CN106745281A - It is a kind of with the method for filobactivirus templated synthesis manganese dioxide nanowire and application - Google Patents
It is a kind of with the method for filobactivirus templated synthesis manganese dioxide nanowire and application Download PDFInfo
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- CN106745281A CN106745281A CN201610271529.6A CN201610271529A CN106745281A CN 106745281 A CN106745281 A CN 106745281A CN 201610271529 A CN201610271529 A CN 201610271529A CN 106745281 A CN106745281 A CN 106745281A
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- manganese dioxide
- dioxide nanowire
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- nanowire
- filobactivirus
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- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 title claims abstract description 211
- 239000002070 nanowire Substances 0.000 title claims abstract description 104
- 238000000034 method Methods 0.000 title claims abstract description 29
- 230000015572 biosynthetic process Effects 0.000 title claims description 18
- 238000003786 synthesis reaction Methods 0.000 title claims description 18
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims abstract description 23
- 238000002360 preparation method Methods 0.000 claims abstract description 16
- 238000006243 chemical reaction Methods 0.000 claims abstract description 15
- 238000006555 catalytic reaction Methods 0.000 claims abstract description 13
- 239000003990 capacitor Substances 0.000 claims abstract description 5
- 230000002255 enzymatic effect Effects 0.000 claims abstract 2
- 239000000243 solution Substances 0.000 claims description 19
- 239000003054 catalyst Substances 0.000 claims description 13
- 239000003153 chemical reaction reagent Substances 0.000 claims description 9
- 238000001514 detection method Methods 0.000 claims description 8
- 239000007864 aqueous solution Substances 0.000 claims description 7
- OHDRQQURAXLVGJ-HLVWOLMTSA-N azane;(2e)-3-ethyl-2-[(e)-(3-ethyl-6-sulfo-1,3-benzothiazol-2-ylidene)hydrazinylidene]-1,3-benzothiazole-6-sulfonic acid Chemical compound [NH4+].[NH4+].S/1C2=CC(S([O-])(=O)=O)=CC=C2N(CC)C\1=N/N=C1/SC2=CC(S([O-])(=O)=O)=CC=C2N1CC OHDRQQURAXLVGJ-HLVWOLMTSA-N 0.000 claims description 7
- 230000008569 process Effects 0.000 claims description 7
- 239000006228 supernatant Substances 0.000 claims description 7
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 6
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 6
- 238000001556 precipitation Methods 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- 239000003513 alkali Substances 0.000 claims description 4
- 238000011161 development Methods 0.000 claims description 4
- 239000007788 liquid Substances 0.000 claims description 4
- 229940071125 manganese acetate Drugs 0.000 claims description 4
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims description 4
- 230000003647 oxidation Effects 0.000 claims description 4
- 238000007254 oxidation reaction Methods 0.000 claims description 4
- -1 Diamine salts Chemical class 0.000 claims description 3
- ZOMNIUBKTOKEHS-UHFFFAOYSA-L dimercury dichloride Chemical class Cl[Hg][Hg]Cl ZOMNIUBKTOKEHS-UHFFFAOYSA-L 0.000 claims description 3
- 239000002270 dispersing agent Substances 0.000 claims description 3
- 238000000835 electrochemical detection Methods 0.000 claims description 3
- 239000012467 final product Substances 0.000 claims description 3
- 239000011259 mixed solution Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 229910052697 platinum Inorganic materials 0.000 claims description 3
- 230000004044 response Effects 0.000 claims description 3
- UAIUNKRWKOVEES-UHFFFAOYSA-N 3,3',5,5'-tetramethylbenzidine Chemical compound CC1=C(N)C(C)=CC(C=2C=C(C)C(N)=C(C)C=2)=C1 UAIUNKRWKOVEES-UHFFFAOYSA-N 0.000 claims description 2
- 229910021380 Manganese Chloride Inorganic materials 0.000 claims description 2
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 claims description 2
- 235000011114 ammonium hydroxide Nutrition 0.000 claims description 2
- 239000007772 electrode material Substances 0.000 claims description 2
- 229910021397 glassy carbon Inorganic materials 0.000 claims description 2
- 239000011565 manganese chloride Substances 0.000 claims description 2
- 235000002867 manganese chloride Nutrition 0.000 claims description 2
- 229940099607 manganese chloride Drugs 0.000 claims description 2
- 229940099596 manganese sulfate Drugs 0.000 claims description 2
- 239000011702 manganese sulphate Substances 0.000 claims description 2
- 235000007079 manganese sulphate Nutrition 0.000 claims description 2
