CN112812750A - Application of silane coupling agent in new energy storage material and new solar energy heat supply system - Google Patents
Application of silane coupling agent in new energy storage material and new solar energy heat supply system Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- 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
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F24—HEATING; RANGES; VENTILATING
- F24D—DOMESTIC- OR SPACE-HEATING SYSTEMS, e.g. CENTRAL HEATING SYSTEMS; DOMESTIC HOT-WATER SUPPLY SYSTEMS; ELEMENTS OR COMPONENTS THEREFOR
- F24D15/00—Other domestic- or space-heating systems
- F24D15/02—Other domestic- or space-heating systems consisting of self-contained heating units, e.g. storage heaters
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
- F28D20/00—Heat storage plants or apparatus in general; Regenerative heat-exchange apparatus not covered by groups F28D17/00 or F28D19/00
- F28D20/02—Heat storage plants or apparatus in general; Regenerative heat-exchange apparatus not covered by groups F28D17/00 or F28D19/00 using latent heat
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/14—Thermal energy storage
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E70/00—Other energy conversion or management systems reducing GHG emissions
- Y02E70/30—Systems combining energy storage with energy generation of non-fossil origin
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
Abstract
Disclosed is the use of a silane coupling agent in energy storage materials and new solar energy heating systems, wherein the silane coupling agent is selected from the compounds represented by formula (1). The new energy storage material has better heat conductivity and higher latent heat of phase change; and the heat and mass transfer efficiency of the new energy storage material is improved compared with the prior art. In addition, the new energy storage material has better stability and is not easy to leak.
Description
Technical Field
The invention belongs to the technical field of solar energy; relates to the application of a silane coupling agent in a new energy storage material and a new solar energy heating system.
Background
With the development of global economy, the energy demand is increasing day by day, and the problem of energy exhaustion is gradually highlighted. The environmental pollution problem caused by the traditional fossil energy is also becoming more serious, and the development and utilization of new energy are becoming the key points of research in various countries. Among various new energy sources, solar energy has the advantages of cleanness, no pollution, sustainability and the like. However, the breadth of our country is broad, and especially in the vast western and northern regions, the solar energy resource is abundant, and the solar energy resource has considerable development potential.
However, due to the influence of factors such as weather, geography, illumination time and the like, solar energy has the defects of low energy storage density, discontinuity and the like, and cannot provide continuous and stable high-density energy, so that the application and development of the solar energy are greatly restricted. In order to increase the utilization of solar energy, it is often necessary to use energy storage devices to store the heat collected by the solar energy.
Among the energy storage devices, the most widely used core material is a phase change energy storage material. Phase change materials are mainly classified into organic, inorganic and composite phase change materials according to their chemical compositions. In the field of medium and low temperature phase change heat storage of solar heating and storage, organic phase change materials such as alkanes, fatty acids and polyols are mostly researched. Among them, paraffin is typically used as the alkane.
The paraffin is colorless, nontoxic and free of pungent smell, stable in physical and chemical properties, large in heat storage density, free of supercooling, low in vapor pressure and widely applied to the field of medium and low temperature phase change heat storage. However, paraffin has the disadvantages of poor heat conductivity, large volume expansion coefficient, poor stability, easy leakage and the like.
Chinese patent application CN105733516A discloses a composite phase change film material based on graphene and a preparation method thereof. In the preparation method, the graphene oxide aqueous solution with a certain concentration is continuously extruded at a constant speed from a preparation device with a linear outlet, enters a solidification liquid, and is put into liquid nitrogen for quick freezing. And then, obtaining a graphene oxide aerogel film through freeze drying, sending the graphene oxide aerogel film into a high-temperature furnace for high-temperature 1300-3000 ℃ heat treatment in an inert atmosphere, then soaking the graphene oxide aerogel film in dichloromethane solutions of paraffin with different concentrations, and fully absorbing the solution to obtain the graphene-based composite phase change film material. The graphene composite phase-change film material has an excellent paraffin packaging effect, the paraffin filling amount is 0.1-99.9%, the film-paraffin composite is uniform, and after multiple heating and cooling cycles, the melting phase-change enthalpy and the solidification phase-change enthalpy of the material basically keep unchanged, so that efficient heat energy storage is realized. However, this patent application uses the dichloromethane solution of graphite alkene aerogel and paraffin to carry out compound, and dichloromethane volatilizees and can lead to compound phase change membrane material to appear a large amount of holes to it is more to lead to its heat conduction efficiency and heat accumulation density to descend. Meanwhile, methylene dichloride is used as a toxic reagent in the patent application, and potential danger is caused to human bodies and the environment.
