Journal
FARADAY DISCUSSIONS
Volume 206, Issue -, Pages 141-157Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7fd00171a
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Funding
- German-Israeli Foundation for Scientific Research and Development [2306-2310.14/2011]
- Excellence Initiative [DFG/ GSC 266]
- Danish National Research Foundation
- Danish Strategic Research Council through project 'ReLiable'
- DANSCATT
- Max Planck Society
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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.
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