Molecularly Imprinted Polymer Enables High-Efficiency Recognition and Trapping Lithium Polysulfides for Stable...

Using molecularly imprinted polymer to recognize various target molecules emerges as a fascinating research field. Herein, we applied this strategy for the first time to efficiently recognize and trap long-chain polysulfides (Li₂S_x, x = 6-8) in lithium sulfur battery to minimize the polysulfide shuttling between anode and cathode, which enables us to achieve remarkable electrochemical performance including a high specific capacity of 1262 mAh g^-1 at 0.2 C and superior capacity retention of over 82.5% after 400 cycles at 1 C. The outstanding performance is attributed to the significantly reduced concentration of long-chain polysulfides in electrolyte as evidenced by in situ UV/vis spectroscopy and Li₂S nucleation tests, which were further confirmed by density functional theory calculations. The molecular imprinting is demonstrated as a promising approach to effectively prevent the free diffusion of long-chain polysulfides, providing a new avenue to efficiently recognize and trap lithium polysulfides for high-performance lithium sulfur battery with greatly suppressed shuttle effect.