CN102507671B - Porous silicon biochip and preparation method thereof - Google Patents
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Abstract
The invention relates to the field of biotechnology, and discloses a porous silicon biochip and a preparation method thereof. The porous silicon preparation method provided by the invention comprises the steps of adopting electrochemical anodic oxidation technology to corrode a single face polished silicon wafer to obtain the porous silicon, wherein the oxidation mode is constant current electrolysis, the current density is 3mA/cm2 and the electrolysis time is 500-700 seconds; then performing modified decoration for the surface of the porous silicon by a functional silane coupling agent to obtain a modified layer containing active groups; and then preparing the porous silicon biochip by the functional porous silicon as a carrier. The preparation method provided by the invention is simple and convenient, requires fewer devices and is suitable for volume-production. The porous silicon biochip obtained by the method of the invention has the advantages of high sensitivity, good selectivity, good repeatability and the like, and can be used to study the interaction among biological macromolecules.
Description
Technical field
The present invention relates to biological technical field, relate to specifically a kind of porous silicon biochip and preparation method thereof.
Background technology
Porous silica material is a kind of novel silicon nano material that forms, has spongy structure by electrochemical oxidation monocrystalline silicon, due to its unique institutional framework and quantum effect, make it there is high efficiency photoluminescence and electroluminescence characters, therefore, porous silicon is considered to one of material had the huge applications prospect.Simultaneously, as silica-base material, porous silicon not only has good physics photoelectron performance, also there is huge specific surface area, good chemical activity and biocompatibility, this is all the transducer sensor that porous silicon is applied to biomolecule, cell and tissue, the aspects such as inorganic non-metallic biomaterial and biomedicine provide possibility (silicon materials and device, Silicon-Based Material and Devices, Edited by Hari Singh Nalwa, 2001, Academic Press).
At present, in the bio-sensing field, the porous silicon optical sensor prepared according to the Fabry-Perot interference effect is most widely used, it utilizes the variation of porous silicon reflection interference spectrum figure, can realize detection (science, Science, 1997 to biomolecule, bacterium, virus etc., 278,840-842; U.S. chemical institute magazine, J.Am.Chem.Soc., 1998,120,12108-12116; U.S. chemical institute magazine, J.Am.Chem.Soc., 2005,127,11636-11645; Analytical chemistry, Anal.Chem., 2007,79,1502-1506; Practical new material, Adv.Funct.Mater., 2010,20,2269-2277; Analytical chemistry, Anal.Chem., 2011,83,3282-3289).
Biochip is the important tool of current genomics, protein science research, has the advantages such as high flux, robotization, sample consumption be little.But at present, biochip mainly be take glass as carrier, thus the diversity of detection means and and other highly sensitive detection technique integrated aspect still have certain disadvantages.Therefore, the application of expansion semiconductor material aspect biochip carrier is significant to its development.The porous silicon semiconductor material is combined with biochip technology, contribute to promote the application in the biochip field of microelectric technique and photoelectron technology.
Summary of the invention
In view of this, it is good that the object of the invention is to provide a kind of selection type, highly sensitive porous silicon biochip and preparation method thereof.
For realizing purpose of the present invention, the present invention adopts following technical scheme:
A kind of preparation method of porous silicon biochip comprises:
Step 1: the polished surface of single-sided polishing silicon chip is contacted with electrolytic solution and connects cathode voltage by electrolytic solution, the back side and conductor contact also connect anode voltage by conductor, then carry out electrochemical anodic oxidation and obtain porous silicon, wherein, described oxidation model is constant-current electrolysis, current density 3mA/cm
2, electrolysis time is 500～700 seconds;
Step 2: the porous silicon that step 1 is made carries out functional modification, then utilizes the biochip point sample system evenly drip the biomacromolecule titer and get final product.
The present invention adopts the electrochemical anodic oxidation technology to corrode and obtain porous silicon the single-sided polishing silicon chip.Wherein, it is 1-10 Ω/cm that described single-sided polishing silicon chip is preferably resistivity, the p-type boron-doping monocrystalline silicon that crystal orientation is<100 > single-sided polishing.
The oxidation model of electrochemical anodic oxidation of the present invention is constant-current electrolysis, current density 3mA/cm
2, electrolysis time is 500～700 seconds.Being preferably electrolysis time is 600 seconds.
