Combined experimental and modeling approaches of the thermal runaway of fresh and aged lithium-ion batteries

Abstract

Li-ion secondary rechargeable batteries are becoming the preferred solution to store energy on board of new generation electric and hybrid vehicles or manage renewable energy in stationary applications. However, Li-ion batteries (LIBs) are still suffering limited lifetime, high cost and significant safety issues increasing their time to mass market. Thermal runaway is still nowadays considered as a major hazard of LIBs. This multiscale and multistep phenomenon originating at the microscale level potentially leads to uncontrolled fire and explosion of the battery. This work is focused on the development and validation of a 3D physical model of the LIB electro-thermal behavior nearby thermal runaway conditions. A combined modeling and experimental investigation provides a better understanding of the mechanisms leading to thermal runaway of LIBs, and of the ageing influence on this process. One major outcome of this work is also the proven fact that calendar ageing leads to a delayed onset of the cell self-heating temperature with a thermal runaway starting at a lower temperature. This is supported by computer simulations showing that the thickening of the solid electrolyte interface (SEI) hinders the diffusion of Li ions, which delays the degradation of the negative electrode and the occurrence of thermal runaway. HIGHLIGHTS  Development of an original 3D thermal runaway model including calendar ageing.  Model includes 3D thermal, 3D chemical reaction, and 0D calendar ageing sub-models. Calibration of the model for cylindrical 26650 LFP/C cells using a BTC. Validation of the model for fresh as well as 10% and 30% aged cells in oven tests.  Fresh and aged cells are compared in terms of critical temperatures under overheating 2

Thermal runaway behavior and features of LiFePO 4 /graphite aged batteries under overcharge

“…For aged batteries, some researchers have studied their thermal safety under heating . Abada's and Zhang's group both studied the effect of calendar aging on the thermal safety of batteries using a battery test calorimeter.…”

“…For aged batteries, some researchers have studied their thermal safety under heating . Abada's and Zhang's group both studied the effect of calendar aging on the thermal safety of batteries using a battery test calorimeter. The former found that the self‐heating onset temperature of the LiFePO 4 /graphite cells aged at 30% increased by 12.3°C compared with the new battery, while the onset temperature of thermal runaway decreased by 20.6°C.…”

“…Second, the onset temperature of thermal runaway obviously decreased when the battery aged to 70% SOH. The current research is helpful to understand the thermal safety of aged battery. However, there are few studies on thermal runaway of aged batteries under overcharge.…”

Deciphering the Interface of a High‐Voltage (5 V‐Class) Li‐Ion Battery Containing Additive‐Assisted Sulfolane‐Based Electrolyte

“…As a sharp contrast, 1 m LiDFOB/SL (Movie S1, Supporting Information) and 1 m LiDFOB/SL + 5 wt% TMSP (Figure b; Movie S2, Supporting Information) are hard to be ignited. Accelerating rate calorimetry (ARC) technology has been widely used to study the thermal (safety) properties of battery materials, single battery cell and battery pack . Herein, ARC Heat‐Wait‐Search (HWS) mode is used to reveal the superior thermal stability of 1 m LiDFOB/SL + 5 wt% TMSP than 1 m LiPF 6 carbonates‐based electrolyte (Figure c).…”

“…Accelerating rate calorimetry (ARC) technology has been widely used to study the thermal (safety) properties of battery materials, single battery cell and battery pack. [13,14,[52][53][54][55][56][57][58][59] Herein, ARC Heat-Wait-Search (HWS) mode is used to reveal the superior thermal stability of 1 m LiDFOB/SL + 5 wt% TMSP than 1 m LiPF 6 carbonates-based electrolyte (Figure 1c). The detected self-heating onset temperature of 1 m LiPF 6 carbonates-based electrolyte and 1 m LiDFOB/SL + 5 wt% TMSP is ≈90 °C and ≈230 °C, respectively.…”