As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and “earth-abundant” nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The constructi...

Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

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

The use of solar energy to produce molecular hydrogen and oxygen (H2 and O2) from overall water splitting is a promising means of renewable energy storage. In the past 40 years, various inorganic and organic systems have been developed as photocatalysts for water splitting driven by visible light. These photocatalysts, however, still suffer from low quantum efficiency and/or poor stability. We report the design and fabrication of a metal-free carbon nanodot-carbon nitride (C3N4) nanocomposite and demonstrate its impressive performance for photocatalytic solar water splitting. We measured quantum efficiencies of 16% for wavelength λ = 420 ± 20 nanometers, 6.29% for λ = 580 ± 15 nanometers, and 4.42% for λ = 600 ± 10 nanometers, and determined an overall solar energy conversion efficiency of 2.0%. The catalyst comprises low-cost, Earth-abundant, environmentally friendly materials and shows excellent stability.

http://science.sciencemag.org/content/sci/347/6225/970.full.pdf

Metal-free efficient photocatalyst for stable visible water splitting via a two-electron pathway

Semiconductor-based photocatalysis is considered to be an attractive way for solving the worldwide energy shortage and environmental pollution issues. Since the pioneering work in 2009 on graphitic carbon nitride (g-C3N4) for visible-light photocatalytic water splitting, g-C3N4 -based photocatalysis has become a very hot research topic. This review summarizes the recent progress regarding the design and preparation of g-C3N4 -based photocatalysts, including the fabrication and nanostructure design of pristine g-C3N4 , bandgap engineering through atomic-level doping and molecular-level modification, and the preparation of g-C3N4 -based semiconductor composites. Also, the photo-catalytic applications of g-C3N4 -based photocatalysts in the fields of water splitting, CO2 reduction, pollutant degradation, organic syntheses, and bacterial disinfection are reviewed, with emphasis on photocatalysis promoted by carbon materials, non-noble-metal cocatalysts, and Z-scheme heterojunctions. Finally, the concluding remarks are presented and some perspectives regarding the future development of g-C3N4 -based photocatalysts are highlighted.

Polymeric Photocatalysts Based on Graphitic Carbon Nitride

Metal Oxides and Oxysalts as Anode Materials for Li Ion Batteries

Graphitic carbon nitride nanosheets are extracted, produced via simple liquid-phase exfoliation of a layered bulk material, g-C3N4. The resulting nanosheets, having ≈2 nm thickness and N/C atomic ratio of 1.31, show an optical bandgap of 2.65 eV. The carbon nitride nanosheets are demonstrated to exhibit excellent photocatalytic activity for hydrogen evolution under visible light.

Exfoliated Graphitic Carbon Nitride Nanosheets as Efficient Catalysts for Hydrogen Evolution Under Visible Light

Although lithium ion batteries have gained commercial success owing to their high energy density, they lack suitable electrodes capable of rapid charging and discharging to enable a high power density critical for broad applications. Here, we demonstrate a simple bottom-up approach toward single crystalline vanadium oxide (VO2) ribbons with graphene layers. The unique structure of VO2-graphene ribbons thus provides the right combination of electrode properties and could enable the design of high-power lithium ion batteries. As a consequence, a high reversible capacity and ultrafast charging and discharging capability is achieved with these ribbons as cathodes for lithium storage. A full charge or discharge is capable in 20 s. More remarkably, the resulting electrodes retain more than 90% of the initial capacity after cycling more than 1000 times at an ultrahigh rate of 190C, providing the best reported rate performance for cathodes in lithium ion batteries to date.

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Bottom-up approach toward single-crystalline VO2-graphene ribbons as cathodes for ultrafast lithium storage.

Two-dimensional (2D) atomic layers such as graphene, and metal chalcogenides have recently attracted tremendous attention due to their unique properties and potential applications. Unfortunately, in most cases, the free-standing nanosheets easily re-stack due to their van der Waals forces, and lose the advantages of their separated atomic layer state. Here, a bottom-up approach is developed to build three-dimensional (3D) architectures by 2D nanosheets such as MoS2 and graphene oxide nanosheets as building blocks, the thin nature of which can be well retained. After simply chemical reduction, the resulting 3D MoS2-graphene architectures possess high surface area, porous structure, thin walls and high electrical conductivity. Such unique features are favorable for the rapid diffusions of both lithium ions and electrons during lithium storage. As a consequence, MoS2-graphene electrodes exhibit high reversible capacity of ≈1200 mAh g−1, with very good cycling performance. Moreover, such a simple and low-cost assembly protocol can provide a new pathway for the large-scale production of various functional 3D architectures for energy storage and conversions.

A Bottom‐Up Approach to Build 3D Architectures from Nanosheets for Superior Lithium Storage

Free-standing graphitic C3N4 nanosheets are prepared by liquid phase exfoliation from graphitic C3N4 powders dispersed in various solvents such as isopropanol, N-methylpyrrolidone, water, ethanol, or acetone (sonication for 10 h).

Exfoliated Graphitic Carbon Nitride Nanosheets as Efficient Catalysts for Hydrogen Evolution under Visible Light.

It is demonstrated that graphene-based porous silica sheets can serve as an efficient carrier support for PEI via a simple nanocasting technology. The resulting materials possess thin nature, high PEI loading content and high thermal-conductivity. Such features are favorable for the efficient diffusion and adsorption of CO2 as well as the rapid thermal transfer during the CO2 capture process.

Liang Zhan

Papers

Exfoliated Graphitic Carbon Nitride Nanosheets as Efficient Catalysts for Hydrogen Evolution Under Visible Light

Bottom-up approach toward single-crystalline VO2-graphene ribbons as cathodes for ultrafast lithium storage.

A Bottom‐Up Approach to Build 3D Architectures from Nanosheets for Superior Lithium Storage

Exfoliated Graphitic Carbon Nitride Nanosheets as Efficient Catalysts for Hydrogen Evolution under Visible Light.

Graphene‐Based Porous Silica Sheets Impregnated with Polyethyleneimine for Superior CO2 Capture