Enhanced Chemisorption and Catalytic Effects toward Polysulfides by Modulating Hollow Nanoarchitectures for Long‐Life Lithium–Sulfur Batteries. Issue 4 (23rd December 2019) - Li, Zhonglin
Abstract: Hollow nanostructures with intricate interior and catalytic effects hold great promise for the construction of advanced lithium–sulfur batteries. Herein, a double‐shelled hollow polyhedron with inlaid cobalt nanoparticles encapsulated by nitrogen‐doped carbon (Co/NC) nanodots (Co‐NC@Co9 S8 /NPC) is reported, which is acquired by using imidazolium‐based ionic‐polymer‐encapsulated zeolitic imidazolate framework‐67 as a core‐shelled precursor. The Co/NC nanodots promote redox kinetics and chemical adsorbability toward polysulfides, while the interconnected double shells serve as a nanoscale electrochemical reaction chamber, which effectively suppresses the polysulfide shuttling and accelerates ion/electron transport. Benefiting from structural engineering and reaction kinetics modulation, the Co‐NC@Co9 S8 /NPC‐S electrode exhibits high cycling stability with a low capacity decay of 0.011% per cycle within 2000 cycles at 2 C. The electrode still shows high rate performance and cyclability over 500 cycles even in the case of high sulfur loading of 4.5 mg cm −2 and 75 wt% sulfur content. This work provides one type of new hollow nanoarchitecture for the development of advanced Li–S batteries and other energy storage systems. Abstract : A type of new hollow nanostructure consisting of interconnected double shells with metal‐containing nanodots in the interior voids is developed. The hollow nanostructure serves as a promising chamber for effective confinement of the diffusing polysulfides and electrochemical conversion of internal polysulfides, which endows lithium–sulfur batteries with excellent rate performance, high capacity, and long cycle life.