A continuous and controllable synthesis method and microfluidic synthesis platform for carbon nanotube nanocomposites loaded with nanometal particles

Abstract

The present invention belongs to the field of nanocomposite synthesis, and specifically relates to a method for the continuous and controllable synthesis of a carbon nanotube nanocomposite loaded with nanometal particles and a microfluidic synthesis platform. The method comprises preparing a reaction reagent solution, preparing a first mixed solution, and mixing the first mixed solution with a reducing agent solution to obtain the carbon nanotube nanocomposite loaded with nanometal particles. The method precisely controls reaction conditions at the microscale and achieves uniform mixing of the reaction reagents within milliseconds. The rapid and efficient mixing reduces the variability in the residence time between the reaction reagents, thereby effectively improving the dispersibility and repeatability of the synthesized nanoparticles.

Description

Technical Field

[0001] The present invention belongs to the field of nanocomposite material synthesis, and in particular relates to a continuous and controllable synthesis method of a carbon nanotube nanocomposite material loaded with nano-metal particles and a microfluidic synthesis platform. Background Art

[0002] Carbon nanotubes (CNTs), as a unique one-dimensional nanomaterial, have been widely used in various fields due to their low cost, easy availability, good biocompatibility, controllable physicochemical properties, ability to withstand harsh environments, and excellent electrokinetic properties. Due to their stable chemical properties, high electrical conductivity, thermal stability, and ability to be functionalized with chemically or electrochemically active substances, CNTs are ideal support materials for loading nanometal particles. CNT nanocomposites loaded with nanometal particles exhibit excellent electrocatalytic activity and are widely used in electrocatalytic materials.

[0003] Currently, the preparation of carbon nanotube nanocomposites loaded with nanometal particles is primarily carried out using batch reactors, such as flasks or beakers. However, this traditional batch production method often requires harsh experimental conditions, such as high temperatures, long synthesis times, complex operating procedures, or specific potential deposition. It often suffers from instability in the mixing of reactants and uneven reaction times, making it difficult to provide a homogeneous nucleation and growth environment. This can result in uneven distribution, low dispersibility, and poor reproducibility of the synthesized nanoparticles, making it difficult to obtain electrocatalytic materials with stable catalytic performance. Furthermore, traditional batch methods can also suffer from problems such as discontinuous synthesis, amplification effects, and low yields, which pose challenges to the large-scale production and application of nanocomposites.

[0004] Therefore, providing a method for synthesizing a continuous carbon nanotube nanocomposite material loaded with nano-metal particles and improving the dispersibility and repeatability of the nanomaterials have become urgent issues to be solved. Summary of the Invention

[0005] The main purpose of the present invention is to provide a continuous and controllable synthesis method of carbon nanotube nanocomposites loaded with nano-metal particles and a microfluidic synthesis platform to overcome the shortcomings of the existing technology.

[0006] To achieve the aforementioned object of the invention, the technical solutions adopted by the present invention include:

[0007] According to a first aspect of an embodiment of the present invention, a method for continuously and controllably synthesizing a carbon nanotube nanocomposite material loaded with nano-metal particles is provided, comprising:

[0008] S1, preparing carbon nanotube solution, precursor solution A, precursor solution B and reducing agent solution, and setting them aside;

[0009] S2, using a syringe pump to control the flow rate of the carbon nanotube solution, precursor solution A and precursor solution B, and mixing the carbon nanotube solution, precursor solution A and precursor solution B through a first micromixer to prepare a first mixed solution;

[0010] S3. Use a syringe pump to control the flow rate of the first mixed solution and the reducing agent solution, and mix the first mixed solution and the reducing agent solution through a second micromixer to obtain a second mixed solution, centrifuge and wash the second mixed solution, collect the precipitate, and obtain the carbon nanotube nanocomposite material loaded with nano-metal particles.

[0011] Furthermore, the carbon nanotube solution includes 0.5-10 mg / mL carbon nanotubes and 0.1-10 mg / mL N-methylpyrrolidone.

