It has been well accepted that when an electric field is applied on an electrode, electrical double layer may form at the electrode-electrolyte interface, the structure of which may have a significant effect on the interfacial electrochemistry. However, it has been challenging to molecularly characterize the formation and evolution of electrical double layer due to lack of operando techniques that can provide molecular information with a depth resolution of a few nanometers at solid-liquid interface. Recently, <i>in situ </i>liquid secondary ion mass spectrometry (SIMS) has been developed in Pacific Northwest National Laboratory for molecular investigation of various liquids and liquid interfaces. Using this innovation, we successfully characterized the formation and evolution of electrical double layers at the electrode-electrolyte interface. Besides, in a model rechargeable Li-ion battery we directly observed the formation of electrical double layer at the electrode surface under battery operating conditions and discovered its consequences on the chemical structure of solid-electrolyte interphase layer. The above findings suggest promising applications of <i>in situ</i> liquid SIMS on investigation of complex chemistry occurring at electrode-electrolyte interfaces.

Mass spectrometric investigation of electrical double layer at electrode-electrolyte interfaces

254th National Meeting (2017)

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