Abstract
AbstractPassivating solid electrolyte interphases (SEIs) in Ca metal anodes constitute a long‐standing challenge, as they block Ca2+ transport and inhibit reversible Ca deposition/stripping. Current solutions focus primarily on boron/aluminum‐based electrolytes to mitigate such interfacial issues by producing Ca2+‐conductive species, yet the complex synthetic procedure of these salts restricts the widespread application. Moreover, whether any inorganic phases possess decent Ca2+ conductivity within SEIs remains ambiguous. Herein, we report that a commercially available CaI2‐dimethoxyethane electrolyte supports reversible Ca/Ca2+ redox reactions via forming CaI2‐involved SEI, inspired by our density functional theory calculations where CaI2 species is predicted to possess the lowest Ca2+ diffusion barrier among a range of inorganic phases. We further materialize this finding by introducing a serial of borate ester anion receptors, resulting in the formation of CaI2/borides hybrid SEIs with an enhanced Ca2+ conductivity. Consequently, the resultant electrolytes realize a 7‐fold reduction in deposition/stripping overpotential compared to anion receptor‐free one, allowing for the construction of reversible Ca‐metal full cells with high‐capacity selenium and organic cathodes.
Published Version
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