CN112063370A - Self-repairing composite phase change material with enhanced heat conduction and preparation method and application thereof - Google Patents
Self-repairing composite phase change material with enhanced heat conduction and preparation method and application thereof Download PDFInfo
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Abstract
The invention discloses a self-repairing composite phase change material with enhanced heat conduction and a preparation method and application thereof. The method comprises the following steps: paraffin is used as a phase change material, and graphene is added to improve the heat conduction performance. And adding the obtained sample into SEBS for packaging paraffin, adding a self-repairing material, heating and stirring to obtain the self-repairing composite phase-change material with enhanced heat conduction. The prepared phase-change material has high phase-change latent heat and high thermal conductivity. The phase-change material disclosed by the invention is well packaged by SBES, can prevent the leakage of the phase-change material to a certain extent, improves the use safety, and can be self-repaired after being extruded by external force, thereby prolonging the service life. The SEBS and the paraffin are cheap and easy to obtain, the preparation conditions are easy to realize, the preparation cost of the composite phase-change material is reduced, the environment is friendly, the safety is high, and the popularization and the application of the technology are facilitated.
Description
Technical Field
The invention belongs to the technical field of functional materials, and particularly relates to a self-repairing composite phase change material with enhanced heat conduction, and a preparation method and application thereof.
Background
In recent years, as the problems of energy crisis and environmental pollution are increasingly prominent, effective energy storage is an important solution for improving energy utilization efficiency. The core of the heat storage technology is an energy storage material, and the phase change energy storage technology is to utilize a phase change material as a medium to effectively store and release energy by utilizing the phase change conversion of the phase change material, so that the aim of saving energy is fulfilled. The organic phase-change material is widely applied to solar energy storage due to the characteristics of high energy density, high chemical stability, no corrosion, no toxicity and the like, and is widely applied to the fields of aerospace, building energy conservation, refrigeration equipment, electronic devices and the like. However, the phase-change material such as paraffin has a series of defects of low heat conductivity coefficient, easy leakage in the solid-liquid change process and the like, which greatly limits the application of the phase-change material. Therefore, in order to reduce the requirements of the practical application of the composite phase change material, the phase change material is well packaged to solve the leakage problem, the self-repairing performance is combined, the service performance and the service life of the composite phase change material can be improved, and the development of the composite phase change material with high heat conductivity coefficient is very important.
The Chinese patent application CN109943291A provides a high-thermal-conductivity self-repairing gel-based phase change material and a preparation method thereof, and the obtained material has high thermal conductivity and stable phase change, but the problem of leakage of the phase change material is not well solved. Chinese patent application CN110713728A provides a preparation method of a paraffin-SEBS thermoplastic elastomer composite phase-change material, the obtained material has a thermal conductivity coefficient of 0.15 W.m < -1 > K < -1 >, the phase-change enthalpy value is only 180J/g at the highest, and the leakage problem is solved, but the problems of low thermal conductivity coefficient and low phase-change enthalpy value are not well solved.
Disclosure of Invention
In order to overcome the defects and shortcomings in the background art, the invention provides a self-repairing composite phase change material with enhanced heat conduction and a preparation method and application thereof.
In order to overcome the defects and shortcomings of the prior art, the invention aims to provide the composite phase-change material which has proper phase-change temperature, larger heat conductivity coefficient, stable performance, high phase-change latent heat value and self-repairing capability so as to prolong the service life of the material, and also provides a preparation method and application of the composite phase-change material with simple preparation process.
The purpose of the invention is realized by at least one of the following technical solutions.
