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. © 2025 Elsevier B.V.