Preferably, electrolytic solution described in electrochemical anodic oxidation process of the present invention is the hydrofluorite ethanolic solution that volume fraction is 25%.
According to the present invention, before carrying out galvanic corrosion, need to clean thoroughly silicon chip, to remove the original oxide layer of silicon chip surface, therefore before step 1, also comprise the step of described single-sided polishing silicon chip being carried out to surface clean.
Wherein, as preferably, silicon wafer surface cleaning of the present invention specifically comprises:
Step a: silicon chip is put into to acetone, cyclohexane, acetone, absolute ethyl alcohol successively and carry out ultrasonic cleaning, each scavenging period is 3 minutes, naturally dries;
Step b: the silicon chip dried is put into to the solution that volume ratio is 3: 1 concentrated sulphuric acids and hydrogen peroxide, no longer include Bubble formation to silicon chip surface and take out, first use a large amount of cold deionized water rinsings, the reusable heat deionized water rinsing is clean;
Step c: clean silicon chip immerses the hydrofluoric acid aqueous solution that volume fraction is 5%, soaks 1 minute, then with deionized water, rinses well, puts into absolute ethyl alcohol standby.
The preparation method of porous silicon biochip of the present invention needs porous silicon is carried out to functional modification after making porous silicon, so that porous silicon surface has from different biomacromolecules in conjunction with required functionalization group.In certain embodiments, the described functional modification of preparation method's step 3 of the present invention is that epoxidation is modified, and with in conjunction with glucide, prepares the porous silicon carbohydrate chip.
As preferably, epoxidation of the present invention is modified to be specially and is utilized silane coupling agent under the protection of nitrogen stream, and 120 ℃, stirring and refluxing 24 hours, obtain.Wherein, as preferably, the anhydrous DMF solution that described silane coupling agent is the massfraction γ-glycidyl ether oxygen propyl trimethoxy silicane that is 1%.
Preparation method's step 2 of the present invention, after the porous silicon that step 1 is made carries out functional modification, is utilized the biochip point sample system evenly to drip the biomacromolecule titer and is prepared porous silicon biochip.Wherein, described biomacromolecule comprises the product that albumen, nucleic acid, carbohydrate, lipid and they mutually combine, as glycoprotein, lipoprotein, nucleoprotein etc.In certain embodiments, biomacromolecule of the present invention is carbohydrate, and the porous silicon biochip made is the carbohydrate biochip.In certain embodiments, described carbohydrate is 4-aminophenyl-β-D-gala pyranose or 4-aminophenyl-α-D-mannopyranose, and described sampling liquid also comprises: the 0.3mol/L phosphate buffered solution that contains 0.15mol/L sodium chloride of the glycerine of volume fraction 20% and pH7.5.After point sample, described porous silicon chip, under 25 ℃, vacuum environment, reacts 12 hours, after reaction, after selecting bovine serum albumin(BSA) that massfraction is 0.5% to be sealed unreacted epoxide group and get final product.
The present invention also provides the porous silicon biochip that utilizes preparation method of the present invention to prepare.
Porous silicon preparation method provided by the invention is that the employing oxidation model is constant-current electrolysis, current density 3mA/cm
2, electrolysis time is 500～700 seconds the electrochemical anodic oxidation technology is corroded and obtained porous silicon the single-sided polishing silicon chip, utilize afterwards the silane coupling agent of functionalization to carry out functional modification to porous silicon surface, obtain the decorative layer that contains reactive group, then the porous silicon of functionalization of take is carrier, prepares porous silicon biochip.Preparation method of the present invention is easy, and device requirement is few, the suitable production in enormous quantities in enormous quantities.Utilize porous silicon biochip that the method for the invention prepares to have highly sensitive, the advantage such as the good and reappearance of selectivity is good, can be used for the interactional research of biomacromolecule.Experiment shows, with existing brilliant core
optical grade epoxy substrate is compared, and porous silicon biochip of the present invention can improve two orders of magnitude of detectability to monose and agglutinin.
