CN111422824B - Orientation method of anisotropic nano material - Google Patents

Orientation method of anisotropic nano material Download PDF

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CN111422824B
CN111422824B CN202010377954.XA CN202010377954A CN111422824B CN 111422824 B CN111422824 B CN 111422824B CN 202010377954 A CN202010377954 A CN 202010377954A CN 111422824 B CN111422824 B CN 111422824B
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anisotropic
orientation
nano
polymer material
solvent
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CN111422824A (en
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刘言军
何慧琳
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Southwest University of Science and Technology
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B81—MICROSTRUCTURAL TECHNOLOGY
    • B81C—PROCESSES OR APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OR TREATMENT OF MICROSTRUCTURAL DEVICES OR SYSTEMS
    • B81C1/00—Manufacture or treatment of devices or systems in or on a substrate
    • B81C1/00015—Manufacture or treatment of devices or systems in or on a substrate for manufacturing microsystems
    • B81C1/00206—Processes for functionalising a surface, e.g. provide the surface with specific mechanical, chemical or biological properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B81—MICROSTRUCTURAL TECHNOLOGY
    • B81C—PROCESSES OR APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OR TREATMENT OF MICROSTRUCTURAL DEVICES OR SYSTEMS
    • B81C1/00—Manufacture or treatment of devices or systems in or on a substrate
    • B81C1/00349—Creating layers of material on a substrate
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y40/00—Manufacture or treatment of nanostructures
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D11/00—Inks
    • C09D11/02—Printing inks
    • C09D11/03—Printing inks characterised by features other than the chemical nature of the binder
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D11/00—Inks
    • C09D11/02—Printing inks
    • C09D11/10—Printing inks based on artificial resins
    • C09D11/106—Printing inks based on artificial resins containing macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds
    • C09D11/108—Hydrocarbon resins

Abstract

The invention provides an orientation method of an anisotropic nanomaterial. The orientation method comprises the following steps: dispersing the anisotropic nano material and the high polymer material in a solvent to obtain nano ink; the anisotropic nano material, the high polymer material and the solvent are compatible; and directly writing the obtained nano ink on a substrate, and drying to form an anisotropic nano material film oriented along the direct writing direction. The orientation method provided by the invention utilizes intermolecular acting force of the high polymer material and the anisotropic nano material and shearing force generated by direct writing to promote the orientation of the anisotropic nano material, and has the advantages of simple operation, high orientation speed, flexible and controllable orientation direction, high orientation degree, capability of realizing graphical orientation and convenience for industrial large-scale application.

Description

Orientation method of anisotropic nano material
Technical Field
The invention belongs to the technical field of oriented nano materials, and particularly relates to an orientation method of an anisotropic nano material.
Background
With the rapid development of the information industry, information transmission and information security have attracted a great deal of attention. The anisotropic nano material (such as a semiconductor quantum rod, a gold nano rod and an up-conversion nano rod) can generate unique polarized light emission, so that the anisotropic nano material has wide application prospect in the fields of color display, optical storage, biological imaging, biological sensing, anti-counterfeiting and the like. However, it is often difficult to observe the polarization properties of anisotropic nanomaterials in colloidal solutions or randomly ordered collective systems. Therefore, in order to realize the observation and detection of the polarization characteristics of the nano material and the practical application, research on self-assembled nano rods with uniform orientation is carried out. The self-assembly method of the nanorod mainly comprises a surface modification induction method, a template method, a photo-alignment method, a shear stress induction alignment, an electromagnetic field regulation alignment and the like. The shear stress induced orientation is mainly to disperse the nano rods in a polymer colloid or a stretchable polymer film, and to control the nano rods to be uniformly distributed along the shearing force direction through the external shear stress. The method has the advantages of high doping concentration of the nano material, simple operation and low cost, and can effectively orient the nano rod. The electric field regulating orientation is to disperse nanometer material in polymer medium, and regulate the orientation of liquid crystal via applying electric field to control the uniform orientation of nanometer material. The method can realize flexible and adjustable nanometer orientation and has low cost.
