CN102954994A - Bioelectrochemical tank having anti-interference function - Google Patents
Bioelectrochemical tank having anti-interference function Download PDFInfo
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- CN102954994A CN102954994A CN2011102449882A CN201110244988A CN102954994A CN 102954994 A CN102954994 A CN 102954994A CN 2011102449882 A CN2011102449882 A CN 2011102449882A CN 201110244988 A CN201110244988 A CN 201110244988A CN 102954994 A CN102954994 A CN 102954994A
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- Investigating Or Analysing Biological Materials (AREA)
Abstract
The invention provides a bioelectrochemical tank having an anti-interference function. The bioelectrochemical tank having an anti-interference function comprises 1, an electrode system and 2, a reagent composition for corresponding biological substance detection. After being automatically sucked into the electrode system, a detected sample undergoes a biochemical reaction and an electrochemical reaction with the reagent composition to produce electrons; the electrons are transmitted to a tester by an electrode; and the tester reads data and the data is processed and a detection result is displayed. The bioelectrochemical tank having an anti-interference function improves detection result accuracy, eliminates the influence produced by erythrocytes on detection results, has a high anti-interfering substance capacity, and has an electron transfer rate constant more than 10 times.
Description
Technical field
The present invention relates to a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function.
Background technology
Glucose oxidase (glucose oxidase, GOD), nineteen twenty-eight is by discoveries such as Muller, after this, the priorities such as Nekamatsu, Konelia, Yoshio have been done a large amount of research to it and have been thrown the people and produce, Fiedurek and Rogalski etc. have done a large amount of research work to the increase of enzyme unit, especially prothetic group one flavin adenine dinucleotide (FAD) (FAD) of glucose oxidase has been done deep research, and having provided detailed explanation, this enzyme has been widely used in clinical detection and food industry at present.The glucose biological electrochemical cell is exactly the selectivity of utilizing the glucose oxidase catalytic oxidation of glucose, detects the glucose content in the various materials, and the glucose biological electrochemical cell is at biology and extremely important using value is medically arranged.1962, Clark and Lyons proposed enzyme is combined with electrode, can measure by detecting oxygen that its enzymic catalytic reaction consumes the content of glucose.1967, Updike and Hicks developed first glucose oxidase electrode take platinum (Pt) electrode as matrix first, by the product H of detection of enzymatic reactions
2O
2Measure glucose content.First generation enzyme biotinylated biomolecule electrochemical cell is take the electrocatalytic reaction of oxygen as electronics medium transfer body:
GOD
Ox+ glucose → GOD
Red+ gluconic acid
GOD
red+O
2→GOD
ox+H
2O
2
2H
2O
2→O
2+2H
2O+2e
There are following shortcomings in first generation glucose oxidase enzyme bioelectrochemical pond: 1. the variation of dissolved oxygen DO may affect the fluctuation of electrode response; 2. the solubleness of oxygen is limited, and when dissolved oxygen DO was poor, the respective electrical lumen is aobvious to descend, thereby affects detection limit; 3. the response performance of biotinylated biomolecule electrochemical cell is subjected in the solution impact of pH and temperature very large.
