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Effects of Substrate, Current Density, and Li+ Supply in Sulfide-based Anode-free Solid-state Batteries Lithium nucleation and growth was examined in anode-free Li5.4PS4.4Cl1.6 (LPSC)-based batteries using cryo-TEM and electrochemical measurements. Lithium metal was plated onto TEM grids of various materials, which acted as substrates/current collectors, under varying current and mass loading conditions. Cycling demonstrated that highly lithiophilic materials are ideal substrates for anode-free systems, and that ideality is maintained even with very thin seed layers (20 nm). Surprisingly, copper was found to be unsuitable for sulfur systems, resulting in mossy or ball-like plating. Low mass loadings, shown in previous Li-excess solid state battery work to extend cycle life (due to low volume change), are observed to promote heterogenous lithium nucleation in the anode-free case, though the exact mechanism is unclear.
Sulfide-based solid-electrolytes can be unsuitable in combination with Cu electrode systems due to Cu 2S byproducts, and may show artificially poor nucleation in low mass loading systems.
Source: J Wang, Y Liu, M Ye, G Wang, C Xu, H Zhu Small, 2025
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