CN108441174B - Phase-change heat storage material and preparation method thereof - Google Patents
Phase-change heat storage material and preparation method thereof Download PDFInfo
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- CN108441174B CN108441174B CN201810368446.8A CN201810368446A CN108441174B CN 108441174 B CN108441174 B CN 108441174B CN 201810368446 A CN201810368446 A CN 201810368446A CN 108441174 B CN108441174 B CN 108441174B
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- C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
- C09K5/02—Materials undergoing a change of physical state when used
- C09K5/06—Materials undergoing a change of physical state when used the change of state being from liquid to solid or vice versa
- C09K5/063—Materials absorbing or liberating heat during crystallisation; Heat storage materials
Abstract
The invention provides a phase-change heat storage material and a preparation method thereof, belonging to the technical field of energy storage materials, wherein the phase-change heat storage material comprises 70-95% of an energy storage main material, 0.01-7.5% of a thickening agent, 0.1-10% of a nucleating agent, 1-5% of a reinforcing material and 0.1-5% of an additive, wherein the additive comprises propylene glycol and petrolatum, the mass ratio of the propylene glycol to the petrolatum is 2-3: 1.6-1.8, the mass ratio of the additive to the thickening agent is 1:1-2, the phase separation phenomenon of the phase-change heat storage material is greatly improved by adding a proper additive, and the thermal cycle performance is improved for intensifying the supercooling phenomenon.
Description
Technical Field
The invention relates to the technical field of energy storage materials, in particular to a phase change heat storage material and a preparation method thereof.
Background
With the increasing prominence of the problems of energy shortage and environmental pollution, people pay more and more attention to the utilization of new energy and the improvement of the utilization rate of the energy. Energy storage technology is gaining favor from domestic and foreign enterprises and related research institutions as an important method for solving the problem of energy supply-demand imbalance. Among them, thermal energy storage based on phase change energy storage materials is one of the most widely applied energy storage technologies at present.
The phase-change energy storage is that the phase-change material absorbs or releases heat to store and release energy during phase change, and compared with sensible heat storage, the phase-change energy storage has the advantages of high energy storage density, constant temperature and the like, has wide application in the fields of waste heat and waste heat recycling, solar energy utilization, electric power peak shifting and valley filling, industrial and civil building heating and air conditioning energy saving, aerospace, textile industry and the like, and is vital to realizing sustainable development of economy and society.
The phase change energy storage material is used as a core of phase change energy storage and can be divided into inorganic, organic and polymer phase change materials, the inorganic phase change energy storage material takes inorganic salt hydrate as an example, and has the advantages of fixed melting point, phase change heat delta Hf, high heat conductivity coefficient (about 0.5W/m.DEG C), high volume energy storage density and the like, and the phase change energy storage material has good application prospect due to low cost and simple preparation.
However, the inorganic salt hydrate has the defects of easy supercooling and phase separation, so that the material is easy to separate out, the cycle service life of the material is shortened, and the practical application is severely restricted; compared with organic materials, the thermal conductivity is higher, but in practical application, the thermal conductivity still needs to be improved. Therefore, how to reduce supercooling, reduce phase separation, and improve the thermal conductivity of the material is critical to the practical application of the material.
Disclosure of Invention
The invention aims to provide a phase change heat storage material which can reduce supercooling degree and phase separation phenomenon and has better cycle stability.
Another object of the present invention is to provide a method for preparing a phase change heat storage material, which can prepare a phase change heat storage material with better cycle stability.
The embodiment of the invention is realized by the following steps:
first aspect of the invention: the phase change heat storage material comprises, by weight, 70% -95% of an energy storage main material, 0.01% -10% of a thickening agent, 0.1% -10% of a nucleating agent, 1% -5% of a reinforcing material and 3% -5% of an additive, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2-3: 1.6-1.8.
Preferably, the thickener is selected from one or more of inorganic thickeners, fiber thickeners, polyacrylate thickeners and natural polymer thickeners.
Preferably, the natural polymer-based thickener is selected from one or more of xanthan gum and guar gum.
Preferably, the polyacrylate thickener is selected from one or more of sodium polyacrylate, polyacrylic acid and copolymers thereof.
