CN105445339A - Flexible differential array electrochemical glucose sensor and use method thereof - Google Patents
Flexible differential array electrochemical glucose sensor and use method thereof Download PDFInfo
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- CN105445339A CN105445339A CN201410378649.7A CN201410378649A CN105445339A CN 105445339 A CN105445339 A CN 105445339A CN 201410378649 A CN201410378649 A CN 201410378649A CN 105445339 A CN105445339 A CN 105445339A
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Abstract
A flexible differential array electrochemical glucose sensor and a use method thereof are disclosed, the sensor comprises seven sensor units which are identical in structure and arranged side by side, each sensor unit comprises a flexible substrate and a first three-electrode monomer and a second three-electrode monomer which are arranged on the flexible substrate, and the first three-electrode monomer and the second three-electrode monomer are identical in structure, and both comprise a reference electrode, an auxiliary electrode and a working electrode. The use method is as follows: one sensor unit is used in one day, seven days of continuous measurement can be achieved, and in the manner of transposition measurement, the skin sensibility phenomenon caused by long time extraction of tissue fluid can be reduced. The flexible differential array electrochemical glucose sensor has small size and high precision advantages, can achieve in-situ measurement, also can achieve the integration of glucose concentrations of transdermal extraction tissue fluid and measurement extraction tissue fluid, solves the problems of adhesion of skin and the sensor in the extraction process and the skin sensibility and the like caused by long time extraction, and eliminates the influence of environmental factors on sensor measurement results.
Description
Technical field
The present invention relates to a kind of glucose sensor.Particularly relate to a kind of flexible differential type array electrochemical glucose sensor and the using method that realize the integration of concentration of glucose in the tissue fluid of tissue fluid transdermal extraction and measurement extraction.
Background technology
Along with the raising of people's living standard, the change of dietary structure and living-pattern preservation, the increase of aging population and fat incidence, the incidence of disease of diabetes is in ascendant trend year by year.Continuous blood sugar monitoring to the significance of diabetes diagnosis and treatment more and more be familiar with by people.If the monitoring of painless and continual continuous blood sugar can be carried out to patient, more close blood sugar concentration continually varying data are provided, just can reflect the blood sugar " overall picture " of patient, measure those uncared-for blood glucose information, disclose hiding blood sugar condition, find the peak value etc. of the hypoglycemic episodes repeatedly of those no conscious symptons, dawn phenomenon and hyperglycaemia, for drafting the glucose-lowering treatment scheme of more adduction reason ﹑ individuation, valuable clinical foundation is provided, thus instructs the treatment of diabetes better.
The quick finger tip blood sampling of the many employings of current blood sugar monitoring detects blood sugar.Due to the restriction of detection method, blood sugar monitoring can only complete at isolated time point, the reflection of its result be the moment blood sugar in certain several moment in one day.But moment, blood sugar concentration was easily by the impact of the factors such as motion, diet, medicine, anxious state of mind, there is certain one-sidedness and inaccuracy.In order to more fully reflect the change of human blood glucose concentration, the continuous detecting of blood sugar concentration just must be realized.The continuous detecting of blood sugar concentration is made to become possibility without wound and Wicresoft's detection technique.Noninvasive dynamics monitoring technology does not need to extract the substance in vivo such as blood, and do not need sensor to implant subcutaneous, relying on the interaction of light and human body privileged site tissue to detect the change of blood sugar concentration in patient body, is optimal blood sugar for human body detection method.Wicresoft's blood sugar concentration detection technique is by being implanted by sensor subcutaneous or measuring concentration of glucose in tissue liquid by the method for tissue fluid transdermal extraction, then obtains the concentration of glucose in blood according to the relation of concentration of glucose in tissue fluid and the concentration of glucose in blood.Wicresoft's blood sugar test technology is reducing on the basis of wound to greatest extent, can realize human blood glucose concentration dynamic, monitor continuously, know-why is relatively simple, has the features such as realizability is strong, easy to use, measuring speed is fast.
