Strategy utilizing lithiophilic gradients for dendrite-free lithium metal battery

Lithium metal batteries (LMBs) hold significant promise for next-generation energy storage due to their high energy density. However, uncontrollable lithium dendrite growth and the formation of "dead lithium" at the anode-separator interface hinder their practical application. To address these challenges, we developed a novel strategy using a vertically distributed lithiophilic ZnO gradient on a 3D carbon cloth substrate (GZnO/CC) to regulate lithium deposition in a controlled "bottom-up" manner. The gradient ZnO structure lowers nucleation energy at the bottom, homogenizes Li+ flux, and suppresses dendrite formation at the top. COMSOL Multiphysics simulations further confirm that the GZnO/CC framework effectively balances Li+ ion concentration gradients, promoting uniform lithium deposition. Experimental results demonstrate that the GZnO/CC electrode exhibits an ultra-long cycle life exceeding 2500 h with low overpotential (4.3 mV) at 1 mA cm- 2 in symmetric cells. In a full cell with a commercial LiFePO4 cathode, the Li-GZnO/CC anode achieves a discharge capacity of 149.7mAh g- 1 and retains 90.7 % capacity after 1000 cycles. This study highlights the potential of integrating lithiophilic gradient strategies with 3D frameworks to enable stable, dendrite-free lithium metal anodes, paving the way for safer and more efficient high-energy batteries.