CN114539980A - Phase-change material capable of storing energy at room temperature for long time and preparation and application thereof - Google Patents
Phase-change material capable of storing energy at room temperature for long time and preparation and application thereof Download PDFInfo
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- 239000012782 phase change material Substances 0.000 title claims abstract description 37
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- 229920002401 polyacrylamide Polymers 0.000 claims abstract description 42
- 238000004146 energy storage Methods 0.000 claims abstract description 35
- UNXHWFMMPAWVPI-UHFFFAOYSA-N Erythritol Natural products OCC(O)C(O)CO UNXHWFMMPAWVPI-UHFFFAOYSA-N 0.000 claims abstract description 29
- 239000004386 Erythritol Substances 0.000 claims abstract description 29
- UNXHWFMMPAWVPI-ZXZARUISSA-N erythritol Chemical compound OC[C@H](O)[C@H](O)CO UNXHWFMMPAWVPI-ZXZARUISSA-N 0.000 claims abstract description 29
- 229940009714 erythritol Drugs 0.000 claims abstract description 29
- 235000019414 erythritol Nutrition 0.000 claims abstract description 29
- 238000003756 stirring Methods 0.000 claims abstract description 17
- 230000007774 longterm Effects 0.000 claims abstract description 12
- 238000005338 heat storage Methods 0.000 claims abstract description 9
- 239000000463 material Substances 0.000 claims abstract description 8
- 239000013526 supercooled liquid Substances 0.000 claims abstract description 3
- 239000007864 aqueous solution Substances 0.000 claims description 26
- 239000011232 storage material Substances 0.000 claims description 19
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 18
- 229920000642 polymer Polymers 0.000 claims description 16
- 150000005846 sugar alcohols Chemical class 0.000 claims description 12
- 239000002861 polymer material Substances 0.000 claims description 11
- 238000001035 drying Methods 0.000 claims description 8
- 238000012546 transfer Methods 0.000 claims description 8
- 239000003153 chemical reaction reagent Substances 0.000 claims description 6
- 125000000129 anionic group Chemical group 0.000 claims description 5
- 238000003860 storage Methods 0.000 claims description 3
- 239000012752 auxiliary agent Substances 0.000 claims description 2
- 125000002091 cationic group Chemical group 0.000 claims description 2
- 239000007787 solid Substances 0.000 claims description 2
- 238000006243 chemical reaction Methods 0.000 claims 1
- 238000002156 mixing Methods 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 9
- 239000002918 waste heat Substances 0.000 abstract description 6
- 238000004064 recycling Methods 0.000 abstract 1
- 230000008859 change Effects 0.000 description 12
- 238000002425 crystallisation Methods 0.000 description 9
- 230000008025 crystallization Effects 0.000 description 9
- 239000012071 phase Substances 0.000 description 9
- 239000007788 liquid Substances 0.000 description 6
- 230000008569 process Effects 0.000 description 6
- 238000001816 cooling Methods 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 230000009972 noncorrosive effect Effects 0.000 description 2
- 231100000252 nontoxic Toxicity 0.000 description 2
- 230000003000 nontoxic effect Effects 0.000 description 2
- 229920005862 polyol Polymers 0.000 description 2
- 150000003077 polyols Chemical class 0.000 description 2
- 238000003303 reheating Methods 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 238000002076 thermal analysis method Methods 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229930014626 natural product Natural products 0.000 description 1
- 230000006911 nucleation Effects 0.000 description 1
- 238000010899 nucleation Methods 0.000 description 1
- 239000012074 organic phase Substances 0.000 description 1
- 238000005191 phase separation Methods 0.000 description 1
- 238000002464 physical blending Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000004781 supercooling Methods 0.000 description 1
- 230000001960 triggered effect Effects 0.000 description 1
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Abstract
Description
技术领域technical field
本发明属于相变储能材料及其制备技术领域，涉及了一种可在室温下长期储能的相变材料的设计及其制备技术。The invention belongs to the technical field of phase-change energy storage materials and their preparation, and relates to the design and preparation technology of a phase-change material capable of storing energy for a long time at room temperature.
