Claw‐Like Macromolecular Engineering for Stabilizing Zinc Anodes Under High‐Current Operation

The mismatch between high-current operation and limited mass transport induces steep concentration gradients at the electrode surface, leading to non-uniform zinc deposition and undesirable side reactions. Here, we propose an electrolyte modification strategy that leverages the claw-like structure of Tris(3,6-dioxaheptyl)amine (TDA-1) to stabilize the electrolyte/electrode interface (EEI) under high-current conditions. Theoretical calculations and experimental results reveal that the abundant polar groups on the three branched chains of TDA-1 strongly anchor to the zinc surface, thereby reconstructing the electric double layer (EDL). The TDA-1 additive reduces the Zn²⁺ desolvation energy barrier and extends the ion migration pathway, enabling rapid and uniform zinc deposition and diffusion. The Zn||Zn symmetric batteries with the TDA-1 additive deliver stable cycling for 1000 h at a current density of 20 mA·cm^-2, whereas the Zn||VNNC full batteries exhibit markedly improved capacity retention after 500 cycles at an N/P ratio of 4.29. This study highlights the potential of macromolecular additives, which exploit claw-like spatial structures and abundant functional groups, to enhance the zinc anodes' stability under high-current conditions.