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Exploring the electrochemical and physical stability of lithium-ion cells exposed to liquid nitrogen
(2024)
The transport and storage of lithium-ion (Li-ion) batteries — damaged or in an undefined state — is a major safety concern for regulatory institutions, transportation companies, and manufacturers. Since (electro)chemical reactivity is exponentially temperature-dependent, cooling such batteries is an obvious measure for increasing their safety.
The present study explores the effect of cryogenic freezing on the electrochemical and physical stability of Li-ion cells. For this purpose, three different types of cells were repeatedly exposed to liquid nitrogen (LN2).
Before and after each cooling cycle, electrical and electrochemical measurements were conducted to assess the impact of the individual freezing steps. While the electrochemical behavior of the cells did not change significantly upon exposure to LN2 , it became apparent that a non-negligible number of cells suffered from physical changes (swelling) and functional failures. The latter defect was found to be caused by the current interrupt device of the cylindrical cells. This safety mechanism is triggered by the overpressure of expanding nitrogen which enters the cells at cryogenic temperatures.
This study underlines that the widely accepted reversibility of LN2 -cooling on a material scale does not allow for a direct extrapolation toward the physical integrity of full cells. Since nitrogen enters the cell at cryogenic temperatures and expands upon rethermalization, it can cause an internal overpressure. This can, in turn, lead to mechanical damage to the cell. Consequently, a more appropriate temperature condition — less extreme than direct LN2 exposure — needs to be found
Most high capacity anode materials for lithium-ion batteries (LiB) require a carbonaceous matrix. In this context one promising material is reduced graphene oxide (rGO). Herein, we present the influence of different reduction degrees of rGO on its physico-chemical properties, such as crystallinity, specific surface area, electrical conductivity and electrochemical lithiation/delithiation behavior. It is found that a heat treatment under inert and reducing atmospheres increases the long-range order of rGO up to a temperature of 700 °C. At temperatures around 1000 °C, the crystallinity decreases. With decreasing oxygen content, a linear decrease in irreversible capacity during cycle 1 can be observed, along with a significant increase in electrical conductivity. This decrease in irreversible capacity can be observed despite an increase in specific surface area indicating the more significant influence of the oxygen content on the capacity loss. Consequently, the reversible capacity increases continuously up to a carbon content of 84.4 at% due to the thermal reduction. Contrary to expectations, the capacity decreases with further reduction. This can be explained by the loss of functional groups that will be lithiated reversibly, and a simultaneous reduction of long-range order, as concluded from dq/dU analysis in combination with XRD analysis.