Xintao Zuo1, Mengmeng Zhen1,2 (*), and Cheng Wang1 (*)
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1 Tianjin Key Laboratory of Advanced Functional Porous Materials and Center for Electron Microscopy, Institute for New Energy Materials & Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300071, China 2 Tianjin Key Laboratory of Clean Energy and Pollution Control, School of Energy and Environmental Engineering, Hebei University of Technology, Tianjin 300401, China
Lithium-sulfur batteries (LSBs) have been regarded as one of the most promising energy storage systems to break through the upper limit of
lithium-ion batteries. However, the rampant diffusions of soluble lithium polysulfides (LiPSs) in the electrolyte induced the shuttle effect
between anode and cathode, resulting in low sulfur utilization, low energy efficiency and short cycling life. Herein, we prove the rational design
and construction of Ni nanoparticles filled in vertically grown N-doped bamboo-like carbon nanotubes (CNTs) on graphene nanosheets
(Ni@NG-CNTs) as efficient polysulfide barrier for high-performance LSBs. The unique design integrates graphene nanosheets and CNTs
into hierarchical architectures with one-dimensional (1D) CNTs, two-dimensional (2D) ultrathin nanosheets and abundant carbon nanocages.
This design provides large surface area for lithium polysulfides (LiPSs) adsorption, accelerates electron transport and enhances electrochemical
redox of LiPSs. Benefiting from the unique structural features, the LSBs with the Ni@NG-CNTs as polysulfide barrier keep high reversible
specific capacities of 309.1 and 265.0 mAh·g−1 at 5 and 10 C rates after 500 cycles. This work provides a new strategy for constructing
self-assembled hybrids of CNTs and graphene nanosheets with abundant carbon nanocages for high-performance LSBs.