Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

Weijiang Xue, Mingjun Huang, Yutao Li, Yun Guang Zhu, Rui Gao, Xianghui Xiao, Wenxu Zhang, Sipei Li, Guiyin Xu, Yang Yu, Peng Li, Jeffrey Lopez, Daiwei Yu, Yanhao Dong (), Weiwei Fan, Zhe Shi, Rui Xiong, Cheng-Jun Sun, Inhui Hwang, Wah-Keat Lee, Yang Shao-Horn (), Jeremiah A. Johnson () and Ju Li ()
Additional contact information
Weijiang Xue: Massachusetts Institute of Technology
Mingjun Huang: Massachusetts Institute of Technology
Yutao Li: University of Texas at Austin
Yun Guang Zhu: Massachusetts Institute of Technology
Rui Gao: Massachusetts Institute of Technology
Xianghui Xiao: Brookhaven National Laboratory
Wenxu Zhang: Massachusetts Institute of Technology
Sipei Li: Massachusetts Institute of Technology
Guiyin Xu: Massachusetts Institute of Technology
Yang Yu: Massachusetts Institute of Technology
Peng Li: Massachusetts Institute of Technology
Jeffrey Lopez: Massachusetts Institute of Technology
Daiwei Yu: Massachusetts Institute of Technology
Yanhao Dong: Massachusetts Institute of Technology
Weiwei Fan: Massachusetts Institute of Technology
Zhe Shi: Massachusetts Institute of Technology
Rui Xiong: Massachusetts Institute of Technology
Cheng-Jun Sun: Argonne National Laboratory
Inhui Hwang: Argonne National Laboratory
Wah-Keat Lee: Brookhaven National Laboratory
Yang Shao-Horn: Massachusetts Institute of Technology
Jeremiah A. Johnson: Massachusetts Institute of Technology
Ju Li: Massachusetts Institute of Technology

Nature Energy, 2021, vol. 6, issue 5, 495-505

Abstract: Abstract By increasing the charging voltage, a cell specific energy of >400 W h kg−1 is achievable with LiNi0.8Mn0.1Co0.1O2 in Li metal batteries. However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi0.8Co0.1Mn0.1O2 with a cut-off voltage up to 4.7 V in Li metal batteries. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, stress-corrosion cracking, transition-metal dissolution and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to a compact morphology and low pulverization. Our lithium-metal battery delivers a specific capacity >230 mA h g−1 and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V lithium-metal battery can retain >88% capacity for 90 cycles, advancing practical lithium-metal batteries.

Date: 2021
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DOI: 10.1038/s41560-021-00792-y

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