Accelerating Desolvation and Constructing Dual‐Storage Channels for Zn <sup>2+</sup> by Ligand Field Engineering of Polar Organic Molecules for High‐Performance Zinc‐Ion Batteries
Xiao‐Jie Lu, Lei Chen, Wenxiao Li, Xiaoliang Zhang, Weili Chi, Mao Peng, Chunxia Wang, Yong Liu, Xiangwu Zhang
Abstract
Abstract The growing reliance on renewable energy has heightened the need for affordable, high‐capacity energy storage solutions. Aqueous zinc‐ion batteries (ZIBs) are promising for large‐scale storage due to their low cost, high safety, and environmental friendliness. However, their practical application is hindered by sluggish Zn 2 ⁺ kinetics arising from high desolvation energy barriers at electrode/electrolyte interfaces. To address this challenge, we design an organic/inorganic hybrid cathode through ethylenediaminetetraacetic acid (EDTA) incorporation into MnO 2 . The desolvation and the construction of dual storage channels for Zn 2+ are cooperatively driven by polar organic molecule ligand field engineering. The multipolar groups (‐COOH/ ─NH 2 ) of EDTA can effectively break the solvation sheath of Zn(H 2 O) 6 2+ , accelerate the desolvation process of Zn 2+ ions, and the polar groups can provide additional active sites as electron donors binding to Zn 2+ , forming organic/inorganic dual energy storage. Density functional theory (DFT) reveals that the electron‐withdrawing effect of EDTA optimizes charge distribution at the MnO 2 , and lowers the Zn 2 ⁺ diffusion barrier. This synergistic regulation enables the EDTA‐MnO 2 cathode to deliver a high reversible capacity of 199.2 mA h g⁻¹ after 1000 cycles at 1 A g⁻¹. This hybrid design accelerates Zn 2+ desolvation and constructs an efficient dual‐storage mechanism, offering a new direction for high‐performance ZIBs.