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:
有机类相变材料(PCM)以其高热能密度、合适相变范围以及优异可循环使用性成为高效而有前景的新能源汽车电池热管理策略，但在实用化过程中仍有相应不足之处应予以改善。本文从有机PCM实用物性不足出发，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以提高热导率；添加高分子共聚物提高柔韧性；添加化学阻燃剂提高阻燃效果，分别改善了有机PCM低导热、不易加工和热失控易燃现象。同时进一步基础上评价了其与热管、液冷、空冷等散热方式耦合后对电池热管理系统强化散热效果，对电池组最高温度/最大温差改善做出系统比对。指出耦合热管散热方式，仍主要讨论形状各异的热管排布；耦合液冷和空冷的散热方式其研究侧重对不同液体和气体流道对有机PCM散热的有效增强。最后介绍了模拟仿真分析对有机PCM在电池热管理领域的验证及预测，包括不同耦合散热的影响因素及最佳使用工况的研究。最后总结了目前有机PCM用于电池热管理的进展及不足，其难点仍在于复合柔性PCM虽然可塑性强，但在室温下柔韧性不足；复合阻燃PCM能有效延缓热失控和抑制燃烧，但无法彻底解决其燃烧问题。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，为今后有机PCM用于电池热管理提出一定建议。 添加不同阻燃剂对热失控(TR)时峰值热释放率(HRR)降低对比[59,61,63-66]Comparison of reduction of peak HRR when TR occurs with different flame retardants[59,61,63-66] 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. -
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; EPDM—Ethylene propylene diene monomer; 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. Three kinds of mathematical and physical models commonly used in BTM simulation
Model Equation of definition Parameter Ref. Electrochemical heat
generation model$q = {R_{\rm{i}}}{I^2} - IT\dfrac{{\partial U}}{{\partial T}}$ Where Ri is the equivalent internal resistance of the battery; I is current; T is the temperature of battery; q is heat flux; U is voltage. [92] Effective heat capacity model $\rho {c_{\rm{p}}}(T)\dfrac{{\partial T}}{{\partial t}} = \lambda \dfrac{{{\partial ^2}T}}{{\partial {x^2}}}$
${c_p} = \left\{ \begin{gathered} {c_{\rm ps}},T < {T_{\rm c}} - \Delta T \\ \dfrac{L}{{2\Delta T}} + \dfrac{{{c_{\rm ps}} + {c_{\rm pl}}}}{2},{T_{\rm c}} - \Delta T \leqslant T \leqslant {T_{\rm c}} + \Delta T \\ {c_{\rm pl}},T > {T_{\rm c}} + \Delta T \\ \end{gathered} \right.$L is the liquid fraction; λ is thermal conductivity; t is time; x is distance; cps, cpl are the specific heat capacities of solid and liquid PCM respectively; ΔT is half of the phase change temperature range; Tc is the 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} $ ρ is density; H is the total enthalpy; T0 is the temperature when the enthalpy is 0 kJ·kg−1; β is the liquid fraction; γ is latent heat; Ts and Tl are the solidification and melting temperatures of PCM, respectively [94]
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