The invention provides a preparation method of a self-repairing composite phase change material with enhanced heat conduction, which comprises the following steps:
(1) adding 1, 4-phenyl diboronic acid, a photoinitiator, a surfactant, a cross-linking agent, dimethylaminoethyl methacrylate and a hydrophilic monomer containing hydroxyl into deionized water, and uniformly mixing to obtain a mixed solution;
(2) adding the mixed solution obtained in the step (1) into N, N-dimethylacrylamide, uniformly mixing by ultrasonic waves, then reacting under the irradiation of ultraviolet light, freeze-drying, and removing the solvent in the dispersion to obtain a self-repairing aerogel material;
(3) heating paraffin in a reactor until the paraffin is completely dissolved, adding SEBS and graphene into liquid paraffin, heating and stirring to obtain a phase-change composite material with enhanced heat conduction;
(4) and (3) in a heating state, uniformly mixing the heat conduction enhanced phase change composite material obtained in the step (3) with the self-repairing aerogel material obtained in the step (2), and cooling to room temperature to obtain the heat conduction enhanced self-repairing composite phase change material.
Further, the mixed solution in the step (1) comprises the following components in parts by weight:
further, the photoinitiator in the step (1) is 4-phenylbenzophenone; the cross-linking agent in the step (1) is magnesium lithium silicate; the hydrophilic monomer containing hydroxyl in the step (1) is N-N dimethyl amide; the surfactant in the step (1) is sodium dodecyl benzene sulfonate;
further, the mass ratio of the mixed solution in the step (2) to the N, N-dimethylacrylamide is 1-5: 1; the power of the ultraviolet light in the step (2) is 50-300mW/cm2(ii) a The reaction time under the irradiation of ultraviolet light is 300-500 s; the freeze drying time in the step (2) is 50-60 h.
Further, the heating and stirring temperature in the step (3) is 80-110 ℃, and the heating and stirring time is 10-30 minutes. The heating and stirring adopt constant-temperature magnetic stirring.
Further, the SEBS in the step (3) is a linear triblock copolymer taking polystyrene as a terminal block and an ethylene-butylene copolymer obtained by hydrogenating polybutadiene as a middle elastic block. English is called Styrene Ethylene Styrene; the model of the SEBS is 501T; the mass ratio of the SEBS to the paraffin is 10-50: 100-200.
Further, in the phase change composite material with enhanced heat conduction in the step (3), the mass percentage of the graphene is 0 wt% -5 wt%.
Further, the temperature of the step (4) in the heating state is 80-110 ℃; in the self-repairing composite phase change material with enhanced heat conduction in the step (4), the self-repairing aerogel material is 5-20 wt% in mass percentage.
The invention provides a self-repairing composite phase change material with enhanced heat conduction, which is prepared by the preparation method.
The invention provides application of a self-repairing composite phase change material with enhanced heat conduction in preparation of a solar storage device.
Compared with the prior art, the invention has the following advantages and beneficial effects:
(1) the invention adopts cheap and easily available raw materials for preparation, the preparation conditions are easy to realize, the cost for preparing the self-repairing composite phase-change material with enhanced heat conduction is reduced, and the popularization and the application of the technology are facilitated;
(2) the paraffin is used as the phase-change material, the SEBS is used for packaging the paraffin, leakage is prevented, and the prepared composite phase-change material has high phase-change latent heat; due to the addition of the graphene, the heat conductivity coefficient of the phase-change material is improved;
(3) the self-repairing material is combined with the composite phase-change material with enhanced heat conduction, so that the service life of the composite phase-change material is prolonged to a certain extent, and the use safety of the composite phase-change material is improved;
(4) the phase-change material can be used for storing solar energy, and has a good heat storage effect; the prepared self-repairing composite phase change material with enhanced heat conduction can be widely applied to solar energy storage.
Detailed Description
The following examples are presented to further illustrate the practice of the invention, but the practice and protection of the invention is not limited thereto. It is noted that the processes described below, if not specifically described in detail, are all realizable or understandable by those skilled in the art with reference to the prior art. The reagents or apparatus used are not indicated to the manufacturer, and are considered to be conventional products available by commercial purchase.
The phase change latent heat and the phase change temperature of the self-repairing composite phase change material with enhanced heat conduction prepared by the following embodimentThe degree is measured by the following method: taking 5-8mg of sample, and testing the thermal property of the phase-change material by using a differential scanning calorimeter (DSC, Netzsch, STA 449), wherein the heating (cooling) rate of the sample is 5 ℃ min-1And measuring the temperature range to be 0-100 ℃ to obtain the phase change latent heat and the phase change temperature of the sample.
