CN102825261A - Binary plasma nanoparticle site specificity self-assembling method - Google Patents
Binary plasma nanoparticle site specificity self-assembling method Download PDFInfo
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- CN102825261A CN102825261A CN2012103696487A CN201210369648A CN102825261A CN 102825261 A CN102825261 A CN 102825261A CN 2012103696487 A CN2012103696487 A CN 2012103696487A CN 201210369648 A CN201210369648 A CN 201210369648A CN 102825261 A CN102825261 A CN 102825261A
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Abstract
A binary plasma nanoparticle site specificity self-assembling method belongs to the technical field of material chemistry. The method comprises the following steps of: synthetising gold nanoparticles; synthetising gold nanorods; decorating DNA1 by using the gold nanoparticles; decorating DNA2 by using the gold nanorods; forming a DNA composite connecting arm; and assembling the gold nanoparticles and the gold nanorods. According to the invention, two important plasma nanoparticles, i.e. the gold nanoparticles and the gold nanorods are selected to prepare a discrete binary self-assembling body. The gold nanorods have space geometry and chemical anisotropy, so that the physical properties and the chemical properties of the gold nanorods in different space sites are different. Therefore, the technical method for controlling the space site specificity of binary gold nanomaterials is very important. The method provided by the invention has the advantage that a binary gold nanomaterial assembling body with uniform and controllable structure and sites as well as high yield is prepared.
Description
Technical field
The method of a kind of binary plasma nano particle locus specificity self assembly belongs to material chemistry technical field.
Background technology
Self assembly refers to spontaneous the accumulation in order of basic construction unit and forms ordered structure and express a kind of technology of synergistic function.In this process, the structure that spontaneous tissue or gathering become a geometry appearance stable, that have certain rule under the interaction of basic construction unit through non-covalent bond.In this process, between some structures simultaneously spontaneous generation related and flock together and form an orderly overall structure, this is the simple superposition of weak force between a kind of synergy but not a large amount of atom, the lewis' acid of complicacy of integral body.This basic construction unit generally refers to nano material, micro materials or molecule.Self assembly is one of the most popular in recent years research theme.
Gold nanorods is a kind of bar-shaped golden nanometer particle, and its size generally arrives up to a hundred nanometers in several nanometers.Conduction band electron on the single gold nanorods is owing to exist along the direction of two resonance of the long axis direction of the major axis of rod and vertical bars and also just have two surface plasma peaks---vertically plasma peak and horizontal plasma peak.The preparation method of gold nanorods mainly contains electrochemical method, photochemical method, template and seeded growth method.Advantages such as wherein seeded growth method preparation method is simple, and productive rate is high, and repeatability is strong make becomes the preparation method of at present popular a kind of gold nanorods.Owing to having used softex kw in the process that is equipped with gold nanorods in the seeded growth legal system; And this surfactant is different to the binding ability of the different facial of gold nanorods; The side that is gold nanorods combines densely; End face at gold nanorods then combines comparatively sparsely; Make gold nanorods have space geometry and chemical anisotropy simultaneously, and regulate the longitudinal resonance peak of gold nanorods, make the controllable adjustment of its surface plasma peak of realization at visible light and near infrared region through the draw ratio (being the ratio of diameter of length and the gold nanorods of gold nanorods) that the addition that changes silver nitrate changes gold nanorods.Because of these unique character make gold nanorods can realize as the good raw material of controlled self-assembled material.Golden nanometer particle since faraday in 1857 prepared gold nano colloidal sol for the first time through method of reducing and to its character Primary Study since; Always because its special optical property; The preparation method's is simple, controlled; Stable in properties, bio-compatibility is good etc., and advantage becomes one of research focus that does not go downhill permanently.
