CN101246175A - Silk screen printing method for producing blood sugar test paper - Google Patents
Silk screen printing method for producing blood sugar test paper Download PDFInfo
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- CN101246175A CN101246175A CNA200710037552XA CN200710037552A CN101246175A CN 101246175 A CN101246175 A CN 101246175A CN A200710037552X A CNA200710037552X A CN A200710037552XA CN 200710037552 A CN200710037552 A CN 200710037552A CN 101246175 A CN101246175 A CN 101246175A
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Abstract
The invention provides a blood glucose testing instrument and the producing method thereof, which belongs to the field of bio-sensor technology. The substrate of the testing paper is printed with working electrode, reference electrode and electrical circuit which are formed by carbon-coating, one end of the substrate is printed with wire connected with readout instrument, the working electrode and reference electrode are respectively printed on carbon-coating above substrate conductive silver layer, the working electrode is also printed with enzyme, medium and adhesive. According to bio-sensor and electrochemical principle, the testing paper is made through silk-screen process, not only conductive circuit is printed, but also sensitive bio-element is directly printed on electrode supporter, the print amount of the print material and print area are totally and exactly controlled by computer. Once the testing paper contacts human body fluid, the testing result can be easily and directly read out on corresponding matching instrument, the producing method is easy, and has high precision, low cost, which is convenient for later process and encapsulation, and is good for large-scale production.
Description
Technical field
What the present invention relates to is a kind of test paper and serigraphy method for making thereof, and particularly a kind of and supporting test paper and the serigraphy method for making thereof of blood glucose monitoring system belongs to the biosensor technique field.
Background technology
China's diabetic has surpassed 4,500 ten thousand according to statistics, annually also increases with 1.5% speed of development.One of effective means of control of diabetes development is to implement blood sugar test every day to reach strict control medication and diet, keeps the stable of patient's glycemic index.Its supporting test paper of some blood glucose meter of Chu Xianing adopts general silk-screen technology in the market, this blood sugar test paper manufacture craft simple coarse, after basic electrode is printed and is finished, also need the point sample processing of biomaterial, yield poorly, production cost and rejection rate are all higher, can only reach pilot-scale production, are difficult to carry out heavy industrialization and produce continuously.Find by literature search, U.S. Patent Publication No. is: 2004/0146958, patent name is: Glucose strip sensor and glucose measurement using the glucose stripsensor (utilizing glucose strip sensor determination glucose), introduced a kind of method for making of three-electrode system glucose strip sensor in this patent, include a working electrode in the test macro, a reference electrode also has a verification electrode, its objective is to make system measure tested glucose more accurately.Thereby also having introduced employing control reaction zone space, system make the reaction mixture volume in the reaction chamber obtain the methods such as accuracy that strict control raising is measured.But this method is except adopting multilayer silk-screen technology, also needs to use biological elements point sample equipment with the surface of biology enzyme solution coat to electrode, causes complex manufacturing technologyization, is unfavorable for the industrial-scale production of product.
Summary of the invention
The objective of the invention is to overcome deficiency of the prior art; the method for making of a kind of blood sugar test paper and serigraphy thereof is provided; after making this test paper in a single day contact blood of human body; can above corresponding blood sugar test instrument, just read test result intuitively; its method for making is simple; make things convenient for post-production and encapsulation, help large-scale production.
The present invention is achieved by the following technical solutions, and test paper of the present invention comprises: a substrate, as the PP substrate; Be printed on a working electrode on the substrate; Be printed on a reference electrode on the substrate; Two electrodes constitute electric loop with the continuous blood sugar test of finishing of testing tool; End at substrate is printed on the lead that connects with the readout meter epiphase.The composite print carbon coating constitutes on the substrate conductive silver layer by being imprinted on respectively for working electrode and reference electrode, stamp one deck on the working electrode again and contain the biology enzyme that the catalysis blood-glucose reacts, as glucose oxidase, and a kind of conducting medium and binder that can between enzymic catalytic reaction center and electrode, carry out electron transport, so constitute a circuit loop.According to the height of concentration of glucose in the blood, produce the current signal of corresponding size during reaction, and the detection of tested instrument is read.This test paper has omitted biological elements point sample equipment, and technology is simpler.Tested material can be lactic acid, cholesterol or glucose, and the enzyme of use can be Lactate Oxidase, cholesterol oxidase and glucose oxidase.
