Spontaneous topological silicon quantization for redesigned Si-based Li-ion batteries

Abstract: Nano-structured silicon anodes are attractive alternatives to graphite in lithium-ion batteries; however, despite recent progress in nano-engineered composites, its use remains limited. One of the issues, particularly in silicon-dominated anodes, is the poor Coulombic efficiency of lithium？silicon processes. Previous studies have shown that repeating the amorphous？crystalline hysteretic lithium？silicon phase transformations can abruptly improve irreversibility and eventually minimize cumulative irreversible lithium consumption in exchange of certain parasitic capacity sacrifice. Here, we reveal mechanism behind the phenomenon that the single phase transformation spontaneously and topologically transforms nano-structured silicon into quantum-scale frameworks without gravimetric loss. This is clearly distinct from ever explored formation mechanism of porous nano-structures. Further, we redesign full cells, largely altering the conventional one, by modulating cathode/anode capacity loading balance and prelithiation dose in the anode to embed the unique feature in the cells. We show that the cell preferentially triggers the irreversibility-depletion phenomenon upon cycling and consequently outperforms conventional silicon-based cells.