A High Conductivity 1D pi-d Conjugated Metal-Organic Framework with Efficient Polysulfide Trapping-Diffusion-Catalysis in Lithium-Sulfur Batteries

The shuttling behavior and sluggish conversion kinetics of the intermediate lithium polysulfides (LiPS) represent the main obstructions to the practical application of lithium-sulfur batteries (LSBs). Herein, a 1D pi-d conjugated metal-organic framework (MOF), Ni-MOF-1D, is presented as an efficient sulfur host to overcome these limitations. Experimental results and density functional theory calculations demonstrate that Ni-MOF-1D is characterized by a remarkable binding strength for trapping soluble LiPS species. Ni-MOF-1D also acts as an effective catalyst for S reduction during the discharge process and Li2S oxidation during the charging process. In addition, the delocalization of electrons in the pi-d system of Ni-MOF-1D provides a superior electrical conductivity to improve electron transfer. Thus, cathodes based on Ni-MOF-1D enable LSBs with excellent performance, for example, impressive cycling stability with over 82% capacity retention over 1000 cycles at 3 C, superior rate performance of 575 mAh g(-1) at 8 C, and a high areal capacity of 6.63 mAh cm(-2) under raised sulfur loading of 6.7 mg cm(-2). The strategies and advantages here demonstrated can be extended to a broader range of pi-d conjugated MOFs materials, which the authors believe have a high potential as sulfur hosts in LSBs.