AI Article Synopsis
- Ions and solvent form a nanometer-scale electric double layer (EDL) at electrodes, crucial for battery passivation and (super)capacitor charge storage.
- The study uses in situ vibrational spectroscopy and molecular dynamics simulations to analyze the EDL composition of a Li-ion battery electrolyte.
- Findings reveal notable differences in ion behavior at the EDL compared to bulk conditions, highlighting the need for careful interpretation of electrochemical processes at interfaces.
Article Abstract
At an electrode, ions and solvent accumulate to screen charge, leading to a nanometer-scale electric double layer (EDL). The EDL guides electrode passivation in batteries, while in (super)capacitors, it determines charge storage capacity. Despite its importance, quantification of the nanometer-scale and potential-dependent EDL remains a challenging problem. Here, we directly probe changes in the EDL composition with potential using in situ vibrational spectroscopy and molecular dynamics simulations for a Li-ion battery electrolyte (LiClO in dimethyl carbonate). The accumulation rate of Li ions at the negative surface and ClO ions at the positive surface from vibrational spectroscopy compares well to that predicted by simulations using a polarizable APPLE&P force field. The ion solvation shell structure and ion-pairing within the EDL differs significantly from the bulk, especially at the negative electrode, suggesting that the common rationalization of interfacial electrochemical processes in terms of bulk ion solvation should be applied with caution.
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| http://dx.doi.org/10.1021/acs.jpclett.9b00879 | DOI Listing |
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