CN208705267U - One kind removing interference paper base electrochemical sensor - Google Patents
One kind removing interference paper base electrochemical sensor Download PDFInfo
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- CN208705267U CN208705267U CN201821315722.6U CN201821315722U CN208705267U CN 208705267 U CN208705267 U CN 208705267U CN 201821315722 U CN201821315722 U CN 201821315722U CN 208705267 U CN208705267 U CN 208705267U
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- Investigating Or Analysing Biological Materials (AREA)
Abstract
The utility model discloses one kind to remove interference paper base electrochemical sensor, belongs to electrochemical sensor field.The electrochemical sensor includes paper-based substrate and measuring electrode system;The paper-based substrate is made of the hydrophilic layer in same level with hydrophobic layer, and hydrophilic layer one end is concordant with paper-based substrate side to be used as flow channel entry point, remaining side of hydrophilic layer is surrounded by hydrophobic layer, constitutes water conservancy diversion channel;Have in the water conservancy diversion channel and remove interference section and measuring section, and interference section is gone to be located in water conservancy diversion channel close to the upstream of the flow channel entry point;The measuring electrode system is set to paper-based substrate surface, includes working electrode and reference electrode in measuring electrode system, and the electrode detection end of working electrode and reference electrode is respectively positioned in the measuring section of water conservancy diversion channel, and exit is respectively positioned on the side edge of paper-based substrate.The advantages that there is the utility model chaff interferent sufficiently to react elimination, and measurement is accurate, and the processing is simple, low in cost.
Description
Technical field
The utility model belongs to electrochemical sensor field, and in particular to one kind removes interference paper base electrochemical sensor.
Background technique
Electrochemical sensor is often applied to the measurement of target analyte concentration in fluid sample, wherein based on enzyme biology point
The electrochemica biological sensor of son is one of the electrochemical sensor being most widely used.Blood glucose, the blood ketone, blood lipid being commercialized
Such sensor is belonged to serum creatinine electrochemistry test piece.These electrochemical sensors mostly with PET, PVC, ceramics for substrate,
The catalyst of specific catalytic is often modified on its working electrode, the oxygen generated under catalyst by detecting target analytes
Change or reduction current realizes the quantitative detection to target analytes.
Heat is flutterred however often containing the chemical substance other than target analytes in fluid sample, such as in blood sample
Pain, ascorbic acid, bilirubin, dopamine, gentianic acid, levodopa, uric acid etc. are ceased, such chemical substance also can be in working electrode
Upper generation oxidation or reduction reaction, influence the current-responsive of target analytes, to influence the measurement accuracy of electrochemistry test piece.Cause
This, reduces or removes chaff interferent, and that improves electrochemical sensor removes interference performance, accurate to the measurement for improving electrochemical sensor
Degree is of great significance.
Currently, reducing or eliminating the method for chaff interferent mainly include the following types: (1) covers one layer of band in working electrode surface
Negative electricity macromolecule membrane (such as Nafion), using electrostatic repulsion principle hinder various electronegative chaff interferents (such as ascorbic acid and
Uric acid) reach electrode surface;(2) one layer of size selective membrane is modified in working electrode surface, is imitated using the size selection of film
Answer the chaff interferent of exclusive segment macromolecule that electrochemical reaction occurs in working electrode;(3) it is modified and master in working electrode surface
The corresponding enzyme of chaff interferent is wanted, chaff interferent is removed using enzymatic reaction, prevents chaff interferent from electrochemical reaction occurring on the working electrode (s;
(4) using the electron mediator with lower oxidation reduction potential, the operating voltage for being applied to working electrode is reduced, chaff interferent is reduced and exists
Electrochemical reaction on electrode;(5) increase by the second working electrode in electrochemical sensor, by what is measured on the second working electrode
Interference electric current is deducted from the current signal of working electrode, eliminates interference.Although these above-mentioned methods are in electrochemical sensor
Interference has and has certain effect on eliminating, but can only to eliminate fraction chaff interferent, working electrode overlay film partially thick there are single method
Influence electron transmission, the disadvantages of electrode fabrication process is complicated.Therefore, developing new has extensive anti-interference ability and function admirable
Electrochemical sensor be of great significance.
Summary of the invention
Utility model aims to solve problems of the prior art, and provide one kind and go interference paper base electrification
Learn sensor.
