Abstract
Metallic lithium affords the highest theoretical capacity and lowest electrochemical potential and is viewed as a leading contender as an anode for high-energy-density rechargeable batteries. However, the poor wettability of molten lithium does not allow it to spread across the surface of lithiophobic substrates, hindering the production and application of this anode. Here we report a general chemical strategy to overcome this dilemma by reacting molten lithium with functional organic coatings or elemental additives. The Gibbs formation energy and newly formed chemical bonds are found to be the governing factor for the wetting behavior. As a result of the improved wettability, a series of ultrathin lithium of 10–20 μm thick is obtained together with impressive electrochemical performance in lithium metal batteries. These findings provide an overall guide for tuning the wettability of molten lithium and offer an affordable strategy for the large-scale production of ultrathin lithium, and could be further extended to other alkali metals, such as sodium and potassium.
Highlights
Metallic lithium affords the highest theoretical capacity and lowest electrochemical potential and is viewed as a leading contender as an anode for high-energy-density rechargeable batteries
The poor lithiophilicity of molten Li results in spherical Li beads rather than thin layers formed onto diverse substrates, including planar copper, foamed iron, foamed nickel, carbon fiber, and oxidized graphite, within the temperature range of 180–300 °C (Fig. 2a–f, Supplementary Movie 1)
This reaction dramatically improved the wettability of molten Li and formed ultrathin Li onto those lithiophobic substrates (Fig. 2h–l and Supplementary Movie 2–4)
Summary
Metallic lithium affords the highest theoretical capacity and lowest electrochemical potential and is viewed as a leading contender as an anode for high-energy-density rechargeable batteries. Spreading molten Li on Cu current collectors might be a promising strategy to realize the large-scale and low-cost preparation of ultrathin Li23–26 This method suffers from the poor wettability of molten Li on various substrates. A series of organic functional coatings can perfectly solve the poor wettability of molten Li. Many elemental additives that can react with molten Li can tune the surface energy of molten Li and facilitate the homogenous spreading of metallic Li on various substrates. Many elemental additives that can react with molten Li can tune the surface energy of molten Li and facilitate the homogenous spreading of metallic Li on various substrates Key parameters, such as ΔrG and newly formed chemical bonds, are found to be the governing factor for the improved wettability. The successful application of ultrathin Li anodes in rechargeable batteries highlights the importance of our strategy to improve the wettability of molten Li and further develop Li metal batteries toward next-generation energy storage systems
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