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims description 2
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 claims description 2
- 239000002086 nanomaterial Substances 0.000 abstract description 10
- 239000000463 material Substances 0.000 abstract description 8
- 230000003197 catalytic effect Effects 0.000 abstract description 4
- 108090000565 Capsid Proteins Proteins 0.000 abstract description 2
- 102100023321 Ceruloplasmin Human genes 0.000 abstract description 2
- 238000005287 template synthesis Methods 0.000 abstract description 2
- 241001515965 unidentified phage Species 0.000 description 18
- 238000002474 experimental method Methods 0.000 description 16
- 230000000694 effects Effects 0.000 description 15
- 102000004190 Enzymes Human genes 0.000 description 7
- 108090000790 Enzymes Proteins 0.000 description 7
- 102000003992 Peroxidases Human genes 0.000 description 5
- 238000002484 cyclic voltammetry Methods 0.000 description 5
- 108040007629 peroxidase activity proteins Proteins 0.000 description 5
- 241000700605 Viruses Species 0.000 description 4
- 238000013461 design Methods 0.000 description 4
- 230000031700 light absorption Effects 0.000 description 4
- 235000015097 nutrients Nutrition 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 241000723873 Tobacco mosaic virus Species 0.000 description 3
- 239000007853 buffer solution Substances 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 2
- 238000004458 analytical method Methods 0.000 description 2
- 230000033558 biomineral tissue development Effects 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 238000004891 communication Methods 0.000 description 2
- 230000018109 developmental process Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000001027 hydrothermal synthesis Methods 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 239000002071 nanotube Substances 0.000 description 2
- 230000006911 nucleation Effects 0.000 description 2
- 238000010899 nucleation Methods 0.000 description 2
- 238000005457 optimization Methods 0.000 description 2
- 238000005498 polishing Methods 0.000 description 2
- 108090000623 proteins and genes Proteins 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 239000007974 sodium acetate buffer Substances 0.000 description 2
- BHZOKUMUHVTPBX-UHFFFAOYSA-M sodium acetic acid acetate Chemical compound [Na+].CC(O)=O.CC([O-])=O BHZOKUMUHVTPBX-UHFFFAOYSA-M 0.000 description 2
- 239000000725 suspension Substances 0.000 description 2
- 238000010408 sweeping Methods 0.000 description 2
- QKNYBSVHEMOAJP-UHFFFAOYSA-N 2-amino-2-(hydroxymethyl)propane-1,3-diol;hydron;chloride Chemical compound Cl.OCC(N)(CO)CO QKNYBSVHEMOAJP-UHFFFAOYSA-N 0.000 description 1
- 241000894006 Bacteria Species 0.000 description 1
- 229910018979 CoPt Inorganic materials 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 241000588724 Escherichia coli Species 0.000 description 1
- 241001524679 Escherichia virus M13 Species 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229910005335 FePt Inorganic materials 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- WAEMQWOKJMHJLA-UHFFFAOYSA-N Manganese(2+) Chemical compound [Mn+2] WAEMQWOKJMHJLA-UHFFFAOYSA-N 0.000 description 1
- 229920002594 Polyethylene Glycol 8000 Polymers 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- QTJOIXXDCCFVFV-UHFFFAOYSA-N [Li].[O] Chemical compound [Li].[O] QTJOIXXDCCFVFV-UHFFFAOYSA-N 0.000 description 1
- 238000002835 absorbance Methods 0.000 description 1
- 239000008351 acetate buffer Substances 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 238000013528 artificial neural network Methods 0.000 description 1
- 238000003556 assay Methods 0.000 description 1
- 238000012742 biochemical analysis Methods 0.000 description 1
- 239000012620 biological material Substances 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 239000000090 biomarker Substances 0.000 description 1
- 239000000872 buffer Substances 0.000 description 1
- 229910052980 cadmium sulfide Inorganic materials 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- MQRJBSHKWOFOGF-UHFFFAOYSA-L disodium;carbonate;hydrate Chemical compound O.[Na+].[Na+].[O-]C([O-])=O MQRJBSHKWOFOGF-UHFFFAOYSA-L 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000004070 electrodeposition Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000003018 immunoassay Methods 0.000 description 1
- SBUJHOSQTJFQJX-NOAMYHISSA-N kanamycin Chemical class O[C@@H]1[C@@H](O)[C@H](O)[C@@H](CN)O[C@@H]1O[C@H]1[C@H](O)[C@@H](O[C@@H]2[C@@H]([C@@H](N)[C@H](O)[C@@H](CO)O2)O)[C@H](N)C[C@@H]1N SBUJHOSQTJFQJX-NOAMYHISSA-N 0.000 description 1
- 229930027917 kanamycin Natural products 0.000 description 1