The thermal conductivity of the self-repairing composite phase change material with enhanced thermal conductivity prepared in the following examples was measured by using a thermal conductivity meter (Hot Disk TPS2500S, Sweden).
Example 1
The self-repairing composite phase change material with enhanced heat conduction is prepared according to the following steps:
(1) 3g of dimethylaminoethyl methacrylate, 1g of hydrophilic monomer containing hydroxyl (N-N dimethyl amide), 0.05g of photoinitiator (4-phenyl benzophenone), 0.5g of 1, 4-phenyl diboronic acid, 0.1g of surfactant (sodium dodecyl benzene sulfonate) and 0.1g of cross-linking agent (magnesium lithium silicate) are added with a certain amount of deionized water until the total mass is 10g, and the mixture is uniformly mixed.
(2) Adding the mixed solution in the step (1) into 2g N, N-dimethylacrylamide, and carrying out ultrasonic mixing.
(3) Placing the solution obtained in the step (2) at 200mW/cm2Irradiating for 500s under an ultraviolet lamp.
(4) And (4) carrying out freeze drying on the solution obtained in the step (3) for 56h to remove the solvent in the dispersion, thus obtaining the self-repairing aerogel material.
(5) And (3) heating 10g of paraffin in a 90 ℃ oven until the paraffin is completely dissolved, adding 3g of SEBS (501T) and 0g of graphene into the reactor, heating and stirring by using a constant-temperature magnetic heating stirrer, and continuously heating and stirring for 20 minutes at the temperature of 90 ℃ until the mixture is uniform to prepare the phase-change composite material with enhanced heat conduction.
(6) And (3) placing the sample obtained in the step (5) in a 90 ℃ oven to be heated until the sample is completely melted, adding the self-repairing aerogel material obtained in the step (4), wherein the mass ratio of the phase-change material to the self-repairing material is 10:1, forming gel, and cooling to obtain the self-repairing composite phase-change material with enhanced heat conduction.
Heat conduction enhanced self-repairing composite phase change prepared by the embodimentThe phase change temperature of the material is 65.3 ℃, the phase change latent heat is 209.4J/g, and the heat conductivity coefficient is 0.2696W m-1K-1The self-repairing rate of the damaged part can reach 70 percent.
Example 2
The self-repairing composite phase change material with enhanced heat conduction is prepared according to the following steps:
(1) 3g of dimethylaminoethyl methacrylate, 1g of hydrophilic monomer containing hydroxyl (N-N dimethyl amide), 0.05g of photoinitiator (4-phenyl benzophenone), 0.5g of 1, 4-phenyl diboronic acid, 0.1g of surfactant (sodium dodecyl benzene sulfonate) and 0.1g of cross-linking agent (magnesium lithium silicate) are added with a certain amount of deionized water until the total mass is 10g, and the mixture is uniformly mixed.
(2) Adding the mixed solution in the step (1) into 2g N, N-dimethylacrylamide, and carrying out ultrasonic mixing.
(3) Placing the solution obtained in the step (2) at 200mW/cm2Irradiating for 500s under an ultraviolet lamp.
(4) And (4) carrying out freeze drying on the solution obtained in the step (3) for 56h to remove the solvent in the dispersion, thus obtaining the self-repairing aerogel material.
(5) And (3) heating 10g of paraffin in a 90 ℃ oven until the paraffin is completely dissolved, adding 3g of SEBS (501T) and 0.1g of graphene into the reactor, heating and stirring by using a constant-temperature magnetic heating stirrer, and continuously heating and stirring for 20 minutes at the temperature of 90 ℃ until the mixture is uniform to prepare the phase-change composite material with enhanced heat conduction.
(6) And (3) placing the sample obtained in the step (5) in a 90 ℃ oven to be heated until the sample is completely melted, adding the self-repairing aerogel material obtained in the step (4), wherein the mass ratio of the phase-change material to the self-repairing material is 10:1, forming gel, and cooling to obtain the self-repairing composite phase-change material with enhanced heat conduction.
