoring.

[0235] Example 7. The linear influence of the adhesive on the test strip detection

[0236] The test strips of Example 6, Comparative Example 1, Comparative Example 2, and Comparative Example 3 were respectively used to make linear graphs based on the test results. See the appendix of the specification Figure 2 .

[0237] The appendix of the specification Figure 2 In the appendix, the 0828 formulation refers to the binder 0828 formulation; the 0726 formulation refers to the binder 0726 formulation; the 0805 formulation refers to the binder 0805 formulation; the 0809 formulation refers to the binder 0809 formulation.

[0238] It was found through the appendix of the specification Figure 2 that the test strips of Comparative Example 1, Comparative Example 2, and Comparative Example 3 had poor linearity and poor repeatability in detection. The test strip of Example 6 had good linearity and good repeatability. This shows that the binder formulations of Comparative Example 1, Comparative Example 2, and Comparative Example 3 had poor linearity and poor repeatability. The binder 0828 formulation of Example 6 had good linearity and good repeatability because the electrode solution diffused sufficiently in the binder 0828 formulation and was paired with an electron mediator, improving the repeatability.

[0239] Comparative Example 1. Binder 0726

[0240] (1) Use a screen-printed electrode sheet containing binder 0726 to detect blood glucose

[0241] Experimental materials: self-prepared electrode solution, screen-printed electrode sheet (Xinde), hydrophilic upper cover sheet (Funai)

[0242] Experimental instruments: dispensing machine, electrochemical workstation (Shanghai Chenhua)

[0243] Experimental operation steps:

[0244] ① The binder 0726 formulation is 0.1% hydroxyethyl cellulose, 1% polyvinylpyrrolidone, 3% potassium ferricyanide, and the balance is deionized water;

[0245] The preparation method of binder 0726 is: prepare 100 mL of binder

[0246] a Calculate and weigh the required cellulose derivatives.

[0247] b Slowly pour it into a beaker containing about 80 mL of deionized water, and stir magnetically for at least 30 minutes until the solution is clear and free of particles to obtain mixture 1.

[0248] c Calculate and weigh the required polyvinylpyrrolidone and pour it into mixture 1, and stir magnetically for about 30 minutes until the solution is clear and free of particles to obtain mixture 2.

[0249] Transfer the mixture 2 into a 100 mL volumetric flask, rinse the beaker with deionized water three times, and incorporate the rinsing liquid into the volumetric flask.

[0250] Then, make up the solution to the 100 mL graduation mark with deionized water and mix well to obtain mixture 3.

[0251] e Long-term storage: After filtering mixture 3 using a 0.22 μm filter membrane, take the filtrate to obtain mixture 4 and store it.

[0252] ② Use the mixture 4 in ① above, weigh 0.1% - 15% of potassium ferricyanide, and mix well to obtain adhesive 0726; use adhesive 0726 to prepare the enzyme solution (electrode solution), and spray the enzyme solution on the reaction area of the screen-printed electrode sheet using a dispensing machine to produce test strips with different formulations.

[0253] ③ Prepare 5 concentration gradients of samples with blood glucose concentrations of approximately 1.80 mmol / L, 3.50 mmol / L, 5.00 mmol / L, 12.00 mmol / L, and 23.5 mmol / L respectively.

[0254] ④ Use an electrochemical workstation to measure the current signal values of the test strips, measure about 5 times at the same horizontal concentration, and calculate the average current and CV at different horizontal concentrations. The theoretical value is the concentration value in mmol units calculated from the current value using the linear formula (Y = AX + B), that is, the electrochemical calculation concentration or the electrochemical determination concentration; where X is the current value; Y is the calculated electrochemical determination concentration, that is, the electrochemical calculation concentration; A is the slope; B is the intercept.

[0255] (2) Biochemical value detection method

[0256] Experimental steps:

[0257] (ⅰ) Use a heparinized whole blood sample to test the test strip to obtain the theoretical concentration value.

[0258] (ⅱ) Set the DLAB high-speed refrigerated centrifuge to 3000 rpm for 5 minutes. Immediately centrifuge the whole blood to obtain plasma.

[0259] (ⅲ) Immediately use the biochemical analyzer BECKMAN - AU680 to measure the blood glucose concentration of the plasma to obtain the biochemical values (1.80 mmol / L, 3.56 mmol / L, 5.39 mmol / L, 12.84 mmol / L, 23.49 mmol / L).

