A Highly Conductive 3D Interconnected Framework with Stress Buffering for Enhanced Electrochemical and Mechanical Performance in Thick Cathodes

Abstract

Developing a thick electrode offers a practical route to enhance the energy density of lithium batteries, but its application suffers from sluggish ion/electron transport kinetics and poor structure homogeneity. Herein, a high-crystallinity three-dimensional porous carbon (H-3DC) is designed for enhancing the capacity utilization and mechanical integrity of high-mass-loading cathodes. H-3DC establishes a continuous conductive network that synergistically promotes ion/electron transport kinetics, regulates the distribution of the conductive binder domain, and alleviates localized overpressure. Consequently, the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode with a high loading of 38 mg cm–2 incorporating H-3DC achieves a high discharge capacity of 173.6 mAh g–1 at 8 mA cm–2. When paired with a lithium metal anode, a remarkable energy density of 570.49 Wh kg–1 is achieved. This work underscores the significance of structural design in reconciling the charge transport efficiency and mechanical robustness for thick electrodes, offering a promising pathway for developing high-energy-density batteries.