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Abstract The interfacial decomposition products forming the so‐called solid–electrolyte interphase (SEI) significantly determine the destiny of a Li‐ion battery. Ultimate knowledge of its detailed behavior and better control are required for higher rates, longer life‐time, and increased safety. Employing an electrochemical surface force apparatus, it is possible to control the growth and to investigate the mechanical properties of an SEI in a lithium‐ion battery environment. This new approach is here introduced on a gold model system and reveals a compressible film at all stages of SEI growth. The demonstrated methodology provides a unique tool for analyzing electrochemical battery interfaces, in particular in view of alternative electrolyte formulations and artificial interfaces.

Electrochemical processes strongly depend on the wetting and mobility phenomena at the involved nano-confined interfaces. Here, the authors use a surface forces apparatus to understand the wetting behavior of graphene, gold, and mica surfaces by Li-ion battery electrolytes.