Chinese patent application CN110804420A discloses a phase change composite material based on a high-thermal-conductivity anisotropic graphene framework and a preparation method thereof, wherein ethanol is introduced into a water system for directional freezing to ensure that graphene sheets are regularly arranged, polyimide is introduced into a graphene three-dimensional network and graphitized to connect the graphene sheets so as to reduce contact thermal resistance, interface thermal resistance and phonon scattering caused by defects of the graphene thermal-conductive network, the obtained three-dimensional graphene framework has excellent thermal conductivity, and the phase change composite material obtained by compounding with the phase change material has high thermal conductivity and high phase change latent heat. The preparation process disclosed by the patent application is safe, environment-friendly and pollution-free, is suitable for mass production, solves the problem that the low filling content and the high thermal conductivity of the conventional phase-change composite material cannot be simultaneously met, and obtains the efficient energy storage material. However, in the preparation method of this patent application, the graphene aerogel needs to be graphitized at a high temperature in a graphitization furnace after the imidization reaction, and the high temperature is preferably 2800 ℃. At the high temperature, polyimide is easy to thermally degrade, so that a pre-constructed graphene three-dimensional network has certain defects, the improvement of the heat-conducting property of the phase-change material is influenced, and the latent heat of phase change is reduced more than that of pure paraffin due to the factors such as mass fraction of graphene and pore distribution of aerogel. This leads to inefficient heat and mass transfer of the energy storage material.
On the other hand, as an energy storage material of a solar new energy heating system, the material also needs to have certain stability, that is, the energy storage material should avoid the problems of leakage and the like in the using process, and if not, the material will cause the performance reduction and even failure of the phase change energy storage material, and the problem that the surrounding environment is polluted and the like is seriously caused.
The inventors have found that the above problems can be preferably solved when a specific silane coupling agent is used in a new energy storage material and a new solar energy heating system.
Disclosure of Invention
The invention aims to provide application of a silane coupling agent in new energy storage materials. The invention also aims to provide the application of the silane coupling agent in a solar new energy heating system. The new energy storage material has better heat conductivity and higher latent heat of phase change; and the heat and mass transfer efficiency of the new energy storage material is improved compared with the prior art. In addition, the new energy storage material has better stability and is not easy to leak.
In order to achieve the purpose, the invention provides application of a silane coupling agent in an energy storage material, wherein the energy storage material takes graphene aerogel as a carrier and takes paraffin as a phase change material; the graphene aerogel is prepared from graphene oxide by adopting chemical reduction self-assembly and freeze drying; the graphene oxide is selected from graphene oxide modified by a silane coupling agent; characterized in that the silane coupling agent is selected from compounds represented by formula (1),
wherein A represents a divalent, trivalent or tetravalent organic group of 2 to 50 carbon atoms; l represents an organic group having 1 to 10 carbon atoms; R1-R3 each independently represent a hydrogen atom, an alkyl or alkoxy group of 1-10 carbon atoms optionally substituted by halogen, an alkenyl or alkenyloxy group of 2-10 carbon atoms optionally substituted by halogen, an aryl or aryloxy group of 5-10 carbon atoms optionally substituted by halogen.
The use according to the invention, wherein the silane coupling agent is selected from compounds represented by formula (2),
wherein B represents a cyclic unit fused with an imido ring, and L and R1 to R3 are as described above.
The use according to the invention, wherein the silane coupling agent is selected from compounds represented by formula (3),
wherein R4 to R7 each independently represents a hydrogen atom or a substituent, and L and R1 to R3 are as described above.