Someone invents the continuous monitoring equipment of the blood sugar having made implanted in recent years, subcutaneous by being implanted by glucose sensor, realizes the detection of concentration of glucose in tissue fluid, calculate the concentration of blood sugar at hypodermis.But the use of this equipment has a series of problem, such as, implantable sensor inevitably brings wound to human body, makes human body produce uncomfortable sensation, and the sensor implanted is owing to being use in the coenocorrelation of complexity, As time goes on, can the material such as continuous adsorbed proteins at sensor surface, these materials can hinder sensor to the detection of glucose, make to detect the result obtained to drift about, this constantly adopts the method for blood sampling calibration to correct the testing result of sensor with regard to needing, deepen the misery of detected person, and the absorption of protein can constantly be carried out, until sensor can not work completely, and this process is at most also with regard to several days, which greatly limits the serviceable life of sensor, have impact on the accuracy of detection of sensor.
Present somebody utilizes micro-fluidic chip to realize the transdermal extraction to tissue fluid, then utilizes various method to realize the measurement of the concentration of glucose to the tissue fluid extracted.Although this method also can obtain blood sugar concentration, there is a lot of problem.First it extracts the tissue fluid obtained is be present in skin surface with the form of drop, be difficult to collect, usually need to dilute it with damping fluid, and then measure, this just needs the volume knowing extracted tissue fluid, just corresponding concentration of glucose be can calculate, complexity and the error of measurement added; Secondly use micro-fluidic chip extracting interstitial fluid, need just can complete measurement by after liquid transfer, in the transfer process of liquid, inevitably lose, this will cause measurement result to occur larger error.
Summary of the invention
Technical matters to be solved by this invention is, provides a kind of measuring accuracy is high, volume is little flexible differential type array electrochemical glucose sensor and using method.
The technical solution adopted in the present invention is: a kind of flexible differential type array electrochemical glucose sensor, include and be arranged side by side 7 identical sensor units of structure, each sensor unit includes flexible substrates, and first the three electrode monomer be arranged in described flexible substrates and second three electrode monomer, first described three electrode monomer are identical with second three electrode monomer structure, included contrast electrode, auxiliary electrode and working electrode.
The structure of described contrast electrode is by supreme one deck chromium, one deck inert metal platinum and one deck Ag/AgCl electrode set gradually of flexible substrates, described auxiliary electrode is identical with working electrode structure, all for by supreme one deck chromium, one deck inert metal platinum set gradually of flexible substrates.
Described contrast electrode, auxiliary electrode and working electrode are arc or bar shape.
Described working electrode is solidified with the glucose oxidase for detecting the specificity of glucose molecule.
Working electrode in first described three electrode monomer forms extraction electrode pair together with the working electrode in second three electrode monomer, when adding DC voltage to two working electrodes, working electrode place wherein in first three electrode monomer is the negative pole of the glucose molecule for assembling transdermal extraction tissue fluid, and the working electrode place in second three electrode monomer is the positive pole for assembling the tissue fluid not comprising glucose molecule.
Described working electrode is while being combined as extraction electrode, working electrode in first three electrode monomer, auxiliary electrode form an electrochemical sensor together with contrast electrode, working electrode in second three electrode monomer, auxiliary electrode form another electrochemical sensor together with contrast electrode, thus realize the in site measurement at the glucose molecule of working electrode place tissue fluid extracting point.
First described three electrode monomer are for detecting the concentration of glucose in the tissue fluid of extraction, the impact that second three electrode monomer produces sensor result for detection background tissue fluid and environment, first described three electrode monomer form difference measurement system, in order to eliminate the error caused by environmental change in measuring process together with second three electrode monomer.
A kind of using method of flexible differential type array electrochemical glucose sensor, the array electrochemical glucose sensor be made up of 7 sensor units, use 1 sensor unit every day, reach the continuous coverage realizing 7 days, the mode utilizing transposition to measure reduces the phenomena of cutaneous irritation caused due to the long-time extraction of tissue fluid.