- 238000004502 linear sweep voltammetry Methods 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- 239000000696 magnetic material Substances 0.000 description 1
- 229910001437 manganese ion Inorganic materials 0.000 description 1
- 230000001404 mediated effect Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002121 nanofiber Substances 0.000 description 1
- 239000002135 nanosheet Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 238000005580 one pot reaction Methods 0.000 description 1
- 238000010422 painting Methods 0.000 description 1
- 239000008363 phosphate buffer Substances 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 108090000765 processed proteins & peptides Proteins 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 102000004169 proteins and genes Human genes 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000004611 spectroscopical analysis Methods 0.000 description 1
- 229910052950 sphalerite Inorganic materials 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
- 238000010189 synthetic method Methods 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 229910021642 ultra pure water Inorganic materials 0.000 description 1
- 239000012498 ultrapure water Substances 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
- 229910052984 zinc sulfide Inorganic materials 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G45/00—Compounds of manganese
- C01G45/02—Oxides; Hydroxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/32—Manganese, technetium or rhenium
- B01J23/34—Manganese
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/40—Catalysts, in general, characterised by their form or physical properties characterised by dimensions, e.g. grain size
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- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
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- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/17—Systems in which incident light is modified in accordance with the properties of the material investigated
- G01N21/25—Colour; Spectral properties, i.e. comparison of effect of material on the light at two or more different wavelengths or wavelength bands
- G01N21/31—Investigating relative effect of material at wavelengths characteristic of specific elements or molecules, e.g. atomic absorption spectrometry
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
- G01N27/28—Electrolytic cell components
- G01N27/30—Electrodes, e.g. test electrodes; Half-cells
- G01N27/308—Electrodes, e.g. test electrodes; Half-cells at least partially made of carbon
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
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- C01P2004/10—Particle morphology extending in one dimension, e.g. needle-like
- C01P2004/16—Nanowires or nanorods, i.e. solid nanofibres with two nearly equal dimensions between 1-100 nanometer
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Abstract
The present invention relates to nano material, catalysis and analytical chemistry field, specifically include it is a kind of based on filobactivirus make biological template synthesis manganese dioxide nanowire preparation method and its application in terms of catalysis.The method is using the intrinsic nano structure of filobactivirus and its property of capsid protein, filobactivirus is mixed with divalent manganesetion, normal-temperature reaction is so that filobactivirus Surface Creation manganese dioxide after adding NaOH, so as to obtain the manganese dioxide nanowire of the nm of diameter 10 50.The material has imitative enzymatic characteristic and electrochemical catalysis characteristic simultaneously, it is had broad application prospects in analytical chemistry, capacitor and catalytic field.The method is with natural biological nanostructures as template, and preparation process is simple, reaction condition is gently environmentally friendly, and nanostructured is easily-controllable.
Description
Technical field
The present invention relates to nano material, catalysis and analytical chemistry field, specifically include a kind of based on the preparation method and its application in terms of catalysis, capacitor, chromogenic assay, electrochemical sensing that filobactivirus is biological templated synthesis manganese dioxide nanowire.
Background technology
Nano material refers at least one-dimensional in nanoscale scope in three dimensions（1−100 nm）Material.Nano wire refers to that one kind is limited in less than 100 nanometers in the horizontal（Longitudinal direction does not limit）One-dimentional structure nano material.
