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The impact of electrode conductivity on electrolyte interfacial structuring and its implications on the Na0/+ electrochemical performance
journal contribution
posted on 2023-10-26, 04:27 authored by DA Rakov, J Sun, PV Cherepanov, K Arano, Patrick HowlettPatrick Howlett, AN Simonov, Fangfang ChenFangfang Chen, Maria ForsythMaria ForsythMolecular and ionic assemblies at electrode/liquid electrolyte interfaces, i.e., the electric double layer (EDL), define battery performance by directing the formation of stable interphases. An unstable interphase can hamper metal-cation diffusion, lead to continuous electrolyte consumption, and also promote non-uniform electrochemical processes like dendrite formation. The co-selection of electrolyte chemistry and initial cycling conditions together are generally considered for the design of desirable interphases. At the same time, the dielectric nature of the electrode material is largely ignored, notwithstanding the high unreliability of the assumption that the nature of the EDL and the mechanism of the interphase formation at metallic and semiconductive electrodes are identical. Here we show that the dielectric nature of the charged electrode greatly affects the interfacial metal-anion-solvent composition; therefore, different interphase chemistry will be formed, suggesting different initial cycling conditions need to be established on a case-by-case basis to form the desired interphase. This phenomenon correlates with the metal ion solvation chemistry and the adsorption of species at the electrified electrode due to the competition of van der Waals and coulombic interactions.
History
Journal
Energy and Environmental ScienceVolume
16Pagination
3919-3931Location
London, Eng.Publisher DOI
ISSN
1754-5692eISSN
1754-5706Language
EnglishPublication classification
C1 Refereed article in a scholarly journalIssue
9Publisher
ROYAL SOC CHEMISTRYUsage metrics
Keywords
Science & TechnologyPhysical SciencesTechnologyLife Sciences & BiomedicineChemistry, MultidisciplinaryEnergy & FuelsEngineering, ChemicalEnvironmental SciencesChemistryEngineeringEnvironmental Sciences & EcologyIONIC LIQUID ELECTROLYTESDIFFERENTIAL CAPACITANCEDOUBLE-LAYERLITHIUMTEMPERATUREDYNAMICSSIMULATIONREDUCTIONSOLVATIONOXIDATION
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