Yuxi Xu

Flexible Graphene Films via the Filtration of Water-Soluble Noncovalent Functionalized Graphene Sheets

Flexible graphene films were prepared by the filtration of water-soluble noncovalently functionalized graphene sheets with pyrenebutyrate. The work presented here will not only open a new way for preparing water-soluble graphene dispersions but also provide a general route for fabricating conducting films based on graphene.

Self-Assembled Graphene Hydrogel via a One-Step Hydrothermal Process

Self-assembly of two-dimensional graphene sheets is an important strategy for producing macroscopic graphene architectures for practical applications, such as thin films and layered paperlike materials. However, construction of graphene self-assembled macrostructures with three-dimensional networks has never been realized. In this paper, we prepared a self-assembled graphene hydrogel (SGH) via a convenient one-step hydrothermal method. The SGH is electrically conductive, mechanically strong, and thermally stable and exhibits a high specific capacitance. The high-performance SGH with inherent biocompatibility of carbon materials is attractive in the fields of biotechnology and electrochemistry, such as drug-delivery, tissue scaffolds, bionic nanocomposites, and supercapacitors.

Supercapacitors Based on Flexible Graphene/Polyaniline Nanofiber Composite Films

Composite films of chemically converted graphene (CCG) and polyaniline nanofibers (PANI-NFs) were prepared by vacuum filtration the mixed dispersions of both components. The composite film has a layered structure, and PANI-NFs are sandwiched between CCG layers. Furthermore, it is mechanically stable and has a high flexibility; thus, it can be bent into large angles or be shaped into various desired structures. The conductivity of the composite film containing 44% CCG (5.5 x 10(2) S m(-1)) is about 10 times that of a PANI-NF film. Supercapacitor devices based on this conductive flexible composite film showed large electrochemical capacitance (210 F g(-1)) at a discharge rate of 0.3 A g(-1). They also exhibited greatly improved electrochemical stability and rate performances.

Flexible Solid-State Supercapacitors Based on Three-Dimensional Graphene Hydrogel Films

Flexible solid-state supercapacitors are of considerable interest as mobile power supply for future flexible electronics. Graphene or carbon nanotubes based thin films have been used to fabricate flexible solid-state supercapacitors with high gravimetric specific capacitances (80-200 F/g), but usually with a rather low overall or areal specific capacitance (3-50 mF/cm(2)) due to the ultrasmall electrode thickness (typically a few micrometers) and ultralow mass loading, which is not desirable for practical applications. Here we report the exploration of a three-dimensional (3D) graphene hydrogel for the fabrication of high-performance solid-state flexible supercapacitors. With a highly interconnected 3D network structure, graphene hydrogel exhibits exceptional electrical conductivity and mechanical robustness to make it an excellent material for flexible energy storage devices. Our studies demonstrate that flexible supercapacitors with a 120 μm thick graphene hydrogel thin film can exhibit excellent capacitive characteristics, including a high gravimetric specific capacitance of 186 F/g (up to 196 F/g for a 42 μm thick electrode), an unprecedented areal specific capacitance of 372 mF/cm(2) (up to 402 mF/cm(2) for a 185 μm thick electrode), low leakage current (10.6 μA), excellent cycling stability, and extraordinary mechanical flexibility. This study demonstrates the exciting potential of 3D graphene macrostructures for high-performance flexible energy storage devices.

Three-dimensional self-assembly of graphene oxide and DNA into multifunctional hydrogels.

Graphene and its functionalized derivatives are unique and versatile building blocks for self-assembly to fabricate graphene-based functional materials with hierarchical microstructures. Here we report a strategy for three-dimensional self-assembly of graphene oxide sheets and DNA to form multifunctional hydrogels. The hydrogels possess high mechanical strength, environmental stability, and dye-loading capacity, and a exhibit self-healing property. This study provides a new insight for the assembly of functionalized graphene with other building blocks, especially biomolecules, which will help rational design and preparation of hierarchical graphene-based materials.

Holey graphene frameworks for highly efficient capacitive energy storage

Supercapacitors represent an important strategy for electrochemical energy storage, but are usually limited by relatively low energy density. Here we report a three-dimensional holey graphene framework with a hierarchical porous structure as a high-performance binder-free supercapacitor electrode. With large ion-accessible surface area, efficient electron and ion transport pathways as well as a high packing density, the holey graphene framework electrode can deliver a gravimetric capacitance of 298 F g(-1) and a volumetric capacitance of 212 F cm(-3) in organic electrolyte. Furthermore, we show that a fully packaged device stack can deliver gravimetric and volumetric energy densities of 35 Wh kg(-1) and 49 Wh l(-1), respectively, approaching those of lead acid batteries. The achievement of such high energy density bridges the gap between traditional supercapacitors and batteries, and can open up exciting opportunities for mobile power supply in diverse applications.