[0012] Furthermore, the precursor solution A includes 1 to 30 mM platinum salt, and / or the platinum salt includes any one or a combination of two or more of chloroplatinic acid, potassium chloroplatinate, sodium chloroplatinate, platinum dichloride, platinum trichloride, platinum tetrachloride, potassium tetrachloroplatinate, and platinum nitrate.

[0013] Furthermore, the precursor solution B includes 1-30 mM palladium salt, and / or the palladium salt includes any one or a combination of two or more of sodium chloropalladate, potassium chloropalladate, palladium dichloride, palladium nitrate, palladium sulfate, and palladium nitrate.

[0014] Furthermore, the reducing agent solution includes 1-25 mg / mL morpholine borane.

[0015] Furthermore, the flow ratio between the precursor solution A and the precursor solution B is 0:1 to 1:0,

[0016] The flow ratio of the carbon nanotube solution to the precursor solution A is 1:9 to 9:1.

[0017] The flow ratio of the carbon nanotube solution to the precursor solution B is 1:9 to 9:1.

[0018] The flow ratio of the reducing agent solution to the first mixed liquid is 1:2 to 2:1;

[0019] The total flow rate of the carbon nanotube solution, precursor solution A, precursor solution B and reducing agent solution is 0.5-50 mL / min.

[0020] According to a second aspect of an embodiment of the present invention, there is provided a microfluidic synthesis platform applied to any one of the above methods, comprising a first micromixer, a second micromixer and at least four syringe pumps;

[0021] The first micromixer is used to mix the carbon nanotube solution, the precursor solution A and the precursor solution B;

[0022] The second micro mixer is used to mix the first mixed liquid and the reducing agent solution;

[0023] The at least four injection pumps are used to regulate the flow rates of the carbon nanotube solution, the precursor solution A, the precursor solution B and the reducing agent solution respectively.

[0024] Furthermore, the first micromixer includes a first mixing microchannel and at least three first inlet microchannels, one end of the at least three first inlet microchannels is respectively connected to one end of the first mixing microchannel, the other end of the at least three first inlet microchannels is provided with a first injection hole, the output end of the injection pump is connected to the first injection hole, the other end of the first mixing microchannel is provided with a first liquid outlet, and the second micromixer is connected to the first liquid outlet.

[0025] Furthermore, the second micromixer includes a second mixing microchannel and at least two second inlet microchannels, one end of the at least two second inlet microchannels is respectively connected to one end of the second mixing microchannel, the other end of the at least two second inlet microchannels is provided with a second injection hole, the output end of the injection pump is connected to the second injection hole, and the other end of the second mixing microchannel is provided with a second liquid outlet.

[0026] Furthermore, the total flow rate of the first micromixer and the second micromixer is 0.5 to 50 mL / min.

[0027] Compared with the prior art, the present invention has the following beneficial effects:

[0028] The method for the continuous and controllable synthesis of carbon nanotube nanocomposites loaded with metal nanoparticles, provided by the present invention, precisely controls reaction conditions at the microscale and achieves uniform mixing of reactants within milliseconds. This rapid and efficient mixing reduces variations in the residence time of reactants, thereby effectively improving the dispersibility and repeatability of synthesized nanoparticles. Furthermore, by precisely controlling synthesis parameters such as the reactant flow ratio and total flow rate, the present invention enables rapid and continuous control of the composition, size, and dispersibility of the nanocomposite particles.

[0029] In addition, the microfluidic synthesis platform provided by the present invention can efficiently mix the reaction reagents through a micromixer, promote the generation of a homogeneous reaction, and is beneficial to the nucleation and growth of nanoparticles. BRIEF DESCRIPTION OF THE DRAWINGS

[0030] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the following briefly introduces the drawings required for use in the embodiments or the description of the prior art. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without paying any creative work.

[0031] Figure 1 is a schematic diagram of a microfluidic synthesis platform in a typical embodiment of the present invention;

[0032] Figure 2 is a physical diagram of a first micromixer in a typical embodiment of the present invention;

[0033] Figure 3 is a physical diagram of a second micromixer in a typical embodiment of the present invention;

[0034] Figure 4a is a transmission electron micrograph of the nanocomposite material synthesized in Example 1 of the present invention;

[0035] Figure 4b yes Figure 4a A local enlarged schematic diagram in FIG.

