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Abstract  Continued growth of the solid–electrolyte interphase (SEI) is the major reason for capacity fade in modern lithium‐ion batteries. This growth is made possible by a yet unidentified transport mechanism that limits the passivating ability of the SEI towards electrolyte reduction. We, for the first time, differentiate the proposed mechanisms by analyzing their dependence on the electrode potential. Our calculations are compared to recent experimental capacity‐fade data. We show that the potential dependence of SEI growth facilitated by solvent diffusion, electron conduction, or electron tunneling qualitatively disagrees with the experimental observations. Only diffusion of Li interstitials results in a potential dependence matching the experiments. Therefore, we identify the diffusion of neutral radicals, such as Li interstitials, as the cause of long‐term SEI growth.

Identifying the Mechanism of Continued Growth of the Solid–Electrolyte Interphase