PNNL

Abstract

Lithium-sulfur (Li-S) battery is one of the most promising energy storage systems because of its high specific capacity of 1675 mAh g-1 based on sulfur. However, the rapid capacity degradation, mainly caused by polysulfide dissolution, remains a significant challenge prior to practical applications. Here, we report a novel Ni-based metal organic framework (Ni-MOF), Ni6(BTB)4(BP)3 (BTB = benzene-1,3,5-tribenzoate and BP = 4,4'-bipridyl), that can remarkably immobilize polysulfides within the cathode structure through physical and chemical interactions at the molecular level. The capacity retention achieves up to 89% after 100 cycles at 0.1 C. The interwoven mesopores (~2.8 nm) and micropores (~1.4 nm) of Ni-MOF firstly provide an ideal matrix to confine polysulfides. Additionally, the strong interactions between Lewis acidic Ni(II) center and the polysulfides base significantly slow down the migration of soluble polysulfides out of the pores, which leads to the excellent cycling performance of Ni-MOF/S composite.