In situ inorganic conductive network formation in high-voltage single-crystal Ni-rich cathodes.

Fan, Xinming; Ou, Xing; Zhao, Wengao; Liu, Yun; Zhang, Bao; Zhang, Jiafeng; Zou, Lianfeng; Seidl, Lukas et al. · Nat Commun · 2021

basic_science · Level V

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Abstract

High nickel content in LiNi<sub>x</sub>Co<sub>y</sub>Mn<sub>z</sub>O<sub>2</sub> (NCM, x ≥ 0.8, x + y + z = 1) layered cathode material allows high specific energy density in lithium-ion batteries (LIBs). However, Ni-rich NCM cathodes suffer from performance degradation, mechanical and structural instability upon prolonged cell cycling. Although the use of single-crystal Ni-rich NCM can mitigate these drawbacks, the ion-diffusion in large single-crystal particles hamper its rate capability. Herein, we report a strategy to construct an in situ Li<sub>1.4</sub>Y<sub>0.4</sub>Ti<sub>1.6</sub>(PO<sub>4</sub>)<sub>3</sub> (LYTP) ion/electron conductive network which interconnects single-crystal LiNi<sub>0.88</sub>Co<sub>0.09</sub>Mn<sub>0.03</sub>O<sub>2</sub> (SC-NCM88) particles. The LYTP network facilitates the lithium-ion transport between SC-NCM88 particles, mitigates mechanical instability and prevents detrimental crystalline phase transformation. When used in combination with a Li metal anode, the LYTP-containing SC-NCM88-based cathode enables a coin cell capacity of 130 mAh g<sup>-1</sup> after 500 cycles at 5 C rate in the 2.75-4.4 V range at 25 °C. Tests in Li-ion pouch cell configuration (i.e., graphite used as negative electrode active material) demonstrate capacity retention of 85% after 1000 cycles at 0.5 C in the 2.75-4.4 V range at 25 °C for the LYTP-containing SC-NCM88-based positive electrode.