Graphene, despite being the best known strong and electrical/thermal conductive material, has found limited success in practical applications, mostly due to difficulties in the formation of desired large-scale highly organized structures. Our discovery of a liquid crystalline phase formation in graphene oxide dispersion has enabled a broad spectrum of highly aligned graphene-based structures, including films, fibers, membranes, and mesoscale structures. In this review, the current understanding of the structure-property relationship of graphene oxide liquid crystals (GOLCs) is overviewed. Various synthetic methods and parameters that can be optimized for GOLC phase formation are highlighted. Along with the results from different characterization methods for the identification of the GOLC phases, the typical characteristics of different types of GOLC phases introduced so far, including nematic, lamellar and chiral phases, are carefully discussed. Finally, various interesting applications of GOLCs are outlined together with the future prospects for their further developments.

Inspired by mussel adhesive polydopamine (PDA), effective reinforcement of graphene-based liquid crystalline fibers to attain high mechanical and electrical properties simultaneously is presented. The two-step defect engineering, relying on bioinspired surface polymerization and subsequent solution infiltration of PDA, addresses the intrinsic limitation of graphene fibers arising from the folding and wrinkling of graphene layers during the fiber-spinning process. For a clear understanding of the mechanism of PDA-induced defect engineering, interfacial adhesion between graphene oxide sheets is straightforwardly analyzed by the atomic force microscopy pull-off test. Subsequently, PDA could be converted into an N-doped graphitic layer within the fiber structure by a mild thermal treatment such that mechanically strong fibers could be obtained without sacrificing electrical conductivity. Bioinspired graphene-based fiber holds great promise for a wide range of applications, including flexible electronics, multifunctional textiles, and wearable sensors.

We report graphene@polymer core-shell fibers (G@PFs) composed of N and Cu codoped porous graphene fiber cores uniformly coated with semiconducting polymer shell layers with superb electrochemical characteristics. Aqueous/organic interface-confined polymerization method produced robust highly crystalline uniform semiconducting polymer shells with high electrical conductivity and redox activity. When the resultant core-shell fibers are utilized for fiber supercapacitor application, high areal/volume capacitance and energy densities are attained along with long-term cycle stability. Desirable combination of mechanical flexibility, electrochemical properties, and facile process scalability makes our G@PFs particularly promising for portable and wearable electronics.

Phosphorene, a newly emerging graphene analogous 2D elemental material of phosphorous atoms, is unique on the grounds of its natural direct band gap opening, highly anisotropic and extraordinary physical properties. This review highlights the current status of phosphorene research in energy and catalytic applications. The initial part illustrates the typical physical properties of phosphorene, which successfully bridge the prolonged gap between graphene and 2D metal chalcogenides. Various synthetic methods available for black phosphorus (BP) and the exfoliation/growth techniques for single to few-layer phosphorene are also overviewed. The latter part of this review details the working mechanisms and performances of phosphorene/BP in batteries, supercapacitors, photocatalysis, and electrocatalysis. Special attention has been paid to the research efforts to overcome the inherent shortcomings faced by phosphorene based devices. The relevant device performances are compared with graphene and 2D metal chalcogenides based counterparts. Furthermore, the underlying mechanism behind the unstable nature of phosphorene under ambient condition is discussed along with the various approaches to avoid ambient degradation. Finally, comments are offered for the future prospective explorations and outlook as well as challenges lying in the road ahead for phosphorene research.

Cost effective scalable method for uniform film formation is highly demanded for the emerging applications of 2D transition metal dichalcogenides (TMDs). We demonstrate a reliable and fast interfacial self-assembly of TMD thin films and their heterostructures. Large-area 2D TMD monolayer films are assembled at air-water interface in a few minutes by simple addition of ethyl acetate (EA) onto dilute aqueous dispersions of TMDs. Assembled TMD films can be directly transferred onto arbitrary nonplanar and flexible substrates. Precise thickness controllability of TMD thin films, which is essential for thickness-dependent applications, can be readily obtained by the number of film stacking. Most importantly, complex structures such as laterally assembled 2D heterostructures of TMDs can be assembled from mixture solution dispersions of two or more different TMDs. This unusually fast interfacial self-assembly could open up a novel applications of 2D TMD materials with precise tunability of layer number and film structures.