To satisfy the increasing energy density requirements for electric vehicles and grid-scale energy storage systems, Ni-rich layered oxide cathode materials are often fabricated as micron-sized secondary spherical particles consisting of nanosized single crystals. Unfortunately, the hierarchical structure inevitably induces intergranular cracks and parasitic reactions at the cathode-electrolyte interphase, aggravating chemomechanical instability and seriously hindering their practical application. Here, we propose a nanowelding strategy to build consolidation points at the grain boundary of the primary particles, which dramatically enhances the capacity retention and chemomechanical stability. Meanwhile, the oxygen vacancies in the ceria-based solid electrolyte possessing oxygen adsorbing and storage capability can restrain the active oxygenates in the surficial lattice to avoid oxygen evolution. Experimental characterization further confirms that this unique architecture can effectively prevent the liquid electrolyte from penetrating into the active material along the grain boundary and consequently eliminate the adverse effects, including intergranular cracks, cathode electrolyte interface formation and growth, and the layered structure-rock salt phase irreversible transition. This finding provides a promising approach to realize the rapid commercialization of highly stabilized nickel-rich cathode materials for high-performance lithium-ion batteries.
Keywords: Ni-rich layered oxide cathode materials; chemomechanical instability; intergranular crack; nanowelding strategy; parasitic reactions.