The accompanying drawing explanation
Fig. 1 shows porous silicon carbohydrate chip and the brilliant core that 4-aminophenyl-β-D-gala pyranose concentration is 50mM made with the different etching times of the method for the invention
the typical curve of epoxy chip detection castor bean agglutinin (RCA120); Wherein, a: the porous silicon carbohydrate chip of etching time 500s, b: the porous silicon carbohydrate chip of etching time 600s, c: the porous silicon carbohydrate chip of etching time 700s, d: brilliant core
the epoxy chip;
Fig. 2 shows porous silicon carbohydrate chip and the brilliant core that castor bean agglutinin (RCA 120) concentration that makes with the different etching times of the method for the invention is 100 μ g/mL
the typical curve of epoxy chip detection 4-aminophenyl-β-D-gala pyranose; Wherein, a: the porous silicon carbohydrate chip of etching time 500s, b: the porous silicon carbohydrate chip of etching time 600s, c: the porous silicon carbohydrate chip of etching time 700s, d: brilliant core
the epoxy chip;
Fig. 3 shows porous silicon carbohydrate chip and the brilliant core that 4-aminophenyl-α-D-mannopyranose concentration is 50mM made with the different etching times of the method for the invention
the typical curve of epoxy chip detection concanavalin agglutinin (Con A); Wherein, a: the porous silicon carbohydrate chip of etching time 500s, b: the porous silicon carbohydrate chip of etching time 600s, c: the porous silicon carbohydrate chip of etching time 700s, d: brilliant core
the epoxy chip;
Fig. 4 shows porous silicon carbohydrate chip and the brilliant core that concanavalin agglutinin (Con A) concentration that makes with the different etching times of the method for the invention is 100 μ g/mL
the typical curve of epoxy chip detection 4-aminophenyl-α-D-mannopyranose; Wherein, a: the porous silicon carbohydrate chip of etching time 500s, b: the porous silicon carbohydrate chip of etching time 600s, c: the porous silicon carbohydrate chip of etching time 700s, d: brilliant core
the epoxy chip.
Embodiment
The embodiment of the invention discloses a kind of porous silicon biochip and preparation method thereof.Those skilled in the art can use for reference this paper content, suitably improve technological parameter and realize.Special needs to be pointed out is, all similar replacements and change apparent to those skilled in the artly, they all are deemed to be included in the present invention.Product of the present invention and method are described by preferred embodiment, and the related personnel obviously can be changed method as herein described or suitably change and combination within not breaking away from content of the present invention, spirit and scope, realizes and apply the technology of the present invention.
In order further to understand the present invention, below in conjunction with embodiment, the present invention is described in detail.
The detection of embodiment 1:4-aminophenyl-β-D-gala pyranose
Before carrying out galvanic corrosion, clean thoroughly silicon chip.The concrete steps of cleaning are as follows: by resistivity, be that acetone, cyclohexane are put into successively for<100 > single-sided polishing p-type boron-doping monocrystalline silicon silicon chip in 1-10 Ω cm, crystal orientation, acetone, carry out ultrasonic cleaning in absolute ethyl alcohol, each scavenging period is 3 minutes, after take out nature and dry; When silicon chip being put into to solution to silicon chip surface that concentrated sulphuric acid hydrogen peroxide volume ratio is 3: 1 again and no longer including Bubble formation, take out, first use a large amount of cold deionized water rinsings, the reusable heat deionized water rinsing is clean; Silicon chip through above processing immerses 5% hydrofluoric acid aqueous solution, soaks and removes oxide layer in 1 minute, with deionized water, rinses well, puts into absolute ethyl alcohol stand-by.
The hydrofluorite ethanolic solution that is 25% with percent by volume by the polished surface of cleaned silicon chip contacts, and the back side contacts with copper sheet to draw and connects anode voltage, and solution connects cathode voltage, with constant-current electrolysis, and current density 3mA/cm
2, etching time is respectively 500 seconds, 600 seconds and 700 seconds.The porous silicon of preparing cleans with deionized water and ethanol immediately, at nitrogen, flows down and dries up.
The porous silicon dried up is heat-treated in constant temperature oven, 150 ℃ of insulations, within 24 hours, carry out slow oxidation; Porous silicon chip after oxidation is put into successively respectively acetone, cyclohexane, acetone and absolute ethyl alcohol and is carried out ultrasonic cleaning 3 minutes, after take out nature and dry; Porous silicon chip after cleaning is placed in vacuum drying chamber, and 100 ℃ of vacuum drying are more than 12 hours; After drying, porous silicon chip is put into there-necked flask, adds 150mL to contain the anhydrous DMF solution that massfraction is 1% γ-glycidyl ether oxygen propyl trimethoxy silicane, under the protection of nitrogen stream, is heated to 120 ℃ of stirring and refluxing 24 hours; After reaction finishes, silicon chip is used anhydrous DMF successively, acetone, absolute ethyl alcohol ultrasonic cleaning 3 minutes; After be placed in vacuum drying chamber, 50 ℃ of vacuum drying 1 hour, obtain the porous silicon chip that epoxide group is modified, and puts into 4 ℃ of preservations of refrigerator stand-by.
