In Situ Mg/MgO-Embedded Mesoporous Carbon Derived from Magnesium 1,4-Benzenedicarboxylate Metal Organic Framework as Sustainable Li-S Battery Cathode Support.

Abstract

Development of advanced carbon cathode support with the ability to accommodate high sulfur (S) content as well as effective confinement of the sulfur species during charge–discharge is of great importance for sustenance of Li–S battery. A facile poly(vinylpyrrolidone)-assisted solvothermal method is reported here to prepare Mg–1,4-benzenedicarboxylate metal organic framework (MOF) from which mesoporous carbon is derived by thermal treatment, where the hexagonal sheetlike morphology of the parent MOF is retained. Existence of abundant pores of size 4 and 9 nm extended in three dimensions with zigzag mazelike channels helps trapping of S in the carbon matrix through capillary effect, resulting in high S loading. When tested as a cathode for lithium–sulfur battery, a reversible specific capacity of 1184 mAh g–1 could be achieved at 0.02 C. As evidenced by X-ray photoelectron spectroscopy, in situ generated Mg in the carbon structure enhances the conductivity, whereas MgO provides support to S immobilization through chemical interactions between Mg and sulfur species for surface polarity compensation, restricting the dissolution of polysulfide into the electrolyte, the main cause for the “shuttle phenomenon” and consequent capacity fading. The developed cathode shows good electrochemical stability with reversible capacities of 602 and 328 mAh g–1 at 0.5 and 1.0 C, respectively, with retentions of 64 and 67% after 200 cycles. The simple MOF-derived strategy adopted here would help design new carbon materials for Li–S cathode support.