The common shear stress induced orientation method has the defects that the orientation of the nano material is single and not adjustable, the film forming thickness is not controllable, and a uniform single-layer orientation film is difficult to form, so that the application range of the method is limited. The electric field regulation and control orientation method based on the liquid crystal system has the key problems of weak light emission and poor polarization of the nanorods due to low dispersion concentration and poor dispersion of the nanorods in the liquid crystal system, which is a limitation of the application of the method.
Therefore, there is a need in the art to develop an orientation method for anisotropic nanomaterials with flexible and controllable orientation direction and high degree of orientation.
Disclosure of Invention
Aiming at the defects existing in the prior art, the invention aims to provide an orientation method of an anisotropic nanomaterial. The method is simple to operate, the anisotropic nano material is high in orientation speed, flexible and controllable in orientation direction and high in orientation degree, and can realize graphical orientation, so that the method is convenient for industrial large-scale application.
To achieve the purpose, the invention adopts the following technical scheme:
the invention provides an orientation method of an anisotropic nanomaterial, which comprises the following steps:
(1) Dispersing the anisotropic nano material and the high polymer material in a solvent to obtain nano ink;
the anisotropic nanomaterial is an anisotropic nanomaterial modified by nonpolar or neutral organic ligand, the polymer material is a nonpolar polymer material, and the solvent is a nonpolar solvent; or the anisotropic nanomaterial is an anisotropic nanomaterial modified by a polar organic ligand, the polymer material is a polar polymer material, and the solvent is a polar solvent;
(2) And (3) directly writing the nano ink obtained in the step (1) on a substrate, and drying to form an anisotropic nano material film oriented along the direct writing direction.
In the method provided by the invention, when nano ink is directly written on the substrate, nano ink fluid can be subjected to shearing action along the direct writing direction, so that the molecular chains of the high polymer material are oriented along the shearing force direction; in the solvent evaporation process, the high polymer material can promote the gelation of the nano ink, weaken the Brownian motion of the anisotropic nano material, and enable the anisotropic nano material to be distributed along the molecular chain orientation direction of the high polymer material under the action of intermolecular acting force (such as Van der Waals force, hydrogen bond and the like) between the high polymer material and the low polymer material, so as to form an anisotropic nano material film of nematic phase, and the thickness of the film can be adjusted by changing the concentration of the anisotropic nano material in the nano ink; in addition, the existence of the high polymer material is also helpful to increase the adhesion of the anisotropic nano material film to the substrate.
It should be noted that, in the present invention, it is necessary to ensure that the anisotropic nanomaterial, the polymer material, and the solvent form a compatible system. Typically, the dipole moment of the polar organic ligand is above 4, and the dipole moment of the nonpolar organic ligand and the neutral organic ligand is less than 4.
As a preferred technical scheme of the invention, the anisotropic nanomaterial is a nanorod or a nanowire.
Preferably, the nanorods are selected from one or a combination of at least two of up-conversion nanorods, gold nanorods, and quantum rods.
The up-conversion nano rod can absorb infrared light to emit visible light, and the gold nano rod can enhance up-conversion luminous intensity and polarization degree. By adjusting the ratio of the two, different up-conversion luminous intensities and polarization degrees can be obtained. The mixed system of the up-conversion nanorod and the gold nanorod is adopted as an anisotropic nanomaterial to perform orientation arrangement, so that the method has wide application prospect in the aspects of display and anti-counterfeiting.
As a preferable technical scheme of the invention, the length-diameter ratio of the anisotropic nano material is more than or equal to 2, for example, 2, 3, 4, 5, 6, 8, 10, 12, 15, 18, 20, 25, 30, 35, 40, 45 or 50 and the like; more preferably not less than 6.
