In situ growing of CoO nanoparticles on g-C3N4 composites with highly improved photocatalytic activity for hydrogen evolution.
ABSTRACT: CoO/g-C3N4 hybrid catalyst is facilely prepared for application to photocatalytic H2 evolution from water splitting by the vacuum rotation-evaporation and in situ thermal method. The physical and chemical properties of CoO/g-C3N4 are determined by a series of characterization methods. The g-C3N4 with 0.6 wt% Co loading exhibits superior photocatalytic hydrogen evolution activity with an H2 evolution amount of 23.25 mmol g-1 after 5 h. The obtained 0.6 wt% CoO/g-C3N4 can split water to generate 0.39 mmol g-1 H2 without sacrificial agent and noble metal, while the pure g-C3N4 is inactive under the same reaction conditions. The remarkable enhancement of photocatalytic H2 evolution activity of CoO/g-C3N4 composites is mainly ascribed to the effective separation of electron-hole pairs and charge transfer. The work creates new opportunities for the design of low-cost g-C3N4-based photocatalysts with high photocatalytic H2 evolution activity from overall water splitting.
Project description:We report the direct splitting of pure water by light-excited graphitic carbon nitride (g-C3N4) modified with Pt, PtO x , and CoO x as redox cocatalysts, while pure g-C3N4 is virtually inactive for overall water splitting by photocatalysis. The novelty is in the selective creation of both H2 and O2 cocatalysts on surface active sites of g-C3N4via photodeposition triggering the splitting of water for the simultaneous evolution of H2 and O2 gases in a stoichiometric ratio of 2?:?1, irradiated with light, without using any sacrificial reagents. The photocatalyst was stable for 510 hours of reaction.
Project description:Na and cyano-group co-modified g-C3N4 was easily synthesized and its physicochemical property was completely analyzed. The results manifested that Na and cyano-group modification could heighten visible light absorbed ability and accelerate photoinduced charge separation. When resultant Na and cyano-group co-modified g-C3N4 was splitting water H2 evolution, its H2 evolution rate was obviously improved. Furthermore, it also kept excellent stable capacity of H2 evolution and stability of chemical structure. Hence, this present study does not only develop an efficient strategy to boost photocatalytic property of g-C3N4 based catalysts, but also provides useful guidance for designing more effective photocatalysts.
Project description:Due to low charge separation efficiency and poor stability, it is usually difficult for single-component photocatalysts such as graphitic carbon nitride (g-C3N4) and silver chromate (Ag2CrO4) to fulfill photocatalytic hydrogen production efficiently. Z-scheme charge transport mechanism that mimics the photosynthesis in nature is an effective way to solve the above problems. Inspired by photosynthesis, we report Ag2CrO4 nanoparticles-decorated g-C3N4 nanosheet as an efficient photocatalyst for hydrogen evolution reaction (HER) with methanol as sacrificial agent. The formation of Z-scheme g-C3N4/Ag2CrO4 nanosheets photocatalysts could inhibit the recombination of photogenerated electron-hole pairs, promote the generation of hydrogen by photosplitting of water. The experiment results indicate that g-C3N4/Ag2CrO4 nanocomposites present enhanced photocatalytic activity and stability in the H2 evolution of water splitting. And the nanocomposites g-C3N4/Ag2CrO4(23.1%) show the 14 times HER efficiency compared to that of bare g-C3N4.
Project description:A one-dimensional (1D) nanostructure having a porous network is an exceptional photocatalytic material to generate hydrogen (H2) and decontaminate wastewater using solar energy. In this report, we synthesized nanoporous 1D microrods of graphitic carbon nitride (g-C3N4) via a facile and template-free chemical approach at room temperature. The use of concentrated acids induced etching and lift-off because of strong oxidation and protonation. Compared with the bulk g-C3N4, the porous 1D microrod structure showed five times higher photocatalytic degradation performance toward methylene blue dye (MB) under visible light irradiation. The photocatalytic H2 evolution of the 1D nanostructure (34??mol g(-1)) was almost 26 times higher than that of the bulk g-C3N4 structure (1.26??mol g(-1)). Additionally, the photocurrent stability of this nanoporous 1D morphology over 24?h indicated remarkable photocorrosion resistance. The improved photocatalytic activities were attributed to prolonged carrier lifetime because of its quantum confinement effect, effective separation and transport of charge carriers, and increased number of active sites from interconnected nanopores throughout the microrods. The present 1D nanostructure would be highly suited for photocatalytic water purification as well as water splitting devices. Finally, this facile and room temperature strategy to fabricate the nanostructures is very cost-effective.
