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The demonstrated technique provides insights into both the optimized structures of composite electrodes and the underlying mechanisms of interfacial degradation at active material/solid electrolyte interfaces.Binders play a crucial role in the development of silicon (Si) anodes for lithium-ion batteries with high specific energy. The large volume change of Si (∼300%) during repeated discharge and charge processes causes the destruction and separation of electrode materials from the copper (Cu) current collector and ultimately results i