The development of long-term stable Zn anodes capable of operating at high current densities and/or capacities remains a huge challenge. Herein, through the rapid potassium permanganate solution treatment and laser lithography, we have developed a gradient Zn anode (LLP@Treated Zn) with the insulating and hydrophobic passivated-layer at the top and conductive and hydrophilic fresh-zinc-layer at the bottom. This makes the passivation layer prevent the Zn anodes from corrosion and side reactions and induce the preferential deposition of Zn at the bottom of the microchannel without dendrite growth. As a consequence, the LLP@Treated Zn anodes exhibit a stable cycle life for over 700 h at 10 mA cm–2 and 5 mAh cm–2. Moreover, the Zn anodes with different surface morphologies (ring, lattice, etc.) could also be obtained by laser lithography, which proves the flexibility of the pulsed laser lithography strategy in the preparation of battery materials.

The continuous growth of Li dendrites and volumetric deformation of Li severely impede the commercial application of Li metal anodes. To regulate Li stripping/plating, electrodeposition or magnetron sputtering is extensively utilized to fabricate lithiophilic‐metal deposited 3D Li hosts. However, the binding force between lithiophilic‐metal and host is weak, inevitably leading to numerous cracks/defects of lithiophilic‐surface‐layer during Li plating/stripping. Herein, a quasi‐gradient (Cu‐Cu3Sn‐Sn‐SnO2) 3D skeleton consisting of hierarchical Sn/SnO2 composite metallurgically bonded to copper foam through Cu3Sn alloy (LAD‐SSC@CF) is designed, and prepared in one‐step by a nanosecond‐pulsed‐laser‐assisted deposition strategy. The homogeneous Li nucleation sites provided by Li22Sn5 formed by the reaction of Sn/SnO2 with Li can inhibit Li dendrites growth. Meanwhile, the porous space and strong bonding of Cu3Sn layer avoid structural deterioration of anodes. Consequently, a symmetric cell based on LAD‐SSC@CF@Li exhibits an outstanding cycling stability of 1500 h at 1 mA cm−2. In particular, a full cell with LiFePO4 cathode provides good capacity retention of 81.3% at 5 C after 600 cycles. Moreover, the successful preparation of other composite materials (In, Zn, Sn‐Bi, etc.) loading on various substrates (Kapton film, ceramic, copper foil, etc.) demonstrates the versatility of pulsed‐laser‐assisted deposition strategy for preparing battery materials.

No abstract