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초록

Anode-less all-solid-state batteries offer a promising route to maximize stack-level volumetric energy density by eliminating pre-installed lithium (Li) and forming the anode in situ on a bare current collector. However, in thin-film microbatteries, anode-less operation is highly sensitive to Li loss, which occurs via interphase formation, dead-Li isolation, and stripping-induced contact loss. Here, we develop an anode-less thin-film battery platform using lithiated vanadium oxide (LVO) cathodes and a lithium phosphorus oxynitride solid electrolyte, targeting the critical challenge of stabilizing Li nucleation and stripping at the solid-solid anode interface. Systematic screening of ultrathin current-collector modifications, including carbon-only, metal-only, and metal/carbon bilayers (Au, Ag, Zn, Al, and Sn), identifies Sn/C as the most effective seed layer, yielding the lowest nucleation overpotential, reduced voltage hysteresis, improved galvanostatic stability, and the most uniform Li plating morphology. To further mitigate first-cycle Li loss, a reversed-structure prelithiation step introduces a controlled Li reservoir on the seeded collector, enabling gradual activation and stable cycling. The optimized anode-less full cell with a 2-& micro;m-thick LVO cathode achieves a volumetric energy density of 235.13 Wh L-1 at the 100th cycle. These results establish practical guidelines for interlayer selection and interface engineering to enable durable anode-less thin-film batteries.

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