Willians in 1970 etc. attempt to adopt the molecule conducting medium to replace the trial that oxygen molecule carries out the transmission of redox electronics.They have used the successful implementation of the potassium ferricyanide one potassium ferrocyanide conducting medium system electrochemical gaging of blood-glucose has also been measured blood lactic acid with same electro-chemical systems simultaneously.Although this initiative electro-chemical test principle is widely used in the development and production practice of company's blood glucose meter in the future.Second generation enzyme biotinylated biomolecule electrochemical cell is take the electro-catalysis of artificial electronics medium transfer body as the basis:
GOD
Ox+ glucose → GOD
Red+ gluconic acid
GOD
red+M
ox→GOD
ox+M
red
M
red-ne→M
ox
Second generation glucose oxidase enzyme bioelectrochemical pond has utilized artificial electronics medium transfer body, its objective is in order to enlarge electrode can survey the material concentration scope and improve mensuration sensitivity
Adopt glucose oxidase technique, although not disturbed by the non-glucose glucides such as maltose, disturb but be subject to oxygen, need the patient of oxygen uptake such as ICU critically ill patient or other, owing to a large amount of oxygen intakes, often make the oxygen content of blood greatly depart from normal level.Adopt glucose dehydrogenase (GDH-PQQ) technology then can to react with carbohydrate such as maltose, galactose and the wood sugar etc. of some non-glucose, and cause the blood glucose meter reading false higher.If the patient receives treatment according to this false high value, hypoglycemia (hypoglycemia), stupor even death that may Anomalies Caused.13 parts of death reports relevant with GDH-PQQ blood sugar test test paper that U.S. FDA is received all are subjected to the interference of the glucide of maltose or other non-glucose.In addition, the factor that affects the blood glucose measurement blood sugar test paper also has hematid specific volume, and hematid specific volume too high or too low (take Hct 42% as reference point) all can affect test result.The impact that hematid specific volume is measured blood sugar test paper is extensively paid attention to; the hematid specific volume usable range of general blood sugar test paper is between 20～60%; but have a lot of diabetics often hematid specific volume exceed this scope, usually can cause blood sugar test false higher or on the low side.A lot of infants' hematid specific volume causes the false on the low side of blood sugar test value far above this scope; Some are suffered from simultaneously exsanguine Erythrocyte on Diabetes Mellitus specific volume and are lower than again this scope and cause the false higher of blood sugar test value; These two kinds of phenomenons all might mislead the medication measure of taking subsequently and cause injury to patient.Standard permission result's of blood sugar test in this scope of existing ISO15197:2003 version error range can be ± 20%; And be transferred on the scope that the standard of the new edition that is about to publicize and implement handle allows ± 15%.In addition; Adopt the electrochemical enzyme electrode mode to carry out the impact that blood sugar test also will be subject to galvanochemistry interfering material in the blood.The interfering material that U.S.'s clinical diagnosis central standard is listed has 16 kinds, and is as shown in table 1.The degree that blood sugar test paper is disturbed should be controlled in the scope of ISO15197 appointment, makes the least possible impact that is subjected to these interfering materials of test result.
16 kinds of galvanochemistry interfering materials that table 1 U.S. clinical diagnosis central standard is listed
Electrode system and specific reagent that the combined type spatial structure is introduced in bioelectrochemistry of the present invention pond form, and are improving test accuracy, and reducing or eliminating affects the factor of blood glucose measurement aspect method is provided.
Summary of the invention
In order to overcome the technical matters that exists in the prior art, the invention provides a kind of bioelectrochemistry pond of the electrode system with the combined type spatial structure, specific reagent composition is contained in this bioelectrochemistry pond, cooperates tester can accomplish the impact of raising accuracy, reduction disturbing factor; Accuracy and confidence level to test result have greatly been improved.
To achieve these goals, the invention provides following technical scheme:
A kind of bioelectrochemistry pond that possesses anti-interference function comprises
A. at least two insulated substrate (100) and (300) that be used for to consist of electrode system;
B. the electrode system that consists of at substrate (104), (105) and (107) wherein (104) and (107) are auxiliary electrode, and (105) are working electrode;
C. consist of the substrate (200) of sample cell;
D. consist of the contact (102) of combined switch;
E. automatically open with switch (101);
F. vent port (109);
H. be coated in chemistry and biological chemical reagent on (104) and (105) electrode;
Auxiliary electrode and working electrode and combined switch contact are opened automatically with switch on same substrate, are distributed in the same face or separately distribute on the substrate two sides.
Preferably, it comprises the system of two or two above auxiliary electrodes.
Preferably, the thickness of the substrate of formation sample cell can be also can be uniformly the system of the substrate splicing of thickness more than two kinds.
Preferably, auxiliary electrode (107) and tester connecting pin are by the structure of bottom by connecting hole (103) conducting.
Further, the combination beginning contact the same face that can be distributed in substrate also can be distributed in two faces of substrate.
Preferably, include glucose oxidase, glucose dehydrogenase (GDH-FAD, GDH-PQQ), horseradish peroxidase, urate oxidase, beta-hydroxybutyric dehydrogenase, one or more in the enzymes such as cholesterol oxidase.
