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

ABSTRACT 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 Zn 2+ 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.