Preferably, the energy storage host material is a crystalline hydrated salt, and the crystalline hydrated salt is barium hydroxide octahydrate.
Preferably, the nucleating agent is selected from one or more of aluminum potassium sulfate dodecahydrate, calcium sulfate dihydrate, barium chloride, disodium hydrogen phosphate dodecahydrate and sodium sulfate.
Preferably, the reinforcing material is one or more of a nanoscale metal or metal oxide powder, a carbon material, a foam material, and nanoparticles.
Preferably, the nanoparticles comprise copper nanoparticles and/or carbon nanotubes.
Preferably, the foam material comprises graphite foam, metal aluminum foam or copper foam.
Second aspect of the invention: the preparation method of the phase-change heat storage material is provided, and the phase-change heat storage material is obtained by uniformly mixing the raw materials, heating until the energy storage main body material is melted, and uniformly stirring.
The embodiment of the invention has the beneficial effects that: by adding the additive into the phase change energy storage material, the technical problem that the phase separation phenomenon is easy to occur in the conventional phase change energy storage material is solved, and the circulation stability of the phase change energy storage material is remarkably improved.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below. The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer. The reagents or instruments used are not indicated by the manufacturer, and are all conventional products available commercially.
The phase-change heat storage material and the preparation method thereof of the present invention are specifically described below.
The phase change energy storage material comprises, by weight, 70% -95% of an energy storage main body material, 0.01% -10% of a thickening agent, 0.1% -10% of a nucleating agent, 1% -5% of a reinforcing material and 3% -5% of an additive, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2-3: 1.6-1.8.
The petrolatum is called petroleum ester, namely vaseline, and the main raw material of the petrolatum is cerate separated from residual oil left after the crude oil is subjected to atmospheric pressure and vacuum distillation.
The reason why the poor circulation stability of the phase change energy storage material occurs is that after multiple uses, the energy storage main body material is subjected to multiple energy storage cycles, and then agglomeration and other phenomena occur, which are caused by uneven dispersion of the energy storage main body material in the phase change energy storage material after multiple energy storage cycles, and generally, the situation can be improved by using the lubricant, but the conventional lubricant becomes extremely viscous after being mixed with the thickener, so that the energy storage main body material is not easy to disperse, and the circulation stability is reduced.
Meanwhile, the lubricant has high fluidity, and can increase the supercooling phenomenon of the phase change heat storage material after being applied to the phase change heat storage material, and the defects can cause that the phase change energy storage material is not suitable for adding the lubricant in the prior art.
The applicant finds that the defects can be avoided and the phase separation phenomenon can be improved by compounding part of the lubricant and reasonably adjusting the proportion of the lubricant and the thickening agent, so that the technical purpose of improving the circulation stability is achieved. The applicant finds that propylene glycol and petrolatum have a good lubricating effect, and the energy storage main body material can be better dispersed by utilizing the good lubricating effect in the process of preparing the phase change energy storage material, so that the problem of poor circulation stability caused by agglomeration of the energy storage main body material in the recycling process is avoided. Meanwhile, as the propylene glycol and the petrolatum belong to organic alcohol or ester substances, the differences of the fluidity of the propylene glycol and the petrolatum are not too large compared with the thickening agent, the phase separation phenomenon of the phase change heat storage material can be obviously improved when the propylene glycol and the petrolatum are compounded, and meanwhile, the supercooling phenomenon has no obvious difference compared with the situation before the additive compounded by the propylene glycol and the petrolatum is not added.
In light of the foregoing, the relative proportion of the thickener and the additive is very important, and excessive thickener can reduce the lubricating effect of the lubricant, and cannot improve the circulation stability, and excessive additive will cause the phenomenon of excessive fluidity of the phase change energy storage material and aggravation of supercooling.
The applicant finds that in the phase change energy storage material, the mass percent of the thickening agent is controlled to be 0.01-10%, the mass percent of the additive is controlled to be 0.1-5%, and the ratio of the additive to the thickening agent is controlled to be in a range of 1: 1-2.