The lower the aspect ratio of the anisotropic nanomaterial, the more difficult it is to orient. The method provided by the invention utilizes intermolecular acting force between the high polymer material and the anisotropic nano material to limit the movement of the anisotropic nano material, so that the anisotropic nano material with lower length-diameter ratio can be well oriented.
In a preferred embodiment of the present invention, the nonpolar or neutral organic ligand is an organic ligand containing a fatty segment having 16 or more carbon atoms.
The fatty chain segment is helpful for enhancing the acting force between the anisotropic nano material and the nonpolar polymer material and promoting the orientation of the anisotropic nano material. If the fatty segment is too short, the binding effect of the nonpolar polymer material on the anisotropic nanomaterial is weakened, and the orientation of the anisotropic nanomaterial may be affected.
Preferably, the non-polar or neutral organic ligand-modified anisotropic nanomaterial is selected from one or a combination of at least two of oleic acid-modified up-conversion nanorods, thiol-terminated polystyrene-modified gold nanorods, and oleic acid or oleylamine-modified quantum rods.
Preferably, the nonpolar polymer material is a polyolefin.
Preferably, the nonpolar solvent is n-hexane or cyclohexane.
As a preferred embodiment of the present invention, the polar organic ligand is a nematic liquid crystal molecule (e.g., 5CB, E7, etc.).
Preferably, the polar solvent is ethanol, diethyl ether or acetone.
As a preferable technical scheme of the invention, the mass ratio of the anisotropic nano material to the high polymer material is 100:0.5-10; for example, it may be 100:0.5, 100:1, 100:1.5, 100:2, 100:2.5, 100:3, 100:4, 100:5, 100:6, 100:7, 100:8, 100:9, or 100:10, etc.
If the mass ratio of the anisotropic nanomaterial to the polymer material is too large, the binding effect of the polymer material on the anisotropic nanomaterial may be insufficient, and the risk of irregular orientation of the anisotropic nanomaterial may be increased.
As a preferable technical scheme of the invention, the content of the polymer material in the nano ink is 0.5-8.5wt%; for example, it may be 0.5wt%, 1wt%, 1.5wt%, 2wt%, 2.5wt%, 3wt%, 3.5wt%, 4wt%, 5wt%, 6wt%, 7wt%, 8wt% or 8.5wt%, etc.
As a preferable technical scheme of the invention, the direct writing speed in the step (2) is more than or equal to 0.03m/s; for example, it may be 0.03m/s, 0.04m/s, 0.05m/s, 0.06m/s, 0.07m/s, 0.08m/s, 0.09m/s, 0.1m/s, or the like.
The write-through rate can affect the amount of shear force to which the nanoink is subjected. If the write-through rate is too low and the shear force is too small, the risk of irregular orientation of the molecular chains of the high polymer material is increased, and the orientation of the anisotropic nano material is further affected.
In the direct writing process of the step (2), the infrared lamp can be used for heating the nano ink on the substrate or directly heating the substrate so as to accelerate the evaporation of the solvent.
As a preferable technical scheme of the invention, the direct writing method in the step (2) comprises the following steps: and (3) taking the nano ink obtained in the step (1), moving an injection port along a preset route on the substrate, and simultaneously enabling the nano ink to flow out of the injection port.
As a preferred embodiment of the present invention, the orientation method includes the steps of:
(1) Adding oleic acid modified up-conversion nanorods and/or mercapto-terminated polystyrene modified gold nanorods into n-hexane, performing ultrasonic dispersion, placing the obtained dispersion liquid into a polypropylene centrifuge tube, aging for more than 20 hours, and dissolving a part of polypropylene into the dispersion liquid to obtain nano ink;
(2) And (3) attaching the injection port to the substrate, moving the injection port along a preset route on the substrate, enabling the nano ink to flow from the injection port to the substrate, and drying to form an anisotropic nano material film oriented along the moving direction of the injection port.
