CN103323512A - Process for preparing electrode membrane based on glucose oxidase and product thereof - Google Patents
Process for preparing electrode membrane based on glucose oxidase and product thereof Download PDFInfo
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- CN103323512A CN103323512A CN2013102197541A CN201310219754A CN103323512A CN 103323512 A CN103323512 A CN 103323512A CN 2013102197541 A CN2013102197541 A CN 2013102197541A CN 201310219754 A CN201310219754 A CN 201310219754A CN 103323512 A CN103323512 A CN 103323512A
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Abstract
The invention discloses a process for preparing an electrode membrane based on glucose oxidase, and further discloses the glucose oxidase electrode membrane prepared by the process. The glucose oxidase electrode membrane provided by the invention can prevent reducing electroactive substances in samples from reaching the surface of an electrode to be subjected to an oxidation reaction, so that an anti-interference capacity of the electrode is enhanced; and a leakage of glucose oxidase macromolecules is prevented effectively because pores of an outer membrane, a polycarbonate (PC) membrane, are small, and the service life of the electrode is increased.
Description
Technical field
The present invention relates to the enzyme electrode field, be specifically related to a kind of preparation method based on the glucose oxidase electrode film and products thereof.
Background technology
Biology sensor is that a kind of selectivity with the biological response element and one can produce the analytical equipment that signal transmitter proportional to testing concentration combines.Selectivity is good, highly sensitive, analysis speed is fast, cost is low because it has, can carry out the on-line continuous monitoring in complex system, demonstrates wide application prospect in fields such as biology, medical science, environmental monitoring, food, medicine and military medicines.
Enzyme electrode refers to that electrode sensitive film surface coverage has one deck to contain the gel of enzyme or a class biology sensor of suspending liquid.During measurement, the test substance in the sample spreads in film, reacts under the catalytic action of enzyme, and product is responded by ion electrode, by measuring corresponding electric current or current potential, can obtain the concentration of determinand in the sample.Enzyme electrode with the advantages such as the selectivity of enzyme reaction and sensitivity and electrochemical reaction easy and simple to handle, measuring speed is fast etc., and advantage combines, a kind of analyzing and testing means of competitive superiority have been formed, thereby in Biochemical Research, the aspects such as biological monitoring can play an important role.
Glucose oxidase electrode is the earliest the biology sensor of coming out, and the enzyme electrode take it as representative also is the study hotspot of field of biosensors.But compare with the temperature of laboratory study, the practical process of glucose oxidase electrode is quite slow, and sensing range is generally too small, and antijamming capability is relatively poor, serviceable life shorter grade these all so that its in the application of clinical detection, be restricted.
Summary of the invention
Goal of the invention: first purpose of the present invention provides a kind of preparation method based on the glucose oxidase electrode film.Second purpose of the present invention provides above-mentioned glucose oxidase electrode film.With the assembly of kind electrode film as glucose sensor, can improve the usability of sensor, be applied to the biomedical sectors such as medicine equipment and clinical detection.
Technical scheme: in order to address the above problem, technical scheme of the present invention provides a kind of preparation method based on the glucose oxidase electrode film, may further comprise the steps 1～3 or step 1～4:
1) cellulose acetate is dissolved in the mixed liquor of cyclohexanone that volume ratio is 1:1 and acetone, obtain 1%～5% colourless cellulose acetate film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get one deck cellulose acetate film;
2) preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 20～60mg/ml glucose oxidase (GOD) and 20～50mg/ml trehalose solution;
3) with step 2) solution of preparation is added drop-wise to the cellulose acetate film surface that step 1) makes and obtains the individual layer glucose oxidase film, and the ground floor polycarbonate membrane is fitted on the individual layer glucose oxidase film, redundant solution is extruded, namely got double-deck glucose oxidase film after drying;
The potpourri that 4) will contain 50～120mg/ml bovine serum albumin(BSA) and 0.2～0.5% glutaraldehyde drops to the double-deck glucose oxidase film that obtains on the ground floor polycarbonate membrane of the double-deck glucose oxidase film that step 3) makes with potpourri, be fitted on the double-deck glucose oxidase film with potpourri with second layer polycarbonate membrane, and redundant solution extruded, namely get three layers of glucose oxidase electrode film after drying.
Cellulose acetate film thickness in the described step 1) is 2～10 μ m.
The aperture of ground floor polycarbonate membrane is that 15～50nm, thickness are 2～20 μ m in the described step 3).
The aperture of second layer polycarbonate membrane is that 50～100nm, thickness are 4～10 μ m in the described step 4).
By the glucose oxidase electrode film that described preparation method obtains, described glucose oxidase electrode film is double-deck enzyme electrode film or three layers of enzyme electrode film.
