Enabling the high-voltage operation of layered ternary oxide cathodes via thermally tailored interphase

• Main Authors: Zhu, Zhiqiang, Cao, Shengkai, Ge, Xiang, Xi, Shibo, Xia, Huarong, Zhang, Wei, Lv, Zhisheng, Wei, Jiaqi, Chen, Xiaodong
• Other Authors: School of Materials Science and Engineering
• Format: Article
• Language: English
• Published: 2022
• Subjects: Engineering::Materials::Energy materials; Cathode/Electrolyte Interphase; Thermally-Tailored Interphase; Layered Ternary Oxides; High-Voltage Cathodes; Lithium-Ion Batteries
• Online Access: https://hdl.handle.net/10356/161486
• Institution: Nanyang Technological University

Layered ternary oxides LiNix Mny Coz O2 are promising cathode candidates for high-energy lithium-ion batteries (LIBs), but they usually suffer from the severe interfacial parasitic reactions at voltages above 4.3 V versus Li+ /Li, which greatly limit their practical capacities. Herein, using LiNi1/3 Mn1/3 Co1/3 O2 (NMC111) as the model system, a novel high-temperature pre-cycling strategy is proposed to realize its stable cycling in 3.0-4.5 V by constructing a robust cathode/electrolyte interphase (CEI). Specifically, performing the first five cycles of NMC111 at 55 °C helps to yield a uniform CEI layer enriched with fluorine-containing species, Li2 CO3 and poly(CO3 ), which greatly suppresses the detrimental side reactions during extended cycling at 25 °C, endowing the cell with a capacity retention of 92.3% at 1C after 300 cycles, far surpassing 62.0% for the control sample without the thermally tailored CEI. This work highlights the critical role of temperature on manipulating the interfacial properties of cathode materials, opening a new avenue for developing high-voltage cathodes for Li-ion batteries.