High‐Performance, Low‐Cost, and Dense‐Structure Electrodes with High Mass Loading for Lithium‐Ion Batteries

Abstract Lithium‐ion batteries have undergone a remarkable development in the past 30 years. However, conventional electrodes are insufficient for the ever‐increasing demand of high‐energy batteries. Here, reported is a thick electrode with a dense structure, as an alternative to the commonly recognized porous framework. A low‐temperature sintering technology with the aid of aqueous solvent, high pressure, and an ion‐conductive additive is originally developed for preparing the LiCoO 2 (LCO)/Li 4 Ti 5 O 12 (LTO) dense‐structure electrode as the representative cathode/anode material. The 400 µm thick cathode with 110 mg cm −2 mass loading achieves a high specific capacity of 131.2 mAh g −1 with a good capacity retention of 96% over 150 cycles, far exceeding the commercial counterpart (≈40 µm) of 54.1 mAh g −1 with 39%. The ultrathick electrode of 1300 µm thickness presents a remarkable area capacity of 28.6 mAh cm −2 that is 16 times that of the commercial electrode. The full cell based on the dense electrodes delivers an extremely high areal capacity of 14.4 mAh cm −2 . The ion‐diffusion coefficients of the densely sintered electrodes increase by nearly three orders of magnitude. This design opens up a new avenue for scalable and sustainable material manufacturing towards various practical applications.