The structure of interfacial water on gold electrodes studied by x-ray absorption spectroscopy

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Science  23 Oct 2014:
DOI: 10.1126/science.1259437

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The molecular structure of the electrical double layer determines the chemistry in all electrochemical processes. Using x-ray absorption spectroscopy (XAS) we probed the structure of water near gold electrodes and its bias dependence. Electron yield XAS detected at the same gold electrode, revealed that the interfacial water molecules have a different structure than those in the bulk. First principles calculations revealed that ~50% of the molecules lie flat on the surface with saturated hydrogen bonds and another significant fraction with broken hydrogen bonds that do not contribute to the XAS spectrum because their core-excited states are delocalized by coupling with the gold substrate. At negative bias the population of flat lying molecules with broken hydrogen bonds increases, producing a spectrum similar to that of bulk water.

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