Journal
NANO RESEARCH
Volume 16, Issue 3, Pages 3855-3863Publisher
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-4852-y
Keywords
liquid electrolyte; high nickel ternary cathode; wide temperature; interface; sheath structure
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In this study, a new local high-concentration sulfolane-based electrolyte (DLi) is proposed, which can be stably applied to high nickel ternary cathode in a wide operating temperature range, improving the high-temperature storage performance and capacity retention of the battery.
An adequate wide temperature electrolyte for high nickel ternary cathode is urgent to further develop high energy density batteries. Herein, a comprehensive double-salt local high-concentration sulfolane-based electrolyte (DLi) is proposed with specific sheath structure to build stable interface on the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode at wide operating temperature between -60 and 55 degrees C. Lithium perchlorate (LiClO4) in combination with high concentration lithium bis-(trifluoromethanesulfonyl) imide (LiTFSI) strengthens the internal interaction between anion and cation in the solvation structure, increasing Li+ transference number of the electrolyte to 0.61. Moreover, the structure and component characteristics of the passive interface layer on NCM811 are modulated, decreasing desolvation energy of Li+ ions, benefiting Li+ transport dynamics especially at low temperature, and also ensuring the interfacial stability at a wide operating temperature range. As a result, the cathode with DLi exhibits excellent high-temperature storage performance and high capacity retention of 80.5% in 100 cycles at 55 degrees C. Meanwhile, the Li parallel to NCM811 cells can deliver high discharge capacity of 160.1, 136.1, and 110.3 mAh.g(-1) under current density of 0.1 C at -20, -40, and -60 degrees C, maintaining 84.5%, 71.8%, and 58.2% of the discharge capacity at 30 degrees C, respectively. Moreover, it enables NCM811 cathode to achieve a reversible capacity of 142.8 mAh.g(-1) in 200 cycles at -20 degrees C and 0.2 C. Our studies shed light on the molecular strategy of wide operational temperature electrolyte for high nickel ternary cathode.
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