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A critical aging mechanism in lithium-ion batteries is the decomposition of the electrolyte at the negative electrode forming a solid electrolyte interphase (SEI) layer that increases impedance and consumes cyclable lithium. In contrast to the typical nanometer SEI layer generally discussed, this paper reports on the formation of a micrometer thick film on top of and within the upper part of a porous graphite electrode in a deep-cycled commercial cylindrical LiFePO4/graphite cell. Morphological, chemical, and electrochemical characterizations were performed by means of cross-sectional electron microscopy in combination with energy dispersive X-ray spectroscopy and focused ion-beam milling, time-of-flight secondary ion mass spectrometry, and electrochemical impedance spectroscopy (EIS) to evaluate the properties and impact of the uneven film. It is shown that the film is enriched in P–O and carbonate species but is otherwise similar in composition to the thin SEI formed on a calendar-aged electrode and clogs the pores in the electrode closest to the separator. Performance evaluation by physics-based EIS modeling supports a local porosity decrease, impeding the effective electrolyte transport in the electrode. The local variation of electrode properties implies that current distribution in the porous electrode under these cycling conditions causes inefficient material utilization and sustained uneven electrode degradation.

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Thermal effects are linked to all main barriers to the widespread commercialization of lithium-ion battery powered vehicles. This paper presents a coupled 2D electrochemical – 3D thermal model of a large-format prismatic lithium-ion battery, including a thermal management system with a heat sink connected to the surface opposite the terminals, undergoing the dynamic current behavior of a plug-in hybrid electric (PHEV) vehicle using a load cycle with a maximum current of 8 C, validated using potential and temperature data. The model fits the data well, with small deviations at the most demanding parts of the cycle. The maximum temperature increase and temperature difference of the jellyroll is found to be 9.7°C and 3.6°C, respectively. The electrolyte is found to limit the performance during the high-current pulses, as the concentration reaches extreme values, leading to a very uneven current distribution. Two other thermal management strategies, short side and long side surfaces cooling, are evaluated but are found to have only minor effects on the temperature of the jellyroll, with maximum jellyroll temperatures increases of 9.4°C and 8.1°C, respectively, and maximum temperature differences of 3.7°C and 5.0°C, respectively.

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An important step toward safer and more reliable lithium-ion battery systems is the improvement of methods for detection and characterization of battery degradation. In this work, we develop and track aging indicators over the life of 18650-format lithium-ion batteries with a blended NMC532-LMO positive electrode and graphite negative electrode. Cells are cycled until reaching 80% of their original capacity under combinations of four cycling conditions: ambient and sub-ambient temperatures (29 °C and 10 °C) and fast and mild rates (2.7 and 1.0C). Loss of lithium inventory dominates aging for all cases, with additional loss of NMC capacity under the combination of sub-ambient temperature and mild rate. A novel, easily acquired polarization factor complements capacity fade analysis; it correlates well with impedance and galvanostatic cycle life and indicates changes in active aging processes. These processes are further revealed by differential voltage analysis (DVA) and incremental capacity analysis (ICA). New indicators and aging scenarios are evaluated for these techniques and supported by post mortem analysis. From in operando cycling data and a single, slow discharge curve, these four methods (capacity fade, polarization factor, DVA, and ICA) comprise a simple, explanatory, and non-invasive toolbox for evaluating aging in lithium-ion battery systems.