The use according to the invention, wherein the silane coupling agent is selected from compounds represented by formula (4),
the application of the invention is that the weight ratio of graphene oxide to silane coupling agent is 1: (1.5-2.5).
The use according to the invention, wherein the modification conditions are: the reaction temperature is 60-80 ℃, and the reaction time is 12-48 h.
The application of the graphene aerogel provided by the invention is characterized in that the graphene aerogel is further subjected to heat treatment at the temperature of 250-350 ℃.
The application is further applied to a solar new energy heating system.
The invention has the beneficial effects that: compared with the prior art, when the specific silane coupling agent is used in the new energy storage material and the new solar energy heating system, the new energy storage material has better heat conductivity and is increased to more than 3 times of the pure phase change material; meanwhile, the latent heat of phase change is higher and is at least more than 85 percent of that of the pure phase change material. In addition, after the energy storage new material undergoes multiple cold and hot cycles, the energy storage new material has better stability and is not easy to leak.
Without wishing to be bound by any theory, the use of the specific silane coupling agents of the present invention improves the above-mentioned properties of new energy storage materials.
Detailed Description
The present invention will be further described with reference to the following examples, which are not intended to limit the scope of the invention. Unless otherwise indicated, percentages in the examples are uniformly percentages by mass.
Example 1
(1) Modification of graphene oxide: mixing 200mg of graphene oxide (synthesized by Hummers method of Beijing Deke island gold technologies Co., Ltd.) with 100mL of deionized water, and performing ultrasonic treatment for 2 hours to form a uniform graphene oxide dispersion liquid; dropwise adding a mixed solution of anhydrous ethanol-toluene (volume ratio is 1:1) containing 400mg of silane coupling agent gamma-phthalimidopropyltrimethoxysilane (CAS: 154717-09-6) into the graphene oxide dispersion liquid under stirring; after the addition, the pH was adjusted to 5.0 using acetic acid. Then reacted at 70 ℃ for 24 hours, cooled to room temperature, centrifuged, and the precipitate was washed 3 times each with anhydrous ethanol and deionized water to remove unreacted silane coupling agent. And drying in vacuum to obtain modified graphene oxide powder.
FT-IR spectrum shows that the modified graphene oxide powder is increased by 2960cm compared with unmodified graphene oxide-1(CH3)、2890cm-1(CH2)、1740cm-1(-C＝O)、1600cm-1(benzene ring-H) 1465cm-1(benzene ring-H), 1050cm-1(Si-O-C) and the like, indicating that the modified GO powder is grafted with the silane coupling agent.
(2) Preparing the graphene aerogel: adding 60mg of modified graphene oxide powder into 12mL of deionized water, and carrying out ultrasonic treatment for 0.5h to form a uniform modified graphene oxide dispersion liquid. And (3) injecting 100 mu L of Ethylenediamine (EDA) into the modified graphene oxide dispersion liquid, and reacting at 90 ℃ for 12h to obtain the graphene hydrogel. The graphene hydrosol was washed 3 times each with anhydrous ethanol and deionized water. Pre-freezing the graphene hydrosol at-20 ℃ for 12h, then placing the pre-frozen graphene hydrosol in a freeze dryer, and carrying out vacuum drying for 24h to obtain the graphene aerogel.
(3) And (3) heat treatment of the graphene aerogel: and (2) placing the graphene aerogel in a tube furnace, heating the graphene aerogel to 300 ℃ from room temperature at a heating rate of 2 ℃/min in a nitrogen atmosphere, then preserving heat for 6 hours, and then cooling to room temperature, wherein the cooling rate is the same as the heating rate, so that the heat-treated graphene aerogel is obtained.
(4) Preparing a phase change energy storage material: the graphene aerogel is used as a carrier, the paraffin is used as a phase-change material, and the weight ratio of the graphene aerogel to the paraffin is 1: 9. and heating the phase change material to a molten state, adding graphene aerogel, and carrying out vacuum adsorption for 2 h. And cooling to room temperature to obtain the phase change energy storage material.
Comparative example 1
Step (3) is not carried out; the other conditions were the same as in example 1.
Comparative example 2
KH550 is used as the silane coupling agent in the step (1); the other conditions were the same as in example 1.
