Parabolic-growth universality and its nucleation-driven breakdown across lithium-battery anode chemistries

TL;DR

This study reveals that solid-electrolyte interphase growth follows a universal parabolic law across most lithium battery chemistries, with deviations indicating nucleation-driven breakdown in certain configurations.

Contribution

It demonstrates the kinetic scaling law of SEI growth across multiple chemistries and identifies nucleation effects in anode-free configurations, simplifying modeling approaches.

Findings

SEI growth obeys a parabolic law in three chemistries

Anode-free configurations deviate with a super-parabolic exponent

The universality reduces modeling complexity to a single rate constant

Abstract

Solid-electrolyte interphase (SEI) growth is widely modeled cell-by-cell with chemistry-specific closures, yet its underlying kinetic scaling is rarely tested across chemistries. By compiling cycle-resolved data from public long-cycle datasets covering four anode configurations -- graphite, silicon composite, lithium metal, and anode-free -- we show that the cumulative interphase-loss index Lambda_int obeys the parabolic law Lambda_int = A_chem * sqrt(1 - Theta_Li) in three of the four chemistries, with an exponent indistinguishable from alpha = 1/2 within experimental uncertainty. The chemistry-specific prefactor A_chem spans an order of magnitude, but the diffusion-limited parabolic kinetics is preserved. The fourth chemistry, anode-free configurations, deviates with a super-parabolic exponent alpha approx 0.77, consistent with a nucleation-controlled growth regime. We rationalize the result using the Tammann-Deal-Grove parabolic-growth framework adapted to interphase formation and identify the conditions under which universality is recovered. The observed regularity reduces SEI modeling complexity to a single rate constant per chemistry and provides a sharp falsifiable test for next-generation cell formats.