Specific technical solution used by the utility model is as follows:
One kind removing interference paper base electrochemical sensor comprising paper-based substrate and measuring electrode system;The paper-based substrate
It is made of the hydrophilic layer in same level with hydrophobic layer, hydrophilic layer one end is concordant with paper-based substrate side to be entered as runner
Mouthful, remaining side of hydrophilic layer is surrounded by hydrophobic layer, constitutes water conservancy diversion channel;Have in the water conservancy diversion channel and goes interference section and measurement
Section, and interference section is gone to be located in water conservancy diversion channel close to the upstream of the flow channel entry point;The measuring electrode system is set to
Paper-based substrate surface, includes working electrode and reference electrode in measuring electrode system, and the electrode of working electrode and reference electrode is examined
It surveys end to be respectively positioned in the measuring section of water conservancy diversion channel, exit is respectively positioned on the side edge of paper-based substrate.
Further, described to go in interference section to be equipped with the first reagent dropwise region, the working electrode of the measuring section is attached
Closely it is equipped with the second reagent dropwise region.
Further, go to interfere the first reagent dropwise region in section to have multiple, and along water conservancy diversion channel between journey
Every laying.
Further, the measuring electrode system is three-electrode system, wherein it is additionally provided with auxiliary electrode, auxiliary electrode
Test side also is located in the measuring section of water conservancy diversion channel, and exit is also disposed on the side edge of paper-based substrate.
Further, the material of the paper-based substrate be filter paper, chromatographic paper, pvdf membrane, NC film, blotting paper and
One of Kleenex paper handkerchief is a variety of.
Further, electrode material is carbon slurry in the measuring electrode system, the carbon of Ag/AgCl, doped graphene is starched,
Carbon nanotube is Prussian blue.
Further, the exit of each electrode is all connected with Electrochemical detector in the measuring electrode system.
Compared with prior art, the utility model has the beneficial effects that
(1) the utility model will with the target jamming substance reaction to be removed in analyte sample fluid but not with it is to be detected
First biological chemical reagent of target substance reaction is arranged in water conservancy diversion channel, rather than directly modifies on the working electrode (s.?
When test, analyte sample fluid flows in water conservancy diversion channel, and chaff interferent therein can be tried with the first biochemistry of interference range is gone
Agent comes into full contact with reaction, and when analyte sample fluid flows to measurement zone, chaff interferent therein is consumed totally substantially, sample to be tested
Object reacts again in liquid.Thus the utility model is not necessarily to add the electron mediator of lower oxidation reduction potential, and no setting is required
Second working electrode has many advantages, such as that chaff interferent sufficiently reacts elimination, and measurement is accurate, processing technology is succinct.
(2) the utility model distinguishes the first biological chemical reagent with measurement, rather than directly with the second biochemistry
Reagent is modified on the working electrode (s jointly.In this way, chaff interferent and object subregion in analyte sample fluid are reacted,
It can reduce the overlay film thickness on working electrode, exclude influence of first biological chemical reagent to working electrode, also exclude first
Influence of the biological chemical reagent to the second biological chemical reagent.Thus have the advantages that electron transmission is rapid, measurement is accurate.
(3) electrode basement that the utility model uses is paper base.Using paper as substrate, paper is utilized and absorbs water, be easy to get, inexpensively
The advantages that, thus invented go interference paper base electrochemical sensor do not need special hydrophilic treated, have the processing is simple, at
Sheet is cheap, is conducive to the advantages that industrialized mass production.
Detailed description of the invention
Fig. 1 is a kind of structure top view for embodiment that the utility model removes interference paper base electrochemical sensor;
Fig. 2 is a kind of structural side view for embodiment that the utility model removes interference paper base electrochemical sensor;
In figure: paper-based substrate 100, hydrophobic layer 101, hydrophilic layer 102, water conservancy diversion channel 103, goes interference section at electrode layer 200
104, measuring section 105, the first reagent dropwise region 106, the second reagent dropwise region 107, working electrode 201, reference electrode
202, auxiliary electrode 203.
Specific embodiment
The utility model is further elaborated and is illustrated with reference to the accompanying drawings and detailed description.In the utility model
The technical characteristic of each embodiment can carry out the corresponding combination under the premise of not conflicting with each other.
As shown in Figure 1, as an implementation, the interference paper base electrochemical sensor that goes of the utility model mainly includes
Paper-based substrate 100 and measuring electrode system 200.