Chemically Converted Graphene Induced Molecular Flattening of 5,10,15,20-Tetrakis(1-methyl-4-pyridinio)porphyrin and Its Application for Optical Detection of Cadmium(II) Ions

Complexation of cationic 5,10,15,20-tetrakis(1-methyl-4-pyridinio)porphyrin (TMPyP) and negatively charged chemically converted graphene (CCG) sheets was performed by simply mixing the diluted aqueous solutions of both components. During this process, a large bathochromic shift of porphyrin Soret band from 421 to 458 nm was observed, which is attributed to the flattening of TMPyP molecules induced by CCG through electrostatic and pi-pi stacking cooperative interactions. Furthermore, the coordination reaction between TMPyP and Cd(2+) ions was greatly accelerated from 20 h to 8 min under ambient conditions by introducing CCG sheets. On the basis of this phenomenon, we used the complex of TMPyP and CCG as an optical probe for rapid and selective detection of Cd(2+) ions in aqueous media.

Functionalized Graphene Hydrogel‐Based High‐Performance Supercapacitors

Functionalized graphene hydrogels are prepared by a one-step low-temperature reduction process and exhibit ultrahigh specific capacitances and excellent cycling stability in the aqueous electrolyte. Flexible solid-state supercapacitors based on functionalized graphene hydrogels are demonstrated with superior capacitive performances and extraordinary mechanical flexibility.

Self-Assembled Three-Dimensional Graphene Macrostructures: Synthesis and Applications in Supercapacitors

Graphene and its derivatives are versatile building blocks for bottom-up assembly of advanced functional materials. In particular, with exceptionally large specific surface area, excellent electrical conductivity, and superior chemical/electrochemical stability, graphene represents the ideal material for various electrochemical energy storage devices including supercapacitors. However, due to the strong π-π interaction between graphene sheets, the graphene flakes tend to restack to form graphite-like powders when they are processed into practical electrode materials, which can greatly reduce the specific surface area and lead to inefficient utilization of the graphene layers for electrochemical energy storage. The self-assembly of two-dimensional graphene sheets into three-dimensional (3D) framework structures can largely retain the unique properties of individual graphene sheets and has recently garnered intense interest for fundamental investigations and potential applications in diverse technologies. In this Account, we review the recent advances in preparing 3D graphene macrostructures and exploring them as a unique platform for supercapacitor applications. We first describe the synthetic strategies, in which reduction of a graphene oxide dispersion above a certain critical concentration can induce the reduced graphene oxide sheets to cross-link with each other via partial π-π stacking interactions to form a 3D interconnected porous macrostructure. Multiple reduction strategies, including hydrothermal/solvothermal reduction, chemical reduction, and electrochemical reduction, have been developed for the preparation of 3D graphene macrostructures. The versatile synthetic strategies allow for easy incorporation of heteroatoms, carbon nanomaterials, functional polymers, and inorganic nanostructures into the macrostructures to yield diverse composites with tailored structures and properties. We then summarize the applications of the 3D graphene macrostructures for high-performance supercapacitors. With a unique framework structure in which the graphene sheets are interlocked in 3D space to prevent their restacking, the graphene macrostructures feature very high specific surface areas, rapid electron and ion transport, and superior mechanical strength. They can thus be directly used as supercapacitor electrodes with excellent specific capacitances, rate capabilities, and cycling stabilities. We finally discuss the current challenges and future opportunities in this research field. By regarding the graphene as both a single-atom-thick carbon sheet and a conjugated macromolecule, our work opens a new avenue to bottom-up self-assembly of graphene macromolecule sheets into functional 3D graphene macrostructures with remarkable electrochemical performances. We hope that this Account will promote further efforts toward fundamental investigation of graphene self-assembly and the development of advanced 3D graphene materials for their real-world applications in electrochemical energy storage devices and beyond.

Assembly of chemically modified graphene: methods and applications

Chemically modified graphenes (CMGs) are unique building blocks for “bottom up” nanotechnology because of their single-atom thickness, two-dimensional conjugated structure, and exceptional physical and chemical properties. Various hierarchical structures and functional nanocomposites based on CMGs have been prepared by self-assembly. Here, we review the recent advances in the assembly of CMGs in solution or at interfaces, and demonstrate the wide application of the resulting materials.