One of the present invention flexible differential type array electrochemical glucose sensor and using method, there is the advantage that volume is little, precision is high, can in site measurement, achieve the integration of concentration of glucose in the tissue fluid of tissue fluid transdermal extraction and measurement extraction, and the problem such as allergic that the adhesion problem and extracting for a long time solving sensor and skin in extraction process causes, remove environmental factor to the impact of sensor measurement, realize the detection to low concentration glucose simultaneously.Tool of the present invention has the following advantages:
1, be make on flexible substrates by sensor, utilize the character of flexible substrate, allow sensor deformation along with the deformation of skin, sensor is closely connected with skin, thus allow the work that sensor can be stable, obtain measurement result accurately.
2, sensor utilizes two working electrode formative tissue liquid in a sensor unit to extract electrode pair, the transdermal extraction for tissue is realized with this, realize the measurement to the concentration of glucose in the tissue fluid extracted by two group of three electrode again, achieve the integration of concentration of glucose in the tissue fluid of tissue fluid transdermal extraction and measurement extraction.
3, sensor make use of the principle of difference in measuring process, (measuring object one has glucose to realize difference by the common measurement under the same conditions of group three electrodes of two in sensor unit, one does not have), the error of the measurement result caused by environmental change in measuring process can be removed.Here utilize the method for in site measurement simultaneously, be conducive to the concentration obtaining glucose more accurately.
4, sensor is the array-type sensor formed by seven sensor units, uses 1 sensor unit every day, and the used unit of first day of tearing for second day, utilizes new sensor unit to measure, can realize the continuous coverage of 7 days.This test position being equivalent to every day is different, and this difference can describe the mode into utilizing transposition to measure, and this mode can effectively reduce the phenomena of cutaneous irritation caused due to long-time extracting interstitial fluid.
Accompanying drawing explanation
Fig. 1 is the one-piece construction schematic diagram of first embodiment of the invention;
Fig. 2 is the one-piece construction schematic diagram of second embodiment of the invention;
Fig. 3 is the structural representation of first embodiment of the invention sensor unit;
Fig. 4 is the structural representation of second embodiment of the invention sensor unit;
Fig. 5 is the structural representation of first, second three electrodes monomer in first embodiment of the invention;
Fig. 6 is the structural representation of first, second three electrodes monomer in second embodiment of the invention.
In figure
1: sensor unit 2: the first three electrode monomers
3: the second three electrode monomers 4: flexible substrates
21,31: contrast electrode 22,32: auxiliary electrode
23,33: working electrode
Embodiment
Below in conjunction with embodiment and accompanying drawing, one of the present invention flexible differential type array electrochemical glucose sensor and using method are described in detail.
As shown in Figure 1, Figure 2, Figure 3, Figure 4, one of the present invention flexible differential type array electrochemical glucose sensor, include and be arranged side by side 7 identical sensor units 1 of structure, each sensor unit 1 includes flexible substrates 4, and first the three electrode monomer 2 be arranged in described flexible substrates 4 and second three electrode monomer 3, described flexible substrates 4 is flexible PET base, utilize the character of flexible substrate well to bond to make sensor and skin, thus allow the work of sensor stabilization.First described three electrode monomer 2 are identical with second three electrode monomer 3 structure, included contrast electrode 21,31, auxiliary electrode 22,32 and working electrode 23,33.Described contrast electrode 21,31, auxiliary electrode 22,32 and working electrode 23,33 be arc or bar shape.
The structure of described contrast electrode 21,31 is by supreme one deck chromium, one deck inert metal platinum and one deck Ag/AgCl electrode set gradually of flexible substrates 4, described auxiliary electrode 22,32 is identical with working electrode 23,33 structure, all for forming adhesion layer by the supreme one deck chromium set gradually of flexible substrates 4, one deck inert metal platinum forms basal electrode, and described working electrode 23,33 goes back fixing glucose oxidase.
Working electrode 23 in first described three electrode monomer 2 forms extraction electrode pair together with the working electrode 33 in second three electrode monomer 3, when giving two working electrodes 23,33 when adding DC voltage, working electrode 23 place wherein in first three electrode monomer 2 is the negative pole of the glucose molecule for assembling transdermal extraction tissue fluid, and working electrode 33 place in second three electrode monomer 3 is the positive pole for assembling the tissue fluid not comprising glucose molecule.
