Rationalized design of hyperbranched trans-scale graphene arrays for enduring high-energy lithium metal batteries.

Lithium (Li) metal anode have shown exceptional potential for high-energy batteries. However, practical cell-level energy density of Li metal batteries is usually limited by the low areal capacity (<3 mAh cm -2 ) because of the accelerated degradation of high-areal capacity Li metal anodes upon cycling. Here, we report the design of hyperbranched vertical arrays of defective graphene for enduring deep Li cycling at practical levels of areal capacity (>6 mAh cm -2 ). Such atomic-to-macroscopic trans-scale design is rationalized by quantifying the degradation dynamics of Li metal anodes. High-energy Li metal cells are prototyped under realistic conditions with high cathode capacity (>4 mAh cm -2 ), low negative-to-positive electrode capacity ratio (1:1), and low electrolyte-to-capacity ratio (5 g Ah -1 ), which shed light on a promising move toward practical Li metal batteries.