Further, contain 1,4-benzoquinone and quinone derivatives, ferrocene and derivant, the potassium ferricyanide, tri-chlorination six ammino rutheniums, Prussian blue, o-dianisidine, methylene is green, tetrathiafulvalene, Nano Silver, nm of gold particulate, the N-PMS, wherein one or more are as electronics medium transfer body.
Preferably, electrode material is by in carbon, conductive carbon paste, gold, platinum, palladium, silver, the silver/silver chloride one or more.
Preferably, glucose oxidase, tri-chlorination six ammino rutheniums and sulfonic group hydrocarbon compound become the reagent composition simultaneously.
Further, glucose dehydrogenase enzyme (GDH-FAD), tri-chlorination six ammino rutheniums, PMS class and sulfonic group hydrocarbon compound become the reagent composition simultaneously.
Electronics medium transfer body selects toluphenazine sulfuric acid formicester etc. to have dyestuff and the tri-chlorination six ammino ruthenium bielectron medium transfer body systems of redox function when further, using glucose dehydrogenase (GDH-FAD).
Preferably, the length of using hydrocarbon chain forms as reagent as the sulfonic group hydrocarbon compound of C4-C20.
Further, the current-responsive curve that produces for separating of the blood sample of different hematid specific volumes of sulfonic group hydrocarbon compound.
Further, utilize the current-responsive curve that separates to carry out the system of hematid specific volume compensation.
Further, consist of electrochemical cell by working electrode (104) and auxiliary electrode (107), and contain the system of claim 9 or the described component of claim 10, current peak appears in chronoa mperometric plot when applying DC voltage.
The beneficial effect that the present invention brings is:
1, this biotinylated biomolecule electrochemical cell is controlled within the specific limits the impact of testing result red blood cell in the blood sample, so that the accuracy of testing result is improved;
2, this biotinylated biomolecule electrochemical cell also has the function of differentiating hematid specific volume, can separate the signal of different hematid specific volumes, is conducive to tester it is proofreaied and correct, and reaches to eliminate red blood cell to the impact of testing result;
3, the more traditional potassium ferricyanide of electronics medium transfer body tri-chlorination six ammino rutheniums of this bioelectrochemistry pond use has the ability of higher anti-interference material impact and the electron transfer speed constant more than 10 times.
Description of drawings
Fig. 1 is the decomposition diagram of bioelectrochemistry pool structure of the present invention;
Fig. 2 is the figure of bioelectrochemistry of the present invention pond assembling;
Fig. 3 a is the current-time curvel of bioelectrochemistry of the present invention pond when measuring under different hematid specific volumes when not adding the sulfonic group hydrocarbons;
Fig. 3 b is the current-time curvel of bioelectrochemistry of the present invention pond when measuring under different hematid specific volumes behind the interpolation sulfonic group hydrocarbons;
Fig. 4 a is bioelectrochemistry of the present invention pond at the comparison diagram (blood sugar concentration as 75mg/dL time) that is disturbed respectively the material influence degree take the potassium ferricyanide and tri-chlorination six ammino rutheniums during as electronics medium transfer body;
Fig. 4 b is bioelectrochemistry of the present invention pond at the comparison diagram (blood sugar concentration as 320mg/dL time) that is disturbed respectively the material influence degree take the potassium ferricyanide and tri-chlorination six ammino rutheniums during as electronics medium transfer body.
Embodiment
The below is to elaborating preferred embodiment of the present invention by reference to the accompanying drawings, thereby so that advantages and features of the invention can be easier to be it will be appreciated by those skilled in the art that protection scope of the present invention made more explicit defining.