At described working electrode 23,33 while being combined as extraction electrode, working electrode 23 in first three electrode monomer 2, auxiliary electrode 22 form an electrochemical sensor together with contrast electrode 21, working electrode 33 in second three electrode monomer 3, auxiliary electrode 32 form another electrochemical sensor together with contrast electrode 31, thus realize at working electrode 23, the in site measurement of the glucose molecule of 33 place's tissue fluid extracting points.
First described three electrode monomer 2 are for detecting the concentration of glucose in the tissue fluid of extraction, the impact that second three electrode monomer 3 produces sensor result for detection background tissue fluid and environment, first described three electrode monomer 2 form difference measurement system together with second three electrode monomer 3, in order to eliminate the error caused by environmental change in measuring process.
The using method of a kind of flexible differential type array electrochemical glucose sensor of the present invention is, the array electrochemical glucose sensor be made up of 7 sensor units 1,1 sensor unit 1 is used every day to measure, within second day, change next sensor unit to measure, reach the continuous coverage that can realize 7 days, the mode utilizing transposition to measure reduces the phenomena of cutaneous irritation caused due to the long-time extraction of tissue fluid.
The making of a kind of flexible differential type array electrochemical glucose sensor of the present invention is: the mode first utilizing magnetron sputtering or 3D to print sputters one deck chromium and one deck inert metal platinum on the pet substrate successively, wherein layers of chrome is as adhesion layer, namely forms basal electrode.Then utilize the mode of plating electrosilvering on basal electrode, and utilize liquor ferri trichloridi to carry out chlorination process to silver electrode, obtain contrast electrode 21,31.Then with method fixing glucose oxidase on working electrode 23,33 of electrochemical deposition or molecular self-assembling layer by layer, the processing of whole electrode is namely completed.
As shown in Figure 5, Figure 6, described contrast electrode 21,31 includes and is integrally formed and the first connection terminal 21a, the 31a that connect successively, first convergence part 21b, 31b and first electrode tip 21c, 31c, is formed with the angle being greater than 130 degree between first described convergence part 21b, 31b and first electrode tip 21c, 31c.Described auxiliary electrode 22,32 includes and is integrally formed and the second connection terminal 22a, the 32a that connect successively, second convergence part 22b, 32b and second electrode tip 22c, 32c, and second described electrode tip 22c, 32c is half-circle-arc shape.Described working electrode 23,33 includes and is integrally formed and the 3rd connection terminal 23a, the 33a that connect successively, the 3rd convergence part 23b, 33b and the 3rd electrode tip 23c, 33c, and described 23c, 33c are circular piece shape.
As shown in Figure 6, described contrast electrode 21,31 and working electrode 23,33 include and are integrally formed and the 4th connection terminal 21a ', the 31a ' that are connected successively, the 4th convergence part 21b ', 31b ' and the 4th electrode tip 21c ', 31c ', and the 4th described electrode tip 21c ' is strip piece shape.Described auxiliary electrode 22,32 includes and is integrally formed and the 5th connection terminal 22a ', the 32a ' that connect successively, the 5th convergence part 22b ', 32b ' and the 5th electrode tip 22c ', 32c ', and described the 5th electrode tip 22c ', 32c ' are rectangular sheet shape.
One of the present invention flexible differential type array electrochemical glucose sensor and using method, realize the specific detection to glucose by the mode of fixing glucose oxidase on the working electrode (s.
Present invention utilizes two groups of electrochemical glucose sensor be made up of first three electrode monomer 2 and second three electrode monomer 3 and carry out difference measurement, glucose is had in the tissue fluid that one of them (as first three electrode monomer 2) electrochemical glucose sensor is measured, another (as second three electrode monomer 3) electrochemical glucose sensor 3 does not have glucose, eliminates with this error caused by environmental change in measuring process; Achieve the in site measurement to extraction point and working electrode 23,33 interstitial fluid glucose concentration simultaneously, be conducive to the concentration obtaining glucose more accurately.