背景技术Background technique
太阳能的间歇性特点，使其在热能供、需之间存在不匹配问题。例如：夏季太阳热能充沛，很多却不能加以利用，而在冬季天气寒冷，靠太阳能供热并不能满足人们的需求。因此开发可长期相变储能技术、提高能源利用效率对我国能源发展意义重大。相变储能材料在其发生相变过程中能够吸收或者释放大量的相变潜热，储热量远高于传统的显热储能材料；另外，相变过程具有可逆性、循环稳定性；且高效长期相变储能材料能够储存数周或数月的热量，在提高能源利用率和解决能源时空供需不匹配的问题上优于显热储热和化学方法储热。The intermittent nature of solar energy makes it a mismatch between thermal energy supply and demand. For example, there is abundant solar heat energy in summer, but a lot of it cannot be used. In winter, the weather is cold, and solar heating cannot meet people's needs. Therefore, the development of long-term phase change energy storage technology and the improvement of energy utilization efficiency are of great significance to my country's energy development. Phase change energy storage materials can absorb or release a large amount of latent heat of phase change during the phase change process, and the heat storage is much higher than that of traditional sensible heat energy storage materials; in addition, the phase change process is reversible and cyclically stable; and efficient Long-term phase change energy storage materials can store heat for weeks or months, and are superior to sensible heat storage and chemical heat storage in improving energy utilization and solving the mismatch between energy supply and demand in space and time.
目前跨季节相变储能材料应用较多的是无机水合盐体系(中国专利CN 103712255B)，其储热密度高、价格低廉，但无机水合盐对金属具有较强的腐蚀性，且存在相分离和严重过冷现象。而有机类相变材料，如多元醇类对金属设备无腐蚀且具有良好的成核特性、化学特性和热稳定性；此外，多元醇类相变材料之一的赤藓糖醇是天然产物，原料廉价易得；且具有无毒、不易燃、无腐蚀性等优点，是一种性能优异的相变储能材料，在废热传输、太阳能蓄热、汽车废热循环系统领域备受关注。赤藓糖醇分子间有大量氢键，过冷度高，可通过外加物质与其形成氢键，使其在冷却过程中不结晶，而在再加热过程中出现冷结晶以及随后的熔化。因此本发明的重点在于通过物理共混制备赤藓糖醇基可室温下长期储能的相变材料，该材料具有制备工艺简单、储热密度高、放热可控等优点，适用于太阳能热能储存、废热传输等领域。At present, the inorganic hydrated salt system (Chinese patent CN 103712255B) is widely used for inter-seasonal phase change energy storage materials, which has high heat storage density and low price, but the inorganic hydrated salt has strong corrosiveness to metals, and there is phase separation. and severe overcooling. However, organic phase change materials, such as polyols, are non-corrosive to metal equipment and have good nucleation properties, chemical properties and thermal stability; in addition, erythritol, one of polyol phase change materials, is a natural product. The raw material is cheap and easy to obtain; and has the advantages of non-toxic, non-flammable, non-corrosive, etc., it is a phase-change energy storage material with excellent performance, and has attracted much attention in the fields of waste heat transmission, solar thermal storage, and automobile waste heat cycle systems. Erythritol has a large number of hydrogen bonds between molecules and has a high degree of supercooling. It can form hydrogen bonds with it by adding substances, so that it does not crystallize during the cooling process, but cold crystallization and subsequent melting occur during the reheating process. Therefore, the focus of the present invention is to prepare an erythritol-based phase change material with long-term energy storage at room temperature through physical blending. The material has the advantages of simple preparation process, high heat storage density, controllable heat release and the like, and is suitable for solar thermal energy storage, waste heat transfer, etc.
