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We develop a novel microtemplate strategy to prepare unique carbon aerogels. The designed cathode materials present excellent electrochemical performance.

A carbon aerogel composite modified with ZnS (ZnS-CA) was successfully prepared through a simple in situ synthesis and used as a cathode for lithium-sulfur batteries. The nanopore ZnS-CA composites with a high specific surface area and rich mesoporous structure exhibit stronger adsorption and immobilization ability for polysulfides. The ZnS-CA/S cathode materials offer excellent electrochemical performances with lasting cycling stability and high specific capacity. In particular, the 6ZnS-CA/S sample achieves an initial capacity of 1352 mAh g À 1 at 0.2 C and maintains a high capacity of 1119 mAh g À 1 after 100 cycles. Furthermore, after 300 long cycles, it still maintains a high capacity of 730 mAh g À 1 at 1 C. These excellent performance features are attributed to the strong affinity of ZnS for Li 2 S n species, thus polysulfide shuttling can be effectively inhibited from the cathode source. Furthermore, the strong adsorption energy between ZnS and polysulfides was validated by using first-principles theory calculations, which reveals the anchoring and catalytic mechanism.