[0036] Figure 5a This is a high-magnification transmission electron microscopy image of the nanocomposite material synthesized in Example 1 of the present invention;

[0037] Figure 5b yes Figure 5a A local enlarged schematic diagram in FIG.

[0038] Figure 6a This is the element distribution diagram of the C element energy dispersion spectrum of the nanocomposite material synthesized in Example 1 of the present invention;

[0039] Figure 6b 1 is an element distribution diagram of the Pt element energy dispersion spectrum of the nanocomposite material synthesized in Example 1 of the present invention;

[0040] Figure 6c This is the element distribution diagram of the Pd element energy dispersion spectrum of the nanocomposite material synthesized in Example 1 of the present invention;

[0041] Figure 7 is the X-ray powder diffraction pattern of the nanocomposite material synthesized in Example 1 of the present invention;

[0042] Figure 8 is an X-ray photoelectron spectrum of the nanocomposite material synthesized in Example 1 of the present invention;

[0043] Figure 9 This is a transmission electron micrograph of the nanocomposite material synthesized in Example 2 of the present invention;

[0044] Figure 10 This is a transmission electron micrograph of the nanocomposite material synthesized in Example 3 of the present invention;

[0045] Figure 11 This is a transmission electron micrograph of the nanocomposite material synthesized in Example 4 of the present invention;

[0046] Figure 12 This is a transmission electron micrograph of the nanocomposite material synthesized in Example 5 of the present invention;

[0047] Figure 13 This is a transmission electron micrograph of the nanocomposite material synthesized in Example 6 of the present invention;

[0048] Figure 14 This is a transmission electron microscope image of the nanocomposite material synthesized in Example 7 of the present invention.

[0049] Markings in the figure: first micromixer 1, first mixing microchannel 101, first inlet microchannel 102, first injection hole 103, first liquid outlet hole 104, second micromixer 2, second mixing microchannel 201, second inlet microchannel 202, second injection hole 203, second liquid outlet hole 204, syringe 3, container 4. DETAILED DESCRIPTION

[0050] To make the objectives, technical solutions, and advantages of the present invention more apparent, the technical solutions of the present invention will be described in detail below. Obviously, the embodiments described are only some of the embodiments of the present invention, not all of them. Based on the embodiments of the present invention, all other implementations obtained by those of ordinary skill in the art without inventive effort are within the scope of protection of the present invention.

[0051] The present invention provides a method for continuously and controllably synthesizing a carbon nanotube nanocomposite material loaded with nano-metal particles, comprising:

[0052] S1. Prepare a carbon nanotube solution, a precursor solution A, a precursor solution B and a reducing agent solution for use; the carbon nanotube solution includes 0.5-10 mg / mL carbon nanotubes and 0.1-10 mg / mL N-methylpyrrolidone; the precursor solution A includes 1-30 mM platinum salt, and the platinum salt includes any one or a combination of two or more of chloroplatinic acid, potassium chloroplatinate, sodium chloroplatinate, platinum dichloride, platinum trichloride, platinum tetrachloride, potassium tetrachloroplatinate, and platinum nitrate; the precursor solution B includes 1-30 mM palladium salt, and the palladium salt includes any one or a combination of two or more of sodium chloropalladate, potassium chloropalladate, palladium dichloride, palladium nitrate, palladium sulfate, and palladium nitrate; the reducing agent solution includes 1-25 mg / mL morpholine borane.

[0053] S2. Use a syringe pump to regulate the flow rate of the carbon nanotube solution, precursor solution A and precursor solution B, and mix the carbon nanotube solution, precursor solution A and precursor solution B through a first micromixer to obtain a first mixed solution, and the precursor solution A and the precursor solution B contain different metal ions; the flow ratio between the precursor solution A and the precursor solution B is 0:1~1:0, the flow ratio of the carbon nanotube solution to the precursor solution A is 1:9~9:1, and the flow ratio of the carbon nanotube solution to the precursor solution B is 1:9~9:1.

