Self-assembled polysilane artificial solid electrolyte interphase layer towards highly reversible zinc electrochemistry

This paper introduces a design strategy for a self-assembled artificial solid electrolyte interface (SEI) layer with adjustable functional group integration, aimed at enhancing the performance of AZIBs. [Display omitted] •The self-assembled artificial SEI layer can securely adhere to the zinc surface through covalent bonding.•The resulting CF3-PSiOX layer acts as a hydrophobic shield, effectively isolating water and inhibiting corrosion.•The strong interaction between −CF3 and Zn2+ guides the diffusion and deposition processes of Zn2+, optimizing the de-solvation process. Commercial applications of aqueous Zn batteries primarily encounter challenges related to surface corrosion and dendrite formation. In this study, a hydrophobic polysilane layer functionalized with −CF3 groups (CF3-PSiOX) is tailored for Zn anode through a two-step process involving self-assembly and condensation. The CF3-PSiOX layer functions as a protective barrier, effectively isolating water and inhibiting corrosion. Moreover, the primary interactions between −CF3 and Zn2+ guides the diffusion and deposition processes of Zn2+ while optimizing the de-solvation process, ultimately resulting in dendrite inhibition. Hence, cells with CF3-PSiOX layer boasts a high Coulombic efficiency (∼99.8 % after 1500 cycles), a long lifespan (over 2400 h), and optimized capacity retention (73.3 % over 1000 cycles). The self-assembled polysilane layer with customizable groups offers a novel approach for tuning the interface properties of Zn anodes and establishes a general principle for interface adjustment applicable to alternative metallic electrodes.