Described double-deck enzyme electrode film comprises cellulose acetate film and ground floor polycarbonate membrane, wherein, and cellulose acetate film and the attached glucose oxidase layer of ground floor polycarbonate membrane therebetween.
Described three layers of enzyme electrode film comprise cellulose acetate film, ground floor polycarbonate membrane and second layer polycarbonate membrane, wherein, cellulose acetate film and the attached glucose oxidase layer of ground floor polycarbonate membrane therebetween, the attached bovine serum albumin(BSA) of ground floor polycarbonate membrane and second layer polycarbonate membrane therebetween/glutaraldehyde layer.
Beneficial effect: the present invention since polycarbonate (PC) film that adopts suitable aperture as diffusion restricting membrane, reduced the rate of propagation of glucose molecule, and oxygen can pass through fully, make the diffusion process of glucose molecule become the control procedure of whole reaction, concentration of glucose in the enzyme membrane remains in the lower concentration range, the oxygen capacity can make the glucose of low concentration in the enzyme membrane fully oxidized simultaneously, reaches to enlarge the glucose electrode sensing range and improve linear purpose; Simultaneously, because the physical barrier of adventitia polycarbonate (PC) film and inner membrance cellulose acetate (CA) film, therefore can effectively stop the reductibility electroactive material in the sample to arrive electrode surface generation oxidation reaction, thus the antijamming capability of electrode increased; Moreover, because the aperture of adventitia polycarbonate (PC) film is less, can also effectively prevent the macromolecular leakage of glucose oxidase, prolong the serviceable life of electrode.
Description of drawings
Fig. 1 is the structural representation of the embodiment of the invention 1.
Fig. 2 is the structural representation of the embodiment of the invention 2.
Embodiment
Below in conjunction with accompanying drawing the present invention is further described.
A kind of preparation method based on the glucose oxidase electrode film, the first step, cellulose acetate (CA) is dissolved in cyclohexanone and the acetone volume ratio is in the mixed liquor of 1:1, obtain 1% colourless CA film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get the CA film 1 that a layer thickness is 2 μ m; Second step, preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 20mg/ml glucose oxidase (GOD) and 20mg/ml trehalose solution; The 3rd step, the solution of second step preparation is added drop-wise to CA film 1 surface that the first step makes obtains the individual layer glucose oxidase film, and ground floor polycarbonate (PC) film 3 of aperture 15nm, thickness 10 μ m is fitted on the individual layer glucose oxidase film, redundant solution is extruded, namely got double-deck glucose oxidase film after drying.
Such as Fig. 1, the glucose oxidase electrode film that is made by above-mentioned preparation method is double-deck enzyme electrode film, described double-deck enzyme electrode film comprises cellulose acetate film 1 and ground floor polycarbonate membrane 3, wherein, and the attached glucose oxidase layer 2 of cellulose acetate film 1 and ground floor polycarbonate membrane 3 therebetween.
In Fig. 1, when the glucose molecule in the sample is flowed through electrode channel, directly pass glucose oxidase (GOD) reaction in ground floor polycarbonate membrane 3 and the glucose oxidase layer 2, the inner membrance that the hydrogen peroxide that generates continues across cellulose acetate film 1 arrives Pt electrode 4 surfaces that are among the electrolyte solution 6 redox reactions occurs, produce electric signal, AgCl/Ag electrode 5 is as the negative electrode of reaction.The size of concentration of glucose is proportionate in the power of the electric signal that produces and the sample, thereby can calculate the concentration of glucose in the sample.
Embodiment 2:
A kind of preparation method based on the glucose oxidase electrode film, the first step, cellulose acetate (CA) is dissolved in cyclohexanone and the acetone volume ratio is in the mixed liquor of 1:1, obtain 5% colourless CA film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get the cellulose acetate film 1 that a layer thickness is 10 μ m; Second step, preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 60mg/ml glucose oxidase (GOD) and 50mg/ml trehalose solution; The 3rd step, the solution that second step is prepared is added drop-wise to cellulose acetate film 1 surface that makes and obtains the individual layer glucose oxidase film, and ground floor polycarbonate (PC) film 3 of aperture 50nm, thickness 10 μ m is fitted on the individual layer glucose oxidase film, redundant solution is extruded, the middle one deck glucose oxidase layer 2 that forms namely gets double-deck glucose oxidase film after drying; The ground floor PC film 3 that the potpourri that will contain 120mg/ml bovine serum albumin(BSA) (BSA) and 0.5% glutaraldehyde drops to the double-deck enzyme membrane that makes obtains the double-deck glucose oxidase film with potpourri, be fitted on the double-deck glucose oxidase film with potpourri with the second layer PC film 8 of aperture 100nm, thickness 10 μ m, and redundant solution extruded, a middle formation skim is bovine serum albumin(BSA)/glutaraldehyde layer 7, namely gets three layers of glucose oxidase electrode film after drying.
