To enable further development of Ni-rich LiNixMnyCo1−x−yO2 (NMC, x ≥ 0.9) cathodes for commercial applications, fundamental understanding of the synthesis–property–performance relationships in the LiNiO2 (LNO) parent phase is essential. In the present study, we report synthesis approaches to produce well-formed, similar-sized single-crystal LiNiO2 (SC-LNO) with different shapes and dominating surface facets, and reveal the dependence of cathode rate performance and cycling stability on particle morphology and surface. While octahedron-shaped SC-LNO with the (012) surface shows better rate capability and improved ability in utilizing the kinetically slow anodic process in the 3.5 V region, cubic-shaped SC-LNO with the (104) surface delivers superior cycling stability, especially upon cycling at a high upper cutoff voltage of 4.6 V. Improvement in cycling stability is correlated with reduced surface reconstruction and preferential LiF formation through the interaction with the electrolyte on the (104) surface. Our study not only demonstrates the importance of particle morphology and surface design, it also provides key insights into desirable material properties for developing future LNO-based cathode materials with better performance.
BT - Journal of Materials Chemistry A DA - 06/2022 DO - 10.1039/D2TA02492F IS - 24 LA - eng N2 -To enable further development of Ni-rich LiNixMnyCo1−x−yO2 (NMC, x ≥ 0.9) cathodes for commercial applications, fundamental understanding of the synthesis–property–performance relationships in the LiNiO2 (LNO) parent phase is essential. In the present study, we report synthesis approaches to produce well-formed, similar-sized single-crystal LiNiO2 (SC-LNO) with different shapes and dominating surface facets, and reveal the dependence of cathode rate performance and cycling stability on particle morphology and surface. While octahedron-shaped SC-LNO with the (012) surface shows better rate capability and improved ability in utilizing the kinetically slow anodic process in the 3.5 V region, cubic-shaped SC-LNO with the (104) surface delivers superior cycling stability, especially upon cycling at a high upper cutoff voltage of 4.6 V. Improvement in cycling stability is correlated with reduced surface reconstruction and preferential LiF formation through the interaction with the electrolyte on the (104) surface. Our study not only demonstrates the importance of particle morphology and surface design, it also provides key insights into desirable material properties for developing future LNO-based cathode materials with better performance.
PY - 2022 SP - 12890 EP - 12899 ST - J. Mater. Chem. A T2 - Journal of Materials Chemistry A TI - Improving LiNiO2 cathode performance through particle design and optimization UR - http://xlink.rsc.org/?DOI=D2TA02492F VL - 10 SN - 2050-7488 ER -