锂离子电池单层电芯内短路建模与热失控触发特性

doi:10.19799/j.cnki.2095-4239.2024.0396

储能科学与技术 ›› 2024, Vol. 13 ›› Issue (10): 3491-3503.doi: 10.19799/j.cnki.2095-4239.2024.0396

锂离子电池单层电芯内短路建模与热失控触发特性

乔亚军¹(), 任怡茂², 谭子健¹, 张袆柔², 吴伟雄²()

^1.广东电网公司广州供电局，广东广州 510620
^2.暨南大学能源电力研究中心(国际能源学院)，广东珠海 519070

收稿日期:2024-05-06 修回日期:2024-05-31 出版日期:2024-10-28 发布日期:2024-10-30
通讯作者: 吴伟雄 E-mail:20288367@qq.com;weixiongwu@jnu.edu.cn
作者简介:乔亚军（1982—），男，硕士研究生，研究方向为高电压技术和电力设备状态监测技术，E-mail：20288367@qq.com；
基金资助:
国家自然科学基金(52106244);广东省基础与应用基础研究基金(2024A1515030124);南方电网公司科技项目［GDKJXM20230246(030100KC23020017)

Modeling internal short circuit and thermal runaway triggers in single-layer lithium-ion battery cells

Yajun QIAO¹(), Yimao REN², Zijian TAN¹, Huirou ZHANG², Weixiong WU²()

^1.Guangdong Power Grid Guangzhou Power Supply Bureau, Guangzhou 510620, Guangdong, China
^2.Energy and Power Research Center (International Energy Institute), Jinan University, Zhuhai 519070, Guangdong, China

Received:2024-05-06 Revised:2024-05-31 Online:2024-10-28 Published:2024-10-30
Contact: Weixiong WU E-mail:20288367@qq.com;weixiongwu@jnu.edu.cn

摘要/Abstract

摘要：

锂离子电池内短路诱因复杂，为深入研究内短路引起的电池失效问题须构建合适的精细化仿真模型。本工作以NCM/石墨电池为研究对象，围绕电池内短路失效机理，基于电化学-热耦合物理场，建立了考虑热失控放热副反应的三维单层电芯内短路模型，探究了热失控触发边界，并从内外部特征讨论了单层电芯内短路-热失控的演变过程。首先利用Arrhenius公式得到内短路触发的四种放热副反应产热量与反应速率，探究对电池温升影响最大的副反应类别，结果表明内短路过程放热副反应中负极与电解液反应总热量最大。进一步分析单层电芯内四种典型内短路形式的热失控触发特性，综合考虑组分材料导电性和导热性，得到铝-阳极内短路危险程度最高，其短路电阻值与热失控触发时间呈现正相关趋势，且临界短路电阻的高温热点区域面积值约为30 mm²。模拟结果获得了四种形式内短路临界短路电阻值，并揭示了单层电芯内短路-热失控触发时内部锂离子浓度和温度分布的空间演变规律，相关结果可为研究内短路失效机制和设计安全锂离子电池提供理论指导。

关键词: 锂离子电池, 单层电芯, 内短路模型, 热失控触发

Abstract:

Internal short circuits (ISC) present significant challenges in lithium-ion batteries, underscoring the need for accurate simulation models to understand battery failure mechanisms. This study examines NCM/graphite batteries and develops a three-dimensional single-cell ISC model that includes exothermic side reactions with thermal runaway. By utilizing electrochemical-thermal coupling, the study investigates the triggers of thermal runaway and the progression of ISC-induced thermal runaway. Initially, the heat generation and reaction rates of four exothermic side reactions are calculated using the Arrhenius equation. The results indicate that the highest heat is produced by reactions between the negative electrode and the electrolyte. Additionally, an analysis of the thermal runaway triggering characteristics of four typical ISC forms within a single cell reveals that an internal short circuit involving an aluminum anode poses the greatest danger. The resistance value of the short circuit is positively correlated with the time it takes for thermal runaway to be triggered. Additionally, the area of the high-temperature hotspot at the critical short-circuit resistance is determined to be 30 mm². This simulation identifies the critical short-circuit resistance values for four different ISC forms and reveals the internal lithium-ion concentration and temperature distribution when thermal runaway is triggered. These findings offer valuable theoretical insights for investigating ISC failure mechanisms and designing safe lithium-ion batteries.

Key words: lithium-ion battery, single-layer cell, internal short circuit model, thermal runaway trigger

中图分类号:

U 467.1

乔亚军, 任怡茂, 谭子健, 张袆柔, 吴伟雄. 锂离子电池单层电芯内短路建模与热失控触发特性[J]. 储能科学与技术, 2024, 13(10): 3491-3503.

Yajun QIAO, Yimao REN, Zijian TAN, Huirou ZHANG, Weixiong WU. Modeling internal short circuit and thermal runaway triggers in single-layer lithium-ion battery cells[J]. Energy Storage Science and Technology, 2024, 13(10): 3491-3503.

