Variation of Electronic Conductivity within Secondary Particles Revealing a Capacity-Fading Mechanism of Layered Ni-Rich Cathode

Abstract

A remarkable reduction in electronic conductivity in the core region rather than on the surface of secondary particles is proposed as a capacity-fading mechanism of a Ni-rich cathode. This result is confirmed by analyzing the electronic conductivity of the secondary particles of Li[Ni0.98Co0.01Mn0.01]O2 using the scanning spreading resistance microscopy (SSRM) mode of atomic force microscopy. SSRM analysis reveals that a much thicker rocksalt phase, which is transformed from the original layered structure, on the surface of the primary particles in the core region electronically insulates the entire volume of the primary particles from the neighboring particles. Li intercalation–deintercalation is not achievable in the electronically insulated primary particles. Thus, visualization of the local electronic conductivity in the secondary particles confirms that the loss of electronic conductivity in the core region of the secondary particle is a key factor in the capacity fading of a Ni-rich cathode for lith...