Paper-based substrate 100 is the main body of paper base electrochemical sensor, it is by hydrophobic layer 101 in the same plane and parent
Water layer 102 forms.102 one end of hydrophilic layer is concordant with 100 one side edge of paper-based substrate to be used as flow channel entry point, hydrophilic layer 102 remaining
Side is surrounded by hydrophobic layer 101, constitutes water conservancy diversion channel 103.When the runner that analyte sample fluid is added dropwise to 102 end of hydrophilic layer enters
When mouth, since hydrophilic layer 102 has hydrophily, and the hydrophobic layer 101 on its periphery has hydrophobicity, therefore sample liquid can be with hydrophilic
Layer 102 is spread since flow channel entry point to the other end as water conservancy diversion channel 103, forms liquid flowing.In the present embodiment, paper base
The material of bottom 100 can be one of filter paper, chromatographic paper, pvdf membrane, NC film, blotting paper and Kleenex paper handkerchief or a variety of.
Hydrophobic layer 101 and hydrophilic layer 102 can be realized in different ways, splice for example, by using existing hydrophobic material and water wetted material, or
Person just spreads hydrophobic material layer and hydrophilic material on the base layer, as long as can guarantee liquid to be detected along hydrophilic laminar flow i.e.
It can.Certainly, in another embodiment, it is contemplated that manufacture craft simplicity, hydrophobic layer 101 can be on the basis of paper-based substrate 100
By one of photoetching process, wax printing method, ink-jet method, PDMS drawing or a variety of realizations, so that the scraps of paper have hydrophobicity;Similarly
Hydrophilic layer can also by paper-based substrate 100 carry out the realization of plasma hydrophilic treated, make reagent flowing more uniformly (if paper
Basal layer 100 itself has hydrophily, can also be without carrying out hydrophilic treated).
Along Cheng Jinhang function division in water conservancy diversion channel 103, it is provided with one section and removes interference section 104 and one section of measuring section 105.
It goes interference section 104 and measuring section 105 itself is one section be formed by water conservancy diversion channel 103 by hydrophilic layer 102, but due to it
He, which handles difference, causes its function difference also occur.Go the effect of interference section 104 mainly to the target dry in analyte sample fluid
Substance is disturbed to be removed, and the effect of measuring section 105 is to be obtained by Electrochemical Detection and mesh to be detected in analyte sample fluid
Mark the positively related current signal of substance.Therefore, it on location layout, goes interference section 104 that should be located in water conservancy diversion channel 103 and leans on
The upstream of nearly flow channel entry point, i.e. analyte sample fluid first pass through interference section 104 and are flowing to measuring section after flow channel entry point entrance
105。
Electrochemical Detection in measuring section 105 needs to realize by measuring electrode system 200.In the present embodiment, it measures
Electrode system 200 is that electrode material is printed on 100 surface of paper-based substrate by way of silk-screen printing or inkjet printing,
In measuring electrode system 200 electrode material be carbon slurry, Ag/AgCl, the carbon slurry of doped graphene, carbon nanotube, it is Prussian blue in
It is one or more, can be selected as needed.It can certainly be using other electrodes lay modes, as long as can will survey
Amount electrode system 200 is set to 100 surface of paper-based substrate.Measuring electrode system 200 can be using with working electrode 201
With two electrode systems of reference electrode 202, but in the present embodiment, in order to improve between working electrode 201 and reference electrode 202
Voltage stability, also add auxiliary electrode 203 in measuring electrode system 200.It is working electrode 201, reference electrode 202, auxiliary
The electrode detection end of electrode 203 is helped to be respectively positioned in the measuring section 105 of water conservancy diversion channel 103, bottom surface is tightly attached to 102 upper surface of hydrophilic layer
On, it can be contacted with substance to be detected therein and electrochemical reaction occurs.Working electrode 201, reference electrode 202, auxiliary electrode
203 electrode leads to client is respectively positioned on the side edge of paper-based substrate 100, to facilitate lead.When in use, measuring electrode system 200
In the exit of each electrode be all connected with Electrochemical detector, for applying current potential to electrode.
In the present invention, it goes interference section 104 to be independently arranged at 105 upstream of measuring section, is not overlapped between the two.
