Enabling Aluminum-Silicon Electrodes As Monolithic Anodes for Lithium-Ion Batteries

Based on current trends in lithium-ion battery (LIB) production and forecasts for immense demand of these energy storage devices, it is evident that all cell components will need dramatic improvement in the future. Although anode materials may be considered by some to be a lower priority, compared to cathode materials, the cost of the anode (and Cu foil current collector) comprise nearly 25% of the materials cost of a LIB cell, and consume ~30% of the volume. Among the possible alternative anode materials for LIBs to replace slurry-based graphite electrodes, alloying materials such as Si, Sn, Al and Ge are promising candidates. Despite the attractive advantages of aluminum-based electrodes (such as low cost, good geographic dispersity and high abundancy), capacity fade due to a large volume change associated with the α/β (Al/LiAl) phase transformation during cycling is the key problem. Al alloy or composite electrodes are a promising strategy for improving the reliability of Al-based electrodes. Among the Al-based monolithic anode materials for LIBs, to the best of our knowledge, Al-rich Al-Si alloys or composites have rarely been investigated. The present work highlights a new achievement towards realizing monolithic, free-standing alloy anodes which can significantly reduce both the cost and processing complexity of LIB electrodes. Herein, we propose a novel strategy to enable the use of aluminum-silicon alloys as monolithic anodes for LIBs. Accordingly, the microstructural, morphological, and electrochemical evolution of Al-Si thin-films of various compositions were investigated, with a focus on understanding the process of Al-Si-Li ternary phase formation during lithiation (in the particular case of excess Al). Ex situ microscopy observations, along with comprehensive electrochemical analysis, suggests that remarkable performance can be achieved by controlling the electrochemical condition for the formation of Al-Si-Li ternary phase, such that no LiAl (β phase) forms during lithiation. In other words, Al-Si-Li ternary phase is cycled within a soft aluminum matrix, thereby avoiding the degradation associated with the de-/lithiation of the β phase [1]. [1] M. H. Tahmasebi, D. Kramer, R. Mönig, and S. T. Boles, “Insights into Phase Transformations and Degradation Mechanisms in Aluminum Anodes for Lithium-Ion Batteries,” J. Electrochem. Soc., vol. 166, no. 3, pp. A5001–A5007, 2019.

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