Meanwhile, the proportion of the propylene glycol and the petrolatum in the additive is extremely important for controlling the total fluidity of the additive, and the applicant finds that the mass ratio of the propylene glycol to the petrolatum is controlled to be 2-3: 1.6-1.8, the total fluidity of the additive is moderate, and after the additive is mixed with the thickening agent, the probability of the phase separation phenomenon can be reduced, and the supercooling phenomenon can not be aggravated.
More preferably, the phase-change heat storage material comprises 80-95 wt% of energy storage main body material, 0.01-7.5 wt% of thickening agent, 0.1-10 wt% of nucleating agent, 1-5 wt% of reinforcing material and 0.1-5 wt% of additive. Through the reasonable proportion that reduces the thickener, improve the proportion of energy storage host material, can improve phase change energy storage material's energy storage density, simultaneously, reduce the thickener proportion, release mobility, further improve phase change energy storage material's circulation ability.
In some embodiments of the present invention, the thickener is selected from one or more of inorganic thickeners, fiber-based thickeners, polyacrylate-based thickeners, i.e., natural polymer-based thickeners.
In some embodiments of the invention, the natural polymeric thickener is selected from one or more of xanthan gum and guar gum. Xanthan gum is also called xanthan gum, xanthan gum and Xanthan polysaccharide, is a monospore polysaccharide produced by fermentation of pseudoxanthomonas, guar gum is a galactomannan, both are natural polymer thickeners, and when the Xanthan gum and the guar gum are matched with propylene glycol and petrolatum, the fluidity range of the formed system can prevent the phase separation phenomenon caused by agglomeration of an energy storage main body material and improve the circulation capacity of the phase change energy storage material.
In some embodiments of the invention, the polyacrylate thickener is selected from one or more of sodium polyacrylate, polyacrylic acid, and copolymers thereof.
In some embodiments of the invention, the energy storage host material crystallizes a hydrated salt, the crystalline hydrated salt being barium hydroxide octahydrate.
In some embodiments of the invention, the nucleating agent is selected from one or more of potassium aluminum sulfate dodecahydrate, calcium sulfate dihydrate, barium chloride, disodium hydrogen phosphate dodecahydrate, sodium sulfate.
In some embodiments of the invention, the reinforcing material is one or more of a nanoscale metal or metal oxide powder, a carbon material, a foam material, and nanoparticles.
In some embodiments of the invention, the nanoparticles comprise copper nanoparticles and/or carbon nanotubes.
In some embodiments of the invention, the foam material comprises graphite foam, aluminum foam, or copper foam.
As another aspect of the present invention, the present invention also provides a preparation method of the phase change energy storage material, including: and uniformly mixing the raw materials, heating until the energy storage main body material is molten, and uniformly stirring to obtain the energy storage material. The heating temperature is typically 60-90 c, which may be higher depending on the melting point of the energy storage host material.
The phase change energy storage material and the preparation method thereof of the present invention are specifically described below with reference to specific examples.
Example 1
The phase change energy storage material comprises 88% of energy storage main material, 2.5% of thickening agent, 5% of nucleating agent, 2% of reinforcing material and 2.5% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.6, the mass ratio of the additive to the thickening agent is 1:1.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is a mixture of xanthan gum and guar gum, the mixing mass ratio is 2:1, the nucleating agent is calcium sulfate dihydrate, and the reinforcing material is nano copper powder.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 2
The phase change energy storage material comprises 90% of energy storage main body material, 3.3% of thickening agent, 2.7% of nucleating agent, 1% of reinforcing material and 3% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.7, and the mass ratio of the additive to the thickening agent is 1: 1.1.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is sodium polyacrylate, the nucleating agent is aluminum potassium sulfate dodecahydrate, and the reinforcing material is nano copper powder.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 3
The phase change energy storage material comprises 70% of energy storage main body material, 10% of thickening agent, 10% of nucleating agent, 5% of reinforcing material and 5% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.8, and the mass ratio of the additive to the thickening agent is 1:2.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is polyacrylic acid and a copolymer thereof, the nucleating agent is barium chloride, and the reinforcing material is nano copper powder.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 4
The phase change energy storage material comprises, by weight, 92% of an energy storage main material, 0.13% of a thickening agent, 5.27% of a nucleating agent, 2.5% of a reinforcing material and 0.1% of an additive, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2.5: 1.6, and the mass ratio of the additive to the thickening agent is 1: 1.3.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is xanthan gum, the nucleating agent is disodium hydrogen phosphate dodecahydrate, and the reinforcing material is nano copper powder.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 5
The phase change energy storage material comprises 80% of energy storage main body material, 7.5% of thickening agent, 6.5% of nucleating agent, 1.5% of reinforcing material and 4.5% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2.5: 1.7, the mass ratio of the additive to the thickener is about 1: 1.6.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is guar gum, the nucleating agent is sodium sulfate, and the reinforcing material is nano copper powder.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 6
The phase change energy storage material comprises 78% of energy storage main body material, 5% of thickening agent, 9.44% of nucleating agent, 4% of reinforcing material and 3.56% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2.5: 1.8, the mass ratio of the additive to the thickener is about 1: 1.5.
