Abstract

Lithium (Li) metal and alloy anodes are strongly attractive for next high-energy-density batteries, owing to their high theoretical specific capacity and low redox potentials. However, the fast electrode pulverization caused by large volume variation upon cycling inhibits the use of the Li metal and alloy anodes seriously, whereas the sluggish charge transfer and weak electrode/electrolyte interphase are mainly responsible for their uneven volume expansion and surface breaks, respectively. Herein, a versatile F–N–S doped lithiophilic interphase is obtained via a one-pot electrochemical fabrication process with high controllability, which exhibits high robustness, Li affinity and fast Li transfer, and significantly outperforms the single lithiophilic interphase obtained via chemical route. When this advanced interphase is applied to the copper or aluminum electrodes, great stabilizations of Li plating/stripping or Li insertion/extraction processes can be achieved. This work emphasizes the importance of the interphase composition for designing stable high-energy-density electrodes, and gives insights on a general and efficient remedy to boost the performances of the large-volume-change electrodes. • F–N–S doped lithiophilic interphases are fabricated via an electrochemical method. • The F–N–S doping enables fast Li transfer and high robustness of the interphase. • The advanced interphases improve the cycling stability of high-capacity anodes.

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