Testing of Material Properties
The thermal conductivity and latent heat of phase change and relative percentage of the phase change energy storage materials obtained in example 1 and comparative examples 1 to 2 and pure paraffin were measured and calculated, respectively.
Wherein, the heat conductivity coefficient is measured and calculated by adopting a TC3200 heat conductivity coefficient instrument. The instrument adopts the principle of a transient hot wire method, and the measurement range is 0.001-20W/(mK). The latent heat of phase change was measured using a DSC-Q20 differential scanning calorimeter. The test temperature is-10 to 80 ℃, the temperature rising and reducing speed is 10 ℃/min, the nitrogen purging flow rate is 40mL/min, and the phase change latent heat of the material is obtained from the obtained heat flow curve by utilizing the self-contained analysis software of the instrument.
The results are shown in table 1 below.
TABLE 1
| Thermal conductivity (W/(mK)) | Latent heat of phase change (J/g) | Relative percentage (%) | |
| Example 1 | 0.967 | 172.6 | 88.1 |
| Comparative example 1 | 0.620 | 153.9 | 78.5 |
| Comparative example 2 | 0.524 | 141.5 | 72.2 |
| Pure paraffin wax | 0.318 | 196.1 | 100 |
As can be seen from Table 1, the new energy storage material of example 1 of the present application has better heat conductivity; meanwhile, the latent heat of phase change is higher; and the heat and mass transfer efficiency of the new energy storage material is improved compared with the prior art.
Further, the phase change energy storage materials of example 1 and comparative examples 1 to 2 were placed on a glass plate, and the glass plate was placed in a drying oven at 80 ℃, kept for 10min, taken out, cooled to room temperature, and recorded as a cooling-heating cycle. The thermal conductivities of the phase change energy storage materials of example 1 and comparative examples 1-2 were measured again after 100 repetitions, and the thermal conductivities of the three were respectively equivalent to 94.2%, 71.8% and 83.5% of the values in table 1.
It should be understood that the detailed description of the invention is merely illustrative of the spirit and principles of the invention and is not intended to limit the scope of the invention. Furthermore, it should be understood that various changes, substitutions, deletions, modifications or adjustments may be made by those skilled in the art after reading the disclosure of the present invention, and such equivalents are also within the scope of the invention as defined in the appended claims.
Claims (8)
1. The application of the silane coupling agent in the energy storage material takes graphene aerogel as a carrier and takes paraffin as a phase change material; the graphene aerogel is prepared from graphene oxide by adopting chemical reduction self-assembly and freeze drying; the graphene oxide is selected from graphene oxide modified by a silane coupling agent; characterized in that the silane coupling agent is selected from compounds represented by formula (1),
wherein A represents a divalent, trivalent or tetravalent organic group of 2 to 50 carbon atoms; l represents an organic group having 1 to 10 carbon atoms; R1-R3 each independently represent a hydrogen atom, an alkyl or alkoxy group of 1-10 carbon atoms optionally substituted by halogen, an alkenyl or alkenyloxy group of 2-10 carbon atoms optionally substituted by halogen, an aryl or aryloxy group of 5-10 carbon atoms optionally substituted by halogen.
2. The use according to claim 1, wherein the silane coupling agent is selected from compounds represented by formula (2),
wherein B represents a cyclic unit fused with an imido ring, and L and R1 to R3 are as defined in claim 1.
3. The use according to claim 2, wherein the silane coupling agent is selected from compounds represented by formula (3),
wherein R4-R7 each independently represent a hydrogen atom or a substituent, and L and R1-R3 are as defined in claim 1.
4. The use according to claim 3, wherein the silane coupling agent is selected from compounds represented by formula (4),
5. use according to claim 1, wherein the weight ratio of graphene oxide to silane coupling agent is 1: (1.5-2.5).
6. Use according to claim 1, wherein the modification conditions are: the reaction temperature is 60-80 ℃, and the reaction time is 12-48 h.
7. The use as claimed in claim 1, wherein the graphene aerogel is further subjected to a heat treatment at 250-350 ℃.
8. Use according to claim 1, further in a solar new energy heating system.
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