Operando nanoindentation: A new platform to measure the mechanical properties of electrodes during electrochemical reactions

We present an experimental platform of operando nanoindentation that probes the dynamic mechanical behaviors of electrodes during real-time electrochemical reactions. The setup consists of a nanoindenter, an electrochemical station, and a custom fluid cell integrated into an inert environment. We evaluate the influence of the argon atmosphere, electrolyte solution, structural degradation and volumetric change of electrodes upon Li reactions, as well as the surface layer and substrate effects by control experiments. Results inform on the system limitations and capabilities, and provide guidelines on the best experimental practices. Furthermore, we present a thorough investigation of the elastic-viscoplastic properties of amorphous Si electrodes, during cell operation at different C-rates and at open circuit. Pure Li metal is characterized separately. We measure the continuous evolution of the elastic modulus, hardness, and creep stress exponent of lithiated Si and compare the results with prior reports. operando indentation will provide a reliable platform to understand the fundamental coupling between mechanics and electrochemistry in energy materials.