Recent progress in enhancement of physical properties of organic phase change materials and optimization of coupling thermal management of batteries
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摘要: 为满足电动汽车锂离子电池热管理需求，具有优良温控效果的相变材料(PCM)冷却逐渐成为研究热点。本文从有机PCM物性不足出发，概括了目前复合有机PCM的制备及改进方向：添加多维高导热材料(如碳材料、纳米金属、泡沫金属等)强化导热；添加共聚物(如聚乙烯、热塑性弹性体等)提高材料柔韧性和添加阻燃剂(如红磷、聚磷酸铵等)提高阻燃效果以改善其实用性。分别指出膨胀石墨、苯乙烯-乙烯-丁二烯-苯乙烯和复合使用红磷与聚磷酸铵对导热、柔性和阻燃的显著提升。同时描述了有机PCM与热管、液冷、空冷等散热方式耦合后系统强化换热的效果，总结耦合热管时需要考虑不同热管排布；耦合液冷或空冷需要设计合适流道增强换热。随后介绍了通过模拟仿真分析有机PCM用于电池热管理系统影响因素及最佳使用工况的研究。最后总结有机PCM用于电池热管理的进展及不足，其难点仍在于其可燃和导电性的改善以及柔性有机PCM在室温下柔韧性不足，有机PCM耦合传统散热系统的车载可靠性和循环可行性也缺乏相应探讨，并为今后有机PCM用于电池热管理提出一定建议。Abstract: To meet the demand for thermal management of lithium-ion batteries in electric vehicle, the cooling method with phase change materials (PCM) on battery modules has gradually become a research hotspot. Based on the poor physical properties of organic PCM, the preparation and improvement directions of composite organic PCM for battery thermal management (BTM) are summarized, including adding multi-dimensional materials such as carbon materials, nano-metals and metal foams to enhance the heat transfer, and adding copolymer such as polyethylene and thermoplastic elastomer to improve the flexibilities. Additionally, flame retardants such as red phosphorus and ammonium polyphosphate are used to improve the flame retardance for better practicabilities. Among them, expanded graphite, styrene-ethylene-butadiene-styrene, and the composite of red phosphorus and ammonium polyphosphate significantly improve the thermal conductivity, flexibility and flame retardancy respectively. Subsequently, the heat transfer enhancement effects of the system after coupling organic PCM with heat pipe, liquid cooling or air cooling are evaluated, indicating that various arrangements of heat pipe and appropriate flow channels of air and liquid should be considered. Then the optimal operating conditions of organic PCM used in BTM system is determined with numerical calculation. Finally, the progress and shortcomings of organic PCM used in BTM are summarized. It is pointed out that the difficulties of composite organic PCM used in BTM are still accounted for the improvement of flammability and conductivity and the insufficient flexibility of flexible organic PCM at room temperature. Furthermore, the reliability and cycle feasibility of PCM and traditional heat dissipation system in the process of vehicle use are still lack of verification. Totally, several suggestions are put forward for the application of organic PCM in BTM in the future.
