To reflect the dynamic nature of the interface, different interfacial Li + -solvation configurations are sampled from recent MD simulations to assess the average influence of the local coordination environments to the overall current density, revealing that the lowest energy adsorption complexes correspond to a total CN of 4-5 with CNanion of 0-1 and coordination to EC being slightly preferred over EMC, in agreement with the results of Aggarwal et al. For each adsorption state, 𝜔 Li + is computed from a thermochemical cycle referenced to the average 𝜇 Li + of the bulk electrolyte (Note S1. 3 and Scheme S1). As seen in Figure .A, these low-energy complexes yield weakly endergonic Li + free energies of adsorption (𝜔