Affiliation: | 1. Department of Chemistry, Stanford University, Stanford, CA, 94305 USA;2. Department of Materials Science and Engineering Academy for Advanced Interdisciplinary Studies, Southern University of Science and Technology, Shenzhen, Guangdong, 518055 China;3. College of Electrical Engineering and Automation, Shandong University of Science and Technology, Qingdao, 266590 China;4. Department of Chemistry, Stanford University, Stanford, CA, 94305 USA
Department of Chemical Engineering, National Chung Cheng University, Chiayi, 62102 Taiwan;5. Department of Chemistry, Stanford University, Stanford, CA, 94305 USA
Institute of Materials Science and Engineering, National Central University, Taoyuan, 32001 Taiwan;6. Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031 China;7. Key Laboratory of Luminescence and Optical Information Ministry of Education, Department of Physics, School of Science, Beijing Jiaotong University, Beijing, 100044 China;8. Department of Chemical Engineering, National Chung Cheng University, Chiayi, 62102 Taiwan;9. Research Center for Applied Sciences, Academia Sinica, Taipei, 11529 Taiwan |
Abstract: | Rechargeable lithium metal batteries are next generation energy storage devices with high energy density, but face challenges in achieving high energy density, high safety, and long cycle life. Here, lithium metal batteries in a novel nonflammable ionic-liquid (IL) electrolyte composed of 1-ethyl-3-methylimidazolium (EMIm) cations and high-concentration bis(fluorosulfonyl)imide (FSI) anions, with sodium bis(trifluoromethanesulfonyl)imide (NaTFSI) as a key additive are reported. The Na ion participates in the formation of hybrid passivation interphases and contributes to dendrite-free Li deposition and reversible cathode electrochemistry. The electrolyte of low viscosity allows practically useful cathode mass loading up to ≈16 mg cm?2. Li anodes paired with lithium cobalt oxide (LiCoO2) and lithium nickel cobalt manganese oxide (LiNi0.8Co0.1Mn0.1O2, NCM 811) cathodes exhibit 99.6–99.9% Coulombic efficiencies, high discharge voltages up to 4.4 V, high specific capacity and energy density up to ≈199 mAh g?1 and ≈765 Wh kg?1 respectively, with impressive cycling performances over up to 1200 cycles. Highly stable passivation interphases formed on both electrodes in the novel IL electrolyte are the key to highly reversible lithium metal batteries, especially for Li–NMC 811 full batteries. |