[0054] S3. Use a syringe pump to regulate the flow rate of the first mixed liquid and the reducing agent solution, and mix the first mixed liquid and the reducing agent solution through a second micromixer to obtain a second mixed liquid, centrifuge and wash the second mixed liquid, collect the precipitate, and obtain the carbon nanotube nanocomposite material loaded with nano-metal particles; the flow ratio of the reducing agent solution to the first mixed liquid is 1:2 to 2:1; the total inlet flow rate of the carbon nanotube solution, precursor solution A, precursor solution B and reducing agent solution is 0.5 to 50 mL / min.

[0055] The present invention provides a continuous and controllable synthesis method for a carbon nanotube nanocomposite material of loaded nano-metal particles. Reaction conditions are precisely controlled at a microscale, and uniform mixing of reaction reagents can be achieved within a few milliseconds. Rapid and efficient mixing can reduce the difference in residence time between reaction reagents, thereby effectively improving the dispersibility and repeatability of synthesized nanoparticles. Simultaneously, the present invention can rapidly carry out continuous and controllable synthesis of the composition, size, and dispersibility of nanocomposite particles by precisely controlling synthesis parameters such as reaction reagent flow ratio and total flow rate. In addition, the present invention also has the advantages of simple process, low cost, continuous controllability, high efficiency, and avoidance of harsh synthesis conditions such as high temperature and high pressure. The synthesized nanocomposite material has advantages such as uniform particle size, good dispersibility, and good repeatability.

[0056] An embodiment of the present invention further provides a microfluidic synthesis platform for use in any of the above methods, comprising a first micromixer 1, a second micromixer 2, and at least four syringe pumps; the first micromixer 1 is used to mix a carbon nanotube solution, a precursor solution A, and a precursor solution B; the second micromixer 2 is used to mix the first mixed solution and a reducing agent solution; the at least four syringe pumps are used to control the flow rates of the carbon nanotube solution, the precursor solution A, the precursor solution B, and the reducing agent solution, respectively;

[0057] The first micromixer 1 includes a first mixing microchannel 101 and at least three first inlet microchannels 102. One end of the at least three first inlet microchannels 102 is respectively connected to one end of the first mixing microchannel 101. The other end of the at least three first inlet microchannels 102 is provided with a first injection hole 103. The output end of the injection pump is connected to the first injection hole 103. The other end of the first mixing microchannel 101 is provided with a first liquid outlet 104. The second micromixer 2 is connected to the first liquid outlet 104.

[0058] The second micromixer 2 includes a second mixing microchannel 201 and at least two second inlet microchannels 202, one end of the at least two second inlet microchannels 202 is respectively connected to one end of the second mixing microchannel 201, the other end of the at least two second inlet microchannels 202 is provided with a second injection hole 203, the output end of the injection pump is connected to the second injection hole 203, and the other end of the second mixing microchannel 201 is provided with a second liquid outlet 204.

[0059] The total flow rate of the first micromixer 1 and the second micromixer 2 is 0.5-50 mL / min.

[0060] By adopting the microfluidic synthesis platform provided by the present invention, the reaction reagents can be efficiently mixed, promoting the generation of a homogeneous reaction, which is beneficial to the nucleation and growth of nanoparticles;

[0061] The present invention is described in detail below with reference to specific embodiments to facilitate understanding of the technical solutions of the present invention.

[0062] Example 1:

[0063] 1. Adoption Figure 1 The microfluidic synthesis platform shown in FIG. 1 is processed using 3D printing technology to obtain a 3D printed first micro mixer 1 (such as Figure 2 As shown) and the second micro mixer 2 (as Figure 3 shown).

