All-Graphitic Multilaminate Mesoporous Membranes by Interlayer-Confined Molecular Assembly.

Layered mesostructured graphene, which combines the intrinsic advantages of planar graphene and mesoporous materials, has become interestingly important for energy storage and conversion applications. Here, an interlayer-confined molecular assembly method is presented for constructing all-graphitic multilaminate membranes (MMG⊂rGO), which are composed of monolayer mesoporous graphene (MMG) sandwiched between reduced graphene oxide (rGO) sheets. Hybrid assembly of iron-oleate complexes and organically modified GO sheets enables the preferential assembly of iron-oleate precursors at the interlayer space of densely stacked GO, driven by the like-pair molecular van der Waals interactions. Confined pyrolysis of iron-oleate complexes at GO interlayers leads to close-packed, carbon-coated Fe O nanocrystal arrays, which serve as intermediates to template the subsequent formation of MMG⊂rGO membranes. To demonstrate their application potentials, MMG⊂rGO membranes are exploited as dual-functional interlayers to boost the performance of Li-S batteries by concurrently suppressing the shuttle of polysulfides and the growth of Li dendrites. This work showcases the capability of molecular-based hybrid assembly for synthesizing multilayer mesostructured graphene with high packing density and its use in electrochemical energy applications.