"Core-shell" cathodes for high performance Li-ion batteries

Li-rich or Ni-rich layered oxides are considered ideal cathode materials for high-energy Li-ion batteries (LIBs) owing to their high capacity (> 200 mAh g–1) and low cost. However, both are suffering from severe structural instability upon high-voltage cycling (> 4.5 V). In this work, “Li-rich Ni-rich” Li1.08Ni0.9Mn0.1O2 oxides with core-shell architecture are designed and synthesized to improve their cyclability at these high-voltages. These oxides are determined to be composed of a less reactive “Li-rich Mn-rich” shell and a high-capacity “Li-rich Ni-rich” core. As Li-ions gradually enter into the core-shell precursor during the high-temperature lithiation reaction, an interdiffusion of elements across the interphase between the Mn-rich shell and the Ni-rich core successively occurs. Such thermally-driven atomic interdiffusion could lead to a thickness- controllable “Li-rich Mn-rich” shell, which can guarantee an exceptional structural reversibility for the layered “Li-rich Ni-rich” core upon long-term cycling. As a consequence, the optimized core-shell  Li1.08Ni0.9Mn0.1O2 achieves a capacity retention of 96% at 0.1 C after 100 cycles in the voltage range of 2.7–4.6 V. These findings might open up a new avenue for rational design of advanced cathode materials for LIBs and beyond.


Dr. Nicola Casati
Beamline Scientist
PSI, Laboratory for Condensed Matter in the Photon Science Division
Forschungsstrasse 111, 5232 Villigen PSI, Switzerland
Telephone: +41 56 310 5346
E-mail: nicola.casati@psi.ch

Original Publication

Architecting “Li-rich Ni-rich” core-shell layered cathodes for high-energy Li-ion batteries

Z. Jing, S. Wang, Q. Fu, V. Baran, A. Tayal, N. Casati, A. Missyul, L. Simonelli, M. Knapp, F. Li, H. Ehrenberg, S. Indris, C. Sha, W. Hua

Energy Storage Materials 2023, 59, 102775