Stabilizing electrode–electrolyte interfaces to realize high-voltage Li||LiCoO2 batteries by a sulfonamide-based electrolyte

Weijiang Xue; Rui Gao; Zhe Shi; Xianghui Xiao; Wenxu Zhang; Yirui Zhang; Yun Guang Zhu; Iradwikanari Waluyo; Yao Li; Megan R. Hill; Zhi Zhu; Sa Li; Oleg Kuznetsov; Yiman Zhang; Wah-Keat Lee; Adrian Hunt; Avetik Harutyunyan; Yang Shao-Horn; Jeremiah A. Johnson; Ju Li

doi:10.1039/D1EE01265G

Stabilizing electrode–electrolyte interfaces to realize high-voltage Li||LiCoO₂ batteries by a sulfonamide-based electrolyte†

Weijiang Xue,

‡*^a Rui Gao,‡^a Zhe Shi,^ab Xianghui Xiao,^c Wenxu Zhang,^d Yirui Zhang,

^e Yun Guang Zhu,

^f Iradwikanari Waluyo,

^c Yao Li,^g Megan R. Hill,^d Zhi Zhu,^a Sa Li,

^h Oleg Kuznetsov,ⁱ Yiman Zhang,ⁱ Wah-Keat Lee,^c Adrian Hunt,^c Avetik Harutyunyan,ⁱ Yang Shao-Horn,

*^bef Jeremiah A. Johnson

*^d and Ju Li

*^ab

Author affiliations

* Corresponding authors

^a Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
E-mail: xuewj@mit.edu, liju@mit.edu

^b Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
E-mail: shaohorn@mit.edu

^c National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973, USA

^d Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
E-mail: jaj2109@mit.edu

^e Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

^f Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

^g State Key Lab of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai 200240, China

^h Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai, China

ⁱ Honda Research Institute, USA, Inc., San Jose, California 95134, USA

Abstract

High-voltage lithium-metal batteries (LMBs) with LiCoO₂ (LCO) as the cathode have high volumetric and gravimetric energy densities. However, it remains a challenge for stable cycling of LCO >4.5 V_Li. Here we demonstrate that a rationally designed sulfonamide-based electrolyte can greatly improve the cycling stability at high voltages up to 4.7 V_Li by stabilizing the electrode–electrolyte interfaces (EEIs) on both the Li-metal anode (LMA) and high-voltage LCO cathode. With the sulfonamide-based electrolyte, commercial LCO cathodes retain 89% and 85% of their capacities after 200 and 100 cycles under high charging voltages of 4.55 V_Li and 4.6 V_Li, respectively, significantly outperforming traditional carbonate-based electrolytes. The surface degradation, impedance growth, and detrimental side reactions in terms of gas evolution and Co dissolution are well suppressed. Our work demonstrates a promising strategy for designing new electrolytes to realize high-energy Li||LCO batteries.

Energy & Environmental Science

Stabilizing electrode–electrolyte interfaces to realize high-voltage Li||LiCoO₂ batteries by a sulfonamide-based electrolyte†

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Stabilizing electrode–electrolyte interfaces to realize high-voltage Li||LiCoO₂ batteries by a sulfonamide-based electrolyte

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