Crepe Cake Structured Layered Double Hydroxide/Sulfur/Graphene as a Positive Electrode Material for Li-S Batteries

This work was financially supported by National Natural Science Foundation of China (Nos. 21975030 and 11674005), and the Ministry of Science and Technology of China (No. 2016YFB0700600 (National Materials Genome Project)). Solving the polysulfide shuttle problem is one of the core challenges for the industrialization of lithium–sulfur batteries. In this work, a triphasic composite of LDH/sulfur/rGO (LDH: layered double hydroxide, rGO: reduced graphene oxide) with a crepe cake like structure is designed and fabricated as a positive electrode material for lithium–sulfur batteries. Sulfur nanoparticles are embedded in the interlayer space of the composite and thus are well protected physically via three-dimensional wrapping and chemically via strong interaction of LDH nanoflakes with lithium polysulfides, such as ionic bonds and S···H hydrogen bonds. In addition, the flexible lamellar structure of the composite with soft graphene layers can tolerate the volume expansion of sulfur during lithiation as well as facilitate ionic permeability and electron transport, which is favorable for the redox reactions of polysulfide. The present work sheds light on the future development and industrialization of lithium–sulfur batteries. Postprint