In the embodiment, the energy storage main material is sodium thiosulfate pentahydrate, the thickening agent is a mixture of xanthan gum and guar gum, the mixing mass ratio is 2:1, the nucleating agent is a mixture of calcium sulfate dihydrate and barium chloride, and the reinforcing material is nano copper powder.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 7
The phase change energy storage material comprises 88.5% of energy storage main body material, 6.4% of thickening agent, 0.1% of nucleating agent, 1% of reinforcing material and 4% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 3: 1.6, and the mass ratio of the additive to the thickening agent is 1: 1.6.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is a mixture of xanthan gum and guar gum, the mixing mass ratio is 2:1, the nucleating agent is calcium sulfate dihydrate, and the reinforcing material is copper foam.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 8
The phase change energy storage material comprises 88% of energy storage main material, 3.4% of thickening agent, 3.6% of nucleating agent, 3% of reinforcing material and 2% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 3: 1.7, and the mass ratio of the additive to the thickening agent is 1: 1.7.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is a mixture of xanthan gum and guar gum, the mixing mass ratio is 2:1, the nucleating agent is calcium sulfate dihydrate, and the reinforcing material is foamy graphite.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 9
The phase change energy storage material comprises 85% of energy storage main body material, 1.8% of thickening agent, 7.2% of nucleating agent, 5% of reinforcing material and 1% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 3: 1.8, and the mass ratio of the additive to the thickening agent is 1: 1.8.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is a mixture of xanthan gum and guar gum, the mixing mass ratio is 2:1, the nucleating agent is calcium sulfate dihydrate, and the reinforcing material is foamed metal aluminum.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Example 10
The phase change energy storage material comprises 95% of energy storage main body material, 0.19% of thickening agent, 2.71% of nucleating agent, 2% of reinforcing material and 0.1% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2.4: 1.7, and the mass ratio of the additive to the thickening agent is 1: 1.9.
In the embodiment, the energy storage main material is barium hydroxide octahydrate, the thickening agent is a mixture of xanthan gum and guar gum, the mixing mass ratio is 2:1, the nucleating agent is calcium sulfate dihydrate, and the reinforcing material is a carbon nano tube.
And mixing the raw materials in a reaction container, heating after mixing, heating until the energy storage main body material is completely melted, and uniformly stirring to obtain the phase change energy storage material.
Comparative example 1
Comparative example 1 was the same as example 1 except that the additive contained propylene glycol alone and no petrolatum.
Comparative example 2
Comparative example 2 was the same as example 1 except that the additive contained only petrolatum and no propylene glycol.
Comparative example 3
Comparative example 3 differs from example 1 in that no additive is included, and the mass percentages of the thickener, nucleating agent and reinforcing material are the same as in example 1, except that the mass percentage of the energy storage host material is 90.5%.
Comparative example 4
The phase change energy storage material comprises 88% of energy storage main material, 3.43% of thickening agent, 5% of nucleating agent, 2% of reinforcing material and 1.56% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.6, the mass ratio of the additive to the thickener is about 1: 2.2.
Comparative example 5
The phase change energy storage material comprises 88% of energy storage main material, 4% of thickening agent, 5% of nucleating agent, 2% of reinforcing material and 1% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.6, and the mass ratio of the additive to the thickening agent is 1: 4.