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表 1 部分用于电池热管理(BTM)的有机固-液相变材料(PCM)热物性
Table 1. Thermo-physical properties of organic solid-liquid phase change materials (PCM) for battery thermal management (BTM)
PCM Thermal conductivity/(W·m−1·K−1) Latent heat/(kJ·kg−1) Phase change temperature/
℃Ref. Paraffin(PW) 0.2 255 41-44/— [20] PW 0.22 300 36/— [21] PW 0.21 200 40/— [22] Lauric acid 0.15 177 43/— [23] Myristic acid — 187 53.7/— [23] Palmitic acid 0.17 186 62.3/— [23] Stearic acid 0.17 203 70.7/— [23] Capric acid 0.15 152.7 28.9/31.9 [24] Polyethylene glycol (PEG) 600 — 146 20-25 [23] PEG 1000 0.29 142/— 35.9/29.9 [25] PEG 1500 0.31 163.4/— 48.9/42.9 [25] PEG 3400 — 171.6 56.4 [23] Tetradecanol — 205 38 [26] 1-dodecanol — 200 26 [26] 
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表 2 BTM用有机PCM热导率强化及其热物性
Table 2. Thermal conductivity enhancements and thermo-physical properties of organic PCM for BTM
PCM and
additivesMass fraction Thermal conductivity
of pure PCM/
(W·m−1·K−1)Thermal conductivity of
composite PCM/
(W·m−1·K−1)Phase change
temperature/
℃Latent
heat/
(kJ·kg−1)Ref. EG/PW 20∶80 0.15 1.90 — — [29] GNP/PW 20∶80 0.15 0.87 — — [29] CNT/PW 20∶80 0.15 0.37 — — [29] Graphene/PW 20∶80 0.15 0.49 — — [29] Nano-Al/PW 20∶80 0.25 0.78 53.89/49.46 282.50/281.20 [30] Nano-TiO2/PW 20∶80 0.25 0.43 54.28/50.74 283.09/280.64 [30] AlN/EG/ER/PW 20∶3∶27∶50 0.20 4.33 47.20/— 116.30 [33] EG/ER/copper foam/PW — 0.23 2.90 49.80/— 75.00 [36] sw-GS/PW 2.25∶97.75 0.19 2.58 53.50/45.40 172.50/158.90 [37] NPC-Al/PEG 2000 15∶85 0.27 0.41 54.40/— 155.30/— [38] CNT/MOFs/PEG 2000 5.16∶24.84∶70 0.30 0.46 52.40/27.40 96.20/90.10 [39] MWCNT/graphene/PW 0.3∶0.7∶99 0.39 0.87 45.30/40.80 203.80/198.00 [40] EG/PW 10∶90 0.28 6.4 39.50 187.88 [42] CNT/PW 10∶90 0.28 0.39 40.30 172.62 [42] h-BN/Na2SiO3/PW 18∶0.9∶81.1 0.12 0.85 52.30/47.90 165.40/176.10 [43] EG/aluminum foam/graphene/PW — 0.20 7.1 — — [44] NPC/myristic acid-stearic acid 12∶26.4∶61.6 0.17 0.37 49.45/— 164.33/— [45] EG/SiO2/low-density polyethylene/RT 45 7∶5.5∶30∶57.5 — 3.30 44.00 77.80 [46] Notes: EG—Expanded graphite; GNP—Graphene nanosheets; CNT—Carbon nanotubes; ER—Epoxy resin; MWCNT—Multi-walled carbon nanotubes; NPC—N-doped porous carbons; RT 45—Rubitherm 45.
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表 3 BTM用有机PCM柔性强化及其热物性
Table 3. Flexibility enhancements and thermo-physical properties of organic PCM for BTM
PCM and
additivesThermal
conductivity/
(W·m−1·K−1)Phase change
temperature/
℃Latent
heat/
(kJ·kg−1)Mechanical property Ref. Test temperature/℃ Tensile and
bending
strength/MPaModulus of
elasticity/
