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Our work provides insights into the interplay between the molecular structure of Li salts, their physicochemical properties and electrochemical performances. Under fast-cycling conditions (charging: 1.46 mA cm − 2, discharging: 3.66 mA cm − 2), pouch cells maintained 81% capacity after 100 cycles. Pouch cells of 310 Wh kg −1 achieved ~410 W kg −1 power density at the discharging current density of 6.59 mA cm −2. LiFEA-based carbonate electrolytes notably improved fast-cycling performances of Li | |NCM811 cells. It enables carbonate electrolytes with a large apparent donor number and Li + transference number and drives a self-cleaning mechanism for solid–electrolyte interphases, enhancing compatibility with Li-metal anodes even at high current densities. Herein we design an asymmetric Li salt, lithium 1,1,1-trifluoro- N-ethyl] methanesulfonamide (LiFEA) that possesses a pseudo-crown ether-like, folded molecular geometry. Conventional carbonate-based electrolytes with high corrosion towards Li metal result in massive dendrite growth and limited cycling life, particularly true for practical Li-metal batteries with high cathode loading (>3.5 mAh cm − 2).
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