In recent years, manganese dioxide has caused the extensive concern in each field as a kind of metal oxide with essential industry purposes.Scientific research personnel has synthesized the nanometer electrode manganese dioxide of different-shape using various methods, by its unique structure and performance, has been widely used in the fields such as battery, magnetic material, catalyst.Boppana et al. exists《Nanostructured MnO2:
an efficient and robust water oxidation catalyst》MnO is synthesized using hydro-thermal method in one text2Nano wire and nanotube, and as catalyst（Chemical
Communications 2011,47,8973-8975）.Hsu et al. exists《Reversible phase transformation of MnO2 nanosheets in an electrochemical capacitor investigated by
in situRaman spectroscopy》MnO is synthesized using electrochemical deposition method in one text2Nanometer sheet, and use it for capacitor（Chemical
Communications 2011,47,1252-1254）.Dongale et al. exists《Development of nano fiber MnO2
thin film electrode and cyclic voltammetry behavior
modeling using artificial neural network for supercapacitor
application》MnO is synthesized using Polarization technique in one text2Nano wire, and it is used as ultracapacitor（Materials Science in Semiconductor Processing 2015,36,43-48）.Pan et al. exists《Green and
large-scale one-pot synthesis of small-sized graphene-bridged
manganese dioxide nanowire network as new electrode
material for electrochemical sensing》Middle utilization hydro-thermal method has synthesized MnO2Nano wire, and use it for electrochemical sensor（Journal of Sol-Gel Science and
Technology2015,76,341-348）.But, the synthesis of these nano material of manganese dioxide generally requires HTHP, complicated process or equipment, and the size and pattern of material and is difficult to control, easily reunite poor dispersion.Therefore, how homogeneous, the stable nanometer MnO of pattern is obtained using the synthesis of simple method and apparatus in a mild condition2Material is a meaningful job.
Biological template nano material, belongs to Bio-Nano-Materials, i.e., with various natural biomaterials as template, simulate biomineralization process, material of the generation with nanostructured.Biological template method avoids the nano material synthesis step of the use, not gentle synthesis condition and complexity of organic reagent.The Nature full of glamour gives people to provide abundant natural biological template（Such as：Protein, DNA, cell, bacteriophage）.Found through the retrieval to existing document, scientific research personnel utilizes filamentous form virus（Such as：M13 bacteriophages, TMV viruses）Make the various nano wires of templated synthesis, noble metal, transition metal inorganic salts, oxide or sulfide can grow to realize the structure control of nano wire on linear template.Shenton et al. exists《Inorganic–organic nanotube composites from template mineralization of tobacco
mosaic virus》CdS, PbS, ferriferous oxide, SiO are synthesized using TMV viruses in one text2Nano wire（Advanced Materials, 1999,11,253 256）.Mao et al. exists《Virus-based toolkit for the directed synthesis of
magnetic and semiconducting nanowires》Filobactivirus is utilized in one text, by gene regulation, has synthesized ZnS, CdS, CoPt, FePt nano wire（Science
2004,303,213 217）.Nam et al. exists《Peptide-mediated reduction of silver ions on engineered
biological scaffolds》Make templated synthesis Ag nano wires using M13 bacteriophages in one text（ACS Nano, 2008,2,1,480 1486）.Nam et al. exists《Virus-enabled
synthesis and assembly of nanowires for lithium ion
battery electrodes》M13 bacteriophage templated synthesis Co is utilized in one text3O4Nano wire（Science
2006,312,885 888）.Oh et al. exists《M13 virus-directed synthesis of nanostructured
metal oxides for lithium–oxygen batteries》Make templated synthesis Co using M13 bacteriophages in one text3O4Nano wire（Nano Letters 2014,14,4837-4845）.
In sum, the various inorganic nanowires based on filamentous form virus are synthesized, and this template reaction condition is gentle, simple to operate, and the nanotopography of preparation is homogeneous, good biocompatibility.Regrettably, so far, the MnO based on filamentous form virus template or other biological template2There is not been reported for the gentle preparation of nano wire.
The content of the invention
It is an object of the invention to provide a kind of preparation method and applications of the manganese dioxide nanowire based on filobactivirus biological template.
To achieve the above object, the technical solution adopted by the present invention is：
It is a kind of based on the preparation method that filobactivirus is biological templated synthesis manganese dioxide nanowire, it is characterised in that the method comprises the following steps：
(1) filobactivirus is well mixed with the aqueous solution containing divalent manganesetion, stands a period of time；
(2) to adding a certain amount of alkali lye in above-mentioned mixed solution and mixing, oscillating reactions generates yellowish-brown suspension afterwards for a period of time；
(3) above-mentioned reaction solution is centrifuged, removes the supernatant containing unreacted component, collect precipitation, 4 °C preserve with standby；Also purifying manganese dioxide nanowire can be collected by the method dialysed or filter.
Preferably, the aqueous solution containing divalent manganesetion can be formulated by manganese acetate, manganese chloride, manganese sulfate, manganese nitrate etc.；The alkali lye can be formulated by NaOH, potassium hydroxide, ammoniacal liquor etc..
