Abstract
Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithium-metal anode in a reversible manner. Considerable attention has been focused on inhibiting dendrite via interface and electrolyte engineering, while admitting electrolyte-lithium metal reactivity as a thermodynamic inevitability. Here, we report the effective suppression of such reactivity through a nano-porous separator. Calculation assisted by diversified characterizations reveals that the separator partially desolvates Li+ in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li0-deposition occurs. The consequence of such deactivation is realizing dendrite-free lithium-metal electrode, which even retaining its metallic lustre after long-term cycling in both Li-symmetric cell and high-voltage Li-metal battery with LiNi0.6Mn0.2Co0.2O2 as cathode. The discovery that a nano-structured separator alters both bulk and interfacial behaviors of electrolytes points us toward a new direction to harness lithium-metal as the most promising anode.
Highlights
Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithiummetal anode in a reversible manner
Attempts to harness Li0 have been prevented by its extreme reactivity with electrolytes, especially those based on carbonate solvents, which leads to low Coulombic efficiency (CE) and dangerous morphologies such as dendritic and dead Li0 3,4
A uniform nano-porous membrane is synthesized from a multi-vinyl functionalized cluster (Supplementary Fig. 1), the metal-organic cluster consisting of a Zr6O4(OH)[4] core with 12 methacrylic acid (MAA) ligands (Fig. 1a)
Summary
Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithiummetal anode in a reversible manner. We found both Zr-MOC@PP-2 and Zr-MOC@PP-3 separators showed no obvious effect in suppressing lithium dendrite and parasitic reactions
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