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.