High-Rate Ni-Rich Single-Crystal Cathodes with Highly Exposed {010} Active Planes Through In-Situ Zr Doping

Nickel (Ni)-rich cathodes with high energy density will play a crucial role in the rapidly growing electric vehicles sector. However, the large-scale application of Ni-rich cathodes is still limited by structural instability and severe capacity decay. Even though the construction design of single-crystal cathodes alleviates these defects, the sluggish lithium ion (Li + ) diffusion between the larger single-crystal particles restricts its rate performance. We propose an in-situ zirconium (Zr) ion doping strategy to modulate the primary particle morphology of precursors and obtain the single-crystal cathodes with highly exposed {010} planes after calcination. The high percentage of {010} planes will deliver more Li + diffusion channels and improved transportation kinetics. Moreover, the homogeneous doping of Zr inside the bulk phase will significantly suppress the anisotropic shrinkage of c-axis, maintain an intact internal structure and prevent the accumulation of rock-salt phases. As a result, the Zr-doped single-crystal cathode exhibits excellent cycling stability, whether at 25 ℃ or 45 ℃. More importantly, the rate performance of cathodes has been remarkably enhanced after Zr modification. At the ultra-high rate of 10 C, it can maintain a high specific capacity of 121.4 mAh g -1 (81.8% of capacity retention) after 250 cycles in the 3.0-4.3 V range.