CN112940687B - Pressure-driven refrigeration method based on solid-liquid phase change material - Google Patents
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Abstract
The invention aims to protect a pressure-driven refrigeration method based on a solid-liquid phase-change material, relates to the technical field of pressure-card refrigeration, and performs refrigeration by taking the solid-liquid phase-change material as a refrigeration working medium and taking isostatic pressure as a driving force. The invention provides a new application direction of a solid-liquid phase change material, namely, the solid-liquid phase change material is used as a refrigeration working medium of a pressure card refrigeration technology. Compared with solid-solid phase change materials, the solid-liquid phase change materials can be driven to realize more remarkable isothermal entropy change and adiabatic temperature change through lower pressure, and the isothermal entropy change and the adiabatic temperature change are two most key parameters for measuring the refrigerating capacity of the materials. Therefore, the research on the solid-liquid phase-change type pressure card material can provide a novel refrigeration working medium for the pressure card refrigeration technology and promote the development of the pressure card refrigeration technology.
Description
Technical Field
The invention relates to the technical field of pressure card refrigeration, in particular to a pressure-driven refrigeration method based on a solid-liquid phase change material.
Background
With the increasing development of economy, the application of refrigeration technology in the industrial fields of food, medicine, air-conditioning refrigeration and the like and daily life is more and more extensive. However, most of the refrigeration technologies used at present rely on the conventional gas compression cycle, and the energy consumption of the refrigeration industry is about 20% of the total global energy consumption due to the inefficient refrigeration mode. In addition, leakage of gaseous refrigerants (such as freon) also causes severe destruction of the ozone layer, exacerbating the global warming effect. Therefore, the development of new efficient and environmentally friendly refrigeration technologies is currently the direction of intense research.
In recent years, a pressure card refrigeration technology (generating cold by applying pressure or releasing pressure using isostatic pressure as a driving force) based on a phase change heat effect has received great attention. Compared with the gas compression refrigeration technology, the refrigeration technology has high refrigeration efficiency, is environment-friendly and is easy to miniaturize equipment. At present, the exploration of the card pressing material mainly focuses on a solid-solid phase change material system. Research results show that many solid-solid phase change material systems with structural phase change or volume mutation during phase change have the pressure-clamping effect. For example, many magnetic card materials (La (Fe, Si)13、Ni2In type compound and Gd5Si2Ge2) Electrocaloric materials (e.g. BaTiO)3、(NH4)2SO4Etc.), ballistic materials (e.g., Ni-Mn-In, etc.), anti-perovskite structure compounds (GaNMn)3And NiNMn3) Organic-inorganic hybrid perovskite ([ TPrA)][Mn(dca)3]And [ FeL2][BF4]2) Material systems such as fast ion conductors (AgI), high molecular polymers and plastic crystals (neopentyl glycol) have been shown to have a piezo-card effect. For phase-change refrigeration materials, adiabatic temperature change and isothermal entropy change are the two most critical parameters for measuring the refrigeration capacity of the materials. The reversible isothermal entropy change value of most of the solid-state pressure-clamping material systems discovered at present is generally within the range of 10-50J/K kg, and the reversible adiabatic temperature change value is hardly more than 20K. Neopentyl glycol (NPG) is one of the most excellent comprehensive performance systems in the existing pressure card material system, however, when the pressure reaches 250MPa, the reversible isothermal entropy change is still less than 400J/K kg, the adiabatic temperature change is not more than 10K, and the difference is still larger compared with the existing gaseous refrigeration mode. At present, the research of the pressure-clamping effect is mainly developed based on solid-solid phase change materials, which greatly limits the selection of material systems. The expansion of the research idea of the pressure card material is to explore a novel pressure card material system with higher adiabatic temperature change and isothermal entropy change value under lower pressure, and the method is an important research direction for future development in the field.
Disclosure of Invention
Based on the technical problems in the background art, the invention provides a pressure-driven refrigeration method based on a solid-liquid phase change material, and compared with a solid-solid phase change material, the lower pressure can realize more remarkable adiabatic temperature change and isothermal entropy change in the solid-liquid phase change material.
The invention provides a pressure-driven refrigeration method based on a solid-liquid phase-change material, which uses the solid-liquid phase-change material as a refrigeration working medium and uses isostatic pressure as a driving force to carry out refrigeration.
