Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

Recent Advances in Ultrathin Two-Dimensional Nanomaterials

Electrochemical capacitors (i.e. supercapacitors) include electrochemical double-layer capacitors that depend on the charge storage of ion adsorption and pseudo-capacitors that are based on charge storage involving fast surface redox reactions. The energy storage capacities of supercapacitors are several orders of magnitude higher than those of conventional dielectric capacitors, but are much lower than those of secondary batteries. They typically have high power density, long cyclic stability and high safety, and thus can be considered as an alternative or complement to rechargeable batteries in applications that require high power delivery or fast energy harvesting. This article reviews the latest progress in supercapacitors in charge storage mechanisms, electrode materials, electrolyte materials, systems, characterization methods, and applications. In particular, the newly developed charge storage mechanism for intercalative pseudocapacitive behaviour, which bridges the gap between battery behaviour and conventional pseudocapacitive behaviour, is also clarified for comparison. Finally, the prospects and challenges associated with supercapacitors in practical applications are also discussed.

Electrochemical capacitors: mechanism, materials, systems, characterization and applications

We present the science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems, targeting an evolution in technology, that might lead to impacts and benefits reaching into most areas of society. This roadmap was developed within the framework of the European Graphene Flagship and outlines the main targets and research areas as best understood at the start of this ambitious project. We provide an overview of the key aspects of graphene and related materials (GRMs), ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries. We also define an extensive list of acronyms in an effort to standardize the nomenclature in this emerging field.

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Science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems

Ongoing technological advances in diverse fields including portable electronics, transportation, and green energy are often hindered by the insufficient capability of energy-storage devices By taking advantage of two different electrode materials, asymmetric supercapacitors can extend their operating voltage window beyond the thermodynamic decomposition voltage of electrolytes while enabling a solution to the energy storage limitations of symmetric supercapacitors This review provides comprehensive knowledge to this field We first look at the essential energy-storage mechanisms and performance evaluation criteria for asymmetric supercapacitors to understand the wide-ranging research conducted in this area Then we move to the recent progress made for the design and fabrication of electrode materials and the overall structure of asymmetric supercapacitors in different categories We also highlight several key scientific challenges and present our perspectives on enhancing the electrochemical performance of future asymmetric supercapacitors

Design and Mechanisms of Asymmetric Supercapacitors.

Molybdenum disulfide (MoS2) has emerged as a promising electrocatalyst for catalyzing protons to hydrogen via the so-called hydrogen evolution reaction (HER). In order to enhance the HER activity, tremendous effort has been made to engineer MoS2 catalysts with either more active sites or higher conductivity. However, at present, synergistically structural and electronic modulations for HER still remain challenging. In this work, we demonstrate the successfully synergistic regulations of both structural and electronic benefits by controllable disorder engineering and simultaneous oxygen incorporation in MoS2 catalysts, leading to the dramatically enhanced HER activity. The disordered structure can offer abundant unsaturated sulfur atoms as active sites for HER, while the oxygen incorporation can effectively regulate the electronic structure and further improve the intrinsic conductivity. By means of controllable disorder engineering and oxygen incorporation, an optimized catalyst with a moderate degree of ...

Controllable Disorder Engineering in Oxygen-Incorporated MoS2 Ultrathin Nanosheets for Efficient Hydrogen Evolution

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

carbide-derived carbon, [ 12 ] carbon nanotubes (CNTs), [ 14–17 ] and graphene, [ 6 , 7 , 10 , 18 , 19 ] possess notable features including high surface area, high electrical conductivity, and good chemical stability, and therefore they have been widely explored as thinfi lm electrode materials for ASSSs. However, the fabrication of ASSSs generally involves complex solution processing, highpressure pressing, high-temperature sintering, and sputtering techniques. [ 11 , 12 , 14–17 ] Moreover, polymer binders and conductive additives are required to enhance the adhesion between electrode materials and substrates as well as to improve the conductivity of the electrode, which unavoidably leads to decreased energy density of the devices. [ 6 , 20 ] Therefore, several challenges remain in developing ASSSs, such as to: i) explore high-performance electrode materials, ii) enhance the interfacial compatibility between electrode and solid-state electrolyte, and iii) simplify the device fabrication process. Graphene aerogels (GAs) represent a new class of ultralight and porous carbon materials that are associated with high

Three-Dimensional Nitrogen and Boron Co-doped Graphene for High-Performance All-Solid-State Supercapacitors

Three-dimensional graphene-based frameworks (3D-GFs) with hierarchical macro- and meso-porous structures are presented. The interconnected macropores are derived from hydrothermally assembled 3D graphene aerogels (GAs), while the mesopores are generated by the silica networks uniformly grown on the surface of graphene. The resulting 3D-GFs exhibit narrow mesopore size distribution (2–3.5 nm), high surface area, and low mass density. These intriguing features render 3D-GFs a promising template for creating various 3D porous materials. Specifically, 3D GA-based mesoporous carbons (GA-MC) and metal oxide hybrids (GA-Co3O4, GA-RuO2) can be successfully constructed via a nanocasting technology. Benefiting from the integration of meso- and macroporous structures, 3D GA-MC manifests outstanding specific capacitance (226 F g–1), high rate capability, and excellent cycling stability (no capacitance loss after 5000 cycles) when it is applied in electrochemical capacitors.

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Three-Dimensional Graphene-Based Macro- and Mesoporous Frameworks for High-Performance Electrochemical Capacitive Energy Storage

A well-designed nanostructure of transition metal oxides has been regarded as a key to solve their problems of large volume changes during lithium insertion-desertion processes which are associated with pulverization of the electrodes and rapid capacity decay. Here we report an effective approach for the fabrication of porous iron oxide ribbons by controlling the nucleation and growth of iron precursor onto the graphene surface and followed by an annealing treatment. The resultant iron oxide ribbons possess large aspect ratio, porous structure, thin feature and enhanced open-edges. These characteristics are favorable for the fast diffusion of lithium ions and electrons, and meanwhile can effectively accommodate the volume change of iron oxides during the cycling processes. As a consequence, the graphene-induced porous iron oxide ribbons exhibit a high reversible capacity and excellent cycle stability for lithium storage.

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Porous Iron Oxide Ribbons Grown on Graphene for High-Performance Lithium Storage

Three-dimensional (3D) N-doped gra- phene 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.

Yi Sun

Papers

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

Three-Dimensional Nitrogen and Boron Co-doped Graphene for High-Performance All-Solid-State Supercapacitors

Three-Dimensional Graphene-Based Macro- and Mesoporous Frameworks for High-Performance Electrochemical Capacitive Energy Storage

Porous Iron Oxide Ribbons Grown on Graphene for High-Performance Lithium Storage

3D Nitrogen-Doped Graphene Aerogel-Supported Fe 3 O 4 Nanoparticles as Efficient Electrocatalysts for the Oxygen Reduction Reaction