The course of work of a kind of flexible differential type array electrochemical glucose sensor of the present invention and using method is: first day uses first sensor unit, first 23, the 33 pairs of tissue fluid of two working electrodes in range site carry out transdermal extraction, and first three electrode monomer 2 secondly in range site and second three electrode monomer 3 detect the glucose in the tissue fluid extracted; Within second day, tear the sensor unit crossed the previous day, realize the extraction of tissue fluid and the detection to the concentration of glucose in the tissue fluid extracted with new sensor unit; Analogize in proper order until complete the continuous detecting of 7 days.
The transdermal extraction to tissue fluid is realized: as shown in Figure 3, Figure 4 by the working electrode of two in sensor unit, by sensor and adhering skin good after, the electric current of 0.3mA is added to the working electrode 23,33 of sensor unit, namely constant current extraction is carried out to tissue fluid, glucose molecule is made to gather negative pole 23 surface with tissue fluid, tissue fluid not containing glucose molecule gathers positive pole 33 surface, and each extraction time is 3 minutes.
Detection to the concentration of glucose in extracting interstitial fluid: detection system is here first three electrode monomer 2 in sensor unit and second three electrode monomer 3, as Fig. 3, shown in Fig. 4, after extraction process completes, add relative to contrast electrode 21 to be the voltage of-0.6V to working electrode 23, and make to form measuring circuit between working electrode 23 and auxiliary electrode 22, the decomposition of glucose oxidase specific catalytic glucose, electric current potentiostatically in electrochemical reaction in the transfer rate of electronics and electrochemical reaction is directly proportional to the concentration of glucose in liquid to be measured, the concentration of glucose in liquid to be measured just can be obtained by the size detecting this electric current (electric currents namely between 23 and 22).Here difference is mainly reflected in: corresponding identical respectively for the condition that electrode 23 and 33,22 and 32,21 and 31 applies, sole difference when detecting is exactly that there is glucose at 23 places and 33 places do not have glucose, so the change of the electric current detected by working electrode 23 and environmental change are on the impact of electrode, by the difference of working electrode 23 with working electrode 33, the impact of environmental change on glucose measurements can be eliminated.
One of the present invention flexible differential type array electrochemical glucose sensor and using method, traditional sensor construction is improved, by electrode fabrication on flexible substrates, by the character of flexible substrate, make sensor deformation along with the deformation of skin, allow sensor and skin close adhesion, thus allow the work that sensor can be stable, obtain measurement result accurately.Sensor utilizes two working electrode formative tissue liquid in a sensor unit to extract electrode pair, the transdermal extraction for tissue is realized with this, realize the measurement to the concentration of glucose in the tissue fluid extracted by two group of three electrode monomer again, achieve the integration of concentration of glucose in the tissue fluid of tissue fluid transdermal extraction and measurement extraction.Sensor make use of the principle of difference in measuring process, by group three electrode monomers of two in sensor unit, (difference is only three electrode measurement objects glucose under the same conditions, one does not have) common measurement realize difference, the error of the measurement result caused by environmental change in measuring process can be removed.Here also used the principle of in site measurement simultaneously, here in site measurement shows: after completing the transdermal extraction to tissue fluid, do not need collect transfer extract tissue fluid, just in working electrode 23 place in-situ accomplishes to the detection of the concentration of glucose in extracted tissue fluid.Sensor is the array-type sensor formed by seven sensor units, uses 1 sensor unit every day, and first day of tearing for second day had used to obtain unit, utilized new sensor unit to measure, can realize the continuous coverage of 7 days.This test bit being equivalent to every day is equipped with fine distinction, and this fine distinction can describe the mode into utilizing transposition to measure, and this mode can effectively reduce the phenomena of cutaneous irritation caused due to long-time extracting interstitial fluid.
The present invention's all combinations that are open and that disclose can produce by using for reference disclosure herein, although combination of the present invention is described by detailed implementation process, but those skilled in the art obviously can be spliced device as herein described or change not departing from content of the present invention, spirit and scope, or increase and decrease some parts, more particularly, all similar replacements and change apparent to those skilled in the art, they are deemed to be included among spirit of the present invention, scope and content.