Preferably, the phase change temperature-pressure response coefficient | dT/dP | of the solid-liquid phase change material is greater than 0.
In the present invention, the solid-liquid phase-change material covers all solid-liquid phase-change material systems in which the solid-liquid phase-change temperature can be driven by pressure.
Solid-liquid phase change material systems tend to generate more latent heat when solid-liquid phase change occurs than solid-solid phase change material systems, which is also a key reason why such materials can be used as phase change energy storage materials. Most of solid-liquid phase change materials have isothermal entropy change value of 102～103J/K kg, which is about one order of magnitude higher than that of the solid phase change material.
In addition, solid-liquid phase changes often occur with significant volume changes, meaning that such materials have high values of | dT/dP |. The large isothermal entropy change and the high value of | dT/dP | mean that the solid-liquid phase change material can be used as an excellent candidate system of the material for the presscard.
The driving force of the method is isostatic pressure, and various oil pressure and air pressure systems can be used as the driving device of the refrigeration method.
Preferably, the solid-liquid phase change material comprises one or more of straight-chain normal alkane, fatty acid, inorganic hydrated salt and water.
Preferably, the straight-chain normal alkane has a structural general formula of CnH2n+2，n＝12-34。
Preferably, the fatty acid has a structural formula of CnH2nO2，n＝10、12、14、16、18。
Preferably, the inorganic hydrated salts include one or more of mirabilite, calcium chloride hexahydrate, magnesium chloride hexahydrate, disodium hydrogen phosphate dodecahydrate.
Preferably, the straight-chain normal alkane comprises one or more of n-tetradecane, n-hexadecane and n-octadecane.
The research results of the applicant show that the solid-liquid phase change material is a very potential pressure card material system. Compared with solid-solid phase change materials, the lower pressure can realize more remarkable adiabatic temperature change and isothermal entropy change in the solid-liquid phase change materials, and the adiabatic temperature change and the isothermal entropy change are two most critical parameters for measuring the refrigerating capacity of the materials. Therefore, the research on the solid-liquid phase change type pressure clamp material can provide a novel refrigeration working medium for the pressure clamp refrigeration technology, and greatly promote the development of the pressure clamp refrigeration technology.
Drawings
FIG. 1 is an adiabatic temperature change test curve for n-octadecane at 356K, 336K, 315K, 305K, 294K under different applied pressures;
FIG. 2 is an adiabatic temperature change test curve for n-hexadecane at 342K, 336K, 329K, 320K, 313K, 305K, 295K, 286K under different applied pressures;
FIG. 3 is a graph of adiabatic temperature change tests of tetradecane at temperatures of 349K, 322K, 307K, 299K, and 290K under various applied pressures;
FIG. 4 is a statistical effective adiabatic temperature change for n-octadecane;
FIG. 5 is a statistical effective adiabatic temperature change for n-hexadecane;
FIG. 6 is a statistical effective adiabatic temperature change for n-tetradecane;
FIG. 7 is a heat flow curve of n-octadecane after temperature reduction at different temperatures, and the inset is an entropy change curve before and after the phase change of n-octadecane;
FIG. 8 is a heat flow curve of n-hexadecane after temperature reduction at different temperatures, and the inset is an entropy change curve before and after phase change of n-hexadecane;
FIG. 9 is a graph of the differential heating value versus temperature for n-octadecane at different applied pressures; wherein, the insets are the change curve of the phase transition temperature of the n-octadecane along with the pressure;
FIG. 10 is a graph of the heat of difference versus temperature for n-hexadecane at different applied pressures; wherein, the insets are the change curve of the phase transition temperature of the n-hexadecane along with the pressure;
FIG. 11 shows reversible isothermal entropy changes of n-octadecane under different driving pressures;
FIG. 12 shows reversible isothermal entropy changes of n-hexadecane under different driving pressures;
FIG. 13A) is the maximum isothermal entropy change of n-octadecane, n-hexadecane and n-tetradecane at different pressures and compared with literature results; B) the maximum adiabatic temperature change of the n-octadecane and the n-hexadecane under different pressures is shown and compared with the literature result;
FIG. 14 is a graph comparing the maximum reversible isothermal entropy change and reversible adiabatic temperature change of n-octadecane with the existing material system at 50MPa, 100MPa, 150MPa, 200MPa, 250MPa pressure.