The phase-change temperature of the heat-conduction-enhanced self-repairing composite phase-change material prepared by the embodiment is 66.1 ℃, the latent heat of phase change is 207.2J/g, and the heat conductivity coefficient is 0.2743W m-1K-1The self-repairing rate of the damaged part can reach 70 percent.
Example 3
The self-repairing composite phase change material with enhanced heat conduction is prepared according to the following steps:
(1) 3g of dimethylaminoethyl methacrylate, 1g of hydrophilic monomer containing hydroxyl (N-N dimethyl amide), 0.05g of photoinitiator (4-phenyl benzophenone), 0.5g of 1, 4-phenyl diboronic acid, 0.1g of surfactant (sodium dodecyl benzene sulfonate) and 0.1g of cross-linking agent (magnesium lithium silicate) are added with a certain amount of deionized water until the total mass is 10g, and the mixture is uniformly mixed.
(2) Adding the mixed solution in the step (1) into 2g N, N-dimethylacrylamide, and carrying out ultrasonic mixing.
(3) Placing the solution obtained in the step (2) at 300mW/cm2Irradiating for 300s under an ultraviolet lamp.
(4) And (4) carrying out freeze drying on the solution obtained in the step (3) for 60h to remove the solvent in the dispersion, thus obtaining the self-repairing aerogel material.
(5) And (3) taking 10g of paraffin, placing the paraffin in a 110 ℃ oven, heating the paraffin to be completely dissolved, adding 3g of SEBS (501T) and 0.2g of graphene into the reactor, heating and stirring the mixture by adopting a constant-temperature magnetic heating stirrer, and continuously heating and stirring the mixture for 10 minutes at the temperature of 110 ℃ until the mixture is uniform to prepare the phase-change composite material with enhanced heat conduction.
(6) And (3) placing the sample obtained in the step (5) in a drying oven at 110 ℃ to be heated until the sample is completely melted, adding the self-repairing aerogel material obtained in the step (4), wherein the mass ratio of the phase-change material to the self-repairing material is 10:1, forming gel, and cooling to obtain the self-repairing composite phase-change material with enhanced heat conduction.
The phase-change temperature of the heat-conduction-enhanced self-repairing composite phase-change material prepared by the embodiment is 65.3 ℃, the latent heat of phase change is 206.9J/g, and the heat conductivity coefficient is 0.2791W m-1K-1The self-repairing rate of the damaged part can reach 70 percent.
Example 4
The self-repairing composite phase change material with enhanced heat conduction is prepared according to the following steps:
(1) 3g of dimethylaminoethyl methacrylate, 1g of hydrophilic monomer (N-N dimethyl amide) containing hydroxyl, 0.05g of photoinitiator (4-phenyl benzophenone), 0.5g of 1, 4-phenyl diboronic acid, 0.1g of surfactant (sodium dodecyl benzene sulfonate) and 0.1g of crosslinking agent lithium magnesium silicate are added with a certain amount of deionized water until the total mass is 10g, and the components are uniformly mixed.
(2) Adding the mixed solution in the step (1) into 2g N, N-dimethylacrylamide, and carrying out ultrasonic mixing.
(3) Placing the solution obtained in the step (2) at 50mW/cm2Irradiating for 300s under an ultraviolet lamp.
(4) And (4) carrying out freeze drying on the solution obtained in the step (3) for 50h to remove the solvent in the dispersion, thus obtaining the self-repairing aerogel material.
(5) And (3) heating 10g of paraffin in an oven at 80 ℃ until the paraffin is completely dissolved, adding 3g of SEBS (501T) and 0.3g of graphene into the reactor, heating and stirring by adopting a constant-temperature magnetic heating stirrer, and continuously heating and stirring for 30 minutes at the temperature of 90 ℃ until the mixture is uniform to prepare the phase-change composite material with enhanced heat conduction.