[0260] Compare the theoretical values in (1) with the biochemical values in (2) to obtain the relative deviation and the absolute deviation. The requirements are met within the following ranges: when the blood glucose concentration < 5.55 mmol / L, the absolute deviation < 0.83 mmol / L; when ≥ 5.55 mmol / L, the relative deviation < 15%.

[0261] The average current, CV, theoretical values, and the comparison with biochemical values are shown in the following table.

[0262] Table 4. Average current and CV at different levels of concentration

[0263]

[0264] Table 5. Theoretical values at different levels of concentration

[0265]

[0266] Table 6. Comparison with biochemical values

[0267]

[0268] Experimental data analysis:

[0269] ① Repeatability: Calculate the CV of the test results at the same level of concentration. If the current CV exceeds 4.5%, the repeatability is judged to be poor.

[0270] ② Linearity: Compare the average value of the test results with the biochemical values and fit a linear equation. If its R 2 < 0.92, the linearity is judged to be poor.

[0271] Comparative Example 2. Adhesive 0805

[0272] (1) Use a screen-printed electrode sheet containing adhesive 0805 to detect blood glucose

[0273] Experimental materials: Self-prepared electrode solution, screen-printed electrode sheet (Xinde), hydrophilic cover sheet (Funa)

[0274] Experimental instruments: Dispensing machine, electrochemical workstation (Shanghai Chenhua)

[0275] Experimental operation steps:

[0276] ① The formula of adhesive 0805 is 0.3% methyl cellulose, 0.1% polyvinylpyrrolidone, 2% hexammine ruthenium chloride, and the balance is deionized water;

[0277] The preparation method of adhesive 0805 is: Prepare 100 mL of adhesive

[0278] a Calculate and weigh the required cellulose derivatives.

[0279] b Slowly pour the cellulose derivative into a beaker containing about 80 mL of deionized water, and magnetically stir for at least 30 minutes until the solution is transparent and free of particles to obtain Mixture 1.

[0280] c Calculate and weigh the required polyvinylpyrrolidone and pour it into Mixture 1, and magnetically stir for about 30 minutes until the solution is transparent and free of particles to obtain Mixture 2. d Transfer Mixture 2 to a 100 mL volumetric flask, rinse the beaker 3 times with deionized water, pour the rinsing liquid into the volumetric flask, and use deionized water to make up the solution to the 100 mL graduation mark and mix well.

[0281] To obtain Mixture 3.

[0282] e Long-term storage: After filtering Mixture 3 with a 0.22 μm filter membrane, take the filtrate to obtain Mixture 4 and store it.

[0283] ② Use Mixture 4 in ① above, weigh 0.1% - 15% of hexammine ruthenium chloride, and mix well to obtain Adhesive 0805; use Adhesive 0805 to prepare the enzyme solution (electrode solution), and use a dispensing machine to spray the enzyme solution on the reaction area of the screen-printed electrode sheet to produce test strips with different formulations.

[0284] ③ Prepare 5 concentration gradients of samples with blood glucose concentrations of about 1.80 mmol / L, 3.50 mmol / L, 5.00 mmol / L, 12.00 mmol / L, and 23.5 mmol / L respectively.

[0285] ④ Use an electrochemical workstation to test the current signal values of the test strips, test about 5 times at the same horizontal concentration, and calculate the average current and CV at different horizontal concentrations. The theoretical value is the concentration value in mmol units calculated from the current value using the linear formula (Y = AX + B), that is, the electrochemical calculation concentration or electrochemical determination concentration; where X is the current value; Y is the calculated electrochemical determination concentration, that is, the electrochemical calculation concentration; A is the slope; B is the intercept.

[0286] (2) Biochemical value detection method

[0287] Experimental steps:

[0288] (ⅰ) Use a heparinized whole blood sample to test the test strip to obtain the theoretical concentration value.

[0289] (ⅱ) Set the DLAB high-speed refrigerated centrifuge to 3000 rpm for 5 minutes. Immediately centrifuge the whole blood to take out the plasma.

[0290] (ⅲ) Immediately use the biochemical analyzer BECKMAN - AU680 to test the blood glucose concentration in plasma and obtain the biochemical values (1.79 mmol / L, 3.62 mmol / L, 5.47 mmol / L, 12.91 mmol / L, 23.17 mmol / L).