MPaEG/SBS/TPEE/PW(5:10:5:80) 1.20(30℃) 56.7/— 172.6/— 60 0.09/— — [47] EG/TPC-et/PW(10:45:45) 1.64 46.4/— 102.0 25 0.88/0.14 — [48] EG/OBC/PW(10:45:45) 1.57 50.1/— 101.0 25 5.44/1.21 — [48] EVA/EG/PW(47.5:5:47.5) 1.70 53.0 121.0 30 0.83/0.02 — [49] SEPS/EG/PW(9.5:5:85.5) 2.67 48.0/— 211.9 50 — — [50] SBS/AlN/PW(50:15:35) 0.50 46.8 57.1 50 0.16/0.16 67.00 [51] h-BN/SEBS/PW(20:20:60) 2.80 40.1-44.3/— 148.3 — — 0.72 [52] EG/SBS/EPDM/PW(5:12:3:80) 1.25 50.9/— 133 60 0.51/— — [53] OBC/EG/PW(19:5:76) 2.34 39.5 185.4 60 — 63.90 [54] SBS/EG/PW(60:3:57) 0.88 50.6 78.3 — 0.34/0.51 — [55] EG/SEBS/PW(5:20:80) 1.23 47.4 159.2/166.5 — — — [56] OBC/EG/eicosane(20:3:80) 1.21 33.5 170.2 — — — [57] OBC/EG/tetracosane(20:3:80) 1.18 47.4 175.1 — — — [57] HDPE/EG/eicosane(20:3:80) 1.25 33.4 169.0 — — — [57] EG/silicon rubber/h-BN/PW(3:55:5:28) 0.95 47.3/— 62.7 — 0.53/— — [58] Notes: TPC-et—Copolyester thermoplastic elastomer with polyether soft segment; OBC—Olefin block copolymer; EVA—Ethylene vinylacetate; SEPS—Styrene butene propylene styrene; SEBS—Styrene ethylene butylene styrene; HDPE—High density polyethylene.
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表 4 部分BTM用阻燃PCM热物性及阻燃效果
Table 4. Thermo-physical properties and flame retardant effects of flame retardant PCM for BTM
PCM Flame
retardantMass fraction/
wt%Thermal
conductivity/
(W·m−1·K−1)Latent
heat/
(kJ·kg−1)Phase change
temperature/℃LOI/% Temperature
peak of TR/
℃Peak HRR before
and after
antiflaming/
(kW·m−2)Ref. OBC/EG/PW(13:5:70) AlCl3/Sb2O3/
glass fibrePadded 1.48 130.7/— 47.1/— 26.0 — 462.3/190.3 [59] Silica aerogel/PW(60:40) APP/dipentaerythritol Coated 0.05 79.2/— 39.6/— 56.3 691 — [60] Benzoyl peroxide/
EG/1,6-hexanediol diacrylate/octadecyl acrylate(4:12:6:318)Al(OH)3 15 1.26 71.5 46.1 — 639 242.5/204.4 [61] EG/SBS/PW(3:12:70) APP/phosphoric acid/ZnO 15 ~1 120.0 45.3 35.9 — 2980.0/801.0 [63] EG/ER/PW(4:50:80) APP/RP 38 1.10 81.2 45.0-48.0 27.6 — 870.9/313.1 [64] PW Aluminium trihydrate/
Mg(OH)250 — 115.0 50.0 — 364 29.0/15.5(kW) [65] PW APP 50 — 98.1 51.4 — 764 29.0/23.9(kW) [65] Polyester fiber/PEG APP 15 0.38 70.1 — 28.7 — 654.7/385.7 [66] Notes: PEG—Polyethylene glycol; APP—Ammonium polyphosphate; RP—Red phosphorus; TR—Thermal runaway; HRR—Heat release rate.
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表 5 PW耦合热管BTM系统控温优化对比
Table 5. Optimization of temperature control of PW coupled with heat pipe BTM system
PCM Charge/discharge rate T1 max and ΔT1 max/℃ T2 max and ΔT2 max/℃ Ref. RT44 HC 60 W 52.8/—
(heatpipe)45.9/— [70] PW 2 W 48.3/—
(heatpipe)39.0/— [71] EG/PW 10 W 47.2/5.9
(PCM)45.1/4.7 [68] EG/PW 3 C 45.5/2.5(PCM) 44.1/1.7 [74] Copper foam/PW 5 C 52.5/4.2(PCM) 44.9/3.6 [67] Notes: T1 max and ΔT1 max—Maximum temperature and maximum temperature difference with single cooling method; T2 max and ΔT2 max—Maximum temperature and maximum temperature difference with coupled cooling method; RT44 HC—Rubitherm 44 high crystallinity.
