Abstract

As lithium-ion batteries (LIBs) have exploded in popularity due to the consumer electronics and electric vehicle industries, many resources are poured into research. While the simplest cell format requiring the least amount of active material to make in a research laboratory to study various aspects of the cell is usually the coin cell, it is far from the most representative of commercial LIBs. Oftentimes, coin cells are made with a large negative electrode overhang to reduce the risk from positive/negative electrode misalignment, but the overhang region can cause Li+ to become effectively trapped at higher C-rates1. While this is a necessary trade-off in today’s commercial LIB manufacturing, the overhang area is normally a much smaller fraction of the total negative electrode area in a commercial cell than in a laboratory coin cell, which can lead to discrepancies in cycle testing. Moreover, during assembly of commercial stacked or wound cells, there is always a region in which one side of a double-sided coating, typically the negative, is not needed and thus a single-sided electrode should be used. However, not all manufacturers eliminate the outward-facing second side and elect to simply use double-sided coatings throughout. Therefore, studying the effects of excess electrode in single-layer pouch cells will be explored in this presentation. In this presentation, cells made in various formats (coin and stacked pouch) will be compared to single-layer pouch cells made with and without negative electrode overhang. Single-layer pouch cells are the easiest format for assembling full cells without overhang because they are neither too small nor too big for positive/negative electrode alignment to be difficult. Moreover, single-layer pouch cells made with double-sided coatings (without overhang) and cycled using Ultra-High Precision Coulometry (UHPC) will be shown to have poor cycling. This is for two reasons: 1) for a double-sided negative, the outward-facing coating of the electrode can trap Li+ just like the overhang on the inward-facing coating; and 2) the outward-facing positive can be deintercalated and provide more capacity than desired2, possibly even surpassing the negative/positive areal capacity ratio. Single-layer pouch cells with no overhang are shown in Figure 1a to outperform all other cell formats tested, retaining 90% of their original capacity after 500 cycles at C/3 and 40 °C, and have the lowest difference in capacity between typical C/3 and C/20 checkup cycles as shown in Figure 1b. The stacked pouch cells in Figure 1 are composed of 3 positive and 4 negative electrodes that are all double-sided, meaning there are two outward-facing negative electrode coatings that can trap Li+, possibly resulting in the much poorer capacity fade to 80% after 500 cycles illustrated in Figure 1a. Thus, single-layer pouch cells without overhang give the most realistic cycling results for the tested electrode materials. Figure 1. C/3 cycling of full cells of various formats denoted in the legend. Plotted in (a) is the normalized discharge capacity and (b) is the difference in areal discharge capacity between the C/20 checkup cycle and preceding C/3 cycle. REFERENCES Gyenes, B., Stevens, D.A., Chevrier, V.L., and Dahn, J.R. (2015). Understanding Anomalous Behavior in Coulombic Efficiency Measurements on Li-Ion Batteries. J Electrochem Soc 162, A278–A283. 10.1149/2.0191503jes.Smith, A., Stüble, P., Leuthner, L., Hofmann, A., Jeschull, F., and Mereacre, L. (2023). Potential and Limitations of Research Battery Cell Types for Electrochemical Data Acquisition. Batter Supercaps e202300080. doi.org/10.1002/batt.202300080. Figure 1

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