Compared with the prior art, the invention has the following beneficial effects:
the method provided by the invention utilizes the shearing action generated during direct writing to orient the molecular chains of the high polymer material along the direct writing direction, and utilizes the intermolecular acting force between the high polymer material and the anisotropic nano material to promote the anisotropic nano material to be arranged along the orientation direction of the molecular chains of the high polymer material, thereby realizing the orientation of the anisotropic nano material on the substrate and enhancing the adhesive force of the anisotropic nano material to the substrate. The method provided by the invention is simple to operate, the orientation speed of the anisotropic nano material is high, the orientation direction is flexible and controllable, the orientation degree is high (the order degree S reaches 0.89-0.98), the patterned orientation can be realized, and the method is convenient for industrial large-scale application.
The mixed system of the up-conversion nanorod and the gold nanorod is adopted as an anisotropic nanomaterial to perform orientation arrangement, so that the up-conversion fluorescence intensity and the polarization degree are improved, the contrast of patterned orientation is improved, and the method has a certain application prospect in the aspects of display and anti-counterfeiting.
Drawings
FIG. 1 is a schematic diagram of a write-through nanoink according to an embodiment of the invention;
FIG. 2 is an SEM photograph of a nanorod film prepared according to example 1 of the present invention;
FIG. 3 is an SEM photograph of a nanorod film prepared according to example 2 of the invention;
FIG. 4 is an SEM photograph of a nanorod film prepared according to comparative example 1 of the present invention;
fig. 5 is an SEM photograph of the nanorod thin film prepared in comparative example 2 of the present invention.
Detailed Description
The technical scheme of the invention is further described below by the specific embodiments with reference to the accompanying drawings. It should be apparent to those skilled in the art that the detailed description is merely provided to aid in understanding the invention and should not be taken as limiting the invention in any way.
Preparation example 1
Preparation of oleic acid modified up-conversion nanorods:
1.5g of sodium hydroxide was dissolved in 7.5mL of deionized water, stirring was continued, and 25mL of ethanol and 25mL of oleic acid were added sequentially. To the above mixture was added 2mmol of rare earth chloride (composed of yttrium chloride, ytterbium chloride, gadolinium chloride and erbium chloride in a molar ratio of 33:20:45:2) and 5mL of ammonium fluoride (2 mol/L) and stirring was continued for 30 minutes. The above solution was transferred to a 100mL hydrothermal autoclave, kept at 200 ℃ for 2 hours, and then naturally cooled to room temperature. The product obtained by the reaction was collected by centrifugation, washed three times with deionized water and ethanol, respectively, and then kept in an oven at 60 ℃ for 24 hours for drying.
Length and diameter distribution statistics of nanorods: and (3) characterizing the oleic acid modified up-conversion nanorod by adopting a Scanning Electron Microscope (SEM), measuring and counting the length and the diameter of 500 nanorods on an SEM image by using Nano Measurer software, carrying out Gaussian distribution processing on the obtained data by using Origin software to obtain a distribution histogram of the length and the diameter of the nanorods, wherein the length-diameter ratio is the ratio of the average length to the average diameter of the nanorods, and calculating to obtain the length-diameter ratio of the oleic acid modified up-conversion nanorod to be 6.
Preparation example 2
Preparation of oleic acid modified up-conversion nanorods:
the difference from preparation example 1 is that the rare earth chloride consists of yttrium chloride, ytterbium chloride, gadolinium chloride and erbium chloride in a molar ratio of 18:20:60:2. The aspect ratio of the up-conversion nanorods was measured as 4 using the method described above.
Preparation example 3
Preparation of oleic acid ligand-free up-conversion nanorods (hydrophilic):
10mg of the oleic acid modified upconversion nanorods obtained in preparation example 1 were dispersed in 10mL of cyclohexane, and then 4mL of deionized water and a small amount of hydrochloric acid (pH about 4) were added. The solution was magnetically stirred for 2 hours. During this process, oleic acid ligands on the nanorod surface are protonated and mixed with cyclohexane. The ligand-free nanorods will be transferred into deionized water. And then washing with acetone and deionized water for several times, collecting a product obtained by the reaction through centrifugation, and finally dispersing the ligand-free nanorods in deionized water for standby.
