High-Mass Loading Nickel-Rich Cathode Electrode Design Incorporating Multidimensional Carbon Conductive Additives to Minimize Ohmic Contact Resistance for High-Performance Lithium-Ion Batteries.

Lithium-ion batteries serve as a key technology, establishing the advancement of energy storage devices and playing a vital role in the global shift toward sustainable and green energy. However, the growing demand for high capacity nickel (Ni)-rich lithium-ion batteries accelerates the optimization of their energy density. A high-mass loading electrode design is a promising strategy for enhancing the energy density of LIBs, enabling the improved performance for commercial applications. The factors that limit the rate capability of the high-mass loading electrode are associated with the underutilization of active materials and increased polarization, which can be further attributed to slow electronic/ionic transport within the electrode. In this work, the conductive networks and porous characteristics of the Ni-rich LiNiCoMnO (NCM811) cathode electrode is preciously tailored through the incorporation of multidimensional carbon conductive additives, facilitating enhanced electron transport and optimized porosity enhancing lithium-ion diffusion within the high-mass loading electrode. As a result, the NCM811 cathode electrode with dual-multidimensional conductive additives, such as carbon black and carbon nanofiber (CB + CNF), exhibits an outstanding performance, achieving a capacity retention of 94.8% over 100 cycles at 1 C. It is also observed that long-structured CNFs contributes significantly to the formation of efficient conductive networks in a high-mass loading thick electrode (∼23 mg cm) exhibiting excellent performance at 0.2 C. The simple yet fundamental principle uncovered through this work demonstrates that the integration of the dual-carbon system synergistically enhances the conductive networks and optimizes electrode porosity. This microstructural optimization effectively reduces Ohmic contact resistance, contributing to a significantly enhanced electrochemical performance.