Lithiophilic Modification of Self-Supporting Carbon-Based Hosts and Lithium Metal Plating/Stripping Behaviors

自支撑碳基主体材料的亲石改性及其锂金属沉积/剥离行为

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Abstract

Metallic lithium anodes possess the lowest redox potential (-3.04 V vs. SHE) and an ultra-high theoretical capacity (3860 mAh g(-1), 2061 mAh cm(-3)). However, during electrochemical cycling, lithium metal tends to plate unevenly, leading to the formation of lithium dendrites. Moreover, severe electrochemical corrosion occurs at the interface between metallic lithium and traditional copper foil current collectors. To address these issues, we selected corrosion-resistant carbon paper as a lithium metal host and modified a uniform distribution of silver nanoparticles and a F-doped amorphous carbon structure as a highly lithiophilic F-CP@Ag host to enhance lithium-ion transport kinetics and achieve improved affinity with lithium metal. The silver nanoparticles reduced the lithium nucleation energy barrier, while F doping resulted in a LiF-rich solid electrolyte interphase that better accommodated volume changes in lithium metal. These two strategies worked together to ensure uniform and stable lithium metal plating/stripping on the F-CP@Ag host. Consequently, under the conditions of 1 mA cm(-2) and 1 mAh cm(-2), the symmetric cell exhibited stable cycling with a polarization voltage of 8 mV for up to 1400 h. This work highlights the corrosion problem of lithium metal on traditional copper foil current collectors and provides guidance for the long-term cycling stability of lithium metal anodes.

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