Working electrode is the double-deck conductive film of a kind of serigraphy on holder, comprises the enzyme of catalysis biochemical reaction and the conducting medium and the binder that can carry out electron transport between enzymic catalytic reaction is with electrode republishing one deck on the conductive film.This working electrode can transmit the electric current that produces behind the enzymic catalytic reaction.Working electrode and contrast electrode are close, and two electrodes constitute an effecting reaction zone, after connecting with tester, form effective body fluid components test macro.
The present invention adopts bio-sensing and electrochemical principle, make above-mentioned test paper by pure silk reticulated printing technology, the conducting wire is not only printed in serigraphy, also will compare responsive biological elements such as enzyme, conducting medium and binder etc. and be imprinted on the electrode surface by specific process.
Below the inventive method is further described, concrete steps are as follows:
(1) carboxymethyl cellulose of adding 1.2-2.5% in the silk-screen conductive carbon ink, the electronic conduction carrier material of adding 10-20%, as the benzoquinones or the potassium ferricyanide, mixing is standby;
(2) metal of 200-400 order number or nylon polyester material silk screen are fixed on square aluminum metal frame and add, in the darkroom, coat Kodak's photoresists, drying for standby;
(3) working electrode and the reference electrode negative film with computer drawing places on the photoresists, and under 20-40 watt of uviol lamp exposure 15-30 minute, remove the unhardened photoresists that covered by the electrode negative film with the giant flushing, dry back forms the silk-screen template;
(4) the silk-screen template that will have working electrode and a reference electrode figure is installed on the automatic screen printer standby;
(5) be the Lactate Oxidase of 35-60 international unit with activity or active be the glucose oxidase of 200-350 international unit for the cholesterol oxidase of 20-50 international unit or activity, the citric acid of allocating every liter of 60-100 mM into is in liquid, add every liter of 2000-8000 milligram of the benzoquinones or the potassium ferricyanide simultaneously, it is standby to shelve 4 ℃ of refrigerators behind the abundant mixing such as binder such as carboxymethyl cellulose.
Working electrode adopts screen process press that conductive silver ink and conductive carbon ink are imprinted on the substrate earlier; Print enzyme and conducting medium such as benzoquinones or the potassium ferricyanide and binder etc. then, reference electrode is also made with identical method.
The biology enzyme China ink that is used for printing comprises: bonding agent, conducting objects and enzyme.The material of substrate can be a kind of good toughness, the polymeric material that insulativity is high, and such as Polyvinylchloride, polyester or polycarbonate.
The present invention has substantive distinguishing features and marked improvement, and the inventive method has expanded to screen printing technique the printing of biological elements enzyme.Reduce production technology and made requirement; Simplified production equipment; Improved the industrialization level of product.Wire printing material and screen printing device needn't specially be processed, and can obtain by commercially available channel, and cost is very low; Relatively more responsive biological elements such as enzyme, conducting medium and binder etc. are imprinted on the electrode support substrate with screen printing mode, the precision of final products and repeatability are fully ensured.After in a single day test paper of the present invention contacts human body fluid, can conveniently on corresponding supporting testing tool read test result intuitively, method for making is simple, the precision height, and cost is low, makes things convenient for post-production and encapsulation, helps large-scale industrial production.
Description of drawings
Fig. 1 test paper structural representation of the present invention
Embodiment
As shown in Figure 1, test paper of the present invention comprises: a substrate 1, be printed on silver coating lead 2 on the substrate 1, be printed on carbon coating 3 on the substrate 1, end on the substrate 1 is printed on the lead 4 that connects with the readout meter epiphase, be printed on insulating coating 5 on the working electrode of carbon coating and the reference electrode 3, also be printed on enzyme coating 6 on the working electrode of carbon coating and the reference electrode 3, this kind of enzyme be can the catalysis blood-glucose biology enzyme of reaction, as glucose oxidase, and a kind of medium and binder that can between enzymic catalytic reaction center and electrode, carry out electron transport, so constitute a circuit loop, according to the height of concentration of glucose in the blood, produce the current signal of corresponding size during reaction, and the detection of tested instrument is read.Tested material can be lactic acid, cholesterol or glucose, and the enzyme of use can be Lactate Oxidase, cholesterol oxidase and glucose oxidase.On the enzyme coating, also be covered with double faced adhesive tape 7 and hydrophilic film 8, be convenient to blood of human body and enter reaction zone with siphon mode easily.
Content in conjunction with the inventive method provides following examples, and the present invention is further illustrated.
Embodiment 1: tygon (PVC) sheet material, it is standby to be cut into 21 * 9 centimeters substrates in advance.
