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Selective Permeable Lithium-ion Channels on Lithium Metal for Practical Lithium-Sulfur Pouch Cells.

Lithium metal batteries are considered a promising candidate for high-energy-density energy storage. However, the strong reducibility of lithium and highly reactivity when contacting oxidants, such as lithium polysulfides in lithium-sulfur batteries, caused by the serious "shuttle effect" and leads to low Coulombic efficiency. Herein we design selectively permeable lithium-ion channels on lithium metal surface, which allow lithium ions to pass through by electrochemical overpotential, while the polysulfides are effectively blocked due to the much larger steric hindrance than lithium ions. The selective permeation of lithium ion through the channels is further elucidated by the molecular simulation and visualization experiment. Consequently, a prolonged cycle life of 75 cycles and high Coulombic efficiency of 99% are achieved in a practical Li-S pouch cell with limited amounts of lithium and electrolyte, confirming the unique role the selective ion permeation plays in protecting highly reactive alkali metal anodes in working batteries.