发明内容SUMMARY OF THE INVENTION
本发明主要解决的技术问题是克服以上背景技术中提到的不足和缺陷，提供一种可室温下长期储能的相变材料的制备方法，所得材料可在室温下长时间稳定高效储热，且具有优越的化学稳定性、热稳定性和安全性；可用于太阳能热能储存或废热传输等。The main technical problem solved by the present invention is to overcome the deficiencies and defects mentioned in the above background technology, and provide a preparation method of a phase change material that can store energy for a long time at room temperature, and the obtained material can store heat stably and efficiently for a long time at room temperature, And it has excellent chemical stability, thermal stability and safety; it can be used for solar thermal energy storage or waste heat transfer, etc.
本发明采用的技术方案为：The technical scheme adopted in the present invention is:
(1)室温下，将聚合物聚丙烯酰胺在水中搅拌一定时间，配制成一定质量百分比浓度的均相聚丙烯酰胺水溶液；(1) at room temperature, the polymer polyacrylamide is stirred in water for a certain period of time to prepare a homogeneous polyacrylamide aqueous solution with a certain mass percentage concentration;
(2)将一定量的赤藓糖醇加入步骤(1)中制备的聚丙烯酰胺聚合物水溶液中，搅拌一定时间，获得均相糖醇聚合物水溶液共混体系；(2) adding a certain amount of erythritol to the polyacrylamide polymer aqueous solution prepared in step (1), and stirring for a certain period of time to obtain a homogeneous sugar alcohol polymer aqueous solution blend system;
(3)取一定量步骤(2)制备的糖醇聚合物水溶液转移至试剂瓶中，常压，在一定温度、一定时间下烘干水分，制备得可室温下长期储能的相变材料。(3) transfer a certain amount of the sugar alcohol polymer aqueous solution prepared in step (2) into a reagent bottle, dry the water at a certain temperature and a certain time under normal pressure, and prepare a phase change material that can store energy for a long time at room temperature.
进一步地，所述步骤(1)中所用的聚丙烯酰胺为阴离子型、阳离子型、非离子型，且非离子型时最佳；Further, the polyacrylamide used in the step (1) is anionic, cationic, non-ionic, and the non-ionic is the best;
进一步地，所述步骤(1)中所用的聚合物材料聚丙烯酰胺分子量在200-1000万之间。优选为300-700万，且分子量在500万时最佳。Further, the molecular weight of the polymer material polyacrylamide used in the step (1) is between 2 million and 10 million. It is preferably 3 to 7 million, and the molecular weight is optimal when it is 5 million.
进一步地，所述步骤(1)中聚合物材料聚丙烯酰胺在水中搅拌时间为2-8h，优选为4-6h，且在搅拌5h时最佳。Further, in the step (1), the stirring time of the polymer material polyacrylamide in water is 2-8h, preferably 4-6h, and the best time is 5h.
进一步地，所述步骤(1)中聚丙烯酰胺水溶液中聚丙烯酰胺的质量分数为1-5％，优选为1-2％，且质量分数在1％时最佳。。Further, in the step (1), the mass fraction of polyacrylamide in the polyacrylamide aqueous solution is 1-5%, preferably 1-2%, and the mass fraction is the best at 1%. .
进一步地，所述步骤(2)中加入赤藓糖醇后搅拌时间为0.5-2h，且搅拌时间在2h时最佳。Further, the stirring time after adding erythritol in the step (2) is 0.5-2h, and the best stirring time is 2h.
进一步地，所述步骤(2)中相变材料赤藓糖醇于储能材料中的质量含量为85-95％，聚合物材料聚丙烯酰胺于储能材料中的质量含量为5-15％。相变材料赤藓糖醇于储能材料中的质量含量优选为88-92％，最佳为90％。聚合物材料聚丙烯酰胺于储能材料中的质量优选为8-12％，最佳为10％。Further, in the step (2), the mass content of the phase change material erythritol in the energy storage material is 85-95%, and the mass content of the polymer material polyacrylamide in the energy storage material is 5-15% . The mass content of the phase change material erythritol in the energy storage material is preferably 88-92%, and the best is 90%. The mass of the polymer material polyacrylamide in the energy storage material is preferably 8-12%, and the best is 10%.