(1) hydroxyethyl cellulose of adding 1.2% in 1 gram silk-screen conductive carbon ink (ACHESON Acheson423SS), the electronic conduction carrier material benzoquinones of adding 10%, mixing is standby.
(2) metal of 280 order numbers or nylon polyester material silk screen are fixed on square light-weight metal frame and add, in the darkroom, coat Kodak's photoresists, drying for standby.
(3) working electrode and the reference electrode negative film with computer drawing places on the photoresists, and exposure is 15 minutes under 20 watts of uviol lamps.Remove the unhardened photoresists that covered by the electrode negative film with giant flushing.Dry back forms the silk-screen template.
(4) the silk-screen template that will have working electrode and a reference electrode figure is installed on (moral gram DEK-245) type automatic screen printer standby.
(5) be that the Lactate Oxidase of 10 international units is allocated in the citrate buffer solution of every liter of 50 mM with activity, add 200 milligrams every liter of benzoquinones simultaneously, binder etc.It is standby fully to shelve 4 ℃ of refrigerators behind the mixing.
On above-mentioned automatic screen printing machine, add conductive silver ink (ACHESON Acheson 427SS) and carry out print conductive circuits; Dry back adds above-mentioned hybrid conductive silk-screen carbon ink on automatic screen printing machine, the silver-colored line of ink marker road of before having printed is covered, and makes working electrode and reference electrode respectively.The electrode of having printed need be held in 80 ℃ of baking ovens and solidify 20 minutes, forms 50 pairs of work and reference electrode on each sheet PVC substrate, takes out standby then.Making can be tested lactic acid, during the enzyme test peper of cholesterol and glucose, takes out Manufactured element task electrode and reference electrode, will the mixed liquor in above-mentioned (5) adds on the automatic screen printing machine to print.
After above-mentioned silk-screen enzyme electrode was made drying, an about 10mm is wide, and long double faced adhesive tape and the hydrophilic film complex of 220mm covered on the reaction zone heat drying.The electrode slice that prints cools off after 3 hours at heat drying.It is long with shearer dried test pieces to be cut into 30mm, the test-strips finished product that 0.8mm is wide.
With Manufactured test-strips, place tester and apply the 350mV operating voltage for two sections at working electrode and reference electrode, measure the lactic acid of variable concentrations, the result shows that reaction took place after 10 seconds, shows to make good test repeatability and the correlativity of electrode.Through relatively with Biochemical Analyzer, get 50 parts of lactic acid control liquids and 50 parts of patient's blood sample lactic acid contrast tests respectively, the relative standard deviation that its correlativity γ reaches 0.9567 test-strips is CV≤6.5%.
Embodiment 2: polyester (PET) sheet material, it is standby to be cut into 21 * 9 centimeters substrates in advance.
(1) hydroxyethyl cellulose of adding 1.8% in silk-screen conductive carbon ink (ACHESON Acheson423 SS), the electronic conduction carrier material benzoquinones of adding 15%.It is standby to shelve 4 ℃ of refrigerators behind the mixing.
(2) metal of 300 order numbers or nylon polyester material silk screen are fixed on square light-weight metal frame and add, in the darkroom, coat Kodak's photoresists, drying for standby.
(3) working electrode and the reference electrode negative film with computer drawing places on the photoresists, and exposure is 25 minutes under 20 watts of uviol lamps.Remove the unhardened photoresists that covered by the electrode negative film with giant flushing.Dry back forms the silk-screen template.
(4) the silk-screen template that will have working electrode and a reference electrode figure is installed on (moral gram DEK-245) type automatic screen printer standby.
(5) be that the cholesterol oxidase of 25 international units is allocated in the phosphate buffer of every liter of 50 mM with activity, add 800 milligrams every liter of benzoquinones simultaneously, binder etc.It is standby fully to shelve 4 ℃ of refrigerators after the dissolving.
The silk-screen method for making is with example 1, with the test-strips of making, place tester and apply the 300mV operating voltage for two sections at working electrode and reference electrode, measure the cholesterol of variable concentrations respectively, the result shows that reaction took place after 20 seconds, shows to make good test repeatability and the correlativity of electrode.Through relatively with Biochemical Analyzer, get 30 parts of cholesterol control liquids and 20 parts of patient's blood sample cholesterol contrast tests, its correlativity γ reaches 0.967, and the relative standard deviation of test-strips is CV≤5.7%.
Embodiment 3: polyphenol ester (PP) sheet material, it is standby to be cut into 21 * 9 centimeters substrates in advance.
