Abstract

<h2>Summary</h2> The issues of Zn dendrite and severe Zn<sup>2+</sup> transport destabilization in the electrode/electrolyte interface have been the main obstacles to the commercialization of aqueous Zn-based batteries. Here, a disordered zinc silicate (ZSO) artificial solid electrolyte interphase with high Zn<sup>2+</sup> conductivity (9.29 mS·cm<sup>−1</sup>) is proposed to address these dilemmas. The disordered ZSO interphase possesses sufficient tunnels for fast Zn<sup>2+</sup> transport and highly reversible Zn plating/stripping, which can redistribute the Zn<sup>2+</sup> flux and guide uniform Zn deposition to achieve a dendrite-free Zn metal anode. As a proof of concept in zinc-ion batteries, the Zn@ZSO//NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> battery delivers a capacity of 336.8 mAh·g<sup>−1</sup> at 0.2 A·g<sup>−1</sup>, with a capacity retention of 90.1% at 5 A·g<sup>−1</sup> over 1,000 cycles. As for the Zn@ZSO//I<sub>2</sub> battery, by inhibiting I<sub>3</sub><sup>−</sup> diffusion, 97.98% of capacity is retained after shelving for 60 h. This work provides enlightenment into interface designing and iodide diffusion suppression to accelerate the commercialization of high-performance zinc-based batteries.

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