Wherein go chaff interferent removal function in interference section 104, be paper base is modified using biological chemical reagent caused by.It is going
It interferes and is equipped with the first reagent dropwise region 106 in section 104, before being detected using the utility model, can be dripped in each region
Add with the target jamming substance reaction to be removed in analyte sample fluid but the biochemistry do not reacted with target substance to be detected is tried
Agent is denoted as the first biological chemical reagent.It, can be to circumferential diffusion, laterally after reagent dropwise since hydrophilic layer has water imbibition
Span covers whole 103 width of water conservancy diversion channel, vertically infiltrates into hydrophilic layer bottom, therefore actually finally to the dropwise addition position
The entire section of water conservancy diversion channel 103 is modified.When analyte sample fluid diffuses to the region, interfering substance therein can be with
It is reacted with the first biological chemical reagent, but target substance to be detected is without reaction, so that interfering substance is removing interference 104 base of section
Originally it is exhausted, the target substance to be detected without interfering substance can enter in subsequent measuring section 105.Go interference section 104
In to can according to need setting one or more in the first reagent dropwise region 106.When the first reagent dropwise region 106 have it is multiple
When, it can be laid along water conservancy diversion channel 103 along journey interval, the reagent being added dropwise in different zones can be identical, identical reagent
It can be repeated as many times and chaff interferent is removed, reduction chaff interferent as far as possible enters in subsequent measuring section 105.Certainly, if
Containing there are many when chaff interferent in analyte sample fluid, different reagents can also be added dropwise in the first different reagent dropwise regions 106,
Reaction consumption is carried out to different chaff interferents respectively, but different reagents is both needed to guarantee to react with substance to be detected.
Similarly, on the working electrode 201 of measuring section 105 or neighbouring position can also be equipped with the second reagent dropwise region 107, utilize this
Before utility model is detected, it can be added dropwise in the second reagent dropwise region 107 and object to be detected in analyte sample fluid
The biological chemical reagent of qualitative response is denoted as the second biological chemical reagent.Second reagent dropwise region, 107 size is unlimited, as long as
The reagent spread after reagent, which is added dropwise, electrochemical reaction occurs with working electrode contact.
It is above-mentioned go interference paper base electrochemical sensor can batch it is prefabricated, when biological chemical reagent can choose use again voluntarily
It is added dropwise.When sensor is prefabricated, it is only necessary in the reserved first reagent dropwise region 106 in the corresponding position of water conservancy diversion channel 103 and the second examination
Region 107 is added dropwise in agent.Different regions can by scribing line, color distinguish, mark etc. mark modes, facilitate user according to
Corresponding reagent is added dropwise in testing requirements;When certain user itself has identification capability, it is only necessary to which there are blank positions, by user
Position is added dropwise in designed, designed.Certainly, the first biological chemical reagent and the second biological chemical reagent directly prefabricated can be tried in paper base
On piece is just no longer needed to additionally be added dropwise so when in use, be modified paper base or electrode.Specific practice can be according to practical progress
Adjustment.
In the present invention, according to the difference of target analytes, the first biological chemical reagent and the examination of the second biochemistry
Agent is not identical, but can be glucose oxidase, mutarotase, glucose dehydrogenase, lactate oxidase, urate oxidase, gallbladder
Sterol oxidizing ferment, phosphatidase, aminoacidase, horseradish peroxidase, beta-hydroxybutyric dehydrogenase, ascorbinase, it is Prussian blue,
One of reagents such as ferrocene derivatives are a variety of.The specific target substance and interfering substance difference needed according to detection, by
User selects on demand;If you need to prefabricated, need to combine prefabricated a variety of detector classes for different test objects and chaff interferent respectively
Not.First biological chemical reagent can be used as reactant and react with the chaff interferent in analyte sample fluid and generate and react production
Object, the chaff interferent that can also be used as in catalyst analyte sample fluid react and generate reaction product.Second bioid
The object that learning reagent can be used as in reactant and analyte sample fluid reacts and generates reaction product, can also be used as and urges
Object in agent and catalysis analyte sample fluid reacts and generates reaction product.
Below by no prefabricated biological chemical reagent go interference paper base electrochemical sensor for, illustrate be based on such paper
The method that based electrochemical sensor tests analyte sample fluid, its step are as follows:
Before testing, will with the target jamming substance reaction to be removed in analyte sample fluid but not with target to be detected
First biological chemical reagent of substance reaction is added dropwise to the first reagent dropwise region 106, and the first biological chemical reagent is made to penetrate into parent
In water layer 102, one or more sections of water conservancy diversion channel 103 are covered;It will be with the target substance to be detected in analyte sample fluid
Second biological chemical reagent of reaction is added dropwise in the second reagent dropwise region 107, is modified working electrode 201;
Then analyte sample fluid is added dropwise in the flow channel entry point of hydrophilic layer end, makes analyte sample fluid along water conservancy diversion channel
103 constantly diffusions reach the first reagent dropwise regions 106 for going interference section 104, the target jamming substance in analyte sample fluid with
First biological chemical reagent, which reacts, to be removed;Analyte sample fluid continues to diffuse to the of measuring section 105 along water conservancy diversion channel 103
Two reagent dropwise regions 107, the target substance to be detected in analyte sample fluid are reacted with the second biological chemical reagent and are generated anti-
Answer product.Apply certain current potential to measuring electrode system 200 using Electrochemical detector, makes target substance to be detected and second
Electrochemical reaction occurs on working electrode 201 for the reaction product that biological chemical reagent reaction generates, and records on working electrode 201
Electric current, the target substance concentration of analyte sample fluid is calculated using the electric current.