(1) hydroxyethyl cellulose of adding 2.5% in the silk-screen conductive carbon ink, the electronic conduction carrier material potassium ferricyanide of adding 20%, mixing is standby;
(2) metal of 350 order numbers or nylon polyester material silk screen are fixed on square light-weight metal frame and add, in the darkroom, coat Kodak's photoresists, drying for standby;
(3) working electrode and the reference electrode negative film with computer drawing places on the photoresists, and exposure is 30 minutes under 40 watts of uviol lamps, removes the unhardened photoresists that covered by the electrode negative film with giant flushing, and dry back forms the silk-screen template;
(4) the silk-screen template that will have working electrode and a reference electrode figure is installed on the automatic screen printer standby;
(5) be that the glucose oxidase of 300 international units is allocated in the citrate buffer solution of every liter of 120 mM with activity, add 600 milligrams every liter of the potassium ferricyanides simultaneously, binder etc.It is standby fully to shelve 4 ℃ of refrigerators behind the mixing.
The silk-screen method for making is with embodiment 1, with the test-strips of making, place tester and apply the 400mV operating voltage for two sections at working electrode and reference electrode, measure the glucose of variable concentrations respectively, the result shows that reaction took place after 15 seconds, shows to make good test repeatability and the correlativity of electrode.Through relatively with hospital's Biochemical Analyzer, get 50 parts of glucose control liquids and 50 parts of diabetes patient's blood sample glucose contrast tests respectively, its correlativity γ reaches 0.97, and the relative standard deviation of test-strips is CV≤6.8%.
Claims (9)
1. supporting test paper of blood glucose monitoring system, mainly comprise: a substrate (1), be printed on a kind of silver coating (2) on the substrate (1), be printed on a kind of carbon coating (3) on the substrate (1), end at substrate (1) is printed on the lead (4) that connects with the readout meter epiphase, it is characterized in that, working electrode (3) and reference electrode (3) are respectively to be imprinted on the carbon coating that forms on substrate (1) conductive silver layer, be printed on the biology enzyme 6 of catalysis blood-glucose reaction on the working electrode (3), and a kind of medium and binder that can between enzymic catalytic reaction center and electrode, carry out electron transport, be covered with double faced adhesive tape 7 and hydrophilic film 8, so constitute a circuit loop, according to the height of concentration of glucose in the blood, produce the current signal of corresponding size during reaction, and the detection of tested instrument is read.
2. human body fluid test paper according to claim 1 is characterized in that, tested material can be lactic acid, cholesterol or glucose, and the enzyme of use can be Lactate Oxidase, cholesterol oxidase and glucose oxidase.
3. blood sugar test paper according to claim 1, it is characterized in that, working electrode (3) is the multilayer conductive film (6) of a kind of serigraphy on holder, has printed enzyme that comprises the catalysis biochemical reaction and the medium that can carry out electron transport between enzymic catalytic reaction is with electrode in conductive film (6).
4. the supporting test paper of blood glucose monitoring system according to claim 1 is characterized in that, working electrode (3) is close with contrast electrode (3), and two electrodes constitute an effecting reaction zone, after connecting with tester, forms effective body fluid components test macro.
5. the supporting test paper of blood glucose monitoring system according to claim 1 is characterized in that, the polymeric material that the material of substrate is a kind of good toughness, insulativity is high, as: Polyvinylchloride, polyester or polycarbonate.
6. the method for making of a blood sugar test paper, it is characterized in that: adopt bio-sensing and electrochemical principle, make above-mentioned test paper by the screen printing technique method, serigraphy is not limited to print the conducting wire, also will compare responsive biological elements and directly be printed on the electrode support substrate, the amount and the area of printing material are accurately controlled by computer fully.
7. the method for making of blood sugar test paper according to claim 6, its concrete steps are as follows:
(1) hydroxyethyl cellulose of adding 1.2-2.5% in the silk-screen conductive carbon ink, the electronic conduction carrier material of adding 10-20%, as the benzoquinones or the potassium ferricyanide, mixing is standby;
(2) metal of 200-400 order number or nylon polyester material silk screen are fixed on square light-weight metal frame and add, in the darkroom, coat Kodak's photoresists, drying for standby;
(3) working electrode and the reference electrode negative film with computer drawing places on the photoresists, and under 20-40 watt of uviol lamp exposure 15-30 minute, remove the unhardened photoresists that covered by the electrode negative film with the giant flushing, dry back forms the silk-screen template;
(4) the silk-screen template that will have working electrode and a reference electrode figure is installed on the automatic screen printer standby;
(5) be the Lactate Oxidase of 10-30 international unit with activity or active be the glucose oxidase of 200-500 international unit for the cholesterol oxidase of 12-25 international unit or activity, allocate in the citrate buffer solution of every liter of 50-120 mM, add every liter of 200-800 milligram of the benzoquinones or the potassium ferricyanide simultaneously, it is standby to shelve 4 ℃ of refrigerators behind the abundant mixing such as binder.
