Suppressing gliding in Ni-rich single-crystal cathodes by defect engineering

Defect engineering has been used for centuries to enhance the mechanical strength of metals and alloys, but its application to cathodes remains largely unexplored. Conventional cathode synthesis aims for defect-free crystals to maximize capacity, but such structures degrade easily through interlayer gliding and microcracking, both of which are reported for single-crystal LiNi 0.8 Mn 0.1 Co 0.1 O 2 (SC-NMC811). Dopant substitution or surface coating has been explored to address these issues but introduce foreign elements that complicate recycling. Here, we present a scalable method to introduce a controlled amount (<5%) of Li/Ni anti-site defects that act as "rivets" to suppress interlayer gliding. This moderate defect level enhances the shear strength of SC-NMC811 by 88% and inhibits oxygen loss. The optimized cathodes retain 88.1% capacity after 1,800 cycles (4.3 V) and 80.1% after 900 cycles (4.7 V) using a standard carbonate-based electrolyte. This exceeds conventional SC-NMC811 cycling stability without relying on complicated synthesis procedures or introducing dopants that complicate the recycling process.