Mitigating the Microcracks of High-Ni Oxides by <i>In</i> <i>Situ</i> Formation of Binder between Anisotropic Grains for Lithium-Ion Batteries

Increasing attention has been paid to layered high-Ni oxides with high capacity as a promising cathode for high-energy lithium-ion batteries. However, the undesirable microcracks in secondary particles usually occur due to the volume changes of anisotropic primary grains during cycles, which lead to the decay of electrochemical performance. Here, for the first time, a functional electrolyte with di-sec-butoxyaluminoxytriethoxysilane additive integrating the functions of silane and aluminate is proposed to in situ form the binder-like filler between anisotropic primary grains for mitigating the microcracks of high-Ni oxides. It is demonstrated that Li-containing aluminosilicate as a glue layer between the gaps of grains and as a coating layer on the surface of the grains is generated, and these features further enhance the interfacial bonding and surface stability of anisotropic primary grains. Consequently, the microcracks along with side reactions and phase transitions of high-Ni oxides are mitigated. As anticipated, the electrochemical performance and thermal stability of high-Ni oxides are improved, and there is also a capacity retention of 75.4% even after 300 cycles and large reversible capacity of ∼160 mA h g-1 at 5 C. The functional electrolyte offers a simple, efficient, and scalable method to promote the electrochemical properties and applicability of high-Ni oxide cathodes in high-energy lithium-ion batteries.