Because the self-assembly of plasma nano material has very strong plasma coupling effect; Cause good properties such as electromagnetic field enhancing; Binary plasma nano material shows the fascinating character that is different from two kinds of independent plasma nano materials in self-assembled material, make binary plasma nano material become one of research focus.At present the bielement nano particle assembling mainly concentrates on the bielement nano particle irregularly in the formation of aggregation, and discrete assembly rarely has report.But discrete self-assembled material is inconsistent with the character of the aggregation of bielement nano particle again; For example on the chirality of the assembly of nano material; The self-assembled material of discrete controlled nano particle is different fully with its bigger character that aggregation showed, therefore the discrete binary assembly of preparation be necessary fully also be essential.Therefore, we select gold nanorods and these two kinds important plasma nano particles of golden nanometer particle to prepare discrete binary self-assembly.Of preamble; Gold nanorods has space geometry and chemical anisotropy; Make that the gold nanorods different physical property that the site had and chemical property on its space is different, space locus specificity therefore how to control the binary gold nano-material seems particularly important.
Summary of the invention
The purpose of this invention is to provide the method for a kind of binary plasma nano particle locus specificity self assembly, prepare structure and site homogeneous, controlled, the binary gold nano-material assembly that productive rate is high.
Technical scheme of the present invention: the method for a kind of binary plasma nano particle locus specificity self assembly; Comprise that golden nanometer particle is synthetic; Gold nanorods is synthetic, golden nanometer particle modifying DNA 1, gold nanorods modifying DNA 2; The formation of the compound linking arm of DNA, gold nanorods and golden nanometer particle assembling and sign.
Processing step:
(1) golden nanometer particle is synthetic
Golden nanometer particle is synthetic to adopt trisodium citrate to reduce the golden nanometer particle of the synthetic 18nm of three hydration tetra chlorauric acids.
(2) gold nanorods is synthetic
The synthetic synthetic 16nm of the seeded growth method * 50nm gold nanorods that adopts of gold nanorods.
(3) the golden nanometer particle modifying DNA 1
The golden nanometer particle that step (1) is synthesized and the DNA1 of sulfydryl modification carry out the compound that coupling forms golden nanometer particle-DNA1.
(4) the gold nanorods end face is modified
The synthetic gold nanorods of step (2) is modified the compound of the end face formation gold nanorods-DNA2 of gold nanorods through the DNA2 of a certain amount of sulfydryl modification.
(5) formation of the compound linking arm of DNA
Through adding of the locus specificity assembling of corresponding single stranded DNA phase mutual cross in the hybridization buffer formation compound linking arm of DNA with control golden nanometer particle and gold nanorods.Used DNA is DNA3 and DNA4.
(6) assembling of gold nanorods and golden nanometer particle and sign
Step (3) gained golden nanometer particle-DNA1 compound and step (4) gained gold nanorods-DNA2 compound are assembled in hybridization buffer and are formed the end face that golden nanometer particle is assembled into gold nanorods.Adopt TEM that this assembling product is characterized.
The numbering of table 1 DNA, sequence and length
| Numbering | Sequence (5 '-3 ') | Length |
| DNA1 | TAACAATAATCCCTCAAAAAAAAAA-SH | 25 |
| DNA 2 | CGTTAGGACTTACGCAAAAAAAAAA-SH | 25 |
| DNA 3 | GAGGGATTATTGTTACGTTAGGACTTACGCAAAAAAAAAA-NH 2 | 40 |
| DNA 4 | GCGTAAGTCCTAACG | 15 |
Annotate: DNA used in the present invention all gives birth to worker's bioengineering Co., Ltd available from Chinese Shanghai, and carries out purifying through polyacrylamide gel electrophoresis.
Beneficial effect of the present invention: the present invention selects gold nanorods and these two kinds important plasma nano particles of golden nanometer particle to prepare discrete binary self-assembly.Gold nanorods has space geometry and chemical anisotropy; Make that the gold nanorods different physical property that the site had and chemical property on its space is different, therefore solve the site-specific technical method in space how to control the binary gold nano-material and seem particularly important.The method of binary plasma nano particle locus specificity provided by the invention self assembly is prepared structure and site homogeneous, and is controlled, the binary gold nano-material assembly that productive rate is high.
Description of drawings
The assembling assumption diagram of the typical bielement nano particle assembling of Fig. 1 body.
The specific embodiment
Embodiment 1
(1) golden nanometer particle is synthetic
The synthetic schemes of golden nanometer particle is: the ultra-pure water that adds 95mL in the clean conical flask; The concentration that then in ultra-pure water, adds 5mL is the three hydration tetra chlorauric acids of 2g/L, and heating is boiled; And then the freshly prepared citric acid three sodium solution that adds 2.5mL mass concentration 1%; Heat while stirring, solution colour is from the faint yellow redness that becomes, and constantly boiling reacts 10 min.At last, solution is cooled to room temperature, is diluted to 100mL, 4 ℃ of preservations.Promptly make the solution of gold nanoparticles of 18nm.