进一步地，所述储能材料的助剂为水，相变材料赤藓糖醇、聚合物材料聚丙烯酰胺二者于水中的固含量为67-1000mg/ml，优选为80-150mg/ml，且在100mg/ml时最佳。Further, the auxiliary agent of the energy storage material is water, and the solid content of the phase change material erythritol and the polymer material polyacrylamide in water is 67-1000 mg/ml, preferably 80-150 mg/ml, And the best at 100mg/ml.
进一步地，所述步骤(3)中烘干温度为80-120℃，烘干时间为8-48h。烘干温度优选为90-110℃，且在110℃时最佳。烘干时间优选为12-24h，且在16h时最佳。Further, in the step (3), the drying temperature is 80-120° C., and the drying time is 8-48 h. The drying temperature is preferably 90-110°C, and is optimal at 110°C. The drying time is preferably 12-24h, and the best time is 16h.
该方法采用相变材料赤藓糖醇作为蓄热单元，聚丙烯酰胺作为提高过冷液体稳定性材料，制备得到可长期储热且放热可控的相变储能材料。本方法所制备的可室温下长期储能的相变材料具有相变潜热高，储能稳定性好、热稳定性好、操作简单和成本低廉的优点，易于其在太阳能热能存储、废热回收利用等方面的应用。The method adopts the phase change material erythritol as the heat storage unit, and the polyacrylamide as the material for improving the stability of the supercooled liquid, to prepare a phase change energy storage material that can store heat for a long time and has controllable heat release. The phase change material that can store energy for a long time at room temperature has the advantages of high latent heat of phase change, good energy storage stability, good thermal stability, simple operation and low cost, and is easy to use in solar thermal energy storage and waste heat recovery and utilization. and other applications.
本发明与现有技术相比，具有以下优点及突出性效果：本发明所制备的可室温下长期储能的相变材料具有优异的储热性能，其可在室温下储存，具有可通过搅拌等外力触发结晶放热性能，可适用于热能的长期储存。解决了现有热能被动式存储问题，同时发明的可室温下长期储能的相变材料制备工艺简单、操作方便、产品无毒、无污染、可回收再利用、易实现大规模工业生产。Compared with the prior art, the present invention has the following advantages and outstanding effects: the phase change material prepared by the present invention, which can store energy for a long time at room temperature, has excellent heat storage performance, can be stored at room temperature, and can be stored at room temperature. The exothermic performance of crystallization is triggered by external force, which can be suitable for long-term storage of thermal energy. The existing problem of passive thermal energy storage is solved, and at the same time, the invented phase change material capable of storing energy for a long time at room temperature is simple in preparation process, convenient in operation, non-toxic, non-polluting, recyclable, and easy to realize large-scale industrial production.
附图说明Description of drawings
图1为实施例1中所制备的可室温下长期储能的相变材料的热分析曲线(降温曲线上没有出现结晶，再加热过程出现冷结晶)。1 is a thermal analysis curve of the phase change material prepared in Example 1 that can store energy for a long time at room temperature (no crystallization occurs on the cooling curve, and cold crystallization occurs during reheating).
图2为实施例1中所制备的可室温下长期储能的相变材料的搅拌下可控放热图片(图中可以看到，刚开始在室温下材料保持透明的液体状态，经过铁勺搅拌后，液体中开始出现白色的结晶区域。最后结晶结束，材料变成不透明的白色晶体状态)。Fig. 2 is the controllable exothermic picture under stirring of the phase change material prepared in Example 1 that can store energy for a long time at room temperature (as can be seen in the figure, the material is in a transparent liquid state at room temperature at the beginning, and after the iron spoon After stirring, white crystalline areas began to appear in the liquid. Eventually the crystallization ended and the material became an opaque white crystalline state).