Comparative example 6
The phase change energy storage material comprises 88% of energy storage main material, 2.37% of thickening agent, 5% of nucleating agent, 2% of reinforcing material and 2.63% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.6, the mass ratio of the additive to the thickener is about 1: 0.9.
Comparative example 6
The phase change energy storage material comprises 88% of energy storage main material, 1.67% of thickening agent, 5% of nucleating agent, 2% of reinforcing material and 3.33% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2: 1.6, the mass ratio of the additive to the thickener is about 1: 0.5.
Comparative example 7
Comparative example 7 is the same as example 1 except that the additive is polyethylene glycol.
Comparative example 8
Comparative example 8 was the same as example 1 except that the additive was hydrogenated vegetable oil.
Of these, polyethylene glycol and hydrogenated vegetable oils are the more commonly used lubricants.
Test examples
The phase change energy storage materials obtained in examples 1 to 10 and comparative examples 1 to 8 were tested according to the following methods:
measurements were performed using Differential Scanning Calorimetry (DSC), test instrument: DSC-200PC Phox differential scanning calorimeter (Shanghai squarey instruments Co., Ltd.). The enthalpy change Δ H is calculated by testing the DSC curve.
The phase change energy storage materials obtained in examples 1 to 10 and comparative examples 1 to 8 were recycled, and measured Δ H after 500 cycles, 800 cycles, 1200 cycles, and 1500 cycles, respectively, and the results are shown in table 1:
TABLE 1 test results table
As can be seen from the data in table 1, the enthalpy value of comparative examples 1 and 2 decreases sharply after 800 cycles when propylene glycol or petrolatum alone is used, which is lower than that of comparative example 3 where no additive is used. The propylene glycol and the petrolatum have synergistic effect when being compounded, and the circulating stability is not reduced and is effectively improved compared with the circulating stability when no additive is added. Likewise, comparative examples 4-6, which illustrate that when the ratio of additive to thickener is too large or too small, the cycle stability is unstable, especially comparative example 5, the enthalpy drops dramatically after 800 cycles of use.
In addition, comparative examples 7 and 8, in which other additives were used, were compared with examples, and the thermal cycle stability of the phase change heat storage material was drastically deteriorated after 500 cycles. Indicating that the additive capable of lubricating does not have the effect of improving the cycle stability.
The embodiments described above are some, but not all embodiments of the invention. The detailed description of the embodiments of the present invention is not intended to limit the scope of the invention as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Claims (6)
1. The phase change heat storage material is characterized by comprising 70-95% of energy storage main body material, 0.01-7.5% of thickening agent, 0.1-10% of nucleating agent, 1-5% of reinforcing material and 0.1-5% of additive in percentage by weight, wherein the additive comprises propylene glycol and petrolatum, and the mass ratio of the propylene glycol to the petrolatum is 2-3: 1.6-1.8, wherein the mass ratio of the additive to the thickener is 1:1-2, and the thickener comprises one or more of fiber thickeners, polyacrylate thickeners and natural polymer thickeners;
the energy storage main body material is crystalline hydrated salt, and the crystalline hydrated salt is barium hydroxide octahydrate; the reinforcing material is one or more of nanoscale metal or metal oxide powder, carbon material, foam material and nano particles.
2. The phase change heat storage material of claim 1, comprising 80-95% of the energy storage host material, 0.01-10% of the thickener, 0.1-10% of the nucleating agent, 1-5% of the reinforcing material, and 0.1-5% of the additive by weight percent.
3. The phase change heat storage material of claim 1 wherein the natural polymeric thickener is selected from one or more of xanthan gum and guar gum.
4. The phase change heat storage material of claim 1 wherein the nucleating agent is selected from one or more of aluminum potassium sulfate dodecahydrate, calcium sulfate dihydrate, barium chloride, disodium hydrogen phosphate dodecahydrate, and sodium sulfate.
5. The phase change heat storage material of claim 1 wherein the nanoparticles comprise copper nanoparticles and/or carbon nanotubes.
6. The method for preparing phase-change heat storage material according to any one of claims 1 to 5, wherein the heat storage material is prepared by mixing the raw materials uniformly, heating until the energy storage main body material is melted, and stirring uniformly.
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