Such as Fig. 2, the glucose oxidase electrode film that is made by above-mentioned preparation method is three layers of enzyme electrode film, described three layers of enzyme electrode film comprise cellulose acetate film 1, ground floor polycarbonate membrane 3 and second layer polycarbonate membrane 8, wherein, the attached glucose oxidase layer 2 of cellulose acetate film 1 and ground floor polycarbonate membrane 3 therebetween, the attached bovine serum albumin(BSA) of ground floor polycarbonate membrane 3 and second layer polycarbonate membrane 8 therebetween/glutaraldehyde layer 7.
Such as Fig. 2, when the glucose molecule in the sample is flowed through electrode channel, pass first outermost second layer PC film 8 and BSA/ glutaraldehyde layer 7 arrival ground floor PC film 3, pass again glucose oxidase (GOD) reaction in ground floor PC film 3 and the glucose oxidase layer 2, the inner membrance that the hydrogen peroxide that generates continues across cellulose acetate (CA) film 1 arrives Pt electrode 4 surfaces that are among the electrolyte solution 6 redox reactions occurs, produce electric signal, AgCl/Ag electrode 5 is as the negative electrode of reaction.The size of concentration of glucose is proportionate in the power of the electric signal that produces and the sample, thereby can calculate the concentration of glucose in the sample.
A kind of preparation method based on the glucose oxidase electrode film, cellulose acetate (CA) is dissolved in cyclohexanone and the acetone volume ratio is in the mixed liquor of 1:1, obtain 3% colourless CA film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get the cellulose acetate film 1 that a layer thickness is 6 μ m; Preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 40mg/ml glucose oxidase (GOD) and 35mg/ml trehalose solution; The solution for preparing is added drop-wise to cellulose acetate film 1 surface that makes, and aperture 40nm, thickness 6 μ m polycarbonate (PC) films are fitted on the solution form ground floor PC film 3, redundant solution is extruded, the middle one deck glucose oxidase layer 2 that forms namely gets double-deck glucose oxidase film after drying; The ground floor PC film 3 that the potpourri that will contain 85mg/ml bovine serum albumin(BSA) (BSA) and 0.75% glutaraldehyde drops to the double-deck enzyme membrane that makes obtains the double-deck glucose oxidase film with potpourri, on the double-deck glucose oxidase film that is fitted in potpourri with aperture 75nm, thickness 7 μ m second layer PC films 8, and redundant solution extruded, a middle formation skim is bovine serum albumin(BSA)/glutaraldehyde layer 7, namely gets three layers of glucose oxidase electrode film after drying.
A kind of preparation method based on the glucose oxidase electrode film, cellulose acetate (CA) is dissolved in cyclohexanone and the acetone volume ratio is in the mixed liquor of 1:1, obtain 1%～5% colourless CA film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get the cellulose acetate that a layer thickness is 2 μ m (CA) film 1; Preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 20mg/ml glucose oxidase (GOD) and 20mg/ml trehalose solution; The solution for preparing is added drop-wise to cellulose acetate film 1 surface that makes, and aperture 30nm, thickness 2 μ m ground floor polycarbonate (PC) films 3 are fitted on the solution, redundant solution is extruded, and the middle one deck glucose oxidase layer 2 that forms namely gets double-deck glucose oxidase film after drying; The potpourri that will contain 50mg/ml bovine serum albumin(BSA) (BSA) and 0.1% glutaraldehyde drops to the double-deck glucose oxidase film that obtains on ground floor polycarbonate (PC) film 3 of the double-deck enzyme membrane that makes with potpourri, on the double-deck glucose oxidase film that is fitted in potpourri with aperture 50nm, thickness 4 μ m second layer PC films 8, and redundant solution extruded, a middle formation skim is bovine serum albumin(BSA)/glutaraldehyde layer 7, namely gets three layers of glucose oxidase electrode film after drying.
A kind of preparation method based on the glucose oxidase electrode film, cellulose acetate (CA) is dissolved in cyclohexanone and the acetone volume ratio is in the mixed liquor of 1:1, obtain 5% colourless CA film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get the cellulose acetate film 1 that a layer thickness is 10 μ m; Preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 60mg/ml glucose oxidase (GOD) and 50mg/ml trehalose solution; The solution for preparing is added drop-wise to cellulose acetate film 1 surface that makes, and aperture 50nm, thickness 10 μ m ground floor polycarbonate (PC) films 3 are fitted on the solution, redundant solution is extruded, and the middle one deck glucose oxidase layer 2 that forms namely gets double-deck glucose oxidase film after drying; The potpourri that will contain 85mg/ml bovine serum albumin(BSA) (BSA) and 0.5% glutaraldehyde drops to the double-deck glucose oxidase film that obtains on ground floor polycarbonate (PC) film 3 of the double-deck enzyme membrane that makes with potpourri, on the double-deck glucose oxidase film that is fitted in potpourri with aperture 75nm, thickness 7 μ m second layer PC films 8, and redundant solution extruded, a middle formation skim is bovine serum albumin(BSA)/glutaraldehyde layer 7, namely gets three layers of glucose oxidase electrode film after drying.
