Multimodal Degradation Interactions in Electrodes for Energy Storage

Energy storage electrodes exhibit significant capacity and performance degradation with cycling owing to extensive decrepitation of anodes associated with lithiation-delithiation induced volumetric expansion and contraction. Microcrack formation in the active material and solid electrolyte interphase layer contribute to deleterious effects including hindered diffusion, particle isolation, and loss of cyclable active material inventory, with detrimental performance ramifications. Unabated solid electrolyte interphase growth in conjunction with irregular plating on metal/intercalation electrodes can also pose serious safety issues like short-circuit, compromising the integrity of the system. In this work, degradation originating from coupled mechano-electrochemical-transport interactions have been identified with detailed insights into the physical mechanisms contributing to this degradation. Strategies to ameliorate degradation damage inside these systems have been enumerated, with emphasis on graphite and silicon intercalation anodes and lithium metal anode.