Be included in the upper working electrode (104) that forms of insulated substrate (100) according to Fig. 1, the auxiliary electrode (105) that keeps at a certain distance away and form at the insulated substrate same plane with working electrode (104); Form another one auxiliary electrode (107) and form vent port in the top that this auxiliary electrode (107) is spaced a distance at insulated substrate (300); The combined switch contact (102) of the switch (101) of the automatic unlatching tester that forms on insulated substrate (100) top and the automatic identification correction codes that forms at same substrate therewith is included as the sample cell (106) of siphon sample.For being conducted with the upper auxiliary electrode (107) that forms of substrate (300), the connector contact pin of tester formed aperture (103) at substrate (100) and the top end of substrate (200).With substrate (300) and the substrate (200) that scribbles bonding agent to bonding behind the good position, again will be bonding good substrate (300) and substrate (200) and to have applied the substrate (100) of enzyme and electronics medium transfer body bonding; Just consisted of the bioelectrochemistry pond that comprises combined type stereoscopic electric chemical bath that will use with this, its course of work is as follows:
(1) biotinylated biomolecule electrochemical cell of the present invention is inserted tester (400), open tester (400) by switch (101), and select correction codes by combined switch (102) tester of correction codes; To prepare to suck sample;
(2) electrochemical cell in working electrode (104) and auxiliary electrode (107) formation applies certain voltage, reads time dependent current value; Disconnecting circuit;
(3) through between working electrode (104) and auxiliary electrode (105), applying certain voltage after one period reaction time, read time dependent current value;
(4) electric current one time curve that obtains from (2) stage, the information of acquisition hematid specific volume;
(5) electric current one time curve that obtains from (3) stage is determined the concentration of analysans, the information of the hematid specific volume that obtains in conjunction with (4) process is proofreaied and correct draws the preparation result, and the biotinylated biomolecule electrochemical cell take these processes as feature will be used to the mensuration of blood sugar.
When above-mentioned biotinylated biomolecule electrochemical cell is used for testing blood sugar, sucks sample in process (1) and be less than 0.1 microlitre, and do not need pre-service to be directly used in test as feature.
The voltage that applies in above-mentioned biotinylated biomolecule electrochemical cell test (2) process can be direct current, interchange, pulse voltage, and to obtain current-responsive, AC impedance value, capacitance are as feature.
Above-mentioned biotinylated biomolecule electrochemical cell a period of time of opening a way in process (3) reacts as feature, and the voltage that this is after-applied can be direct current, interchange, pulse voltage, and to obtain current-responsive, AC impedance value, capacitance are as feature.
Enzyme and electronics medium transfer body are coated on working electrode (104) and the auxiliary electrode (105) in the above-mentioned biotinylated biomolecule electrochemical cell, to obtain stable and to respond as feature fast.
Above-mentioned biotinylated biomolecule electrochemical cell reagent selects tri-chlorination six ammino rutheniums as electronics medium transfer body in forming, and with the impact of reduce disturbance material on test result, fast reaction speed is feature simultaneously.
Above-mentioned biotinylated biomolecule electrochemical cell reagent is selected sulfonic hydrocarbon compound in forming, and makes the current-responsive of the blood sample of different hematid specific volumes be separated into feature.
Tri-chlorination six ammino ruthenium 5.0g (weight ratio is 40%), polyvinyl alcohol (PVA) 1.0g (weight ratio 8.0%) Triton X-1000.5g (weight ratio 4.0%), it is 6.4 100ml phosphate buffered solution that glucose oxidase 6.0g (weight ratio 48.0%) is dissolved in pH, filters.
Potassium ferricyanide 5.0g (weight ratio is 37.0%), sodium octyl 1.0g (weight ratio 17.4%) polyvinyl alcohol (PVA) 1.0g (weight ratio 7.4%), Triton X-1000.5g (weight ratio 3.7%), it is 6.4 100ml phosphate buffered solution that glucose oxidase 6.0g (weight ratio 44.5%) is dissolved in pH with above-claimed cpd, filters.
Tri-chlorination six ammino ruthenium 5.0g (weight ratio is 37.0%), sodium octyl 1.0g (weight ratio 7.4%) polyvinyl alcohol (PVA) 1.0g (weight ratio 7.4%), Triton X-100 0.5g (weight ratio 3.7%), it is 6.4 100ml phosphate buffered solution that glucose oxidase 6.0g (weight ratio 44.5%) is dissolved in pH with above-claimed cpd, filters.