[0291] Compare the theoretical values in (1) with the biochemical values in (2) to obtain the relative deviation and absolute deviation. The requirements are met within the following ranges: when the blood glucose concentration < 5.55 mmol / L, the absolute deviation < 0.83 mmol / L; when ≥ 5.55 mmol / L, the relative deviation < 15%.

[0292] The average current, CV, theoretical values, and the comparison with biochemical values are shown in the following table.

[0293] Table 7. Average current and CV at different levels of concentration

[0294]

[0295] Table 8. Theoretical values at different levels of concentration

[0296]

[0297] Table 9. Comparison with biochemical values

[0298]

[0299] Experimental data analysis:

[0300] ① Repeatability: Calculate the CV of the test results at the same level of concentration. If the current CV exceeds 4.5%, it is determined that the repeatability is poor.

[0301] ② Linearity: Compare the average value of the test results with the biochemical values and fit a linear equation. If its R 2 < 0.92, it is determined that the linearity is poor.

[0302] Comparative Example 3. Adhesive 0809

[0303] (1) Use a screen - printed electrode sheet containing adhesive 0809 to detect blood glucose

[0304] Experimental materials: Self - prepared electrode solution, screen - printed electrode sheet (Xinde), hydrophilic cover sheet (Funer)

[0305] Experimental instruments: Dispensing machine, electrochemical workstation (Shanghai Chenhua)

[0306] Experimental operation steps:

[0307] ① The formula of adhesive 0809 is 0.5% methyl cellulose, 2% hexammine ruthenium chloride, 0.1% sodium 2,6 - dichlorophenol indophenol, and the balance is deionized water.

[0308] The preparation method of Adhesive 0809 is as follows: Prepare 100 mL of adhesive

[0309] a Calculate and weigh the required cellulose derivative.

[0310] b Slowly pour the cellulose derivative into a beaker containing about 80 mL of deionized water, and stir magnetically for at least 30 minutes until the solution is transparent and free of particles to obtain Mixture 1.

[0311] c Transfer Mixture 1 to a 100 mL volumetric flask, rinse the beaker 3 times with deionized water, pour the rinsing liquid into the volumetric flask, and use deionized water to make up the solution to the 100 mL graduation line and mix well to obtain Mixture 2.

[0312] d Long-term storage: After filtering Mixture 2 with a 0.22 μm filter membrane, take the filtrate to obtain Mixture 3 and store it.

[0313] ② Use Mixture 3 in ① above, and weigh 0.1%-15% of hexammine ruthenium chloride and 0.001%-5.55% of cellulose stabilizer, and mix well to obtain Adhesive 0809; use Adhesive 0809 to prepare an enzyme solution (electrode solution), and use a dispensing machine to spray the enzyme solution on the reaction area of the screen-printed electrode sheet to produce test strips with different formulations.

[0314] ③ Prepare 5 concentration gradients of samples with blood glucose concentrations of about 1.80 mmol / L, 3.50 mmol / L, 5.00 mmol / L, 12.00 mmol / L, and 23.5 mmol / L respectively.

[0315] ④ Use an electrochemical workstation to test the current signal value of the test strip, test about 5 times at the same horizontal concentration, and calculate the current mean and CV at different horizontal concentrations. The theoretical value is the concentration value in mmol units calculated by the current value using the linear formula (Y = AX + B), that is, the electrochemical calculation concentration or the electrochemical determination concentration; where, X is the current value; Y is the calculated electrochemical determination concentration, that is, the electrochemical calculation concentration; A is the slope; B is the intercept.

[0316] (2) Biochemical value detection method

[0317] Experimental steps:

[0318] (ⅰ) Use a heparinized whole blood sample to test the test strip to obtain the theoretical concentration value.

[0319] (ⅱ) Set the DLAB high-speed refrigerated centrifuge to 3000 rpm for 5 minutes. Immediately centrifuge the whole blood to take out the plasma.

[0320] (ⅲ) Immediately use the biochemical analyzer BECKMAN - AU680 to test the blood glucose concentration in the plasma, and obtain the biochemical values (1.82 mmol / L, 3.69 mmol / L, 5.54 mmol / L, 12.99 mmol / L, 23.81 mmol / L).

[0321] Compare the theoretical values in (1) with the biochemical values in (2) to obtain the relative deviation and the absolute deviation. The requirements are met within the following ranges: when the blood glucose concentration < 5.55 mmol / L, the absolute deviation < 0.83 mmol / L; when ≥ 5.55 mmol / L, the relative deviation < 15%.