The brilliant core that the porous silicon chip of modifying with the epoxide group of preparation, Beijing Bo Ao Bioisystech Co., Ltd produce
optical grade epoxy substrate is carrier, utilizes SmartArrayer 48 biochip point sample system point samples, 4-aminophenyl-β that the making concentration gradient is 10 μ M-200mM-D-gala pyranose monose chip, and the point sample amount is the 1nL/ point.In order to obtain the activity of good array point shape uniformly and maintenance biomolecule, the sampling liquid of selecting also comprises except 4-aminophenyl-β-D-gala pyranose solution: the 0.3mol/L phosphate buffered solution that contains 0.15mol/L sodium chloride of the glycerine of volume fraction 20% and pH=7.5.After point sample, at 25 ℃, under vacuum environment, reaction is 12 hours, obtains porous silicon carbohydrate biochip and brilliant core after selecting bovine serum albumin(BSA) that massfraction is 0.5% to be sealed unreacted epoxide group after reaction
epoxy carbohydrate biochip.
Fluorescence labeling porous silicon carbohydrate biochip: the 4-aminophenyl-β that is 10 μ M-200mM by the concentration gradient of making-D-gala pyranose monose chip reacts with the fluorescein-labeled castor bean agglutinin (FITC-RCA 120) of 10ng/mL-200ug/mL respectively, and temperature of reaction is 30 ℃, 1 hour time.After successively by the phosphate buffered solution that contains 0.1% Tween-20, phosphate buffered solution, the clean and centrifuge dripping of washed with de-ionized water, obtain fluorescently-labeled carbohydrate biochip.
Fluoroscopic examination porous silicon carbohydrate biochip: the fluorescently-labeled carbohydrate biochip obtained is put into to microarray scanner (LuxScan-10K/A type, Beijing Bo Ao Bioisystech Co., Ltd) detect, obtain the fluorescence signal of carbohydrate biochip, the typical curve of fluoroscopic examination is shown in Fig. 1.
Using the castor bean agglutinin as sample according to the method for the invention, utilize SmartArrayer 48 biochip point sample systems to make the castor bean lectin chip of variable concentrations gradient, then with the 4-aminophenyl-β of the variable concentrations of agglutinin mark-D-gala pyranose, react, microarray scanner detects the typical curve of fluorescence signal fluoroscopic examination and sees Fig. 2.
The detection of embodiment 2:4-aminophenyl-α-D-mannopyranose
By resistivity, be that the p-type boron-doping monocrystalline silicon silicon chip that 1-10 Ω cm, crystal orientation are<100 > single-sided polishing is put into acetone, cyclohexane successively, acetone, carry out ultrasonic cleaning in absolute ethyl alcohol, and each scavenging period is 3 minutes, after take out nature and dry; When silicon chip being put into to solution to silicon chip surface that concentrated sulphuric acid hydrogen peroxide volume ratio is 3: 1 again and no longer including Bubble formation, take out, first use a large amount of cold deionized water rinsings, the reusable heat deionized water rinsing is clean; Silicon chip through above processing immerses 5% hydrofluoric acid aqueous solution, soaks and removes oxide layer in 1 minute, with deionized water, rinses well, puts into absolute ethyl alcohol stand-by.
The hydrofluorite ethanolic solution that is 25% with percent by volume by the polished surface of cleaned silicon chip contacts, and the back side contacts with copper sheet to draw and connects anode voltage, and solution connects cathode voltage, with constant-current electrolysis, and current density 3mA/cm
2, etching time is respectively 500 seconds, 600 seconds and 700 seconds.The porous silicon of preparing cleans with deionized water and ethanol immediately, at nitrogen, flows down and dries up.