Project description:Energy crises and environmental pollution are two serious threats to modern society. To overcome these problems, graphitic carbon nitride (g-C3N4) nanosheets were fabricated and functionalized with SnO2 nanoparticles to produce H2 from water splitting and degrade 2-chlorophenol under visible light irradiation. The fabricated samples showed enhanced photocatalytic activities for both H2 evolution and pollutant degradation as compared to bare g-C3N4 and SnO2. These enhanced photoactivities are attributed to the fast charge separation as the excited electrons transfer from g-C3N4 to the conduction band of SnO2. This enhanced charge separation has been confirmed by the photoluminescence spectra, steady state surface photovoltage spectroscopic measurement, and formed hydroxyl radicals. It is believed that this work will provide a feasible route to synthesize photocatalysts for improved energy production and environmental purification.
Project description:Design and preparation of noble-metal-free photocatalysts is of great importance for photocatalytic water splitting harvesting solar energy. Here, we report the high visible-light-driven hydrogen evolution upon the hybrid photocatalyst system consisting of CdS nanocrystals and Ni@NiO nanoparticles grown on the surface of g-C3N4. The hybrid system shows a high H2-production rate of 1258.7??mol h(-1) g(-1) in the presence of triethanolamine as a sacrificial electron donor under visible light irradiation. The synergetic catalytic mechanism has been studied and the results of photovoltaic and photoluminescence properties show that efficient electron transfer could be achieved from g-C3N4 to CdS nanocrystals and subsequently to Ni@NiO hybrid.
Project description:Novel photocatalysts -CdSe quantum dots (QDs)/g-C3N4- were successfully constructed. The structure, chemical composition, and optical properties of the prepared samples were investigated via a series of characterization techniques. The results indicated that CdSe QDs/g-C3N4 photocatalysts exhibited remarkably enhanced photocatalytic activity for visible-light-induced H2 evolution compared to pristine g-C3N4 and CdSe QDs and addition of 13.6 wt % CdSe QDs into the composite photocatalyst generated the highest H2 production rate. The enhanced photocatalytic performance of CdSe QDs/g-C3N4 can be attributed to the synergistic effects of excellent visible absorption and high charge separation efficiency from the heterostructure. This work could not only provide a facile method to fabricate semiconductor QDs-modified g-C3N4 photocatalysts but also contribute to the design for heterostructures.
Project description:Direct and efficient photocatalytic overall water splitting is crucial for the sustainable conversion and storage of renewable solar energy. Herein, we present the design of a carbon-rich graphitic carbon nitride (Cco-C3N4), prepared from a layered molecular cocrystal precursor. The cocrystal microsheets were synthesized using a facile hydrothermal process. Following two-step thermal treatment and liquid exfoliation, the product maintains the 2D morphology owing to the toptactic transformation process. The Cco-C3N4 exhibits an enhanced photogenerated electron-hole separation, high charge transport capacity, and prolonged lifetime of the carriers, relative to the g-C3N4 system. In the absence of any sacrificial reagent or co-catalyst, the Cco-C3N4 microsheets exhibit a high photocatalytic activity. The work presented in this report supplies a cocrystal route for the orderly molecular self-assembly of precursor materials to tailor the chemical compositions and electronic structures. Moreover, the generation of a highly efficient water-splitting photocatalyst has larger implications for sustainable energy applications.
Project description:Novel fibrous graphitic carbon nitride (g-C3N4) derivatives prepared from metal organic frameworks (MOFs) were doped with Ce3+ (Ce-C3N4) as photocatalytic materials. Ce-C3N4 was characterized using various techniques, revealing its high specific surface area, excellent photocatalytic activity, and stability for H2 evolution under visible light irradiation. The fluorine modified samples show superior photocatalytic activity under visible light irradiation, which is due to the presence of more active sites and enhanced absorption of solar energy. This work provides a new synthetic route for MOF-derived g-C3N4 that can be doped with different metal ions. The fluorine modified Ce-C3N4 is an efficient photocatalyst with potential for many applications related to energy and the environment.
Project description:Both artificial photosystems and natural photosynthesis have not reached their full potential for the sustainable conversion of solar energy into specific chemicals. A promising approach is hybrid photosynthesis combining efficient, non-toxic, and low-cost abiotic photocatalysts capable of water splitting with metabolically versatile non-photosynthetic microbes. Here, we report the development of a water-splitting enzymatic photocatalyst made of graphitic carbon nitride (g-C3N4) coupled with H2O2-degrading catalase and its utilization for hybrid photosynthesis with the non-photosynthetic bacterium Ralstonia eutropha for bioplastic production. The g-C3N4-catalase system has an excellent solar-to-hydrogen efficiency of 3.4% with a H2 evolution rate up to 55.72 ?mol h-1 while evolving O2 stoichiometrically. The hybrid photosynthesis system built with the water-spitting g-C3N4-catalase photocatalyst doubles the production of the bioplastic polyhydroxybutyrate by R. eutropha from CO2 and increases it by 1.84-fold from fructose. These results illustrate how synergy between abiotic non-metallic photocatalyst, enzyme, and bacteria can augment solar-to-multicarbon chemical conversion.