[0322] The average current, CV, theoretical values, and the comparison with the biochemical values are shown in the following table.

[0323] Table 10. Average current and CV at different level concentrations

[0324]

[0325] Table 11. Theoretical values at different level concentrations

[0326]

[0327] Table 12. Comparison with the biochemical values

[0328]

[0329] Experimental data analysis:

[0330] ① Repeatability: Calculate the CV of the test results at the same level concentration. If the current CV exceeds 4.5%, it is determined that the repeatability is poor.

[0331] ② Linearity: Compare the average value of the test results with the biochemical values and fit a linear equation. If its R 2 < 0.92, it is determined that the linearity is poor.

[0332] The foregoing description of the specific exemplary embodiments of the present disclosure is for purposes of illustration and exemplification. These descriptions are not intended to limit the present disclosure to the precise forms disclosed, and it is obvious that many changes and variations can be made in light of the above teachings. The purpose of selecting and describing the exemplary embodiments is to explain the specific principles of the present disclosure and its practical applications, so that those skilled in the art can implement and utilize various different exemplary embodiments of the present disclosure, as well as various different selections and changes. The scope of the present disclosure is intended to be defined by the claims and their equivalents.

Claims

1. An adhesive for an electrode, the adhesive for the electrode comprising the following components: a cellulose derivative, a water-soluble polymer, an electron mediator, and a cellulose stabilizer.

2. The binder for an electrode according to claim 1, characterized in that, The adhesive for the electrode comprises the following components by mass percentage: 0.001% to 1.55% of a cellulose derivative, 0.1% to 6.8% of a water-soluble polymer, 0.1% to 15% of an electron mediator, and 0.001% to 5.55% of a cellulose stabilizer.

3. The binder for an electrode according to claim 2, characterized in that, The cellulose derivative is selected from at least one of cellulose ethers, cellulose esters, cellulose carbamates, cellulose nitrates, cellulose sulfonates, and cellulose ether esters; The water-soluble polymer is selected from at least one of polyether polymers, polyvinylpyrrolidone, polyvinyl alcohol, and polyacrylamide; The cellulose ethers are selected from at least one of methyl cellulose, hydroxyethyl methyl cellulose, ethyl cellulose, benzyl cellulose, hydroxyethyl cellulose, hydroxypropyl methyl cellulose, carboxymethyl hydroxyethyl cellulose, and phenyl cellulose; The polyether polymers are selected from at least one of polyethylene glycol derivatives and polypropylene glycol derivatives; The electron mediator is selected from at least one of hexammine ruthenium chloride, potassium ferricyanide, and ferrocene formic acid; The cellulose stabilizer is selected from at least one of sodium 2,6-dichloroindophenol, bovine serum albumin, glycerol, gelatin, DTT, glycine, gentamicin, EDTA, and cyclodextrin.

4. The binder for an electrode according to claim 3, characterized in that, The adhesive for the electrode comprises the following components: cellulose ethers, polyether polymers, an electron mediator, and a cellulose stabilizer.

5. The binder for an electrode according to any one of claims 1 to 4, characterized in that, The adhesive for the electrode further comprises water.

6. The binder for an electrode according to claim 5, characterized in that, The water accounts for 85% to 99.7% of the total mass of the adhesive for the electrode.

7. A method for preparing the adhesive for the electrode according to any one of claims 1 to 6, comprising the following steps: adding a formulated amount of a cellulose derivative to a part of the formulated amount of water, then adding a formulated amount of a water-soluble polymer, adding the remaining formulated amount of water, filtering and taking the filtrate, adding a formulated amount of an electron mediator and a cellulose stabilizer to the filtrate, and mixing evenly to obtain the adhesive for the electrode.

8. An electrode liquid, characterized in that, It comprises the adhesive for the electrode according to any one of claims 1 to 6.

9. An electrode, characterized in that, It comprises the adhesive for the electrode according to any one of claims 1 to 6 or the electrode liquid according to claim 8.

10. An electrochemical element, characterized in that, It comprises the electrode according to claim 9; The electrochemical element is selected from one or more of screen-printed electrode sheets, test strips, electrochemical sensors, electrochemical chips, blood glucose detection chips, and blood lipid detection chips.

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