The porous silicon dried up is heat-treated in constant temperature oven, 150 ℃ of insulations, within 24 hours, carry out slow oxidation; Porous silicon chip after oxidation is put into successively respectively acetone, cyclohexane, acetone and absolute ethyl alcohol and is carried out ultrasonic cleaning 3 minutes, after take out nature and dry; Porous silicon chip after cleaning is placed in vacuum drying chamber, and 100 ℃ of vacuum drying are more than 12 hours; After drying, porous silicon chip is put into there-necked flask, adds 150mL to contain the anhydrous DMF solution that massfraction is 1% γ-glycidyl ether oxygen propyl trimethoxy silicane, under the protection of nitrogen stream, is heated to 120 ℃ of stirring and refluxing 24 hours; After reaction finishes, silicon chip is used anhydrous DMF successively, acetone, absolute ethyl alcohol ultrasonic cleaning 3 minutes; After be placed in vacuum drying chamber, 50 ℃ of vacuum drying 1 hour, obtain the porous silicon chip that epoxide group is modified, and puts into 4 ℃ of preservations of refrigerator stand-by.
The brilliant core that the porous silicon chip of modifying with the epoxide group of preparation, Beijing Bo Ao Bioisystech Co., Ltd produce
optical grade epoxy substrate is carrier, utilizes SmartArrayer 48 biochip point sample system point samples, 4-aminophenyl-α that the making concentration gradient is 10 μ M-100mM-D-mannopyranose monose chip, and the point sample amount is the 1nL/ point.In order to obtain the activity of good array point shape uniformly and maintenance biomolecule, the sampling liquid of selecting also comprises except 4-aminophenyl-α-D-mannopyranose solution: the 0.3mol/L phosphate buffered solution that contains 0.15mol/L sodium chloride of the glycerine of volume fraction 20% and pH=7.5.After point sample, at 25 ℃, under vacuum environment, reaction is 12 hours, obtains porous silicon carbohydrate biochip and brilliant core after selecting bovine serum albumin(BSA) that massfraction is 0.5% to be sealed unreacted epoxide group after reaction
epoxy carbohydrate biochip.
Fluorescence labeling porous silicon carbohydrate biochip: the 4-aminophenyl-α that is 10 μ M-100mM by the concentration gradient of making-D-mannopyranose monose chip respectively with fluorescein-labeled concanavalin agglutinin (FITC-Con A) react, temperature of reaction is 30 ℃, 1 hour time.After successively by the phosphate buffered solution that contains 0.1% Tween-20, phosphate buffered solution, the clean and centrifuge dripping of washed with de-ionized water, obtain fluorescently-labeled carbohydrate biochip.
Fluoroscopic examination porous silicon carbohydrate biochip: the fluorescently-labeled carbohydrate biochip obtained is put into to microarray scanner (LuxScan-10K/A type, Beijing Bo Ao Bioisystech Co., Ltd) detect, obtain the fluorescence signal of carbohydrate biochip, the typical curve of fluoroscopic examination is shown in Fig. 3.
Using the concanavalin agglutinin as sample according to the method for the invention, utilize SmartArrayer48 biochip point sample system to make the concanavalin lectin chip of variable concentrations gradient, then with the 4-aminophenyl-α of the variable concentrations of agglutinin mark-D-mannopyranose, react, microarray scanner detects the typical curve of fluorescence signal fluoroscopic examination and sees Fig. 4.
Embodiment 3:
Porous silicon chip and existing brilliant core prepared by the method that the statistics embodiment of the present invention 1 and embodiment 2 provide
the testing result of epoxy chip detection galactose (Gal-β), castor bean agglutinin (RCA 120), mannose (Man-α), concanavalin agglutinin (Con A) is in Table 1.
Table 1. porous silicon carbohydrate chip and brilliant core
the range of linearity of epoxy chip and detectability
From table 1 result, porous silicon chip detection prepared by the preparation method that the oxidization time that utilizes the embodiment of the present invention 1 and embodiment 2 to provide is respectively 500 seconds, 600 seconds, 700 seconds, the detection that the galactose detection is limited to 100～500 μ M, castor bean agglutinin is limited to 300ng/mL～5 μ g/mL, mannose detects the detection that is limited to 100～500 μ M, concanavalin agglutinin and is limited to 500ng/mL～5 μ g/mL.And utilize existing brilliant core
the epoxy chip detection, the detection that the galactose detection is limited to 5mM, castor bean agglutinin is limited to 5 μ g/mL, mannose detects the detection that is limited to 5mM, concanavalin agglutinin and is limited to 5 μ g/mL.Show that porous silicon biochip prepared by preparation method of the present invention is highly sensitive, selectivity is good.