具体实施方式Detailed ways
实施例1Example 1
(1)将0.2g分子量为500W的阴离子型聚丙烯酰胺溶于20ml水中，常温下搅拌5h获得质量百分比浓度为1％的均相聚丙烯酰胺水溶液。(1) Dissolve 0.2 g of anionic polyacrylamide with a molecular weight of 500 W in 20 ml of water, and stir at room temperature for 5 hours to obtain a homogeneous polyacrylamide aqueous solution with a mass percentage concentration of 1%.
(2)向步骤(1)聚丙烯酰胺水溶液中加入1.8g赤藓糖醇，常温下搅拌2h，形成均相糖醇聚合物水溶液。其中赤藓糖醇与聚丙烯酰胺的质量比为90:10。(2) 1.8 g of erythritol was added to the polyacrylamide aqueous solution in step (1), and stirred at room temperature for 2 h to form a homogeneous sugar alcohol polymer aqueous solution. The mass ratio of erythritol to polyacrylamide is 90:10.
(3)将上述所制备的糖醇聚合物水溶液转移至试剂瓶中，常压下110℃，16小时烘干水分，得到负载赤藓糖醇的、可室温下长期储能的相变材料。(3) Transfer the prepared sugar alcohol polymer aqueous solution into a reagent bottle, dry the water at 110° C. under normal pressure for 16 hours, and obtain a phase change material loaded with erythritol and capable of long-term energy storage at room temperature.
制备的可室温下长期储能的相变材料为透明液体，热分析曲线如图1所示，熔融焓为209.19J/g，冷结晶焓为182.44J/g，且降温过程中无结晶。该相变材料可在室温下保持透明液体状态，放置180天状态无任何变化，能通过搅拌等机械方式使其结晶并放热。实现放热可控等相关步骤如图2所示。The prepared phase change material with long-term energy storage at room temperature is a transparent liquid. The thermal analysis curve is shown in Figure 1. The melting enthalpy is 209.19 J/g, the cold crystallization enthalpy is 182.44 J/g, and there is no crystallization during the cooling process. The phase change material can maintain a transparent liquid state at room temperature, and the state does not change after being placed for 180 days, and can be crystallized and exothermic by mechanical means such as stirring. Figure 2 shows the relevant steps to achieve controllable heat release.
实施例2Example 2
(1)将0.4g分子量为500W的非离子型聚丙烯酰胺溶于20ml水中，常温下搅拌5h获得质量百分比浓度为2％的均相聚丙烯酰胺水溶液。(1) Dissolve 0.4 g of nonionic polyacrylamide with a molecular weight of 500 W in 20 ml of water, and stir at room temperature for 5 hours to obtain a homogeneous polyacrylamide aqueous solution with a mass percentage concentration of 2%.
(2)向步骤(1)聚丙烯酰胺水溶液中加入7.6g赤藓糖醇，常温下搅拌2h，形成均相糖醇聚合物水溶液。其中赤藓糖醇与聚丙烯酰胺的质量比为95:5。(2) 7.6 g of erythritol was added to the polyacrylamide aqueous solution in step (1), and stirred at room temperature for 2 h to form a homogeneous sugar alcohol polymer aqueous solution. The mass ratio of erythritol to polyacrylamide is 95:5.
(3)将上述所制备的糖醇聚合物水溶液转移至试剂瓶中，常压下80℃，48小时烘干水分，得到负载赤藓糖醇的、可室温下长期储能的相变材料。(3) Transfer the prepared sugar alcohol polymer aqueous solution into a reagent bottle, dry the water at 80° C. under normal pressure for 48 hours, and obtain a phase change material loaded with erythritol and capable of long-term energy storage at room temperature.