Claims (8)
1. a flexible differential type array electrochemical glucose sensor, it is characterized in that, include and be arranged side by side 7 identical sensor units of structure (1), each sensor unit (1) includes flexible substrates (4), and first the three electrode monomer (2) be arranged in described flexible substrates (4) and second three electrode monomer (3), first described three electrode monomer (2) are identical with second three electrode monomer (3) structure, include contrast electrode (21, 31), auxiliary electrode (22, 32) and working electrode (23, 33).
2. one according to claim 1 flexible differential type array electrochemical glucose sensor, it is characterized in that, the structure of described contrast electrode (21,31) is by supreme one deck chromium, one deck inert metal platinum and one deck Ag/AgCl electrode set gradually of flexible substrates (4), described auxiliary electrode (22,32) is identical with working electrode (23,33) structure, all for by supreme one deck chromium, one deck inert metal platinum set gradually of flexible substrates (4).
3. the differential type array electrochemical glucose sensor of flexibility according to claim 1, it is characterized in that, described contrast electrode (21,31), auxiliary electrode (22,32) and working electrode (23,33) are arc or bar shape.
4. the differential type array electrochemical glucose sensor of flexibility according to claim 1, is characterized in that, described working electrode (23,33) is solidified with the glucose oxidase for detecting the specificity of glucose molecule.
5. one according to claim 1 flexible differential type array electrochemical glucose sensor, it is characterized in that, working electrode (23) in first described three electrode monomer (2) and the working electrode (33) in second three electrode monomer (3) form extraction electrode pair together, when giving two working electrodes (23, 33) when adding DC voltage, working electrode (23) place wherein in first three electrode monomer (2) is the negative pole of the glucose molecule for assembling transdermal extraction tissue fluid, working electrode (33) place in second three electrode monomer (3) is the positive pole for assembling the tissue fluid not comprising glucose molecule.
6. the differential type array electrochemical glucose sensor of flexibility according to claim 5, it is characterized in that, described working electrode (23, 33) while being combined as extraction electrode, working electrode (23) in first three electrode monomer (2), auxiliary electrode (22) and contrast electrode (21) form an electrochemical sensor together, working electrode (33) in second three electrode monomer (3), auxiliary electrode (32) and contrast electrode (31) form another electrochemical sensor together, thus realize at working electrode (23, 33) in site measurement of the glucose molecule of place's tissue fluid extracting point.
7. one according to claim 1 flexible differential type array electrochemical glucose sensor, it is characterized in that, first described three electrode monomer (2) are for detecting the concentration of glucose in the tissue fluid of extraction, the impact that second three electrode monomer (3) produces sensor result for detection background tissue fluid and environment, first described three electrode monomer (2) and second three electrode monomer (3) form difference measurement system, together in order to eliminate the error caused by environmental change in measuring process.
8. the using method of an a kind of flexible differential type array electrochemical glucose sensor according to claim 1, it is characterized in that, the array electrochemical glucose sensor be made up of 7 sensor units (1), use 1 sensor unit (1) every day, reach the continuous coverage realizing 7 days, the mode utilizing transposition to measure reduces the phenomena of cutaneous irritation caused due to the long-time extraction of tissue fluid.
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| CN108627553A (en) * | 2018-05-15 | 2018-10-09 | 青岛理工大学 | Platinum electrode Multifunction Sensor |
| CN110501403A (en) * | 2018-05-18 | 2019-11-26 | 潘新宇 | Single pixel noninvasive dynamics monitoring device |
| CN109813791A (en) * | 2019-01-02 | 2019-05-28 | 北京科技大学 | A kind of microlayer model high-flux electric chemical sensor based on micro-pillar array |
| WO2021024136A1 (en) * | 2019-08-02 | 2021-02-11 | Bionime Corporation | Method for manufacturing implantable micro-biosensor and the implantable micro-biosensor |
| CN111839532A (en) * | 2020-07-14 | 2020-10-30 | 天津大学 | Flexible epidermis electrochemistry biosensor based on conductive hydrogel |
| CN114088788A (en) * | 2021-11-18 | 2022-02-25 | 华东师范大学 | Sweat composition detection device |
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