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

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.