Detailed Description
The technical solution of the present invention will be described in detail below with reference to specific examples.
Example 1
In the research of the pressure-heat effect, adiabatic temperature change and isothermal entropy change are often taken as two most key indexes for evaluating the heat effect of the material. We have systematically studied the above properties of three chain alkanes (including n-octadecane, n-hexadecane and n-tetradecane) by means of an oil pressure test system (with oil as the pressure transmission medium).
(1) Adiabatic temperature change
The system represents the adiabatic temperature change values (figures 1-3) of three alkanes under different pressures in a temperature zone range of about 50K-70K near phase change, when pressure is applied, the average temperature of the three alkanes is increased, and the average temperature of the three alkanes is decreased when the pressure is released. Particularly above the phase transition temperature, the pressurization or depressurization process results in an abnormal increase or decrease in the temperature of the material when the pressure reaches a certain critical value, mainly due to the contribution of the large pressure-induced phase transition (the pressurization-induced liquid-solid phase transition or the depressurization-induced solid-liquid phase transition).
The existing test system is difficult to achieve complete heat insulation, so that the length of the phase change process and the speed of pressure change are related to whether the heat insulation temperature change value is accurate or notThe key factors, namely the fast phase change speed and the pressure change speed can effectively reduce the experimental error and prevent the adiabatic temperature change from being underestimated. The solid-liquid phase change process of the alkane material concerned in the invention has the following characteristics: 1) when the testing temperature is far higher than the solid-liquid phase change temperature, the liquid-solid phase change process induced by pressurization is slow, and the time required for a complete phase change process is often higher than 102S, the absolute value of the actually measured adiabatic temperature change is far lower than the pressure relief process due to long-time heat leakage; on the contrary, when the testing temperature is slightly higher than the phase transition temperature, the solid-liquid phase transition process caused by pressure relief is slow, so that the absolute value of the actually measured adiabatic temperature change is far lower than that of the pressurizing process; therefore, considering the significant effect of the time required to complete the complete phase transition on the adiabatic temperature change results, we mainly counted the test results with time below 60S as valid results. In addition, since the pressure relief process is faster than the pressurization process, the adiabatic temperature change induced by the pressure relief process is closer to the true value for the cases below the phase transition temperature and above the phase transition temperature but the pressure is lower and the solid-liquid phase change is not induced, and is counted as a valid result.
Based on the above two principles, the statistics of the effective adiabatic temperature change results for n-octadecane are shown in FIG. 4. For n-octadecane, when the temperature is much higher than the phase transition temperature, for example, 356K at the test temperature, the adiabatic temperature change starts to increase linearly with increasing pressure, driving the material to undergo an adiabatic temperature change of-7K per 100MPa of pressure change on average, whereas when the pressure is greater than 237MPa, the adiabatic temperature increase suddenly can be attributed to the contribution of the solid-liquid phase change suddenly induced by the large pressure, so that it reaches 45.4K at 367 MPa; when the test temperature is reduced to 336K, the adiabatic temperature change is also linearly increased at the beginning along with the increase of the pressure, the response of the adiabatic temperature change to the pressure is basically consistent with that of 356K, and when the pressure reaches 150MPa, the adiabatic temperature change is suddenly increased, so that 200MPa can drive the adiabatic temperature change of about 32K; when the temperature is reduced to 305K, the testing temperature is slightly higher than the phase transition temperature, and the solid-liquid phase transition can be driven by low pressure, so that the adiabatic temperature transition with enhanced phase transition is obtained, the adiabatic temperature transition can reach 18K under the pressure of 100MPa, and the adiabatic temperature transition can reach 46.9K under the pressure of 350 MPa. 313K, when the pressure is more than 267MPa, the result of the adiabatic temperature change test induced by the pressure is basically consistent with 305K; the test temperature is further lowered below the phase transition temperature, namely 294K, the material is in a solid state, the adiabatic temperature change is basically linear with the pressure, and the adiabatic temperature change of 2.9K can be driven to the material per 100MPa of pressure change on average, and is obviously lower than the response of the adiabatic temperature change to the pressure in a liquid state (7K/100 MPa).
