Interfaces play an important role in nearly all aspects of life, and are essential for electrochemistry. Electrochemical systems ranging from high temperature solid oxide fuel cells (SOFC) to batteries to capacitors have a wide range of important interfaces between solids, liquids, and gases which play a pivotal role in how energy is stored, transferred, and/or converted. The ability to study these interfaces has proven to be difficult and is only further exacerbated by the limited number of techniques capable of operating under <i>in situ/operando</i> environments. To overcome these challenges, we use ambient pressure X-ray Photoelectron Spectroscopy (APXPS) at the tender X-ray regime between ~2 keV to 8 keV to probe the solid/liquid electrochemical interfaces under<i> in situ/operando</i> conditions. APXPS is a photon-in/electron-out process that can provide atomic concentrations, chemical specific, and electric potential information at pressures greater then 20 Torr. However we need to combine experiment with theory to truly understand these complex systems. In this talk I will introduce our APXPS technique for probing solid/liquid interfaces and how we leverage various modeling techniques ranging from analytical models to first-principles calculations to understand the phenomena occurring at the electrochemical interface. The strength of this synergistic approach will be shared through several studies including our ability to directly probe the electrochemical double layer (EDL) and determine the interfacial chemistry occurring at a magnesium electrode/diglyme interface.

Combining tender ambient pressure XPS with theory to unravel the solid/liquid electrochemical interface

254th National Meeting (2017)

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