Lithium metal is the most attractive anode material owing to its lowest electrochemical potential and high theoretical specific capacity. However, uncontrolled dendrite growth leads to severe safety issues and poor electrochemical stability, hindering its practical application. Herein, we report a dendrite-free and reversible Li metal anode enabled by graphene aerogel (GA) host with three-dimensional gradient porous structure. The gradient porous structure facilitates reversible Li plating/stripping with high Li/carbon mass ratio (Li/C = 5) and realizes uniform Li distribution on the electrode surface. This approach achieves a stable voltage profile for a long lifespan (1300 h at 2 mA cm⁻² for 2 mAh cm⁻² and 1000 h at 5 mA cm⁻² for 3 mAh cm⁻²) with superior high symmetric cumulative capacity (2500 mAh cm⁻²). Coupling the LiGA anode with a LiFePO₄ (LFP) cathode, a stable cycling of the full LiGA-LFP cells for 200 cycles at 2 C were achieved, demonstrating the promising practical applications of LiGA in advanced rechargeable batteries.

锂金属由于其最低的电化学势和较高的理论比容量而成为最具吸引力的阳极材料。然而，不受控制的枝晶生长导致严重的安全问题和较差的电化学稳定性，从而阻碍了其实际应用。本文中，我们报道了具有三维梯度多孔结构的石墨烯气凝胶（GA）基质实现的无枝晶且可逆的锂金属阳极。梯度多孔结构有助于以高Li /碳质量比（Li / C = 5）进行可逆的Li电镀/剥离，并在电极表面实现均匀的Li分布。这种方法可实现稳定的电压曲线，使用寿命长（2 mAh cm ^-2的2 mA cm ^-2 1300 h和3 mAh cm ^-2的5 mA cm ^-2 1000 h）具有出色的高对称累积容量（2500 mAh cm ^-2）。将LiGA阳极与LiFePO ₄（LFP）阴极耦合，可在2 C下实现完整LiGA-LFP电池200个循环的稳定循环，这证明了LiGA在高级可充电电池中的有希望的实际应用。