As an example of present embodiment, target analytes are uric acid, what the first reagent dropwise region 106 was added dropwise
First biological chemical reagent is ascorbic acid oxidase, and the second biological chemical reagent that the second reagent dropwise region 107 is added dropwise is
Urate oxidase, analyte sample fluid are ascorbic acid and uric acid mixed solution, and wherein uric acid is target detection thing.In test,
Mixed solution enters from 103 entrance of water conservancy diversion channel, flows through interference section 104, ascorbic acid and ascorbic acid in mixed solution
Enzyme comes into full contact with reaction, and with flowing of the mixed solution in water conservancy diversion channel 103, ascorbic acid is gradually consumed.It is molten when mixing
When liquid flow to measuring section 105, ascorbic acid is not included in mixed solution, at this time the uric acid and measurement zone in mixed solution
Urate oxidase react and generate product, which electrochemical reaction occurs under the current potential that measurement zone applies and generates electrification
Learn electric current.The electrochemical source of current so generated is only positively correlated with the concentration of object uric acid, has achieved the purpose that removal interference.
The uric acid concentration of analyte sample fluid can be calculated according to the correlativity of electric current and uric acid concentration.
It should be pointed out that if the target substance to be detected itself in analyte sample fluid has redox active, that
The second biological chemical reagent of addition can not be had in second reagent dropwise region 107, working electrode 201 can directly detect electricity
Stream.
Embodiment described above is a kind of preferable scheme of the utility model, and so it is not practical to limit
It is novel.Those of ordinary skill in related technical field can be in the case where not departing from the spirit and scope of the utility model
It makes a variety of changes and modification.In addition, measuring electrode system when necessary can also be only with two electrode systems.Therefore all take is equal
The mode technical solution obtained of replacement or equivalent transformation, all falls in the protection scope of the utility model.
Claims (7)
1. one kind removes interference paper base electrochemical sensor, which is characterized in that including paper-based substrate (100) and measuring electrode system
(200);The paper-based substrate (100) is made of the hydrophilic layer (102) in same level with hydrophobic layer (101), hydrophilic layer
(102) one end is concordant with paper-based substrate (100) side is used as flow channel entry point, and hydrophilic layer (102) remaining side is by hydrophobic layer
(101) it surrounds, constitutes water conservancy diversion channel (103);Have in the water conservancy diversion channel (103) and removes interference section (104) and measuring section
(105), and interference section (104) is gone to be located in water conservancy diversion channel (103) close to the upstream of the flow channel entry point;The measurement electricity
Electrode systems (200) are set to paper-based substrate (100) surface, include working electrode (201) and reference in measuring electrode system (200)
The electrode detection end of electrode (202), working electrode (201) and reference electrode (202) is respectively positioned on the measuring section of water conservancy diversion channel (103)
(105) in, exit is respectively positioned on the side edge of paper-based substrate (100).
2. removing interference paper base electrochemical sensor as described in claim 1, which is characterized in that described goes interference section (104)
In be equipped with the first reagent dropwise region (106), the working electrode (201) of the measuring section (105) nearby be equipped with the second reagent drip
Add region (107).
3. removing interference paper base electrochemical sensor as claimed in claim 2, which is characterized in that go the in interference section (104)
One reagent dropwise region (106) have it is multiple, and along water conservancy diversion channel (103) along journey interval lay.
4. removing interference paper base electrochemical sensor as described in claim 1, which is characterized in that the measuring electrode system
It (200) is three-electrode system, wherein being additionally provided with auxiliary electrode (203), the test side of auxiliary electrode (203) also is located at water conservancy diversion channel
(103) in measuring section (105), exit is also disposed on the side edge of paper-based substrate (100).
5. removing interference paper base electrochemical sensor as described in claim 1, which is characterized in that the paper-based substrate
(100) material is one of filter paper, chromatographic paper, pvdf membrane, NC film, blotting paper and Kleenex paper handkerchief or a variety of.
6. removing interference paper base electrochemical sensor as described in claim 1, which is characterized in that the measuring electrode system
(200) electrode material is carbon slurry, Ag/AgCl, the carbon slurry of doped graphene, carbon nanotube or Prussian blue in.
7. removing interference paper base electrochemical sensor as described in claim 1, which is characterized in that the measuring electrode system
(200) exit of each electrode is all connected with Electrochemical detector in.
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