(6) And (3) placing the sample obtained in the step (5) in an oven at 80 ℃ to be heated until the sample is completely melted, adding the self-repairing aerogel material obtained in the step (4), wherein the mass ratio of the phase-change material to the self-repairing material is 10:1, forming gel, and cooling to obtain the self-repairing composite phase-change material with enhanced heat conduction.
The phase-change temperature of the heat-conduction-enhanced self-repairing composite phase-change material prepared by the embodiment is 66.3 ℃, the latent heat of phase change is 208.0J/g, and the heat conductivity coefficient is 0.2855W m-1K-1The self-repairing rate of the damaged part can reach 70 percent.
Example 5
(1) 3g of dimethylaminoethyl methacrylate, 1g of hydrophilic monomer containing hydroxyl (N-N dimethyl amide), 0.05g of photoinitiator (4-phenyl benzophenone), 0.5g of 1, 4-phenyl diboronic acid, 0.1g of surfactant (sodium dodecyl benzene sulfonate) and 0.1g of crosslinking agent lithium magnesium silicate are added with a certain amount of deionized water until the total mass is 10g and mixed evenly.
(2) Adding the mixed solution in the step (1) into 2g N, N-dimethylacrylamide, and carrying out ultrasonic mixing.
(3) Placing the solution obtained in the step (2) at 200mW/cm2Irradiating for 500s under an ultraviolet lamp.
(4) And (4) carrying out freeze drying on the solution obtained in the step (3) for 56h to remove the solvent in the dispersion, thus obtaining the self-repairing aerogel material.
(5) And (3) heating 10g of paraffin in a 90 ℃ oven until the paraffin is completely dissolved, adding 3g of SEBS (501T) and 0.4g of graphene into the reactor, heating and stirring by using a constant-temperature magnetic heating stirrer, and continuously heating and stirring for 20 minutes at the temperature of 90 ℃ until the mixture is uniform to prepare the phase-change composite material with enhanced heat conduction.
(6) And (3) placing the sample obtained in the step (5) in a 90 ℃ oven to be heated until the sample is completely melted, adding the self-repairing aerogel material obtained in the step (4), wherein the mass ratio of the phase-change material to the self-repairing material is 10:1, forming gel, and cooling to obtain the self-repairing composite phase-change material with enhanced heat conduction.
The phase-change temperature of the heat-conduction-enhanced self-repairing composite phase-change material prepared by the embodiment is 66.6 ℃, the latent heat of phase change is 208.9J/g, and the heat conductivity coefficient is 0.2871W m-1K-1The self-repairing rate of the damaged part can reach 70 percent.
Example 6
(1) 3g of dimethylaminoethyl methacrylate, 1g of hydrophilic monomer containing hydroxyl (N-N dimethyl amide), 0.05g of photoinitiator (4-phenyl benzophenone), 0.5g of 1, 4-phenyl diboronic acid and 0.1g of surfactant (sodium dodecyl benzene sulfonate) are added with a certain amount of deionized water until the total mass is 10g, and the mixture is uniformly mixed.
(2) Adding the mixed solution in the step (1) into 2g N, N-dimethylacrylamide, and carrying out ultrasonic mixing.
(3) Placing the solution obtained in the step (2) at 200mW/cm2Irradiating for 500s under an ultraviolet lamp.
(4) And (4) carrying out freeze drying on the solution obtained in the step (3) for 56h to remove the solvent in the dispersion, thus obtaining the self-repairing aerogel material.
(5) And (3) heating 10g of paraffin in a 90 ℃ oven until the paraffin is completely dissolved, adding 3g of SEBS (501T) and 0.5g of graphene into the reactor, heating and stirring by using a constant-temperature magnetic heating stirrer, and continuously heating and stirring for 20 minutes at the temperature of 90 ℃ until the mixture is uniform to prepare the phase-change composite material with enhanced heat conduction.
(6) And (3) placing the sample obtained in the step (5) in a 90 ℃ oven to be heated until the sample is completely melted, adding the self-repairing aerogel material obtained in the step (4), wherein the mass ratio of the phase-change material to the self-repairing material is 10:1, forming gel, and cooling to obtain the self-repairing composite phase-change material with enhanced heat conduction.