(2) gold nanorods is synthetic
The growth of
gold nanorods: seed solution carries out the growth of gold nanorods after synthesizing well.The three hydration tetra chlorauric acid solution of the 2g/L of 5mL join in the 0.2 M softex kw solution of 5mL, add the ultra-pure water of 4mL, mixing.0.125mL 0.01M silver nitrate (AgNO
3) solution joins in the above-mentioned mixed system, mixing, the 0.1M ascorbic acid solution with 65 μ L adds above-mentioned system solution subsequently, 28 ℃ of following stirring reaction 2 min, solution is become colourless by brown.At last, the soft stirring and evenly mixing 20s of seed-solution that adds 0.05mL.28 ℃ of reaction 4h.Promptly get gold nanorods solution.
(3) the golden nanometer particle modifying DNA 1
⑴ with the centrifugal 10min of golden nanometer particle 10000r/min of the 10mL of step (1) preparation, and deposition is with the aqueous dispersion of 1mL, and 10000r/min is centrifugal, and 10min abandons supernatant, contains the PBS buffer solution dispersion of 0.01M of the pH8.0 of 0.01%SDS with 1mL, 4 ℃ of preservations, for use.
⑵ get the golden nanometer particle 100 μ L that above-mentioned ⑴ prepares, and adds the DNA1 of 12 μ L, 100 μ M, mixing; Behind the jolting reaction 20min; The PBS buffer solution of 0.01M with the pH8.0 of the NaCl that contains 0.01%SDS and 2M adds in the reaction system, makes NaCl concentration reach 50mM, ultrasonic 10s; Jolting reaction 20min continued adds this buffer solution to reaction system; Make NaCl concentration reach 100mM, when repeating above-mentioned course of reaction NaCl concentration reach 0.7M to system according to the gradient of every increase by 100 mM of NaCl concentration subsequently, room temperature jolting reaction 12h.
⑶ at the centrifugal 10min of 8000r/min, abandon supernatant with reaction solution among the above-mentioned steps ⑵, and the back disperses deposition with 0.01% the SDS of 100 μ L, and the back with the solution cleaning of 0.01% SDS once 4 ℃ of preservations, gets golden nanometer particle-DNA1 compound, and is for use.
(4) gold nanorods end face modifying DNA 2
Get the DNA2 that gold nanorods 10 μ L that step (2) prepares add the 10 μ M of 1 μ L, mixing, room temperature jolting reaction 12h, the centrifugal 6min of 6000r/min; Abandon supernatant, with the aqueous dispersion of 10 μ L, washing once; 4 ℃ of preservations get gold nanorods-DNA2 compound, and are for use.
(5) formation of the compound linking arm of DNA
Get DNA3 and the DNA4 of the 1 μ M of 5 μ L respectively, add the pH7.5 of 15 μ L, the Tris-HCl hybridization buffer of 0.01M (contains 20mM MgCl
2, 0.01% SDS) in, mixing, standing and reacting 12h, 4 ℃ of preservations, for use.
(6) assembling of gold nanorods and golden nanometer particle and sign
Get the golden nanometer particle-DNA1 compound 5 μ L of preparation in the step (3) respectively, the compound linking arm 0.6 μ L of DNA of the gold nanorods-DNA2 compound 10 μ L of step (4) preparation and step (5) preparation joins the pH7.5 of 16 μ L, the Tris-HCl hybridization buffer of 0.01M (contains 20mM MgCl
2, 0.01% SDS) in, mixing, standing and reacting 12h.Assembling forms the end face that golden nanometer particle is assembled into gold nanorods in hybridization buffer.
The above-mentioned product that assembles is carried out the centrifugal 6min of 5000r/min, abandon supernatant, deposition heavily is distributed in the water of 30 μ L, and washing once.Electronic Speculum characterizes: the sample drop of the above-mentioned processing of 7 μ L is added on the copper mesh of carbon film support, under infrared lamp, carries out drying.The projection Electronic Speculum adopts the Electronic Speculum of JEOL JEM-2100 model, and its accelerating potential is 200 kV.
