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Lithium–sulfur (Li–S) batteries are widely regarded as some of the most promising next-generation energy storage systems due to their cost advantage and high theoretical energy density. However, the shuttle effect arising from the dissolution of polysulfides into organic electrolyte, the insulating nature of sulfur and their discharge products severely restrict the development of high-energy density Li–S batteries. Herein, a porous organic framework containing diketopyrrolopyrrole (DPP) building blocks is reasonably designed and it serves as a shuttle-inhibiting layer to bifunctionally increase the physical and chemical trapping of lithium polysulfides. The frameworks were synthesized through a bottom-up approach, allowing precise control of the network design at the molecular level. As a result, the framework-derived microscale networks with polar units effectively hinder the shuttle effect of polysulfides and promise …