The phase-change temperature of the heat-conduction-enhanced self-repairing composite phase-change material prepared by the embodiment is 66.6 ℃, the latent heat of phase change is 209.4J/g, and the heat conductivity coefficient is 0.2963W m-1K-1The self-repairing rate of the damaged part can reach 70 percent.
The above examples are only preferred embodiments of the present invention, which are intended to be illustrative and not limiting, and those skilled in the art should understand that they can make various changes, substitutions and alterations without departing from the spirit and scope of the invention.
Claims (10)
1. A preparation method of a self-repairing composite phase change material with enhanced heat conduction is characterized by comprising the following steps:
(1) adding 1, 4-phenyl diboronic acid, a photoinitiator, a surfactant, a cross-linking agent, dimethylaminoethyl methacrylate and a hydrophilic monomer containing hydroxyl into water, and uniformly mixing to obtain a mixed solution;
(2) adding the mixed solution obtained in the step (1) into N, N-dimethylacrylamide, uniformly mixing by ultrasonic waves, then reacting under the irradiation of ultraviolet light, and freeze-drying to obtain a self-repairing aerogel material;
(3) heating paraffin until the paraffin is completely dissolved, then adding SEBS and graphene into liquid paraffin, heating and stirring to obtain a phase-change composite material with enhanced heat conduction;
(4) and (3) in a heating state, uniformly mixing the heat conduction enhanced phase change composite material obtained in the step (3) with the self-repairing aerogel material obtained in the step (2), and cooling to room temperature to obtain the heat conduction enhanced self-repairing composite phase change material.
2. The preparation method of the self-repairing composite phase-change material with the enhanced heat conduction of claim 1, wherein the mixed solution in the step (1) comprises the following components in parts by mass:
3. the method for preparing the self-repairing composite phase-change material with the enhanced heat conduction of claim 1, wherein the photoinitiator in the step (1) is 4-phenylbenzophenone; the cross-linking agent in the step (1) is magnesium lithium silicate; the hydrophilic monomer containing hydroxyl in the step (1) is N-N dimethyl amide; the surfactant in the step (1) is sodium dodecyl benzene sulfonate.
4. The preparation method of the self-repairing composite phase-change material with the enhanced heat conduction of claim 1, wherein the mass ratio of the mixed solution in the step (2) to the N, N-dimethylacrylamide is 1-5: 1; the power of the ultraviolet light in the step (2) is 50-300mW/cm2(ii) a The reaction time under the irradiation of ultraviolet light is 300-500 s; the freeze drying time in the step (2) is 50-60 h.
5. The preparation method of the self-repairing composite phase change material with the enhanced heat conduction of claim 1, wherein the heating and stirring temperature in the step (3) is 80-110 ℃, and the heating and stirring time is 10-30 minutes.
6. The preparation method of the self-repairing composite phase change material with the enhanced heat conduction of claim 1, wherein the SEBS obtained in the step (3) is a linear triblock copolymer with polystyrene as a terminal segment and an ethylene-butylene copolymer obtained by hydrogenation of polybutadiene as a middle elastic block; the molecular weight of the SEBS is 60000-100000; the mass ratio of the SEBS to the paraffin is 10-50: 100-200.
7. The preparation method of the heat conduction enhanced self-repairing composite phase-change material as claimed in claim 1, wherein in the heat conduction enhanced phase-change composite material in the step (3), the mass percentage of graphene is 0 wt% -5 wt%.
8. The preparation method of the self-repairing composite phase change material with the enhanced heat conduction of claim 1, wherein the temperature in the heating state in the step (4) is 80-110 ℃; in the self-repairing composite phase change material with enhanced heat conduction in the step (4), the self-repairing aerogel material is 5-20 wt% in mass percentage.
9. The self-repairing composite phase change material with enhanced heat conduction prepared by the preparation method of any one of claims 1-8.
10. Use of the thermally enhanced self-healing composite phase change material of claim 9 in the preparation of a solar storage device.
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