DNA1：5’-TAACAATAAT?CCCTCAAAAA?AAAAA-SH-3’，
DNA2：5’-CGTTAGGACT?TACGCAAAAA?AAAAA-SH?-3’，
DNA3：5’-GAGGGATTAT?TGTTACGTTA?GGACTTACGC?AAAAAAAAAA?-NH
2-3’，
DNA4：5’-GCGTAAGTCC?TAACG?-3’
Claims (1)
1. the method for binary plasma nano particle locus specificity self assembly; It is characterized in that comprising that golden nanometer particle is synthetic, gold nanorods is synthetic, golden nanometer particle modifying DNA 1; Gold nanorods modifying DNA 2; The formation of the compound linking arm of DNA, gold nanorods and golden nanometer particle assembling and sign, processing step:
(1) golden nanometer particle is synthetic
Golden nanometer particle is synthetic to adopt trisodium citrate to reduce the golden nanometer particle of the synthetic 18nm of three hydration tetra chlorauric acids: the ultra-pure water that adds 95mL in the clean conical flask; The concentration that then in ultra-pure water, adds 5mL is the three hydration tetra chlorauric acids of 2g/L, and heating is boiled; And then the citric acid three sodium solution that adds the freshly prepared mass concentration 1% of 2.5mL; Heat while stirring, solution colour is from the faint yellow redness that becomes, and constantly boiling reacts 10min; At last, solution is cooled to room temperature, is diluted to 100mL, and 4 ℃ of preservations promptly make the solution of gold nanoparticles of 18nm;
(2) gold nanorods is synthetic
The synthetic gold nanorods that adopts the synthetic 16nm * 50nm of seeded growth method of gold nanorods:
2. gold nanorods growth: seed solution carries out the growth of gold nanorods after synthesizing well, and the three hydration tetra chlorauric acid solution of the 2g/L of 5mL join in the 0.2 M softex kw solution of 5mL, adds the ultra-pure water of 4mL, mixing; 0.125 the 0.01M liquor argenti nitratis ophthalmicus of mL joins in the above-mentioned mixed system, mixing; 0.1M ascorbic acid solution with 65 μ L adds above-mentioned system solution subsequently, 28 ℃ of following stirring reaction 2 min, and solution is become colourless by brown; At last, add the soft stirring and evenly mixing 20s of seed-solution of 0.05mL, 28 ℃ of reaction 4h promptly get gold nanorods solution;
(3) the golden nanometer particle modifying DNA 1
The golden nanometer particle that step (1) is synthesized and the DNA1 of sulfydryl modification carry out coupling and form golden nanometer particle-DNA1 compound:
⑴ with the centrifugal 10min of golden nanometer particle 10000r/min of the 10mL of step (1) preparation, and deposition is with the aqueous dispersion of 1mL, and 10000r/min is centrifugal, and 10min abandons supernatant, contains the PBS buffer solution dispersion of 0.01M of the pH8.0 of 0.01%SDS with 1mL, 4 ℃ of preservations, for use;
⑵ get the golden nanometer particle 100 μ L that above-mentioned ⑴ prepares, and adds the DNA1 of 12 μ L, 100 μ M, mixing; Behind the jolting reaction 20min; The PBS buffer solution of 0.01M with the pH8.0 of the NaCl that contains 0.01%SDS and 2M adds in the reaction system, makes NaCl concentration reach 50mM, ultrasonic 10s; Jolting reaction 20min continued adds this buffer solution to reaction system; Make NaCl concentration reach 100mM, when repeating above-mentioned course of reaction NaCl concentration reach 0.7M to system according to the gradient of every increase by 100 mM of NaCl concentration subsequently, room temperature jolting reaction 12h;
⑶ at the centrifugal 10min of 8000r/min, abandon supernatant with reaction solution among the above-mentioned steps ⑵, and the back disperses deposition with 0.01% the SDS of 100 μ L, and the back with the solution cleaning of 0.01% SDS once 4 ℃ of preservations, gets golden nanometer particle-DNA1 compound, and is for use;
(4) gold nanorods end face modifying DNA 2