[0064] 2. Prepare a reaction reagent solution, which includes a carbon nanotube solution, a precursor solution A, a precursor solution B, and a reducing agent solution. The carbon nanotube solution is a mixture of 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0065] 3. The reaction reagent solution was placed in syringe 3 and introduced into the micromixer via a quadruple precision syringe pump. The reaction reagent solution was then injected into the two micromixers at a specific flow ratio to obtain a nanocomposite solution. The flow ratio of precursor solution A to precursor solution B was 1:1, the flow ratio of the carbon nanotube solution to precursor solution A was 1:1, and the flow ratio of the carbon nanotube solution to precursor solution B was 1:1. The total flow rate into the first micromixer 1 and the second micromixer 2 was 5 mL / min.

[0066] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol at a speed of 4400 rpm for 5 minutes. The nanocomposite material after centrifugation was placed in a vacuum drying oven at 60°C and dried for 24 hours.

[0067] 5. Conduct transmission electron microscopy characterization of the synthesized nanocomposites, such as Figure 4a As shown, Figure 4b for Figure 4a The enlarged schematic diagram of the box area in the figure; the synthesized nanocomposite material was characterized by high-magnification transmission electron microscopy, such as Figure 5a As shown, Figure 5b for Figure 5a An enlarged schematic diagram of the boxed area; Figure 4a 、 4b , 5a, 5b, it can be seen that uniformly distributed nanoparticles are synthesized on the surface of carbon nanotubes.

[0068] The synthesized nanomaterials were characterized by energy dispersion spectroscopy, as shown in FIG6 ; the synthesized nanomaterials were characterized by X-ray powder diffraction, as shown in FIG6 . Figure 7 As shown; X-ray photoelectron spectroscopy was performed on the synthesized nanomaterials, as shown Figure 8 As shown in Figures 6-8, Pt-Pd nanoparticles were successfully synthesized on the microfluidic synthesis platform.

[0069] Example 2:

[0070] 1. Adoption Figure 1 The microfluidic synthesis platform shown in the figure is shown in Figure 2 and Figure 3 .

[0071] 2. The carbon nanotube solution is 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0072] 3. The reaction reagent solution is placed in a syringe 3 and introduced into the first micromixer 1 and the second micromixer 2 via a quadruple precision syringe pump. The reaction reagent solution is injected into the two micromixers at a specific flow ratio. The flow ratio of precursor solution A to precursor solution B is 3:7, the flow ratio of the carbon nanotube solution to precursor solution A is 1:1, the flow ratio of the carbon nanotube solution to precursor solution B is 1:1, and the flow ratio of the reducing agent solution to the outlet of the second micromixer 2 is 1:1. The total flow rate of the first micromixer 1 and the second micromixer 2 is 5 mL / min.

[0073] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol at a speed of 4400 rpm for 5 minutes. The nanocomposite material after centrifugation was placed in a vacuum drying oven at 60°C and dried for 24 hours.

[0074] 5. Perform transmission characterization on the synthesized nanomaterials, such as Figure 9 As shown in the figure, it can be seen that Pt-Pd nanoparticles are evenly distributed on the surface of carbon nanotubes.

[0075] Example 3:

[0076] 1. Adoption Figure 1 The microfluidic synthesis platform shown in the figure is shown in Figure 2 and Figure 3 .

[0077] 2. The carbon nanotube solution is 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0078] 3. The reaction reagent solution was placed in a syringe 3 and introduced into the first micromixer 1 and the second micromixer 2 via a quadruple precision syringe pump. The reaction reagent solution was injected into the two micromixers at a specific flow ratio. The flow ratio of precursor solution A to precursor solution B was 1:0, the flow ratio of the carbon nanotube solution to precursor solution A was 1:1, and the flow ratio of the carbon nanotube solution to precursor solution B was 1:1. The total flow rate of the first micromixer 1 and the second micromixer 2 was 5 mL / min.

[0079] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol at a speed of 4400 rpm for 5 minutes. The nanocomposite material after centrifugation was placed in a vacuum drying oven at 60°C and dried for 24 hours.

[0080] 5. Perform transmission characterization on the synthesized nanomaterials, such as Figure 10 As shown in the figure, it can be seen that Pt nanoparticles are evenly distributed on the surface of carbon nanotubes.

