A nitrogen-superdoped graphene with diamond-like interlayer bonds is obtained via the radical chemistry of fluorographene, affording a symmetric supercapacitor with an energy density of 200 W h L−1 at a power of 2.6 kW L−1 and 143 W h L−1 at 52 kW L−1.

Graphene decorated with isolated single atoms (SAs) offers new vista to magnetic and spintronic devices up to single-atom catalysts. While sp atoms can be efficiently bound to graphene, d-block atoms require anchoring groups to prevent nanoparticle formation. Identification of suitable binding sites is a challenging task because the interaction among graphene, anchoring groups and adatoms is very complex. Using density functional theory (DFT) we explored strength and nature of interactions of graphene covalently functionalized by − OH, − CN, − F, and − H groups as anchors for Pt SAs. Both theory and experiment showed that − CN groups acted as suitable ligand enabling immobilization of 3.7 wt % single Pt adatoms. The findings imply that CN functionalized graphene, i.e., cyanographene, is a perspective material for anchoring metal adatoms with potential implications as single-atom-catalysts.

Stabilization of ferromagnetic ordering in graphene-based systems up to room temperature remains an important challenge owing to huge scope for applications in electronics, spintronics, biomedicine, and separation technologies. To date, several strategies have been proposed, including edge engineering, introduction of defects and dopants, and covalent functionalization. However, these techniques are usually hampered by limited temperature sustainability of ferromagnetic ordering. Here, we describe a method for the well-controlled sp 3 functionalization of graphene to synthesize zig-zag conjugated sp 2 carbon chains that can act as communication pathways among radical motifs. Zig-zag sp 2 /sp 3 patterns in the basal plane were clearly observed by high-resolution scanning transmission electron microscopy and provided a suitable matrix for stabilization of ferromagnetic ordering up to room temperature due to combined contributions of itinerant π-electrons and superexchange interactions. The results highlight the principal role of sp 2 /sp 3 ratio and super-organization of radical motifs in graphene for generating room temperature non-metallic magnets. KEYWORDS: hydroxofluorographene • fluorographene • magnetic carbon • hydroxyl • DFT calculations • density of states • 2D magnets • spintronicsGraphene, a two-dimensional (2D) layer of sp 2 -bonded carbon atoms arranged in hexagons, has attracted continuous attention of the scientific community over the past decade owing to its exceptional mechanical, electric, transport, and optical properties, which stem from its peculiar atomic organization and electronic structure. 1,2 It has been successfully tested in or proposed for a broad spectrum of applications 3 in various fields, such as electronics, 4 generation and storage of energy, 5,6 optics, 7 medicine, 8 printing technologies, 9 treatment of the environment, 10 and mechanical reinforcements. 11 However, despite its unique physical features, several drawbacks have been identified that hamper its use for specific processes and utilization. They include its high hydrophobicity, zero bandgap, and lack of magnetic response. In many cases, functionalization has been shown to be an effective strategy for overcoming these drawbacks. 12 For instance, it has been used to synthetize a number of graphene derivatives, such as graphene oxide, 13 graphane, 14 fluorographene 15,16 and other halogenated graphenes, 17 thiographene, 18 cyanographene, 19 graphene acid 19,20 and hydroxographene, 21 significantly extending the application potential of graphene-based materials and providing attractive/competitive alternatives in fields where pristine graphene fails.More than two decades ago, it was theoretically suggested that in a single layer of graphite, intrinsically diamagnetic, localized magnetic moments may emerge if an sp 3 -type defect is formed in the hexagonal carbon lattice. Since the first isolation of graphene in 2004, 1 the introduction of defects has become accepted as a promising way to endow graphene with magnetic proper...

Fluorinated graphenes (FGs) are key precursors for the synthesis of many graphene derivatives that significantly expand the application potential of graphene-based materials. The reactivity of FGs is rather surprising because the C−F bond is considered to be one of the strongest single covalent bonds in organic chemistry. However, its strength in FGs varies from 25.6 to 118.2 kcal/mol, depending on the configuration of fluorine ad-atoms. This variability is reflected in the formation of specific structural motifs and topological features during fluorination and defluorination processes; whereas defluorination favors formation of π-conjugated chains, following the path of the weakest C−F bonds, fluorination is driven both by thermodynamics and stochasticity, leading to diverse fluorination patterns. Individual motifs vary in their electronic structures, having either metallic or semiconducting character. We rationalize the complex 2D chemistry of FGs using empirical rules that predict the structural and underlying electronic/magnetic properties of these materials.