For n-hexadecane, a similar law was also presented as for n-octadecane, as shown in fig. 5. When the testing temperature of the n-hexadecane is obviously higher than the phase transition temperature, for example, within the range of 342-313K, the adiabatic temperature increases linearly with the increase of the pressure, and the adiabatic temperature change changes by 7.3K when the pressure changes by 100MPa, which is similar to that of the n-octadecane; the pressure at which the corresponding adiabatic temperature change abruptly changes gradually decreases as the test temperature decreases (about 293, 200, 170, 150, 100MPa, respectively). Due to the enhancement effect of the phase change, the adiabatic temperature change of 14.2K, 21.8K and 42.9K can be driven by 83MPa, 133MPa and 250MPa pressure respectively at 305K, 313K and 336K. When the temperature is reduced to be below the solid-liquid phase change temperature, the pressure can not drive the solid-liquid phase change, at the moment, in the test pressure range, the adiabatic temperature change and the pressure change also have a linear relation, and about every time the pressure changes by 100MPa, the temperature changes by 2.8K, and the adiabatic temperature change is similar to that of n-octadecane.
For n-tetradecane, the law is consistent with n-hexadecane and n-octadecane, as shown in FIG. 6. Under the condition that the testing temperature is higher than the phase transition temperature and no phase transition enhancement exists, the adiabatic temperature change is in a linear relation with the pressure increase, the pressure change is 100MPa, the adiabatic temperature change is 6.9K, and when the testing temperature is 349K, the pressure changes of 400MPa and 500MPa can drive the adiabatic temperature change of 58K and 64.5K respectively.
(2) Reversible isothermal entropy change
The system researches the reversible isothermal entropy change of n-octadecane and n-hexadecane under different pressures. The accurate reversible isothermal entropy change value is obtained mainly based on a heat flow curve at zero pressure (based on a commercial differential scanning calorimeter, namely a DSC device) and temperature-dependent differential thermal signals at different pressures. Specifically, the heat flow curves dQ/dT of n-octadecane and n-hexadecane were measured by DSC over temperatureThe (1/T) (dQ/dT) -T curve after the reduction is shown in FIGS. 7 and 8, where the temperature of the highest peak in the heat flow curve is defined as the solid-liquid phase transition temperature Tt. The entropy change (Δ S) at Tt (considering only the phase change contribution) is obtained by integrating the (1/T) (dQ/dT) -T curves of the rise and fall events, and the results are shown in the insets of FIGS. 7 and 8. The delta S values of the n-octadecane and the n-hexadecane are 727J/K kg and 774J/K kg respectively, which are consistent with the results reported in the literature and are far higher than the reported solid-solid phase transformation type pressure card material system.
For both alkanes, the solid-liquid phase change temperature increased significantly with increasing temperature and was substantially consistent with literature results (see fig. 9, fig. 10). Based on the differential thermal curve and the heat flow curve, we calculated the reversible isothermal entropy change of the two alkanes, shown in fig. 11 and 12. For n-octadecane, when the pressure reaches 40MPa, the reversible entropy change is close to saturation, and the reversible entropy change value is about 690J/K.kg; when the pressure is increased to 80MPa, the reversible entropy change is completely saturated, and the reversible entropy change values are not lower than 716J/K.kg in the temperature range of 304K-310K (namely an inverse platform temperature range). As the pressure continues to increase, the reversible plateau region exhibiting a change in saturation entropy continues to widen. For example, when the pressures are 140MPa, 164MPa and 232MPa respectively, the temperature plateau regions of n-octadecane are 304K-324K, 304K-327K and 304K-341K respectively, and the reversible entropy changes are not lower than 718J/K.kg, 719J/K.kg and 720J/K.kg respectively. For n-hexadecane, when the driving pressure is 22MPa, the reversible entropy change is about 274J/K.kg; when the pressure is increased to 58MPa, the reversible entropy change is close to saturation, and the value is about 755J/K.kg; the reversible entropy change is fully saturated when the pressure is increased to 101MPa, and as the pressure increases, the reversible plateau region exhibiting saturated entropy change continuously widens. When the pressure is 101MPa, 130MPa and 152MPa, the temperature platform areas of the n-hexadecane are 293K-295K, 293K-305K and 293K-313K respectively, and the reversible entropy change is not lower than 776J/K.kg, 784J/K.kg and 787J/K.kg respectively.