图/表 18

图1

表1

表2

图2

表3

表4

模型控制方程"

方程描述	控制方程
固相电势	$- σ s e f f ∂ ϕ s ∂ x = i s$	(2)
电子的迁移过程	$- ∂ i s ∂ x = σ s e f f ∂ 2 ϕ s ∂ x 2 = a F j L i$	(3)
液相电势	$∂ ∂ x σ e e f f ∂ ϕ e ∂ x = - a F j L i + 2 R T 1 - t + 0 F ∂ ∂ x σ e e f f ∂ l n c e ∂ x$	(4)
固相锂离子分布	$∂ c s ∂ t = 1 r 2 ∂ ∂ r D s r 2 ∂ c s ∂ r$	(5)
液相锂离子浓度	$ε e ∂ c e ∂ t = ∂ ∂ x D e e f f ∂ c e ∂ x + 1 - t + 0 a j L i$	(6)
界面电化学反应过程	$j L i = i 0 e x p α n F R T η s - e x p α p F R T η s$	(7)
过电位	$η s = ϕ s - ϕ e - U - j F R S E I$	(8)
热平衡	$ρ c p ∂ T ∂ t = λ x ∂ 2 T ∂ x 2 + λ y ∂ 2 T ∂ y 2 + λ z ∂ 2 T ∂ z 2 + Q t o t a l$	(9)
可逆热	$Q r e v = F a j T ∂ U ∂ T$	(10)
不可逆热	$Q i r r v = F a j ϕ s - ϕ e - U$	(11)
欧姆热	$Q o h m = σ s e f f ∂ ϕ s ∂ x 2 + σ e e f f ∂ ϕ e ∂ x 2 + 2 R T σ e e f f F 1 - t + 0 ∂ l n c e ∂ x ∂ ϕ e ∂ x$	(12)
对流换热	$- λ ∂ T ∂ n = h T s u r f - T ∞$	(13)
放热副反应热	$Q e x = ∑ H i W i R i$	(14)
SEI膜分解反应	$R S E I T, c S E I = - d c S E I d t = A S E I e x p - E S E I R T c S E I, T > 363.15 K$	(15)
负极与电解液反应	$R n e T, c n e = - d c n e d t = A n e e x p - t S E I t S E I 0 e x p - E n e R T c n e, T > 393.15 K$	(16)
正极与电解液反应	$R p e (T, c a) = d c a d t = A p e e x p - E p e R T c a 1 - c a, T > 443.15 K$	(17)
电解液分解反应	$R e l e T, c e l e = - d c e l e d t = A e l e e x p - E e l e R T c e l e, T > 473.15 K$	(18)

表4

图3

图4

图5

图6

图7

图8

图9

图10

图11

图12

图13

图14

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参数	数值
内短路半径R₀/mm	1.2
热导率k/[W/(m·K)]	85
比热容c_p /[J/(kg·K)]	3500
密度ρ/(kg/m³)	535
短路电阻r_short/Ω	5

参数	铜	负极	隔膜	正极	铝
密度ρ/(kg/m³)	8960	1200	525	2860	2770
比热容c_p /[W/(m·K)]	385	1437.4	2050	1150	897
热导率k/[J/(kg·K)]	395	0.4	0.5	0.4	240
最大锂浓度c_{s_max}/(mol/m³)	—	31507	—	49000	—
初始电解质盐浓度c_e,0/(mol/m³)	—	2000	2000	2000	—
电荷转移系数α_a，α_c	—	0.5,0.5	—	0.5,0.5	—
固相锂扩散率D_s/(m²/s)	—	3.9×10^-14	—	1×10^-13	—
电解质扩散率D_e/(m²/s)	—	1.5×10^-11	1.5×10^-11	1.5×10^-11	—
电极固相体积分数ε_s	—	0.471	—	0.297	—
电解质相体积分数ε_e	—	0.357	—	0.444	—
电极颗粒半径r_s/μm	—	14.75	—	10	—
扭曲布鲁格曼系数Brugl	—	2.5	2.15	2.98	—
法拉第常数F/(c/mol)	96485	—	—	—	—
摩尔气体常数R/[J/(mol·K)]	8.314	—	—	—	—
参考温度T_ref/K	273.15	—	—	—	—
固液界面电阻R_SEI/(Ω·m²)	—	0.001	—	0.001	—
比表面积a/m^-1	—	3ε_s/r_s	—	3ε_s/r_s	—
有效电解质扩散率D_e^eff/(m²/s)	—	ε_e^1.5D_e	D_e	ε_e^1.5D_e	—
固相电导率σ_s/(S/m)	5.998×10⁷	100	—	3.8	3.774×10⁷
液相电导率σ_e/(S/m)	—	—	σ_e=f(c_e,T)^[39]	—	—
有效固相电导率σ_s^eff/(S/m)	—	ε_s^1.5σ_s	σ_s	ε_s^1.5σ_s	—
有效液相电导率σ_e^eff/(S/m)	—	ε_e^1.5σ_e	σ_e	ε_e^1.5σ_e	—

参数	SEI膜分解	负极与电解液反应	正极与电解液反应	电解液分解反应
放热量H/(J/kg)	2.57×10⁵	1.71×10⁶	3.14×10⁵	1.55×10⁵
物质含量W/(kg/m³)	413	413	1300	500
频率因子A/s^-1	1.67×10¹⁵	2.5×10¹³	6.67×10¹³	5.14×10²
活性能E/(J/mol)	1.35×10⁵	1.35×10⁵	1.40×10⁵	2.74×10⁵
初始归一化浓度值c	0.15	0.75	0.04	1
初始无量纲SEI膜厚度值t_SEI0	0.033	—	—	—

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锂离子电池单层电芯内短路建模与热失控触发特性

Modeling internal short circuit and thermal runaway triggers in single-layer lithium-ion battery cells

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