Example 1
The embodiment provides an orientation method of an anisotropic nanomaterial, which comprises the following steps:
(1) Dispersing 12mg of oleic acid modified up-conversion nanorods (with the length-diameter ratio of 6) into 1mL of cyclohexane, performing ultrasonic dispersion for 20 minutes to prepare a solution with the concentration of 12mg/mL, and storing the obtained solution in a polypropylene centrifuge tube for ageing for 20 hours to obtain nano ink (the content of the polypropylene is measured to be 0.5%);
(2) As shown in fig. 1, 15 μl of the nano ink obtained in step (1) is sucked by a 100 μl pipette, the pipette tip is dragged in a certain direction on a smooth and flat quartz plate substrate at a dragging rate of 0.035m/s, and the nano ink is injected at the same time, so that the nano ink is directly written on the substrate, the auxiliary solvent is heated by an infrared lamp to volatilize, and a nano rod film is formed on the substrate after drying.
The surface morphology of the nanorod thin film obtained in this example was characterized by using a Scanning Electron Microscope (SEM), and the result is shown in fig. 2. As can be seen from fig. 2, in the nanorod film prepared in this embodiment, the nanorods are arranged in a nematic phase, and the whole is oriented in the direct writing direction, and has a higher degree of orientation. Taking the orientation direction with the largest number of nano rods in the SEM image as a main axis, counting the average included angle theta between the orientation direction of 500 other nano rods and the main axis, and according to the formula s=<2cos 2 θ-1>The degree of order s=0.96 was calculated.
Example 2
(1) Dispersing 12mg of oleic acid modified up-conversion nanorods (with the length-diameter ratio of 4) into 1mL of cyclohexane, performing ultrasonic dispersion for 20 minutes to prepare a solution with the concentration of 12mg/mL, and storing the obtained solution in a polypropylene centrifuge tube for ageing for 20 hours to obtain nano ink (the content of the polypropylene is measured to be 0.5%);
(2) As shown in fig. 1, 15 μl of the nano ink obtained in step (1) is sucked by a 100 μl pipette, the pipette tip is dragged in a certain direction on a smooth and flat quartz plate substrate at a dragging rate of 0.035m/s, and the nano ink is injected at the same time, so that the nano ink is directly written on the substrate, the auxiliary solvent is heated by an infrared lamp to volatilize, and a nano rod film is formed on the substrate after drying.
The surface morphology of the nanorod thin film obtained in this example was characterized by using a Scanning Electron Microscope (SEM), and the result is shown in fig. 3. As can be seen from FIG. 3, the nanorod films prepared in this example have nanorods arranged in a nematic phaseThe whole is oriented along the direct writing direction, and has higher orientation degree. Taking the orientation direction with the largest number of nano rods in the SEM image as a main axis, counting the average included angle theta between the orientation direction of 500 other nano rods and the main axis, and according to the formula s=<2cos 2 θ-1>The degree of order s=0.89 was calculated.
Comparative example 1
The difference from example 1 is that the solution obtained in step (1) was stored in a glass bottle for 20 hours, and the other steps were the same as example 1.
The surface morphology of the nanorod thin film obtained in comparative example 1 was characterized by SEM, and the result is shown in fig. 4. As can be seen from fig. 4, since the nano ink prepared in comparative example 1 does not contain a polymer material, the nanorods are randomly oriented in the obtained nanorod film.
Comparative example 2
The difference from example 1 is that oleic acid modified up-conversion nanorods are replaced with up-conversion nanorods free of an oleic acid ligand, and the other steps are the same as in example 1.
