Ultrathin Two-dimensional Layered Composite Carbosilicates from in situ Unzipped Carbon Nanotubes and Exfoliated Bulk Silica.

A key task in today's inorganic synthetic chemistry is to develop effective reactions, routes, and associated techniques aiming to create new functional materials with specifically desired multilevel structures and properties. Herein, we report an ultrathin two-dimensional layered composite of graphene ribbon and silicate via a simple and scalable one-pot reaction, which leads to the creation of a novel carbon-metal-silicate hybrid family: carbosilicate. The graphene ribbon is in situ formed by unzipping carbon nanotubes, while the ultrathin silicate is in situ obtained from bulk silica or commercial glass; transition metals (Fe or Ni) oxidized by water act as bridging agent, covalently bonding the two structures. The unprecedented structure combines the superior properties of the silicate and the nanocarbon, which triggers some specific novel properties. All processes during synthesis are complementary to each other. The associated synergistic chemistry could stimulate the discovery of a large class of more interesting, functionalized structures and materials.

Interface and Charge Induced Molecular Self-Assembly Strategy for the Synthesis of Reduced Graphene Oxide Coated with Mesoporous Platinum Sheets.

The design of porous noble metal catalysts holds great promise in various electrocatalytic applications. However, it is still a challenge to improve the durability performance through constructing stable framework. Here, an interface and charge induced strategy is developed to synthesize large-sized continuous reduced graphene oxide@mesoporous platinum (denoted as rGO@mPt) sheets under kinetic control by molecular self-assembly design. Graphene oxide (GO) is a promising large-sized growth interface for platinum. Cationic surfactant dioctadecyldimethylammonium chloride bridges the negatively charged GO and platinum precursors, while creating interconnected mesopores. The successful synthesis of rGO@mPt sheets relies on proper kinetic control, which is achieved by controlling pH, temperature, and the complexation of bromide ions. rGO@mPt sheets present strong crystallinity with a pure face-centered cubic Pt phase. Worm-like mesostructures with an average pore size of 2.2 nm exist throughout the sheets. rGO@mPt sheets possess both stable framework and abundant active sites, which markedly improve the durability on methanol oxidation reaction while maintaining relatively good catalytic activity. Long-term stability test shows a slight loss of 1.2% activity after 250 cycles. Amperometric i-t curves reveal the mass current three times higher compared to commercial Pt/C at 3000 s.