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表 6 耦合液冷或空冷后BTM系统控温优化
Table 6. Optimization of temperature control of BTM system coupled with liquid cooling or air cooling
PCM Method of coupling Charge/discharge rate T1 max and ΔT1 max/℃ T2 max and ΔT2 max/℃ Ref. h-BN/SEBS/PW Liquid cooling 5 C 52.9/7.9
(Liquid cooling)44.0/3.2 [52] PEG 1000 Liquid cooling 0.9 C 32.0/1.2(PEG 1000) 30.0/0.6 [79] Copper foam/PW Liquid cooling 12.5 W 60.0/—
(Liquid cooling)45.1/— [83] EG/RT44 HC Liquid cooling 2 C 50.0/4.1
(Liquid cooling)42.0/1.2 [85] EG/Lipin/PW Liquid cooling 3 C 45.10/—
(PCM)41.1/4.0 [86] Copper foam/RT25 HC Liquid cooling 2 C 39.00/—
(RT25 HC)25.0/1.0 [87] Aluminium foam/RT27 Air cooling 1 C — 25.6/— [82] Copper foam/PW Air cooling 5 W 46.6/—
(Air cooling)35.8/— [80] Cetane stearic acid/EG/PW Air cooling 2 C — 51.9/2.6 [81] PEG 1000 Air cooling 2 C — 37.0/— [25] Copper wire/PW Air cooling 2.45 W 43.0/—
(PCM)26.0/— [84]
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表 7 BTM仿真模拟常用的3种数学物理模型
Table 7. 3 kinds of mathematical and physical models commonly used in BTM simulation
Model Equation of definition Parameter Ref. Electrochemical heat
generation model$q = {R_{\rm{i}}}{I^2} - IT\dfrac{{\partial U}}{{\partial T}}$ Notes: Ri—Equivalent internal resistance of the battery; I—Current; T—Temperature of battery; q—Heat flux; U—Voltage. [92] Effective heat capacity model $\rho {c_{\rm{p}}}(T)\dfrac{{\partial T}}{{\partial t}} = \lambda \dfrac{{{\partial ^2}T}}{{\partial {x^2}}}$
${c_{\rm p}} = \left\{ \begin{gathered} {c_{\rm ps}},T < {T_{\rm c}} - \Delta T \\ \dfrac{L}{{2\Delta T}} + \dfrac{{{c_{\rm ps}} + {c_{\rm pl}}}}{2},{T_{\rm c}} - \Delta T \leqslant T \leqslant {T_{\rm c}} + \Delta T \\ {c_{\rm pl}},T > {T_{\rm c}} + \Delta T \\ \end{gathered} \right.$Notes: L—Liquid fraction; λ—Thermal conductivity; t—Time; x—Distance; cps, cpl—Specific heat capacities of solid and liquid PCM respectively; ΔT—Half of phase change temperature range; Tc—Cent temperature of the phase change temperature range. [93] Enthalpy model $\begin{gathered} \rho \dfrac{{\partial H}}{{\partial t}} = \lambda \dfrac{{{\partial ^2}T}}{{\partial {x^2}}} \\ H = \int_{{T_0}}^T {{c_{\rm p}}dT} + \beta \gamma \\ \left\{ \begin{gathered} \beta = 0,T < {T_{\rm s}}{\text{ }} \\ \beta = 0,T > {T_{\rm l}} \\ \beta = \dfrac{{T - {T_{\rm s}}}}{{{T_{\rm l}} - {T_{\rm s}}}},{T_{\rm s}} < T < {T_{\rm l}} \\ \end{gathered} \right. \\ \end{gathered} $ Notes: ρ—Density; H—Total enthalpy; T0—Temperature when the enthalpy is 0 kJ·kg−1; β—Liquid fraction; γ—Latent heat; Ts and Tl—Solidification and melting temperatures of PCM, respectively. [94]
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