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?

Sustainable hydrogen production is an essential prerequisite of a future hydrogen economy. Water electrolysis driven by renewable resource-derived electricity and direct solar-to-hydrogen conversion based on photochemical and photoelectrochemical water splitting are promising pathways for sustainable hydrogen production. All these techniques require, among many things, highly active noble metal-free hydrogen evolution catalysts to make the water splitting process more energy-efficient and economical. In this review, we highlight the recent research efforts toward the synthesis of noble metal-free electrocatalysts, especially at the nanoscale, and their catalytic properties for the hydrogen evolution reaction (HER). We review several important kinds of heterogeneous non-precious metal electrocatalysts, including metal sulfides, metal selenides, metal carbides, metal nitrides, metal phosphides, and heteroatom-doped nanocarbons. In the discussion, emphasis is given to the synthetic methods of these HER electrocatalysts, the strategies of performance improvement, and the structure/composition-catalytic activity relationship. We also summarize some important examples showing that non-Pt HER electrocatalysts could serve as efficient cocatalysts for promoting direct solar-to-hydrogen conversion in both photochemical and photoelectrochemical water splitting systems, when combined with suitable semiconductor photocatalysts.

Noble metal-free hydrogen evolution catalysts for water splitting

The reduction of graphene oxide

Approaches, Derivatives and Applications Vasilios Georgakilas,† Michal Otyepka,‡ Athanasios B. Bourlinos,‡ Vimlesh Chandra, Namdong Kim, K. Christian Kemp, Pavel Hobza,‡,§,⊥ Radek Zboril,*,‡ and Kwang S. Kim* †Institute of Materials Science, NCSR “Demokritos”, Ag. Paraskevi Attikis, 15310 Athens, Greece ‡Regional Centre of Advanced Technologies and Materials, Department of Physical Chemistry, Faculty of Science, Palacky University Olomouc, 17. listopadu 12, 771 46 Olomouc, Czech Republic Center for Superfunctional Materials, Department of Chemistry, Pohang University of Science and Technology, San 31, Hyojadong, Namgu, Pohang 790-784, Korea Institute of Organic Chemistry and Biochemistry, Academy of Sciences of the Czech Republic, v.v.i., Flemingovo naḿ. 2, 166 10 Prague 6, Czech Republic

Functionalization of Graphene: Covalent and Non-Covalent Approaches, Derivatives and Applications

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

Herein we obtained a chemically bonded TiO2 (P25)-graphene nanocomposite photocatalyst with graphene oxide and P25, using a facile one-step hydrothermal method. During the hydrothermal reaction, both of the reduction of graphene oxide and loading of P25 were achieved. The as-prepared P25-graphene photocatalyst possessed great adsorptivity of dyes, extended light absorption range, and efficient charge separation properties simultaneously, which was rarely reported in other TiO2−carbon photocatalysts. Hence, in the photodegradation of methylene blue, a significant enhancement in the reaction rate was observed with P25-graphene, compared to the bare P25 and P25-CNTs with the same carbon content. Overall, this work could provide new insights into the fabrication of a TiO2−carbon composite as high performance photocatalysts and facilitate their application in the environmental protection issues.

P25-Graphene Composite as a High Performance Photocatalyst

The effects of chemical states of Ag on the photoelectrochemical (PEC) properties of Ag−TiO2 composites were investigated with Ag(0)−TiO2 and Ag(I)−TiO2 prepared by photoreduction-thermal treatment (PRT) method. The comparison of photoaction spectra of Ag(0)−TiO2 and Ag(I)−TiO2 showed that only the Ag(0) containing samples had notable photocurrent under visible light (in the range of 400−800 nm), which was attributed to the highly dispersed Ag(0), according to the DRS, XRD and XPS measurements. During the photocurrent spectra measurements of Ag(0)−TiO2, it was demonstrated that Ag(0) was photoexcited because of plasma resonance in the visible light region, and charge separation was accomplished by the transport of photoexcited electrons from Ag(0) to the TiO2 conduction band with the simultaneous formation of Ag(I), which could be partially reduced to the initial active Ag(0) state under the following UV light irradiation. Actually, it was the interconversion of Ag(0) and Ag(I) during the alternating irra...

Tuning Photoelectrochemical Performances of Ag−TiO2 Nanocomposites via Reduction/Oxidation of Ag

To improve the performance of SnO2 as anode materials for lithium battery, a facile and efficient method to prepare the composites of SnO2-nanocrystal/graphene-nanosheets was developed on the basis of the reduction of graphene oxide (GO) by Sn2+ ion. Changing the ratio of Sn2+ and GO led to the morphology changes of SnO2/graphene-nanosheets composite. The performance as anode materials for lithium battery was studied in this report. The results showed that the electrochemical performance of composites was greatly enhanced, indicating that the composites might have a promising future as application in Li-ion battery.

Preparation of SnO2-Nanocrystal/Graphene-Nanosheets Composites and Their Lithium Storage Ability

The original bismuth-based oxyhalide, known as the Sillen family, is an important photocatalyst due to its high photocatalytic oxidation activity. Here, we report a bismuth-based photocatalyst, Bi24O31Br10, with reasonable reduction activity. The photoreduction capability of Bi24O31Br10 in H-2 evolution from water reduction is 133.9 mu mol after 40 h under visible light irradiation. Bi24O31Br10 presents the highest activity among Bi2O3, BiOBr, and Bi24O31Br10 in photocatalytic reduction of the Cr (VI) test, and Cr (VI) ions are totally removed in 40 mm. The Mott-Schottky test shows the bottom of the conduction band fits the electric potential requirements for splitting water to H-2. First-principles calculations indicate the conduction band of Bi24O31Br10 mainly consists of hybridized Bi 6p and Br 4s orbitals, which may contribute to the uplifting of the conduction band.

Xiao-Jun Lv

Papers

P25-Graphene Composite as a High Performance Photocatalyst

Tuning Photoelectrochemical Performances of Ag−TiO2 Nanocomposites via Reduction/Oxidation of Ag

Preparation of SnO2-Nanocrystal/Graphene-Nanosheets Composites and Their Lithium Storage Ability

Bismuth Oxybromide with Reasonable Photocatalytic Reduction Activity under Visible Light

Spectacular photocatalytic hydrogen evolution using metal-phosphide/CdS hybrid catalysts under sunlight irradiation