Carry out the bioelectrochemistry pond by Fig. 1 and Fig. 2 and make, before three substrate mountings, embodiment 1, embodiment 2, embodiment 3 ready reagent are coated in respectively (104) and (105) and are assembled into again three kinds of bioelectrochemistry ponds.The electrochemical cell that consists of in (104) and (105) applies the DC voltage of 0.2V, measures and carries out disconnecting circuit after 5 seconds; Kept for 2 seconds, the electrochemical cell that consists of in (104) and (107) again applies the DC voltage of 0.2V; The current-responsive of two processes is read in test.Information by the relevant hematid specific volume of current-responsive curve acquisition of phase one; By the information of the relevant blood sugar concentration of current-responsive curve acquisition of subordinate phase, comprehensive two kinds of information show the result at tester (401).
The response curve in blood sugar bioelectrochemistry pond when having or not the sulfonic group hydrocarbon compound during experimental example 1, reaction reagent form
Utilize the reagent of embodiment 1 and 3 to form, make and measuring method according to embodiment 4 described blood sugar bioelectrochemistry ponds, obtain the response curve of whole blood sample.Whole blood sample is through centrifuging, separated plasma and haemocyte, and recycling its preparation hematid specific volume is 20,42,60% blood sample adds glucose solution in the blood sample of three kinds of preparations, make the concentration of blood sugar in three kinds of blood samples reach respectively 229,298,296mg/dL for measuring.Fig. 3 a is the response curve in the blood sugar bioelectrochemistry pond when not having the sulfonic group hydrocarbon compound, can see in the response curve that background current is too high, the time in the response curve of three kinds of blood samples during peak current is almost identical, and can't differentiate hematid specific volume is 20,42,60% blood sample.And Fig. 3 b is the response curve that has added the blood sugar bioelectrochemistry pond of sulfonic group hydrocarbon compound; Along with the increase background current step-down of the hematid specific volume of blood sample, and the position of peak current obviously is subjected to displacement with the increase of hematid specific volume, namely is easy to differentiate the blood sample of three kinds of hematid specific volumes; Utilize this characteristic just can be easy to this is compensated, obtain accurately result.
Experimental example 2, blood sugar bioelectrochemistry pond are to response curve and the calibration curve of blood sample
Utilize the reagent of embodiment 3 to form and blood sugar bioelectrochemistry pond that the method for embodiment 4 is made, measure with blood sample and obtain response curve and draw test result through the data processing again.47.8,129,394mg/dL the hematid specific volume of blood sample of preparation is respectively 15,20,25,30,42,50,55,60,65%, and the concentration of blood sugar divides three groups to be respectively:.Measurement result is as shown in table 2.The result show hematid specific volume in 15% to 65% scope deviation in ± 18, and in 20% to 60% scope deviation only in ± 10.
The test result of three kinds of blood sugar concentrations of table 2 when different hematid specific volume
Experimental example 3, interfering material are on blood sugar test result's impact
Utilize embodiment 2,3 reagent to form, the blood sugar bioelectrochemistry pond Ascorbic Acid that utilizes the method for embodiment 4 to make, dopamine, the impact of paracetamol testing result is tested.The hematid specific volume of blood sample is mixed with 42%, blood-glucose is transferred to 75mg/dL and two kinds of concentration of 320mg/dL, the blood sample of every kind of concentration is divided into three parts again, each adds ascorbic acid, dopamine, paracetamol is respectively 3mg/dL, 13mg/dL, 20mg/dL, utilize these blood samples obtain a result as Fig. 4 a and Fig. 4 b from figure, can compare the bioelectrochemistry pond that utilizes tri-chlorination six ammino ruthenium electronics medium transfer bodies on the impact of interfering material much smaller than the bioelectrochemistry pond that utilizes the potassium ferricyanide.
The above; it only is one of the specific embodiment of the present invention; but protection scope of the present invention is not limited to this; any those of ordinary skill in the art are in the disclosed technical scope of the present invention; variation or the replacement that can expect without creative work all should be encompassed within protection scope of the present invention.Therefore, protection scope of the present invention should be as the criterion with the protection domain that claims were limited.
