Preparation apparatus for nanocomposite material and self-assembly preparation method

Abstract

The present invention relates to a self-assembly preparation method of a nanocomposite material, and more particularly, relates to a self-assembly preparation method of a nanocomposite material comprising steps of: spraying a drug-containing solution onto metal aerosol nanoparticles to form a drug layer on the metal aerosol nanoparticles; and spraying a polymer-containing solution onto the metal aerosol nanoparticles, on which the drug layer is formed, to form a polymer layer on the drug layer, whereby since the method involves no liquid chemical process upon producing the metal aerosol nanoparticles, the processes are simple and can be performed even at a low temperature to suppress deformation of an organic or a drug, and the release rate of the drug, or the like can be easily controlled through metal types of metal aerosol nanoparticles, modification, and the like.

Claims

1. A preparation apparatus for a nanocomposite material comprising: a discharge part which comprises a pair of conductive rods spaced apart at a predetermined interval to form an interval and containing a metal, and a power supply part for applying a voltage to the conductive rods, wherein metal nanoparticles are generated at the interval between the conductive rods by spark discharge; a first spray part which comprises a drug injector for injecting a drug-containing solution onto the metal nanoparticles generated in the interval between the conductive rods, and forms a drug layer surrounding the metal nanoparticles; and a second spray part which comprises a polymer injector for injecting a polymer-containing solution onto the metal nanoparticles on which the drug layer is formed, and forms a polymer layer surrounding the drug layer, wherein the drug injector and the polymer injector comprise a nozzle having an ejection opening, wherein the nozzle of the first spray part and the nozzle of the second spray part are charged with different electric charges.

2. The preparation apparatus for a nanocomposite material according to claim 1, wherein the metal is one or more selected from the group consisting of a transition metal, a transition metal oxide, a transition metal sulfur group element adduct, a lanthanide metal, a lanthanide metal oxide, bismuth, a bismuth sulfur group element adduct and an alloy thereof.

3. The preparation apparatus for a nanocomposite material according to claim 1, wherein the discharge part, the first spray part and the second spray part are maintained under one or more carrier gas atmospheres selected from the group consisting of nitrogen, an inert gas and oxygen.

4. The preparation apparatus for a nanocomposite material according to claim 1, wherein the ejection opening has irregularities on its inner wall.

5. The preparation apparatus for a nanocomposite material according to claim 1, wherein the ejection opening has a diameter of 0.05 mm to 0.5 mm.

Description

BRIEF DESCRIPTION OF DRAWINGS

(1) FIG. 1 is a diagram schematically showing a preparation apparatus of the present application.

(2) FIG. 2 is photographs of processes that a nanocomposite material is formed according to a preparation method of the present application.

(3) FIG. 3 is a diagram schematically showing a cross-section of a nanocomposite material produced according to a preparation method of the present application.

(4) FIG. 4 is a graph of the results that the particle diameters of the nanocomposite materials of Example 2 and Comparative Example are measured by a scanning mobility particle sizer in a gas phase.

(5) FIG. 5 is a graph of the results that the particle diameters of the nanocomposite materials of Example 2 and Comparative Example are measured by a dynamic light scattering particle sizer (Nano ZS90, Malvern Instruments, UK) in a liquid phase.

BEST MODE

(6) Hereinafter, the above-described contents will be described in more detail through Examples and Comparative Examples, but the scope of the present application is not limited by the following contents.

Example 1

(7) Using the apparatus of FIG. 1, a nanocomposite material was produced by the procedure shown in FIG. 2.

(8) 1. Preparation of Metal Aerosol Nanoparticles

(9) A voltage of the following conditions was applied to a spark generator of the following specifications to generate metal vapor, and the vapor was condensed outside the spark generation point to obtain metal aerosol nanoparticles.

(10) <Spark Generator Specifications and Conditions>

(11) Positive electrode: Au

(12) Negative electrode: FePt

(13) Electrode diameter: 3 mm

(14) Electrode length: 100 mm

(15) Resistance: 0.5 M

(16) Capacitance: 1.0 nF

(17) Load current: 2.0 mA

(18) Applied voltage: 3 kV

(19) Frequency: 1 kHz

(20) 2. Formation of Drug Layer

(21) A nitrogen gas (99.99999%>) was supplied between both the metal electrodes to move the metal aerosol nanoparticles along the flow of nitrogen. The flow rate of nitrogen was set to 1.0 to 5.0 L/min, and the number concentration of the metal aerosol nanoparticles was 10.sup.4 to 10.sup.8/cm.sup.3.

(22) A drug-containing solution was sprayed onto the metal aerosol nanoparticles moving along the flow of nitrogen.

(23) The drug-containing solution was prepared by dissolving doxorubicin in a solvent, and the concentration of the drug was adjusted to 0.01 to 10% by volume.

(24) The spraying was performed through a nozzle having a 0.3 mm diameter ejection opening.

(25) Then, the drug layer was dried by passing the metal aerosol nanoparticles, on which the drug layer was formed, through a heat pipe near 100 C.

(26) 3. Formation of Polymer Layer

(27) Prior to formation of a polymer layer, the flow rate of nitrogen as the carrier gas was increased 5 times to dilute the metal aerosol nanoparticles on which the drug layer was formed.

(28) A polymer-containing solution was sprayed onto the metal aerosol nanoparticles, on which the drug layer was formed, moving along the flow of nitrogen.

