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Molecular scale structure and dynamics at an ionic liquid/electrode interface
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DOI：10.1039/c7fd00171a.png)
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Abstract
En 中文
After a century of research, the potential-dependent ion distribution at electrode/electrolyte interfaces is still under debate. In particular for solvent-free electrolytes such as room-temperature ionic liquids, classical theories for the electrical double layer are not applicable. Using a combination of in situ high-energy X-ray reflectivity and impedance spectroscopy measurements, we determined this distribution with sub-molecular resolution. We find oscillatory charge density profiles consisting of alternating anion-and cation-enriched layers at both cathodic and anodic potentials. This structure is shown to arise from the same ion-ion correlations dominating the liquid bulk structure. The relaxation dynamics of the interfacial structure upon charging/discharging were studied by impedance spectroscopy and time resolved X-ray reflectivity experiments with sub-millisecond resolution. The analysis revealed three relaxation processes of vastly different characteristic time scales: a 2 ms scale interface-normal ion transport, a 100 ms scale molecular reorientation, and a minute scale lateral ordering within the first layer.
Keywords:
X-RAY REFLECTIVITY
ELECTRICAL DOUBLE-LAYER
LIQUID INTERFACE
ELECTROCHEMICAL-CELL
SURFACE-STRUCTURE
TEMPERATURE
CAPACITANCE
SCATTERING
METAL
RECONSTRUCTION
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