Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes

Abstract

Coupling thin Li metal anodes with high-capacity/high-voltage cathodes such as LiNi0.8Co0.1Mn0.1O2 (NCM811) is a promising way to increase lithium battery energy density. Yet, the realization of high-performance full cells remains a formidable challenge. Here, we demonstrate a new class of highly coordinated, nonflammable carbonate electrolytes based on lithium bis(fluorosulfonyl)imide (UFSI) in propylene carbonate/fluoroethylene carbonate mixtures. Utilizing an optimal salt concentr ation (4 M LiFSI) of the electrolyte results in a unique coordination structure of Li+-FSI-solvent cluster, which is critical for enabling the formation of stable interfaces on both the thin Li metal anode and high-voltage NCM811 cathode. Under highly demanding cell configuration and operating conditions (Li metal anode = 35 mu m, areal capacity/charge voltage of NCM811 cathode = 4.8 mAh cm(-2)/4 .6 V, and anode excess capacity [relative to the cathode] = 0.83), the Li metal-based full cell provides exceptional electrochemical performance (energy densities = 679 Wh kg(cell)(-1)/1,024 Wh L-cell(-1)) coupled with nonflammability.