(29) The polymer-containing solution was prepared by dissolving polyethyleneimine in a solvent, and the concentration of the polymer was adjusted to 0.1 to 10% by volume.

(30) The spraying was performed through a nozzle having a 0.3 mm diameter ejection opening.

(31) Then, the polymer layer was dried by passing the metal aerosol nanoparticles, on which the polymer layer was formed, through a heat pipe near 100 C.

Example 2

(32) Using the apparatus of FIG. 1, a nanocomposite material was produced by the procedure shown in FIG. 2.

(33) Metal vapor was produced by a spark generator (manufactured by inventors themselves), and the vapor was condensed outside the spark generation point to obtain gold aerosol nanoparticles. Specifically, the spark generation operating conditions was set at an interval of 1 mm between the gold electrodes, an operating voltage of 3 kV and a current of 4.1 mA. The spark frequency was controlled by applying a capacitor of 1 nF and the gold electrode vaporized by the high temperature spark channel was condensed along the nitrogen gas flow to produce gold aerosol nanoparticles. The particle diameters of the prepared gold aerosol nanoparticles were measured by a scanning mobility particle sizer (SMPS) provided with an electrostatic classifier (3085, TSI, USA), a condensation particle counter (3776, TSI, USA) and an aerosol charge neutralizer (4530, HCT, Korea), and the measured particle diameters were 4 to 200 nm. Nitrogen gas (>99.99999% purity) was supplied between the gold electrodes to move the gold aerosol nanoparticles along the flow of nitrogen. The flow rate of nitrogen was 3.0 L/min and the number concentration of gold aerosol nanoparticles was 3.210.sup.7/cm.sup.3.

(34) To produce uniform sized gold-triton aggregates using a collision atomizer (containing 2.5 v/v % Triton X-100 and 0.1 w/v % doxorubicin), gold aerosol nanoparticles were first prepared through the spark generator in the compressed nitrogen gas and then the nitrogen gas that the prepared gold aerosol nanoparticles floated was used as a working fluid for the collision atomizer. The collision atomizer was operated at a fluid pressure of 0.25 MPa, the total diameter of the nozzles was 0.3 mm, and an orifice having a plurality of projections with a diameter of 0.05 mm was mounted on the inner wall surface of the nozzle. The solution containing gold aerosol nanoparticles in the collision atomizer passed through the nozzle, to which irregularities were applied, to be uniformly subjected to droplets and then dried, where the uniform sized nanocomposite material was produced.

(35) Thereafter, a drug-containing solution was sprayed onto the gold aerosol nanoparticles moving along the flow of nitrogen. The drug-containing solution was prepared by dissolving 2.5 v/v % Triton X-100 and 0.1 w/v % doxorubicin in a hexane solvent, where the drug concentration was controlled by changing the relative ratio of doxorubicin. The drug-containing solution was sprayed with the nozzle to which irregularities were applied. The total diameter of the nozzle was 0.3 mm, and the inner wall surface of the nozzle included a plurality of protrusions having a diameter of 0.05 mm. The irregularities were electrostatically positively charged at an intensity of 2.7 kV/cm to have electrical repulsion between droplets. As the drug-containing solution collided with the first prepared gold aerosol nanoparticles at the nozzle portion, the gold aerosol nanoparticles were encapsulated by the drug-containing solution and passed through a heat pipe near 100 C. to vaporize the solvent component in the drug solution.

(36) To add targeting ability of the prepared particles to biological tissues, a cationic polymer-containing solution was sprayed onto the gold aerosol nanoparticles, on which the drug layer was formed, moving along the flow of nitrogen. The polymer-containing solution was prepared by dissolving polyethyleneimine in an ethanol solvent, where the concentration of the polymer was adjusted to 0.1 v/v %. The polymer-containing solution was sprayed with a nozzle having the same specification as that of the nozzle used in the drug-containing solution, and the irregularities were also electrostatically positively charged at an intensity of 2.7 kV/cm to have electrical repulsion between the droplets, where size uniformity by agglomeration between the droplets was maintained. As the droplets of the polymer-containing solution collided with the gold aerosol nanoparticles on which the drug layer was formed, the drug layer was encapsulated by the polymer-containing layer and passed through a heat pipe near 100 C. to vaporize the solvent, whereby a nancomposite material having a multi-layered structure (layer-by-layer) was prepared as shown in FIG. 3.

Comparative Example

(37) A nanocomposite material was prepared in the same manner as in Example 2 except that irregularities were not formed on the inner wall of the nozzle.

Experimental ExampleParticle Diameter Measuring Method and Result Analysis

(38) The particle diameters of the nanocomposite materials of Example 2 and Comparative Example were measured with a scanning mobility particle sizer in the gas phase and with a dynamic light scattering particle sizer (Nano ZS90, Malvern Instruments, UK) in the liquid phase, and the results were shown in FIGS. 4 and 5, respectively.

(39) As shown in FIG. 4, from the scanning mobility particle sizer measurement results, in the case of Comparative Example (solid line), the particle size distribution was not uniform and the width was very wide, but in the case of Example 2 (dotted line), the particle size distribution became remarkably uniform.

(40) Also, as shown in FIG. 5, from the dynamic scattering particle sizer measurement results, in the case of Comparative Example (solid line), the particle size distribution was not uniform and the width was very wide, but in the case of Example 2 (dotted line), the particle size distribution was remarkably uniform.

(41) As the irregularities are applied to the nozzle, this is because the physical conditions applied to the droplets passing through the nozzle are made uniform.