[0081] Example 4:

[0082] 1. Adoption Figure 1 The microfluidic synthesis platform shown in the figure is shown in Figure 2 and Figure 3 .

[0083] 2. The carbon nanotube solution is 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0084] 3. The reaction reagent solution is placed in a syringe 3 and introduced into the first micromixer 1 and the second micromixer 2 via a quadruple precision syringe pump. The reaction reagent solution is injected into the two micromixers at a specific flow ratio. The flow ratio of precursor solution A to precursor solution B is 1:1, the flow ratio of the carbon nanotube solution to precursor solution A is 3:7, the flow ratio of the carbon nanotube solution to precursor solution B is 3:7, and the flow ratio of the reducing agent solution to the outlet of the second micromixer 2 is 1:1. The total flow rate of the first micromixer 1 and the second micromixer 2 is 5 mL / min.

[0085] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol at a speed of 4400 rpm for 5 minutes. The nanocomposite material after centrifugation was placed in a vacuum drying oven at 60°C and dried for 24 hours.

[0086] 5. Perform transmission characterization on the synthesized nanomaterials, such as Figure 11 As shown in the figure, Pt-Pd nanoparticles with a large size are synthesized on the surface of carbon nanotubes.

[0087] Example 5:

[0088] 1. Adoption Figure 1The microfluidic synthesis platform shown in the figure is shown in Figure 2 and Figure 3 .

[0089] 2. The carbon nanotube solution is 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0090] 3. Place the reaction reagent solution in syringe 3 and introduce it into the first micromixer 1 and the second micromixer 2 via a quadruple precision syringe pump. The reaction reagent solution is injected into the two micromixers at a specific flow ratio. The flow ratio of precursor solution A to precursor solution B is 1:1, the flow ratio of the carbon nanotube solution to precursors A and B is 7:3, and the flow ratio of the reducing agent solution to the outlet of the second micromixer 2 is 1:1. The total flow rate into the micromixer is 5 mL / min.

[0091] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol at a speed of 4400 rpm for 5 minutes. The nanocomposite material after centrifugation was placed in a vacuum drying oven at 60°C and dried for 24 hours.

[0092] 5. Perform transmission characterization on the synthesized nanomaterials, such as Figure 12 As shown in the figure, it can be seen that fewer Pt-Pd nanoparticles are synthesized on the surface of carbon nanotubes.

[0093] Example 6:

[0094] 1. Adoption Figure 1 The microfluidic synthesis platform shown in the figure is shown in Figure 2 and Figure 3 .

[0095] 2. The carbon nanotube solution is 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0096] 3. Place the reaction reagent solution in syringe 3 and introduce it into the first micromixer 1 and the second micromixer 2 via a quadruple precision syringe pump. The reaction reagent solution is injected into the two micromixers at a specific flow ratio. The flow ratio of precursor solution A to precursor solution B is 1:1, the flow ratio of the carbon nanotube solution to precursors A and B is 1:1, and the flow ratio of the reducing agent solution to the outlet of the second micromixer 2 is 1:1. The total flow rate into the micromixer is 1 mL / min.

[0097] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol. The centrifugation speed was 4400 rpm and the centrifugation time was 5 min. The nanocomposite material was placed in a vacuum drying oven at 60°C and dried for 24 h.

[0098] 5. Perform transmission characterization on the synthesized nanomaterials, such as Figure 13 As shown in the figure, large-sized Pt-Pd nanoparticles were synthesized on the surface of carbon nanotubes.

[0099] Example 7:

[0100] 1. Adoption Figure 1 The microfluidic synthesis platform shown in the figure is shown in Figure 2 and Figure 3 .

[0101] 2. The carbon nanotube solution is 1.5 mg / mL multi-walled carbon nanotubes (MWCNT) and 3 mg / mL NMP; the precursor solution A is 9 mM chloroplatinic acid; the precursor solution B is 9 mM sodium chloropalladate; the reducing agent solution is 6 mg / mL morpholine borane (C4H 12 BNO).

