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Solid-state zinc (Zn) batteries offer anew candidate for emerging applications sensitive to volume,safety and cost. However,c urrent solid polymeric or ceramic electrolyte structures remain poorly conductive for the divalent Zn 2+ , especially at room temperature.C onstructing aheterogeneous interface whichallows Zn 2+ percolation is aviable option, but this is rarely involved in multivalent systems.H erein, we construct as olid Zn 2+ -ion conductor by inducing crystallization of tailored eutectic liquids formed by organic Zn salts and bipolar ligands.H igh-entropye utectic-networks weaken the ion-association and form interfacial Zn 2+ -percolated channels on the nucleator surfaces,r esulting in as olid crystal with exceptional selectivity for Zn 2+ transport (t Zn 2þ = 0.64) and appreciable Zn 2+ conductivity (s Zn 2þ = 3.78 10 À5 Scm À1 at 30 8 8C, over 2o rders of magnitude higher than conventional polymers), and finally enabling practical ambient-temperature Zn/V 2 O 5 metal solid cells.T his design principle leveraged by the eutectic solidification affords new insights on the multivalent solid electrochemistry suffering from slow ion migration.

Silicon (Si) has been regarded as an alternative anode material to traditional graphite owing to its higher theoretical capacity (4200 vs. 372 mAh g−1). However, Si anodes suffer from the inherent volume expansion and unstable solid electrolyte interphase, thus experiencing fast capacity decay, which hinders their commercial application. To address this, herein, an endotenon sheath-inspired water-soluble double-network binder (DNB) is presented for resolving the bottleneck of Si anodes. The as-developed binder shows excellent adhesion, high mechanical properties, and a considerable self-healing capability mainly benefited by its supramolecular hybrid network. Apart from these advantages, this binder also induces a Li3N/LiF-rich solid electrolyte interface layer, contributing to a superior cycle stability of Si electrodes. As expected, the DNB can achieve mechanically more stable Si electrodes than traditional polyacrylic acid and pectin binders. As a result, DNB delivers superior electrochemical performance of Si/Li half cells and LiNi0.8Co0.1Mn0.1O2/Si full cells, even with a high loading of Si electrode, to traditional polyacrylic acid and pectin binders. The bioinspired binder design provides a promising route to achieve long-life Si anode-assembled lithium batteries. "Image missing"

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