The application of above-mentioned manganese dioxide nanowire, it is characterised in that：The manganese dioxide nanowire has the catalysis activity of imitative peroxidase, can be used as the catalyst of analysis detection.
Preferably, the manganese dioxide nanowire can be used for H as catalyst2O2Detection.
It is further to be preferably, the detection H2O2When add organicvisualization reagent；The organicvisualization reagent is 2,2 '-connection nitrogen-bis-（3- ethyl benzo thiazole phenanthroline -6- sulfonic acid）Diamine salts（ABTS）Or 3,3 ', 5,5 '-tetramethyl benzidine（TMB）.
The application of above-mentioned manganese dioxide nanowire, it is characterised in that：The manganese dioxide nanowire has electrochemical catalysis activity, the application of the catalyst that can be analyzed as qualitative/quantitative.
Preferably, the manganese dioxide nanowire can be used for H as electrochemical catalyst2O2Electrochemical Detection.
It is further to be preferably, detect H2O2When, using three-electrode system, it is placed on and contains various concentrations H2O2PBS solution in, the speed of sweeping with 25 mV/s under the electrochemical window of -0.2+0.8 V is circulated voltammetric determination.H is determined by peak current response2O2Concentration.
The three-electrode system is included manganese dioxide nanowire modified electrode（Working electrode）, saturated calomel electrode（Reference electrode）, platinum electrode（To electrode）.
The manganese dioxide nanowire modified electrode preparation method is as follows, and manganese dioxide nanowire is distributed in water.Then, dispersant liquid drop is coated in the good glassy carbon electrode surface of pre-polish(ing), dries and obtain final product manganese dioxide nanowire modified electrode.
Effect of the invention is：
1. the present invention utilizes biological template method and one-step synthesis method manganese dioxide nanowire, and synthetic method is simple, gentle, environmental protection, and the manganese dioxide nanowire pattern for obtaining is homogeneous（The nm of diameter 10 50,0.8 1.8 μm of length）, and with good dispersiveness and stability, the shortcomings of the process that solves the manganese dioxide nanowire of conventional method synthesis is complicated, energy consumption is big, nano wire pattern is difficult to control to.
2. the manganese dioxide nanowire of the filobactivirus template in the present invention has the catalysis activity and electro catalytic activity of imitative peroxidase, due to the dimensional effect of nano wire, its catalysis activity is apparently higher than the manganese dioxide nanowire without synthesis in the presence of filobactivirus, therefore the manganese dioxide nanowire can be used for H as catalyst2O2Color developing detection and Electrochemical Detection.
3. it is nontoxic to human body because biological template of the present invention is M13 bacteriophages, it is a kind of biological template of environmental protection.Also, there is good biocompatibility by the manganese dioxide nanowire that biological template method synthesizes, will be had a good application prospect in biochemical analysis fields such as biomarker, immunoassay, bio-sensings.
Brief description of the drawings
Fig. 1 prepares reaction solution photo for material provided in an embodiment of the present invention；
Fig. 2 is the transmission electron microscope photo of manganese dioxide nanowire provided in an embodiment of the present invention；
Fig. 3 is the Mimicry enzyme design sketch with ABTS as substrate of manganese dioxide nanowire provided in an embodiment of the present invention；
Fig. 4 is the Mimicry enzyme design sketch with TMB as substrate of manganese dioxide nanowire provided in an embodiment of the present invention；
Fig. 5 is the pH effect of optimization figures of manganese dioxide nanowire provided in an embodiment of the present invention；
The temperature stability design sketch of Fig. 6 manganese dioxide nanowire Mimicry enzymes provided in an embodiment of the present invention.
Fig. 7 is development process quantitative determination H provided in an embodiment of the present invention2O2Standard working curve；
Fig. 8 is the electro-chemical activity design sketch of manganese dioxide nanowire provided in an embodiment of the present invention.Curve a, b are respectively bare electrode in the H containing 0,300 μM2O2PBS solution in cyclic voltammogram.Curve c, d, e are respectively manganese dioxide nanowire modified electrode in the H containing 0,100,200,300 μM2O2PBS solution liquid in cyclic voltammogram.
Fig. 9 is that electrochemical sensing standard measure provided in an embodiment of the present invention detects H2O2Cyclic voltammogram.
