Abstract

Exploring multifunctional sulfur host materials with high immobilization ability and catalytic activity is of great significance for realizing high-performance Lithium-sulfur (Li–S) batteries. Recently, cellulose nanocrystals (CNCs) receive extensive attention for advanced energy storage applications owing to their intrinsically exceptional physical/chemical properties and natural abundance. Herein, a highly dispersed cobalt clusters/nanoparticles embedded into CNC derived carbon aerogel composite (CA/Co-2) is for the first time synthesized. Benefiting from the interconnected hierarchical porous structure, homogeneously anchored Co clusters/nanoparticles and N-doped species, the designed CA/Co-2 could enable rapid electron/ion transport, efficient sulfur utilization, effective suppression of the shuttle effect and fast catalytic conversion of polysulfides, thereby contributing to outstanding electrochemical performance. Consequently, CA/Co-2@S cathode delivers high initial discharge capacity (1553.1 mAh g−1 at 0.1C) and superior cycle stability. Moreover, a remarkable rate performance of 681.4 mAh g−1 at 5.0C and exceptional long-term cycling stability with an ultralow capacity decay of 0.028 % per cycle at 5.0C over 1000 cycles could be achieved when coupled with carbon paper interlayer. This work develops a workable strategy for fabricating multifunctional sulfur host derived from the fascinating bio-nanomaterial of CNC, which provides valuable guidance for the future design of high-performance Li–S batteries.

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