Geoscience‐Inspired Pore Topology Engineering for Ultra‐Thick Cathodes Toward High‐Energy‐Density Zinc‐Ion Batteries

Abstract

ABSTRACT Zinc‐ion batteries (ZIBs) are promising for safe and large‐scale energy storage, yet the construction of high‐performance ultrathick and high‐loading cathodes hinders their application due to sluggish ion/electron transport. Herein, drawing upon the structure‐activity relationships of pore topology in geoscience, we propose an efficient pore network regulation strategy using an ammonium acetate porogen to prepare a high‐performance ultrathick cathode through integrating this architecture with a graphene/carbon nanotubes framework synergistically enhances both ionic and electronic conductivity. Specifically, micro‐computed tomography (Micro‐CT) and pore network modeling reveal a highly optimized pore topology with remarkably increased connectivity (64.9%), coordination number (77.8%), and throat diameter (25%) despite a mere 13% increase in porosity by using ammonium acetate porogen. This architecture preserves conductive network robustness during wetting and enhances mass/ion transport, as validated by Avizo permeability simulations. As expected, the cathode delivers 17.96 mAh cm −2 (97.2% retention after 106 cycles) and a competitive energy density of 152.8 Wh kg −1 (N/ P = 1.3) in coin cells with an ultra‐high loading of 56.8 mg cm −2 . A practical 4 × 4.5 cm pouch cell using this cathode achieves a full‐cell energy density of 69.2 Wh kg −1 as well as82.6% retention over 96 cycles. This scalable topology‐guided strategy bridges geoscience and battery engineering for ZIBs.