Figure 10 is that electrochemical sensing standard measure provided in an embodiment of the present invention detects H2O2Standard working curve.
Specific embodiment
In order in depth illustrate present disclosure, some embodiments will be further enumerated below, but the present invention is not limited to cited embodiment.Specific experiment condition or method are for example unreceipted in the following example, are carried out by the normal condition or method of this area.
Embodiment 1
The preparation of M13 bacteriophages：
Take 1 μ L phasmid PC89 solution, conversion is to e. coli tg1 competent cell, single bacterium colony is chosen after flat board culture to be inoculated in the SOC nutrient solutions of 2 mL Amp resistances, 37 °C of h of shaken cultivation 2, it is transferred in the SOC nutrient solutions of 400 mL Amp resistances, 37 °C of shaken cultivations, when the absorbance of 600 nm is about 0.4, add about 1 × 10 to nutrient solution12Individual helper phage M13KO7, the h of shaken cultivation 1, add the kanamycins of final concentration of 25 μ g/mL and the isopropyl-β-d- thiogalactosides of final concentration of 1 mM, and 37 °C of shaken cultivations are overnight.
Embodiment 2
The purification of M13 bacteriophages：
Nutrient solution is placed in 70 °C of min of water-bath 20,50 mL centrifuge tubes are then sub-packed in, 15 min are centrifuged（Rotating speed 5000rpm）, collect supernatant；PEG8000 to 40 g/L, NaCl to 30 g/L, the h of ice bath 1 are added, 5 min are centrifuged in 4 °C（Rotating speed 12000rpm）, abandon supernatant；Precipitate and dissolved with the PBS of 5 mL, 5 min are centrifuged in 4 °C（Rotating speed 12000rpm）, discard insoluble matter.It is repeated 1 times by the above process, collects supernatant, 4 °C of preservations.The concentration of M13 bacteriophages is determined by the method for common painting number of plates plaque in supernatant.
Embodiment 3
The preparation of the manganese dioxide nanowire based on filobactivirus M13 templates：
(1) filobactivirus is well mixed with the aqueous solution of manganese acetate, stands 1 h；
(2) to adding the aqueous solution of NaOH in above-mentioned mixed solution and mixing, yellowish-brown suspension is generated after the h of oscillating reactions 24；
(3) above-mentioned reaction solution is centrifuged, removes the supernatant containing unreacted component, collect precipitation, 4 °C preserve with standby；Also purifying manganese dioxide nanowire can be collected by the method dialysed or filter.
Separately do a control experiment：Synthesize manganese dioxide in the presence of without M13 bacteriophages, other experiment conditions and step are identical with above-mentioned experiment.
As shown in Figure 1, the mixed reaction solution of M13 bacteriophages and manganese acetate produces a large amount of precipitations after being acted on through NaOH, and control experiment to go out only produce a small amount of precipitation, illustrates under conditions of no M13 bacteriophages template, the generation of manganese dioxide lacks nucleation site, and the manganese dioxide solid of generation is less；And M13 bacteriophages template provides substantial amounts of nucleation site to the generation of manganese dioxide, manganese dioxide is formed on M13 surfaces and crystallized, manganese dioxide nanowire is generated, this phenomenon also illustrate that M13 phage surfaces capsid protein has the property interacted with manganese ion or manganese dioxide.The preparation method of this nano wire is simply controllable, so as to solve the problems, such as that manganese dioxide nanowire is difficult to prepare.
Embodiment 4
The morphology analysis of manganese dioxide nanowire：
By the hanging drop of manganese dioxide nanowire on copper mesh, room temperature dry after using its pattern of tem study.
As shown in Fig. 2 the manganese dioxide nanowire for obtaining maintains original linear structure of M13, pattern is homogeneous, the nm of diameter 10 50, length 0.8 1.8
µm。
Embodiment 5
The Mimicry enzyme of manganese dioxide nanowire：
Experimental system a：Catalystic converter system is comprising H2O2（5 mM）, above-described embodiment obtain manganese dioxide nanowire（5 µg）, organicvisualization reagent ABTS（3 mM）Acetate buffer solution（pH 3.5）.In room temperature（25 °C）After lower reaction 10 minutes, it is the spectrogram in the range of 380 500 nm to record it in wavelength using ELIASA.