The surface morphology of the nanorod thin film obtained in comparative example 2 was characterized by SEM, and the result is shown in fig. 5. As can be seen from fig. 5, since the nanorods used in comparative example 2 were not modified, the acting force between the nanorods and the nonpolar polymer material was weak, and thus the nanorods were randomly oriented in the obtained nanorod film.
The applicant declares that the above is only a specific embodiment of the present invention, but the scope of the present invention is not limited thereto, and it should be apparent to those skilled in the art that any changes or substitutions that are easily conceivable within the technical scope of the present invention disclosed by the present invention fall within the scope of the present invention and the disclosure.

Claims (8)

1. A method of orienting anisotropic nanomaterials, the method comprising the steps of:
(1) Dispersing the anisotropic nano material and the high polymer material in a solvent to obtain nano ink;
the anisotropic nanomaterial is an anisotropic nanomaterial modified by nonpolar or neutral organic ligand, the polymer material is a nonpolar polymer material, and the solvent is a nonpolar solvent; or the anisotropic nanomaterial is an anisotropic nanomaterial modified by a polar organic ligand, the polymer material is a polar polymer material, and the solvent is a polar solvent;
(2) Writing the nano ink obtained in the step (1) on a substrate directly, and drying to form an anisotropic nano material film oriented along the direct writing direction;
the anisotropic nanomaterial is an up-conversion nanorod;
the length-diameter ratio of the anisotropic nano material is 2-6;
the non-polar or neutral organic ligand modified anisotropic nanomaterial is selected from oleic acid modified up-conversion nanorods;
the nonpolar polymer material is polyolefin;
the nonpolar solvent is cyclohexane.
2. The method of claim 1, wherein the polar organic ligand is a nematic liquid crystal molecule.
3. The orientation method according to claim 1, wherein the polar solvent is ethanol, diethyl ether or acetone.
4. The method of claim 1, wherein the mass ratio of the anisotropic nanomaterial to the polymeric material is 100:0.5-10.
5. The method of claim 1, wherein the nanoink has a content of the polymer material of 0.5 to 8.5wt%.
6. The method of claim 1, wherein the write-through rate in step (2) is not less than 0.03m/s.
7. The orientation method according to claim 1, wherein the direct writing method in step (2) is: and (3) taking the nano ink obtained in the step (1), moving an injection port along a preset route on the substrate, and simultaneously enabling the nano ink to flow out of the injection port.
8. The orientation method according to claim 1, characterized in that the orientation method comprises the steps of:
(1) Adding oleic acid modified up-conversion nanorods into cyclohexane, performing ultrasonic dispersion, placing the obtained dispersion liquid into a polypropylene centrifuge tube, aging for more than 20 hours, and dissolving a part of polypropylene into the dispersion liquid to obtain nano ink;
(2) And (3) taking the nano ink obtained in the step (1), moving an injection port on a substrate along a preset route, enabling the nano ink to flow from the injection port to the substrate, and drying to form an anisotropic nano material film oriented along the moving direction of the injection port.
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JP2013016293A (en) * 2011-07-01 2013-01-24 Konica Minolta Holdings Inc Transparent conductive film and manufacturing method therefor, organic electronic element, organic light-emitting element, and organic power generation element
CN105254336A (en) * 2015-09-16 2016-01-20 浙江大学 Method for preparing oriented carbon nanotube on surface of substrate and product
CN105788708A (en) * 2013-12-25 2016-07-20 中山大学 Manufacturing method of orderly-distributed conductive thin film

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013016293A (en) * 2011-07-01 2013-01-24 Konica Minolta Holdings Inc Transparent conductive film and manufacturing method therefor, organic electronic element, organic light-emitting element, and organic power generation element
CN105788708A (en) * 2013-12-25 2016-07-20 中山大学 Manufacturing method of orderly-distributed conductive thin film
CN105254336A (en) * 2015-09-16 2016-01-20 浙江大学 Method for preparing oriented carbon nanotube on surface of substrate and product

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