Stable Lithium-Carbon Composite Enabled by Dual-Salt Additives

Highlights It is the first report that using dual-salt additives of LiPF6 and LiNO3 to significantly improve the cycling performance of the Li-CNT negative electrode.The mechanism why the combined use of LiPF6 and LiNO3 additive can improve the cycling performance and rate capability of the Li-CNT negative electrode was investigated.An average cycling Coulombic efficiency as high as 99.30% was obtained for the Li-CNT negative electrode at a current density of 2.5 mA cm−2 and an negative electrode to positive electrode capacity (N/P) ratio of 2. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-021-00633-3.
Lithium metal is regarded as the ultimate negative electrode material for secondary batteries due to its high energy density. However, it suffers from poor cycling stability because of its high reactivity with liquid electrolytes. Therefore, continuous efforts have been put into improving the cycling Coulombic efficiency (CE) to extend the lifespan of the lithium metal negative electrode. Herein, we report that using dual-salt additives of LiPF6 and LiNO3 in an ether solvent-based electrolyte can significantly improve the cycling stability and rate capability of a Li-carbon (Li-CNT) composite. As a result, an average cycling CE as high as 99.30% was obtained for the Li-CNT at a current density of 2.5 mA cm–2 and an negative electrode to positive electrode capacity (N/P) ratio of 2. The cycling stability and rate capability enhancement of the Li-CNT negative electrode could be attributed to the formation of a better solid electrolyte interphase layer that contains both inorganic components and organic polyether. The former component mainly originates from the decomposition of the LiNO3 additive, while the latter comes from the LiPF6-induced ring-opening polymerization of the ether solvent. This novel surface chemistry significantly improves the CE of Li negative electrode, revealing its importance for the practical application of lithium metal batteries. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-021-00633-3.