Separately do three control experiments：Control experiment b, manganese dioxide nanowire is replaced with equivalent without the manganese dioxide synthesized in the presence of M13 bacteriophages, and spectrogram is recorded after being reacted 10 minutes under with above-mentioned experimental system similarity condition；Control experiment c, without manganese dioxide nanowire, spectrogram is recorded after standing 10 minutes under with above-mentioned experimental system similarity condition；Control experiment d, manganese dioxide nanowire is replaced with equivalent without the manganese dioxide synthesized in the presence of M13 bacteriophages, and spectrogram is recorded after standing 10 minutes under with above-mentioned experimental system similarity condition.
As shown in figure 3, experimental system a shows obvious peak near 416 nm, it is higher by much than experimental system c, illustrates that manganese dioxide nanowire has the activity of obvious imitative peroxidase；Control experiment b has weaker peak near 416 nm, illustrates that the catalysis activity without the manganese dioxide synthesized in the presence of M13 bacteriophages is low compared with Template synthesis manganese dioxide nanowire；The response curve of control experiment d is similar to control experiment c, illustrates M13 in itself without catalysis activity.In sum, experiment shows that the manganese dioxide nanowire of present invention preparation has good catalysis activity.
Further to prove the Mimicry enzyme of manganese dioxide nanowire, do substrate with another organicvisualization reagent TMB to replace ABTS, respectively with manganese dioxide nanowire（Experimental system a）, without in the presence of M13 bacteriophages synthesize manganese dioxide（Experimental system b）, water（Experimental system c）Make catalyst, other experiment conditions are consistent with above-mentioned experiment.
As shown in Figure 4, experimental system a shows obvious peak near 652 nm, and experimental system b, c near 652 nm without obvious peak, illustrate manganese dioxide nanowire there is the activity of obvious imitative peroxidase and without the manganese dioxide synthesized in the presence of M13 bacteriophages to TMB catalytically inactives.
Embodiment 6
The pH optimizations of manganese dioxide nanowire Mimicry enzyme：
Catalystic converter system is comprising H2O2（5 mM）, manganese dioxide nanowire（5 µg）, organicvisualization reagent ABTS（3 mM）Different pH buffer solution（PH 2.0, glycine-HCI buffer solution；PH 3.0 6.0, Acetic acid-sodium acetate buffer solution；PH 7.0 8.0, phosphate buffer；PH 9.0 10.0, Tris- hydrochloride buffer；PH 11.0 12.0, sodium acid carbonate-sodium hydrate buffer solution）.In room temperature（25 °C）After lower reaction 10 minutes, the light absorption value in its 416 nm is detected using spectrophotometer.As shown in figure 5, manganese dioxide nanowire is in pH
Optimal peroxidase activity is shown at 3.5.
Embodiment 7
The temperature stability of manganese dioxide nanowire Mimicry enzyme：
The aqueous solution of manganese dioxide nanowire is in different temperatures（4−90 °C）It is lower to be incubated 2 hours.Then, manganese dioxide nanowire is added in catalystic converter system, detects it 416
Light absorption value at nm, as shown in fig. 6, less than the 70 °C manganese dioxide nanowires being incubated almost retain whole vigor, and the manganese dioxide nanowire being incubated under 90 °C also remains more than 80% vigor.
Embodiment 8
H2O2Development process quantitative determination：
Catalystic converter system is the H comprising various concentrations2O2（0−600
µM）, manganese dioxide nanowire（5 µg）, organicvisualization reagent ABTS（3 mM）Acetic acid-sodium acetate buffer solution（pH 3.5）.In room temperature（25 °C）After lower reaction 10 minutes, the light absorption value in its 390 550 nm is detected using ELIASA.H is drawn out by the light absorption value of 416 nm2O2Standard working curve.As shown in fig. 7,20 400 μM of the range of linearity.
Embodiment 9
The modification of electrode and application method：
(1) glass-carbon electrode（GCE）Pretreatment：First by glass-carbon electrode successively with 1.0,0.3,0.05 μm of Al2O3Polishing powder carries out sanding and polishing in flat mirror, is then cleaned with absolute ethyl alcohol, ultra-pure water successively, dries stand-by.
(2) preparation of manganese dioxide nanowire modified electrode：First, the manganese dioxide nanowire of 250 μ g is distributed in the water of 1 mL.Then, the dispersant liquid drop for drawing 10 μ L is coated on the GCE electrode surfaces for having pre-processed, and room temperature is dried, and obtains final product manganese dioxide nanowire modified electrode.
