Graphene has attracted tremendous research interest in recent years, owing to its exceptional properties. The scaled-up and reliable production of graphene derivatives, such as graphene oxide (GO) and reduced graphene oxide (rGO), offers a wide range of possibilities to synthesize graphene-based functional materials for various applications. This critical review presents and discusses the current development of graphene-based composites. After introduction of the synthesis methods for graphene and its derivatives as well as their properties, we focus on the description of various methods to synthesize graphene-based composites, especially those with functional polymers and inorganic nanostructures. Particular emphasis is placed on strategies for the optimization of composite properties. Lastly, the advantages of graphene-based composites in applications such as the Li-ion batteries, supercapacitors, fuel cells, photovoltaic devices, photocatalysis, as well as Raman enhancement are described (279 references).

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Graphene-based composites

Graphene based materials: Past, present and future

Graphene, a two-dimensional, single-layer sheet of sp(2) hybridized carbon atoms, has attracted tremendous attention and research interest, owing to its exceptional physical properties, such as high electronic conductivity, good thermal stability, and excellent mechanical strength. Other forms of graphene-related materials, including graphene oxide, reduced graphene oxide, and exfoliated graphite, have been reliably produced in large scale. The promising properties together with the ease of processibility and functionalization make graphene-based materials ideal candidates for incorporation into a variety of functional materials. Importantly, graphene and its derivatives have been explored in a wide range of applications, such as electronic and photonic devices, clean energy, and sensors. In this review, after a general introduction to graphene and its derivatives, the synthesis, characterization, properties, and applications of graphene-based materials are discussed.

Graphene-Based Materials: Synthesis, Characterization, Properties, and Applications

Supercapacitors have drawn considerable attention in recent years due to their high specific power, long cycle life, and ability to bridge the power/energy gap between conventional capacitors and batteries/fuel cells. Nanostructured electrode materials have demonstrated superior electrochemical properties in producing high-performance supercapacitors. In this review article, we describe the recent progress and advances in designing nanostructured supercapacitor electrode materials based on various dimensions ranging from zero to three. We highlight the effect of nanostructures on the properties of supercapacitors including specific capacitance, rate capability and cycle stability, which may serve as a guideline for the next generation of supercapacitor electrode design.

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Supercapacitor electrode materials: nanostructures from 0 to 3 dimensions

Three-dimensional (3D) N-doped graphene aerogel (N-GA)-supported Fe3O4 nanoparticles (Fe3O4/N-GAs) as efficient cathode catalysts for the oxygen reduction reaction (ORR) are reported. The graphene hybrids exhibit an interconnected macroporous framework of graphene sheets with uniform dispersion of Fe3O4 nanoparticles (NPs). In studying the effects of the carbon support on the Fe3O4 NPs for the ORR, we found that Fe3O4/N-GAs show a more positive onset potential, higher cathodic density, lower H2O2 yield, and higher electron transfer number for the ORR in alkaline media than Fe3O4 NPs supported on N-doped carbon black or N-doped graphene sheets, highlighting the importance of the 3D macropores and high specific surface area of the GA support for improving the ORR performance. Furthermore, Fe3O4/N-GAs show better durability than the commercial Pt/C catalyst.

3D Nitrogen-Doped Graphene Aerogel-Supported Fe3O4 Nanoparticles as Efficient Electrocatalysts for the Oxygen Reduction Reaction

Near infrared (NIR) imaging-guided photodynamic therapy (PDT) is attractive, especially the utilization of one dye as both a photosensitizer and fluorescent probe, and the as-synthesized BODIPY-Br2 molecule is a candidate. Here, a galactose targeted amphiphilic copolymer of a polypeptide was synthesized and its micelles work as nanocarriers for BODIPY for targeting the NIR imaging-guided PDT of hepatoma cancer cells. At the same time, BODIPY could light up the cytoplasm for real-time imaging and kill cancer cells when the light was switched on. In vitro tests performed on both HepG2 and HeLa cells confirmed that the as-prepared PMAGP-POEGMA-PLys-B micelles showed efficient cell suppression of the cells with galactose receptors in the presence of light under an extremely low energy density (6.5 J cm−2). This protocol highlights the potential of polypeptides as biodegradable carriers for NIR image-guided and confined targeting photodynamic therapy.

Near infrared imaging-guided photodynamic therapy under an extremely low energy of light by galactose targeted amphiphilic polypeptide micelle encapsulating BODIPY-Br2

Dissolution of highly molecular weight cellulose isolated from wheat straw in deep eutectic solvent of Choline/l-Lysine hydrochloride

Summary: The structural relationship of cellulose, hemicellulose, and lignin in plant cell walls is still a mystery needing to be explored. By using atomic force microscopy (AFM) the surface of straw at different layers was directly observed, and the structural characteristics were analyzed by topographic analysis and FT-IR spectra. It was found that a compact layer of wax covered the outside of the straw, which protects the straw from insects and microorganisms. At the boundary of the primary and second wall there appears a network structure of cellulose and hemicellulose, with some lignin localised on the surface of the network. It is consistent with the model of a cell wall suggested by Vincent. Inside the second cell wall, there is a layer mainly composed of a cellulose crystalline region. High-resolution AFM observation reveals that the crystalline structure consists of both triclinic and monoclinic unit cells.

An AFM phase image showing the structural relation between cellulose microfibrils, hemicellulose, and lignin in the straw cell wall.

Direct Visualization of Straw Cell Walls by AFM

pH-Sensitive doxorubicin conjugated polymeric micelles entrapped with near infrared (NIR) photosensitizer BODIPY (which works as an imaging agent at the same time) were designed and synthesized by ring opening polymerization of N-carboxyanhydride with mPEG-NH2 as the initiator, following reaction with doxorubicin to form the hydrazone-bond linker for pH responsiveness. Then the NIR dye (BODIPY) was loaded in the micelles for both bioimaging and photodynamic therapy (PDT). A significant cytotoxicity of NIR imaging-guided combined PDT and chemotherapy could be found by MTT assays, which was also confirmed with a fluorescence microscope, indicating a new kind of polymeric nanoparticle for potential theranostic treatment of cancers. In addition, the energy density of the laser for the PDT is extremely low.

NIR imaging-guided combined photodynamic therapy and chemotherapy by a pH-responsive amphiphilic polypeptide prodrug

Transparent free-standing films of graphene oxide (GO) have been prepared by a dried foam method using different oxygen-containing GO sheets as feedstocks. Then a humidity sensor was fabricated using the films as transparent and flexible sensing materials. The impedances of the films were measured at different relative humidity, and the results revealed that the relationship between impedance and relative humidity depends on both the oxygen content and the thickness of the GO films, and a linear relationship corresponds to an ultrathin film (in thickness of about 100 nm) while a non-linear relationship for thick films. In addition, the thin film can also show a dynamic switch behavior for humidity sensing. The transparent free-standing GO film has potential application working as an optical window combing the humidity sensing property.

Lifeng Yan

Papers

Near infrared imaging-guided photodynamic therapy under an extremely low energy of light by galactose targeted amphiphilic polypeptide micelle encapsulating BODIPY-Br2

Dissolution of highly molecular weight cellulose isolated from wheat straw in deep eutectic solvent of Choline/l-Lysine hydrochloride

Direct Visualization of Straw Cell Walls by AFM

NIR imaging-guided combined photodynamic therapy and chemotherapy by a pH-responsive amphiphilic polypeptide prodrug

Free-standing dried foam films of graphene oxide for humidity sensing