The above only is preferred implementation of the present invention; be noted that for those skilled in the art; under the prerequisite that does not break away from the principle of the invention, can also make some improvements and modifications, these improvements and modifications also should be considered as protection scope of the present invention.
Claims (7)
1. the preparation method based on the glucose oxidase electrode film is characterized in that, may further comprise the steps 1～3 or step 1～4:
1) cellulose acetate is dissolved in the mixed liquor of cyclohexanone that volume ratio is 1:1 and acetone, obtain 1%～5% colourless cellulose acetate film forming liquid, and the film forming liquid that obtains evenly is tiled in the glass plate surface, treat in air, to dry and namely get one deck cellulose acetate film;
2) preparation contains 60mmol/L succinic acid, 0.2mmol/L EDTANa
2, 1.5% glutaraldehyde, 20～60mg/ml glucose oxidase (GOD) and 20～50mg/ml trehalose solution;
3) with step 2) solution of preparation is added drop-wise to the cellulose acetate film surface that step 1) makes and obtains the individual layer glucose oxidase film, and the ground floor polycarbonate membrane is fitted on the individual layer glucose oxidase film, redundant solution is extruded, namely got double-deck glucose oxidase electrode film after drying;
The potpourri that 4) will contain 50～120mg/ml bovine serum albumin(BSA) and 0.2～0.5% glutaraldehyde drops to the double-deck glucose oxidase film that obtains on the ground floor polycarbonate membrane of the double-deck glucose oxidase film that step 3) makes with potpourri, be fitted on the double-deck glucose oxidase film with potpourri with second layer polycarbonate membrane, and redundant solution extruded, namely get three layers of glucose oxidase electrode film after drying.
2. the preparation method based on the glucose oxidase electrode film according to claim 1 is characterized in that, the cellulose acetate film thickness in the described step 1) is 2～10 μ m.
3. the preparation method based on the glucose oxidase electrode film according to claim 1 is characterized in that, the aperture of ground floor polycarbonate membrane is that 15～50nm, thickness are 2～20 μ m in the described step 3).
4. the preparation method based on the glucose oxidase electrode film according to claim 1 is characterized in that, the aperture of second layer polycarbonate membrane is that 50～100nm, thickness are 4～10 μ m in the described step 4).
5. the glucose oxidase electrode film that is obtained by each described preparation method of claim 1～4 is characterized in that, described glucose oxidase electrode film is double-deck glucose oxidase electrode film or three layers of glucose oxidase electrode film.
6. glucose oxidase electrode film according to claim 5, it is characterized in that, described double-deck glucose oxidase electrode film comprises cellulose acetate film and ground floor polycarbonate membrane, wherein, and cellulose acetate film and the attached glucose oxidase layer of ground floor polycarbonate membrane therebetween.
7. glucose oxidase electrode film according to claim 5, it is characterized in that, described three layers of glucose oxidase electrode film comprise cellulose acetate film, ground floor polycarbonate membrane and second layer polycarbonate membrane, wherein, cellulose acetate film and the attached glucose oxidase layer of ground floor polycarbonate membrane therebetween, the attached bovine serum albumin(BSA) of ground floor polycarbonate membrane and second layer polycarbonate membrane therebetween/glutaraldehyde layer.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104198556A (en) * | 2014-08-11 | 2014-12-10 | 南京普朗医疗设备有限公司 | Preparation method of electrode membrane based on lactate oxidase and product prepared by the method |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4759828A (en) * | 1987-04-09 | 1988-07-26 | Nova Biomedical Corporation | Glucose electrode and method of determining glucose |
| US5352348A (en) * | 1987-04-09 | 1994-10-04 | Nova Biomedical Corporation | Method of using enzyme electrode |
| CN102712946A (en) * | 2009-10-30 | 2012-10-03 | 爱德华兹生命科学公司 | Sensor layers and methods related thereto |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4759828A (en) * | 1987-04-09 | 1988-07-26 | Nova Biomedical Corporation | Glucose electrode and method of determining glucose |
| US5352348A (en) * | 1987-04-09 | 1994-10-04 | Nova Biomedical Corporation | Method of using enzyme electrode |
| CN102712946A (en) * | 2009-10-30 | 2012-10-03 | 爱德华兹生命科学公司 | Sensor layers and methods related thereto |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104198556A (en) * | 2014-08-11 | 2014-12-10 | 南京普朗医疗设备有限公司 | Preparation method of electrode membrane based on lactate oxidase and product prepared by the method |
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Application publication date: 20130925 |