The absolute values of the maximum adiabatic temperature change values (including n-octadecane, n-hexadecane, n-tetradecane) and the maximum reversible entropy change (n-octadecane, n-hexadecane) are summarized in fig. 13A and 13B and compared with literature results, respectively. Note, in literature results, etcReversible change in temperature entropy change (Δ S)r) And irreversible (Δ S)ir) Dividing into (1) and (b); adiabatic temperature change is then measured directly (. DELTA.T)d) Reversible (Δ T)r) Irreversible fraction (. DELTA.T)ir). In general,. DELTA.SirAnd Δ TirWill be higher than the real result, and Δ TdIt is often lower than the true value because of the difficulty in obtaining a completely adiabatic environment during testing. Furthermore, | Δ S ∞ is not calculation according to the results we have discussed earliermaxIn practice it is also severely underestimated. Even so, as shown in fig. 13A and 13B, the adiabatic and isothermal entropy change values for the three alkanes are significantly higher than other prior material systems. For example, compared to the star presscard material system NPG: under the pressure of about 200MPa, the maximum reversible adiabatic temperature change of NPG is less than 7K, and the reversible adiabatic temperature change of three alkanes is more than 30K; the maximum reversible entropy change of the n-octadecane can reach 690J/K kg under the pressure of 40MPa, the maximum reversible entropy change of the n-hexadecane can reach 755J/K kg under the pressure of 58MPa, the maximum reversible entropy change of the n-hexadecane can reach 274J/K kg under the pressure of 22MPa, and the maximum reversible entropy change of the NPG is still less than 200J/K kg under the driving pressure of between NPG and 200 MPa.
A good material system for pressing card is to combine large and reversible isothermal entropy change and adiabatic temperature change. We compared the maximum reversible entropy change and adiabatic temperature change of n-octadecane and n-hexadecane with existing material systems (for objectivity of comparison, only focus on Δ Sr、ΔTr、ΔTdEtc.) are set to five pressures of 50MPa, 100MPa, 150MPa, 200MPa, and 250MPa, respectively (as shown in fig. 14). We can find that under the lower pressure of 50MPa, only a few material systems such as n-octadecane, n-hexadecane, C60, silicone rubber and the like are reported to have reversible pressure-heat effect (which may also be related to the large thermal hysteresis of the phase change material system), and both isothermal entropy change and adiabatic temperature change of n-octadecane and n-hexadecane are significantly better than those of the other two material systems; with the increase of pressure, a material system with reversible piezothermal effect gradually increases, but the n-octadecane and the n-hexadecane always keep very remarkable advantages in the two aspects of isothermal entropy change and adiabatic temperature change, which means a great application prospect.
Claims (1)
1. A pressure-driven refrigeration method based on solid-liquid phase-change materials is characterized in that the solid-liquid phase-change materials are used as refrigeration working media, and isostatic pressure is used as driving force for refrigeration; the phase change temperature-pressure response coefficient | dT/dP | of the solid-liquid phase change material is more than 0; the solid-liquid phase change material is straight-chain normal alkane; the structural general formula of the straight-chain normal alkane is CnH2n+2N is 12-34; the straight-chain normal alkane comprises one or more of n-tetradecane, n-hexadecane and n-octadecane.
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| CN113652203B (en) * | 2021-07-23 | 2022-10-04 | 中国科学院金属研究所 | Application of halogen compound containing ammonium ion in solid refrigeration |
| CN113604204B (en) * | 2021-07-27 | 2022-05-31 | 中国科学院金属研究所 | Application of inorganic plastic crystal material in solid refrigeration |
| CN115960360B (en) * | 2021-10-09 | 2024-04-09 | 中国科学院物理研究所 | Press-clamping effect material and preparation method and application thereof |
| CN114350325B (en) * | 2022-01-13 | 2023-10-03 | 中国科学院金属研究所 | Glass crystal-based actively controllable solid-state phase change heat storage and release method, device and application of press card material |
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