Preservation of cycling behavior: Understanding the changes in interfaces between electrode and electrolyte during battery cycling, including the formation of the solid-electrolyte interphase (SEI), is key to the development of longer lasting batteries. Z. Zhang et al . adapt a thin-film vitrification method to ensure the preservation of liquid electrolyte so that the samples taken for analysis using microscopy and spectroscopy better reflect the state of the battery during operation. A key finding is that the SEI is in a swollen state, in contrast to current belief that it only contained solid inorganic species and polymers. The extent of swelling can affect transport through the SEI, which thickens with time, and thus might also decrease the amount of free electrolyte available for battery cycling. —MSL

LiNi_xMn_yCo_zO₂ (NMC) is the current choice of cathode for high-performance Li-ion batteries. The structural and mechanical stability of NMC plays a vital role in determining the electrochemical performance of batteries. However, the dynamic mechanical properties of NMC during Li reactions are widely unknown because of the microscopic heterogeneity of composite electrodes as well as the challenge of mechanical measurement for air-sensitive battery materials. We employ instrumented nanoindentation in an inert environment to measure the elastic modulus, hardness, and interfacial fracture strength of NMC of a hierarchical meatball structure as a function of the state of charge and cycle number. The mechanical properties significantly depend on the lithiation state and degrade as the electrochemical cycles proceed. The results are further compared with the properties of bulk NMC pellets. We perform first-principles theoretical modeling to understand the evolution of the elastic property of NMC on the basis of the electronic structure. This work presents the first time systematic mechanical measurement of NMC electrodes which characterizes damage accumulation in battery materials over cycles.