The synthetic gold nanorods of step (2) is modified the end face formation gold nanorods-DNA2 compound of gold nanorods through the DNA2 of a certain amount of sulfydryl modification:
Get the DNA2 that gold nanorods 10 μ L that step (2) prepares add the 10 μ M of 1 μ L, mixing, room temperature jolting reaction 12h, centrifugal 6 min of 6000r/min; Abandon supernatant, with the aqueous dispersion of 10 μ L, washing once; 4 ℃ of preservations get gold nanorods-DNA2 compound, and are for use;
(5) formation of the compound linking arm of DNA
Through adding of the locus specificity assembling of corresponding single stranded DNA phase mutual cross in the hybridization buffer formation compound linking arm of DNA with control golden nanometer particle and gold nanorods; Used DNA is DNA3 and DNA4; Get DNA3 and the DNA4 of the 1 μ M of 5 μ L respectively, what add 15 μ L contains 20mM MgCl
2In the Tris-HCl hybridization buffer of the pH 7.5 of 0.01% SDS, 0.01M, mixing, standing and reacting 12h, 4 ℃ of preservations, for use;
(6) assembling of gold nanorods and golden nanometer particle and sign
Get the golden nanometer particle-DNA1 compound 5 μ L of preparation in the step (3) respectively, the gold nanorods-DNA2 compound 10 μ L of step (4) preparation and the compound linking arm 0.6 μ L of DNA that step (5) prepares, what join 16 μ L contains 20mM MgCl
2In the Tris-HCl hybridization buffer of the pH 7.5 of 0.01% SDS, 0.01M, mixing, standing and reacting 12h; Assembling forms the end face that golden nanometer particle is assembled into gold nanorods in hybridization buffer;
Adopt TEM that this assembling product is characterized;
DNA1：5’-TAACAATAAT?CCCTCAAAAA?AAAAA-SH-3’，
DNA2：5’-CGTTAGGACT?TACGCAAAAA?AAAAA-SH?-3’，
DNA3：5’-GAGGGATTAT?TGTTACGTTA?GGACTTACGC?AAAAAAAAAA?-NH
2-3’，
DNA4：5’-GCGTAAGTCC?TAACG?-3’。
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| CN103341623A (en) * | 2013-06-25 | 2013-10-09 | 江南大学 | Method for preparing gold nanorod assemblies induced by static electricity acting force |
| CN104399974A (en) * | 2014-12-16 | 2015-03-11 | 天津工业大学 | Continuous control method for gold nanometer particle aggregate microstructure |
| CN104525938A (en) * | 2014-12-23 | 2015-04-22 | 国家纳米科学中心 | Molybdenum disulfide/gold nanorod composite, preparation method and application |
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| CN110586949A (en) * | 2019-10-23 | 2019-12-20 | 四川大学 | Gold nanorod modification method and DNA-modified gold nanorod |
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| CN102127542A (en) * | 2010-12-27 | 2011-07-20 | 江南大学 | Preparation method of self-assembly material having surface-enhanced Raman activity |
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| CN103341623A (en) * | 2013-06-25 | 2013-10-09 | 江南大学 | Method for preparing gold nanorod assemblies induced by static electricity acting force |
| CN104399974A (en) * | 2014-12-16 | 2015-03-11 | 天津工业大学 | Continuous control method for gold nanometer particle aggregate microstructure |
| CN104525938A (en) * | 2014-12-23 | 2015-04-22 | 国家纳米科学中心 | Molybdenum disulfide/gold nanorod composite, preparation method and application |
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| CN110586949A (en) * | 2019-10-23 | 2019-12-20 | 四川大学 | Gold nanorod modification method and DNA-modified gold nanorod |
| CN110586949B (en) * | 2019-10-23 | 2021-01-05 | 四川大学 | Gold nanorod modification method and DNA-modified gold nanorod |
| CN111085692A (en) * | 2019-12-27 | 2020-05-01 | 季华实验室 | Irregular alloy nano material synthesis method based on high-temperature water phase reaction |
| CN111408732A (en) * | 2020-04-23 | 2020-07-14 | 江南大学 | Method for synthesizing chiral nano material by utilizing DNA induction and chiral light auxiliary growth |
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Application publication date: 20121219 |