Anode-free batteries, employing garnet-type solid-state electrolytes, offer a promising avenue for developing safe and high-energy-density battery technologies. However, their practical implementation is hampered by internal strain resulting from the repetitive plating and stripping of lithium metal. To address this challenge, we propose a novel approach utilizing titanium nitrate nanotubes and a silver-carbon interlayer. These components effectively mitigate the anisotropic stress arising from the recurrent formation of lithium deposition layers during cycling. The titanium nitrate nanotubes exhibit a mixed ionic-electronic conducting nature, facilitating the entry of reduced lithium into their free volume space via interfacial diffusion creep. This design achieves nearly strain-free operation with nearly tenfold volume suppression capability compared to conventional copper anodes during lithiation. Notably, our fabricated initial-anode-free quasi-solid-state battery, based on Li6.4La3Zr1.7Ta0.3O12 (LLZTO), paired with a high-voltage cathode infused with an ionic liquid electrolyte, demonstrates remarkable room temperature cyclability, exceeding 600 cycles at 1 mA cm-2, with an impressive average coulombic efficiency of 99.8%. This advancement holds significant promise for overcoming the barriers to practical realization of safe and high-performing battery technologies, paving the way for the development of next-generation energy storage solutions.
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