[0102] 3. Place the reaction reagent solution in syringe 3 and introduce it into the first micromixer 1 and the second micromixer 2 via a quadruple precision syringe pump. The reaction reagent solution is injected into the two micromixers at a specific flow ratio. The flow ratio of precursor solution A to precursor solution B is 1:1, the flow ratio of the carbon nanotube solution to precursors A and B is 1:1, and the flow ratio of the reducing agent solution to the outlet of the second micromixer 2 is 1:1. The total flow rate into the micromixer is 15 mL / min.

[0103] 4. The generated nanocomposite solution was collected in a centrifuge tube, which was placed in a container 4 filled with ice water. The collected solution was centrifuged three times and washed with anhydrous ethanol at a speed of 4400 rpm for 5 minutes. The nanocomposite material after centrifugation was placed in a vacuum drying oven at 60°C and dried for 24 hours.

[0104] 5. Perform transmission characterization on the synthesized nanomaterials, such as Figure 14 As shown in the figure, small-sized Pt-Pd nanoparticles are synthesized on the surface of carbon nanotubes.

[0105] The above description is merely a specific embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any modifications or substitutions that can be easily conceived by a person skilled in the art within the technical scope disclosed in the present invention should be included in the scope of protection of the present invention. Therefore, the scope of protection of the present invention should be based on the scope of protection of the claims.

Claims

1. A continuous and controllable synthesis method of carbon nanotube nanocomposites loaded with nano-metal particles, characterized in that: The method comprises the following steps: S1, preparing carbon nanotube solution, precursor solution A, precursor solution B and reducing agent solution, and setting them aside; S2, using a syringe pump to control the flow rate of the carbon nanotube solution, precursor solution A and precursor solution B, and mixing the carbon nanotube solution, precursor solution A and precursor solution B through a first micromixer to prepare a first mixed solution; S3. Use a syringe pump to control the flow rate of the first mixed solution and the reducing agent solution, and mix the first mixed solution and the reducing agent solution through a second micromixer to obtain a second mixed solution, centrifuge and wash the second mixed solution, collect the precipitate, and obtain the carbon nanotube nanocomposite material loaded with nano-metal particles.

2. The method for continuous and controllable synthesis of carbon nanotube nanocomposites loaded with nano-metal particles according to claim 1, characterized in that: The carbon nanotube solution includes 0.5-10 mg / mL carbon nanotubes and 0.1-10 mg / mL N-methylpyrrolidone.

3. The method for continuous and controllable synthesis of carbon nanotube nanocomposites loaded with nano-metal particles according to claim 1, characterized in that: The precursor solution A includes 1-30 mM platinum salt, and the platinum salt includes any one or a combination of two or more of chloroplatinic acid, potassium chloroplatinate, sodium chloroplatinate, platinum dichloride, platinum trichloride, platinum tetrachloride, potassium tetrachloroplatinate, and platinum nitrate.

4. The method for continuous and controllable synthesis of carbon nanotube nanocomposites loaded with nanometal particles according to claim 1, characterized in that: The precursor solution B includes 1-30 mM palladium salt, and the palladium salt includes any one or a combination of two or more of sodium chloropalladate, potassium chloropalladate, palladium dichloride, palladium nitrate, palladium sulfate, and palladium nitrate.

5. The method for continuous and controllable synthesis of carbon nanotube nanocomposites loaded with nano-metal particles according to claim 1, characterized in that: The reducing agent solution includes 1-25 mg / mL morpholine borane.

6. The method for continuously and controllably synthesizing carbon nanotube nanocomposites loaded with nano-metal particles according to claim 1, characterized in that: The flow ratio between the precursor solution A and the precursor solution B is 0:1~1:0, The flow ratio of the carbon nanotube solution to the precursor solution A is 1:9 to 9:

1. The flow ratio of the carbon nanotube solution to the precursor solution B is 1:9 to 9:

1. The flow ratio of the reducing agent solution to the first mixed solution is 1:2 to 2:1; The total flow rate of the carbon nanotube solution, precursor solution A, precursor solution B and reducing agent solution is 0.5-50 mL / min.

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