制备的可室温下长期储能的相变材料为透明液体，熔融焓为238.22J/g，冷结晶焓为179.37J/g，且降温过程中无结晶。可在室温下保持液体状态，放置180天状态无任何变化，能通过搅拌等机械方式结晶放热。The prepared phase change material that can store energy for a long time at room temperature is a transparent liquid, the melting enthalpy is 238.22 J/g, the cold crystallization enthalpy is 179.37 J/g, and there is no crystallization during the cooling process. It can be kept in a liquid state at room temperature, and the state will not change for 180 days. It can crystallize and release heat by mechanical means such as stirring.
实施例3Example 3
(1)将0.32g分子量为500W的阴离子型聚丙烯酰胺溶于16ml水中，常温下搅拌5h获得质量百分比浓度为2％的均相聚丙烯酰胺水溶液。(1) Dissolve 0.32 g of anionic polyacrylamide with a molecular weight of 500 W in 16 ml of water, and stir at room temperature for 5 hours to obtain a homogeneous polyacrylamide aqueous solution with a mass percentage concentration of 2%.
(2)向步骤(1)聚丙烯酰胺水溶液中加入3.68g赤藓糖醇，常温下搅拌2h，形成均相糖醇聚合物水溶液。其中赤藓糖醇与聚丙烯酰胺的质量比为92:8。(2) 3.68 g of erythritol was added to the polyacrylamide aqueous solution in step (1), and stirred at room temperature for 2 h to form a homogeneous sugar alcohol polymer aqueous solution. The mass ratio of erythritol to polyacrylamide is 92:8.
(3)将上述所制备的糖醇聚合物水溶液转移至试剂瓶中，常压下110℃，16小时烘干水分，得到负载赤藓糖醇的、可室温下长期储能的相变材料。(3) Transfer the prepared sugar alcohol polymer aqueous solution into a reagent bottle, dry the water at 110° C. under normal pressure for 16 hours, and obtain a phase change material loaded with erythritol and capable of long-term energy storage at room temperature.
实施例4Example 4
(1)将0.3g分子量为500W的阴离子型聚丙烯酰胺溶于30ml水中，常温下搅拌5h获得质量百分比浓度为1％的均相聚丙烯酰胺水溶液。(1) Dissolve 0.3 g of anionic polyacrylamide with a molecular weight of 500 W in 30 ml of water, and stir at room temperature for 5 hours to obtain a homogeneous polyacrylamide aqueous solution with a mass percentage concentration of 1%.
(2)向步骤(1)聚丙烯酰胺水溶液中加入1.7g赤藓糖醇，常温下搅拌2h，形成均相糖醇聚合物水溶液。其中赤藓糖醇与聚丙烯酰胺的质量比为85:15。(2) 1.7 g of erythritol was added to the polyacrylamide aqueous solution in step (1), and stirred at room temperature for 2 h to form a homogeneous sugar alcohol polymer aqueous solution. The mass ratio of erythritol to polyacrylamide is 85:15.
(3)将上述所制备的糖醇聚合物水溶液转移至试剂瓶中，常压下110℃，16小时烘干水分，得到负载赤藓糖醇的、可室温下长期储能的相变材料。(3) Transfer the prepared sugar alcohol polymer aqueous solution into a reagent bottle, dry the water at 110° C. under normal pressure for 16 hours, and obtain a phase change material loaded with erythritol and capable of long-term energy storage at room temperature.
显然，上述实施例仅仅是为清楚地说明所作的举例，而并非对实施方式的限定。对于所属领域的普通技术人员来说，在上述说明的基础上还可以做出其它不同形式的变化或变动。这里无需也无法对所有的实施方式予以穷举。而由此所引伸出的显而易见的变化或变动仍处于本发明创造的保护范围之中。Obviously, the above-mentioned embodiments are only examples for clear description, and are not intended to limit the implementation manner. For those of ordinary skill in the art, changes or modifications in other different forms can also be made on the basis of the above description. There is no need and cannot be exhaustive of all implementations here. And the obvious changes or changes derived from this are still within the protection scope of the present invention.
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