Abstract
Despite lithium-ion batteries (LIBs) being state-of-the-art commercial rechargeable batteries, there are still significant challenges. For example, heat generation during cycling can lead to performance degradation and safety issues1-2. During the process of charging and discharging, the heat that is generated from the chemical reactions taking placing is ideally distributed uniformly in space, to dissipate out the cell easily. However, in practice, heat generation tends to be heterogeneous throughout the battery, leading to localized overheating3. This phenomenon can result in e.g. decomposition of the solid-state electrolyte interphase (SEI) layer, triggering electrode reactions with the electrolyte and degradation of the electrolyte (producing combustible gases) and even melting of the separator4. Hence, comprehending the origins of temperature generation and its heterogeneity is crucial.To address this challenge, operando X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) are applied to monitor the structural changes in the electrode materials during charge and discharge, while simultaneous temperature measurements are conducted using a thermal camera, as such obtaining spatial resolved structure/temperature/performance relationships. We have focused on state-of-the-art nickel rich NMC (Nickel Manganese Cobalt Oxide) versus graphite batteries and by comparing the structural changes of the electrode materials during cycling in ‘hot’ versus ‘cool’ areas of the electrode and battery, we were able to establish a structure-temperature relationships, on top of the electrochemical structure-performance relationships and as such unravel “heat-generation” process and reactions. The real-time temperature distribution was compared to the computational models using COMSOL, and insights in thermal processes and their possible control measures could be obtained.References Lain, M. & Kendrick, E. Understanding the limitations of lithium-ion batteries at high rates. Journal of Power Sources. Volume 493, 229690 (2021).Ma, S., et al. Temperature effect and thermal impact in lithium-ion batteries: A review. Progress in Natural Science: Materials International. Volume 28, Issue 6, Pages 653-666 (2018).Rafael, M., et al. Operando Radiography and Multimodal Analysis of Lithium–Sulfur Pouch Cells—Electrolyte Dependent Morphology Evolution at the Cathode. Adv. Energy Mater. 2103432 (2022).Joris, J., et al. A comprehensive review of future thermal management systems for battery electrified vehicles. Journal of Energy Storage 31, 101551(2020).
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