The explanation of above embodiment is just for helping to understand method of the present invention and core concept thereof.It should be pointed out that for those skilled in the art, under the premise without departing from the principles of the invention, can also carry out some improvement and modification to the present invention, these improvement and modification also fall in the protection domain of the claims in the present invention.
Claims (8)
1. the preparation method of a porous silicon biochip, is characterized in that, comprising:
Step 1: the polished surface of single-sided polishing silicon chip is contacted with electrolytic solution and connects cathode voltage by electrolytic solution, the back side and conductor contact also connect anode voltage by conductor, then carry out electrochemical anodic oxidation and obtain porous silicon, wherein, described oxidation model is constant-current electrolysis, current density 3mA/cm
2, electrolysis time is 500～700 seconds;
Step 2: the porous silicon that step 1 is made carries out functional modification, then utilizes the biochip point sample system evenly drip the biomacromolecule titer and get final product;
Wherein, the described functional modification of step 2 is that epoxidation is modified;
Described biomacromolecule is carbohydrate;
Described carbohydrate is 4-aminophenyl-β-D-gala pyranose or 4-aminophenyl-α-D-mannopyranose.
2. preparation method according to claim 1, is characterized in that, described silicon chip is that resistivity is 1-10 Ω/cm, the p-type boron-doping monocrystalline silicon that crystal orientation is<100 > single-sided polishing.
3. preparation method according to claim 1, is characterized in that, described electrolytic solution is the hydrofluorite ethanolic solution that volume fraction is 25%.
4. preparation method according to claim 1, is characterized in that, before step 1, also comprises the step of described single-sided polishing silicon chip being carried out to surface clean, specifically comprises:
Step a: the single-sided polishing silicon chip is put into to acetone, cyclohexane, acetone, absolute ethyl alcohol successively and carry out ultrasonic cleaning, each scavenging period is 3 minutes, naturally dries;
Step b: the silicon chip dried is put into to the solution that volume ratio is the 3:1 concentrated sulphuric acid and hydrogen peroxide, no longer include Bubble formation to silicon chip surface and take out, first use a large amount of cold deionized water rinsings, the reusable heat deionized water rinsing is clean;
Step c: clean silicon chip immerses the hydrofluoric acid aqueous solution that volume fraction is 5%, soaks 1 minute, then with deionized water, rinses well, puts into absolute ethyl alcohol standby.
5. preparation method according to claim 1, is characterized in that, the described electrolysis time of step 1 is 600 seconds.
6. preparation method according to claim 1, is characterized in that, described epoxidation is modified to and utilizes silane coupling agent under the protection of nitrogen stream, and 120 ℃, stirring and refluxing 24 hours, obtain.
7. preparation method according to claim 6, is characterized in that, the anhydrous DMF solution that described silane coupling agent is the massfraction γ-glycidyl ether oxygen propyl trimethoxy silicane that is 1%.
8. the porous silicon biochip that prepared by the described preparation method of claim 1～7 any one.
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| CN103979543B (en) * | 2014-05-08 | 2015-12-30 | 新疆大学 | A kind of modifying method of porous silicon and the purposes as biosensor thereof |
| CN107375936A (en) * | 2017-06-21 | 2017-11-24 | 南京师范大学 | A kind of curcumin porous silicon and preparation method thereof |
| CN107296802B (en) * | 2017-08-03 | 2020-11-20 | 南京师范大学 | Hydrophobic porous silicon curcumin micro-gel with antioxidant activity and preparation method thereof |
| CN107473175B (en) * | 2017-08-15 | 2019-09-06 | 薛宁 | A kind of nerve electrode and its manufacture craft and application based on porous silicon and polymer |
| CN111139515A (en) * | 2020-01-09 | 2020-05-12 | 广州大学 | Tool and method for manufacturing thin-film photoelectric sensing material |
| CN114524622B (en) * | 2022-03-07 | 2023-09-08 | 安吉世纪康敏生物科技有限公司 | Preparation method of epoxy modified substrate, microarray chip and application of microarray chip |
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Effective date of registration: 20161214 Address after: Changzhou City, Jiangsu province Hehai road 213000 No. 9 Patentee after: Changzhou Institute of Energy Storage Materials & Devices Address before: 130000 Jilin City, Changchun province people's street, No. 5625 Patentee before: Changchun Applied Chemistry Inst., Chinese Academy of Sciences |