Claims (15)
1. a bioelectrochemistry pond that possesses anti-interference function comprises
A. at least two insulated substrate (100) and (300) that be used for to consist of electrode system;
B. the electrode system that consists of at substrate (104), (105) and (107) wherein (104) and (107) are auxiliary electrode, and (105) are working electrode;
C. consist of the substrate (200) of sample cell;
D. consist of the contact (102) of combined switch;
E. automatically open with switch (101);
F. vent port (109);
H. be coated in chemistry and biological chemical reagent on (104) and (105) electrode;
It is characterized in that: auxiliary electrode and working electrode and combined switch contact, automatically open with switch on same substrate, be distributed in the same face or separately distribute on the substrate two sides.
2. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1, it is characterized in that: it comprises the system of two or two above auxiliary electrodes.
3. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: the thickness that consists of the substrate of sample cell can be also can be uniformly the system of the substrate splicing of thickness more than two kinds.
4. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function of biology according to claim 1 is characterized in that: auxiliary electrode (107) and tester connecting pin are by the structure of bottom by connecting hole (103) conducting.
5. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: the same face that combination beginning contact can be distributed in substrate also can be distributed in two faces of substrate.
6. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1, it is characterized in that: include glucose oxidase, glucose dehydrogenase (GDH-FAD, GDH-PQQ), horseradish peroxidase, urate oxidase, beta-hydroxybutyric dehydrogenase, one or more in the enzymes such as cholesterol oxidase.
7. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: contain 1,4-benzoquinone and quinone derivatives, ferrocene and derivant, the potassium ferricyanide, tri-chlorination six ammino rutheniums, Prussian blue, o-dianisidine, methylene is green, tetrathiafulvalene, Nano Silver, nm of gold particulate, the N-PMS, wherein one or more are as electronics medium transfer body.
8. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: electrode material is by in carbon, conductive carbon paste, gold, platinum, palladium, silver, the silver/silver chloride one or more.
9. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function of biology according to claim 1 is characterized in that: glucose oxidase, tri-chlorination six ammino rutheniums and sulfonic group hydrocarbon compound become simultaneously that reagent forms.
10. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: glucose dehydrogenase enzyme (GDH-FAD), tri-chlorination six ammino rutheniums, PMS class and sulfonic group hydrocarbon compound become simultaneously that reagent forms.
11. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: electronics medium transfer body selects toluphenazine sulfuric acid formicester etc. to have dyestuff and the tri-chlorination six ammino ruthenium bielectron medium transfer body systems of redox function when using glucose dehydrogenase (GDH-FAD).
12. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1 is characterized in that: the length of using hydrocarbon chain forms as reagent as the sulfonic group hydrocarbon compound of C4-C20.
13. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 13 is characterized in that: the current-responsive curve that the sulfonic group hydrocarbon compound produces for separating of the blood sample of different hematid specific volumes.
14. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 14 is characterized in that: utilize the current-responsive curve that separates to carry out the system of hematid specific volume compensation.
15. a kind of a kind of bioelectrochemistry pond that possesses anti-interference function that possesses anti-interference function according to claim 1, it is characterized in that: consist of electrochemical cell by working electrode (104) and auxiliary electrode (107), and contain the system of claim 9 or the described component of claim 10, current peak appears in chronoa mperometric plot when applying DC voltage.
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| CN104730134A (en) * | 2015-03-31 | 2015-06-24 | 曲阜师范大学 | Ferrocene/graphene oxide/sol-gel silicon film as well as preparation method thereof and glucose biosensor |
| CN105283757A (en) * | 2013-03-15 | 2016-01-27 | 豪夫迈·罗氏有限公司 | Methods of failsafing electrochemical measurements of an analyte as well as devices, apparatuses and systems incorporating the same |
| US10416114B2 (en) | 2016-05-26 | 2019-09-17 | Industrial Technology Research Institute | Structures and manufacture method of electrochemical units |
| US10983087B2 (en) | 2016-05-26 | 2021-04-20 | Industrial Technology Research Institute | Structures and manufacture method of electrochemical units |
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| US10983087B2 (en) | 2016-05-26 | 2021-04-20 | Industrial Technology Research Institute | Structures and manufacture method of electrochemical units |
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