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

Coupling thin Li metal anodes with high-capacity/high-voltage cathodes such as LiNi _0.8 Co _0.1 Mn _0.1 O ₂ (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 (LiFSI) in propylene carbonate/fluoroethylene carbonate mixtures. Utilizing an optimal salt concentration (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 μm, 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.
Competing Interests: Declaration of Interests The authors declare no competing interests.
(Copyright © 2020 The Author(s). Published by Elsevier Inc. All rights reserved.)