8. according to the method for making of claim 6 or 7 described blood sugar test papers, it is characterized in that working electrode adopts screen printing technique that conductive silver ink and conductive carbon ink are imprinted on the substrate earlier; Print enzyme and electron transit mediator then, as benzoquinones or the potassium ferricyanide and binder, reference electrode is made with identical method.
9. according to the method for making of claim 6 and 7 described blood sugar test papers, it is characterized in that the printing ink that is used for the silk screen brush comprises: bonding agent, conducting objects and enzyme.
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| CNA200710037552XA CN101246175A (en) | 2007-02-14 | 2007-02-14 | Silk screen printing method for producing blood sugar test paper |
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Cited By (9)
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| CN103149255A (en) * | 2013-02-25 | 2013-06-12 | 长沙理工大学 | Method for quickly determining lead content in blood |
| CN103235015A (en) * | 2012-10-24 | 2013-08-07 | 长沙理工大学 | Dry chemical test strip used in quantitative test of uric acid |
| CN103525695A (en) * | 2012-07-04 | 2014-01-22 | 长沙中生众捷生物技术有限公司 | Portable kidney function detecting system |
| CN104569063A (en) * | 2015-02-02 | 2015-04-29 | 周佩龙 | Blood glucose test strip |
| CN104931549A (en) * | 2014-03-19 | 2015-09-23 | 深圳市艾瑞生物科技有限公司 | Electrochemical test paper for quantitatively measuring homocysteine and preparation method thereof |
| CN105738432A (en) * | 2016-01-27 | 2016-07-06 | 杭州瑞健科技有限公司 | Hydrophilic film having stable and reliable performances and used for blood glucose test paper |
| CN106546643A (en) * | 2015-09-23 | 2017-03-29 | 香港生产力促进局 | High-sensitivity biological sensor prepared by nano-particle technology and preparation method thereof |
| CN106680347A (en) * | 2017-02-16 | 2017-05-17 | 常州鹤田生物技术有限公司 | Finger blood test strip and use method and preparation method thereof |
| US10399851B2 (en) | 2014-09-30 | 2019-09-03 | 3M Innovative Properties Company | Electrically conductive patterns with wide line-width and methods for producing same |
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- 2007-02-14 CN CNA200710037552XA patent/CN101246175A/en active Pending
Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103525695A (en) * | 2012-07-04 | 2014-01-22 | 长沙中生众捷生物技术有限公司 | Portable kidney function detecting system |
| CN103525695B (en) * | 2012-07-04 | 2015-05-20 | 长沙中生众捷生物技术有限公司 | Portable kidney function detecting system |
| CN103235015A (en) * | 2012-10-24 | 2013-08-07 | 长沙理工大学 | Dry chemical test strip used in quantitative test of uric acid |
| CN103149255A (en) * | 2013-02-25 | 2013-06-12 | 长沙理工大学 | Method for quickly determining lead content in blood |
| CN104931549A (en) * | 2014-03-19 | 2015-09-23 | 深圳市艾瑞生物科技有限公司 | Electrochemical test paper for quantitatively measuring homocysteine and preparation method thereof |
| US10399851B2 (en) | 2014-09-30 | 2019-09-03 | 3M Innovative Properties Company | Electrically conductive patterns with wide line-width and methods for producing same |
| CN104569063A (en) * | 2015-02-02 | 2015-04-29 | 周佩龙 | Blood glucose test strip |
| CN106546643A (en) * | 2015-09-23 | 2017-03-29 | 香港生产力促进局 | High-sensitivity biological sensor prepared by nano-particle technology and preparation method thereof |
| CN105738432A (en) * | 2016-01-27 | 2016-07-06 | 杭州瑞健科技有限公司 | Hydrophilic film having stable and reliable performances and used for blood glucose test paper |
| CN105738432B (en) * | 2016-01-27 | 2018-05-11 | 杭州瑞健科技有限公司 | Blood sugar test paper hydrophilic film stable and reliable for performance |
| CN106680347A (en) * | 2017-02-16 | 2017-05-17 | 常州鹤田生物技术有限公司 | Finger blood test strip and use method and preparation method thereof |
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Application publication date: 20080820 |