(3) application method of electrode：Using manganese dioxide nanowire modified electrode or bare electrode as working electrode, saturated calomel electrode as reference electrode, platinum electrode as to electrode, so as to constitute three-electrode system.Three-electrode system is placed in and contains various concentrations H2O2PBS solution in, the speed of sweeping with 25 mV/s under the electrochemical window of -0.2+0.8 V is circulated voltammetric determination.
Embodiment 10
The checking of electro-chemical activity：
By above-mentioned experimental procedure, test manganese dioxide nanowire modified electrode and bare electrode are to H2O2Electro catalytic activity.As shown in figure 8, with H2O2The increase of concentration, oxidation peak current of the manganese dioxide nanowire at+0.65 V（i pa）Response gradually rises, and bare electrode does not have obvious peak and electric current is without significant change.Illustrate manganese dioxide nanowire of the invention to H2O2With certain electro catalytic activity.
Embodiment 11
H2O2Electrochemical sensing standard measure detection：
In H2O2Concentration is 0 600
In the range of μM, the cyclic voltammetry curve of manganese dioxide nanowire modified electrode is determined by the methods described of embodiment 9（Fig. 9）, by 0.65 V oxidation peak currents（i pa）Deduct blank（Without H2O2When）Electric current（Δi pa）After draw out H2O2Standard working curve.As shown in Figure 10, the range of linearity 5 500
µM。
Claims (10)
1. it is a kind of based on the preparation method that filobactivirus is biological templated synthesis manganese dioxide nanowire, it is characterised in that the method comprises the following steps：
(1) filobactivirus is well mixed with the aqueous solution containing divalent manganesetion, stands a period of time；
(2) to adding a certain amount of alkali lye in above-mentioned mixed solution and mixing, oscillating reactions is for a period of time；
(3) above-mentioned reaction solution is centrifuged, removes the supernatant containing unreacted component, collect precipitation, 4 °C preserve with standby；Also purifying manganese dioxide nanowire can be collected by the method dialysed or filter.
2. the preparation method of the manganese dioxide nanowire as described in claim 1, it is characterised in that the aqueous solution containing divalent manganesetion can be formulated by manganese acetate, manganese chloride, manganese sulfate, manganese nitrate etc.；The alkali lye can be formulated by NaOH, potassium hydroxide, ammoniacal liquor etc..
3. the manganese dioxide nanowire as described in claim 1 or 2, it is characterised in that：The manganese dioxide nanowire has the characteristic of imitative enzymatic, the catalyst that can be analyzed as qualitative/quantitative.
4. the application of the manganese dioxide nanowire as described in claim 3, it is characterised in that：The manganese dioxide nanowire can be used for H as catalyst2O2Development process detection and medical catalyst.
5. the application of the manganese dioxide nanowire as described in claim 4, it is characterised in that：The detection H2O2When add organicvisualization reagent；The organicvisualization reagent is 2,2 '-connection nitrogen-bis-（3- ethyl benzo thiazole phenanthroline -6- sulfonic acid）Diamine salts（ABTS）Or 3,3 ', 5,5 '-tetramethyl benzidine（TMB）.
6. the manganese dioxide nanowire as described in claim 1 or 2, it is characterised in that：The manganese dioxide nanowire has electrochemical catalysis characteristic, can be used as the electrode material of capacitor.
7. the application of the manganese dioxide nanowire as described in claim 1 or 2, it is characterised in that：The manganese dioxide nanowire can be used for H as electrochemical catalyst2O2Electrochemical Detection.
8. the application of the manganese dioxide nanowire as described in claim 7, it is characterised in that：Detection H2O2When, using three-electrode system, contain various concentrations H2O2Be placed in PBS solution, be circulated voltammetric determination under the electrochemical window of -0.2+0.8 V, by oxidation peak current response determine H2O2Concentration.
9. the application of the manganese dioxide nanowire as described in claim 8, it is characterised in that：The three-electrode system is included manganese dioxide nanowire modified electrode（Working electrode）, saturated calomel electrode（Reference electrode）, platinum electrode（To electrode）.
10. the application of the manganese dioxide nanowire as described in claim 9, it is characterised in that：The manganese dioxide nanowire modified electrode preparation method, manganese dioxide nanowire is distributed in water, then, is drawn dispersant liquid drop and is coated in the glassy carbon electrode surface for having pre-processed, and is dried and is obtained final product manganese dioxide nanowire modified electrode.
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