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Immobilizing photogenerated electrons from graphitic carbon nitride for an improved visible-light photocatalytic activity.

ABSTRACT: Reducing the recombination probability of photogenerated electrons and holes is pivotal in enhancing the photocatalytic ability of graphitic carbon nitride (g-C3N4). Speeding the departure of photogenerated electrons is the most commonly used method of achieving this. To the best of our knowledge, there is no report on suppressing the recombination of photogenerated electron-hole pairs by immobilizing the electrons with ester functional groups. Here, for the first time the mesoporous g-C3N4 (mpg-C3N4) was integrated with polymethyl methacrylate, a polymer abundant in ester groups, which showed a photocatalytic activity unexpectedly higher than that of the original mpg-C3N4 under visible-light irradiation. Experimental observations, along with theoretical calculations, clarified that the impressive photocatalytic ability of the as-modified mpg-C3N4 was mainly derived from the immobilization of photogenerated electrons via an electron-gripping effect imposed by the ester groups in the polymethyl methacrylate. This novel strategy might also be applied in improving the photocatalytic performance of other semiconductors.

SUBMITTER: Sun H

PROVIDER: S-EPMC4779999 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Improving the Visible-Light Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Black Doping.

Project description:Hydrogen production by water splitting and the removal of aqueous dyes by using a catalyst and solar energy are an ideal future energy source and useful for environmental protection. Graphitic carbon nitride can be used as the photocatalyst with visible light irradiation. However, it typically suffers from the high recombination of carriers and low electrical conductivity. Here, we have developed a facile mix-thermal strategy to prepare carbon black-modified graphitic carbon nitrides, which possess high electrical conductivity, a wide adsorption range of visible light, and a low recombination rate of carriers. With the help of carbon black, highly crystallized graphitic carbon nitrides with built-in triazine and heptazine heterojunctions are obtained. Improved photocatalytic activities have been achieved in carbon black-modified graphitic carbon nitride. The dye removal rate can be three times faster than that of pristine graphitic carbon nitride and the photocatalytic H2 generation is 234 μmol h-1 g-1 under visible light irradiation.

| S-EPMC6643869 | biostudies-literature

Dual-defect-modified graphitic carbon nitride with boosted photocatalytic activity under visible light.

Project description:The development of photocatalysts that efficiently degrade organic pollutants is an important environmental-remediation objective. To that end, we report a strategy for the ready fabrication of oxygen-doped graphitic carbon nitride (CN) with engendered nitrogen deficiencies. The addition of KOH and oxalic acid during the thermal condensation of urea led to a material that exhibits a significantly higher pseudo-first-order rate constant for the degradation of bisphenol A (BPA) (0.0225 min-1) compared to that of CN (0.00222 min-1). The enhanced photocatalytic activity for the degradation of BPA exhibited by the dual-defect-modified CN (Bt-OA-CN) is ascribable to a considerable red-shift in its light absorption compared to that of CN, as well as its modulated energy band structure and more-efficient charge separation. Furthermore, we confirmed that the in-situ-formed cyano groups in the Bt-OA-CN photocatalyst act as strong electron-withdrawing groups that efficiently separate and transfer photo-generated charge carriers to the surface of the photocatalyst. This study provides novel insight into the in-situ dual-defect strategy for g-C3N4, which is extendable to the modification of other photocatalysts; it also introduces Bt-OA-CN as a potential highly efficient visible-light-responsive photocatalyst for use in environmental-remediation applications.

| S-EPMC6795803 | biostudies-literature

Highly efficient photocatalytic H₂ evolution from water using visible light and structure-controlled graphitic carbon nitride.

Project description:The major challenge of photocatalytic water splitting, the prototypical reaction for the direct production of hydrogen by using solar energy, is to develop low-cost yet highly efficient and stable semiconductor photocatalysts. Herein, an effective strategy for synthesizing extremely active graphitic carbon nitride (g-C3N4) from a low-cost precursor, urea, is reported. The g-C3N4 exhibits an extraordinary hydrogen-evolution rate (ca. 20,000 μmol h(-1) g(-1) under full arc), which leads to a high turnover number (TON) of over 641 after 6 h. The reaction proceeds for more than 30 h without activity loss and results in an internal quantum yield of 26.5% under visible light, which is nearly an order of magnitude higher than that observed for any other existing g-C3N4 photocatalysts. Furthermore, it was found by experimental analysis and DFT calculations that as the degree of polymerization increases and the proton concentration decreases, the hydrogen-evolution rate is significantly enhanced.

| S-EPMC4257501 | biostudies-literature

Cadmium Sulfide and Nickel Synergetic Co-catalysts Supported on Graphitic Carbon Nitride for Visible-Light-Driven Photocatalytic Hydrogen Evolution.

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 μmol 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.

| S-EPMC4770297 | biostudies-literature

Graphitic Carbon Nitride for Photocatalytic Air Treatment.

Project description:Graphitic carbon nitride (g-C3N4) is a conjugated polymer, which recently drew a lot of attention as a metal-free and UV and visible light responsive photocatalyst in the field of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability and earth-abundant nature. In the present work, bulk g-C3N4 was synthesized by thermal decomposition of melamine. This material was further exfoliated by thermal treatment. S-doped samples were prepared from thiourea or further treatment of exfoliated g-C3N4 by mesylchloride. Synthesized materials were applied for photocatalytic removal of air pollutants (acetaldehyde and NOx) according to the ISO 22197 and ISO 22197-1 methodology. The efficiency of acetaldehyde removal under UV irradiation was negligible for all g-C3N4 samples. This can be explained by the fact that g-C3N4 under irradiation does not directly form hydroxyl radicals, which are the primary oxidation species in acetaldehyde oxidation. It was proved by electron paramagnetic resonance (EPR) spectroscopy that the dominant species formed on the irradiated surface of g-C3N4 was the superoxide radical. Its production was responsible for a very high NOx removal efficiency not only under UV irradiation (which was comparable with that of TiO2), but also under visible irradiation.

| S-EPMC7372426 | biostudies-literature

Nitrogen-doped Carbon Nanospheres-Modified Graphitic Carbon Nitride with Outstanding Photocatalytic Activity.

Project description:Metals and metal oxides are widely used as photo/electro-catalysts for environmental remediation. However, there are many issues related to these metal-based catalysts for practical applications, such as high cost and detrimental environmental impact due to metal leaching. Carbon-based catalysts have the potential to overcome these limitations. In this study, monodisperse nitrogen-doped carbon nanospheres (NCs) were synthesized and loaded onto graphitic carbon nitride (g-C3N4, GCN) via a facile hydrothermal method for photocatalytic removal of sulfachloropyridazine (SCP). The prepared metal-free GCN-NC exhibited remarkably enhanced efficiency in SCP degradation. The nitrogen content in NC critically influences the physicochemical properties and performances of the resultant hybrids. The optimum nitrogen doping concentration was identified at 6.0 wt%. The SCP removal rates can be improved by a factor of 4.7 and 3.2, under UV and visible lights, by the GCN-NC composite due to the enhanced charge mobility and visible light harvesting. The mechanism of the improved photocatalytic performance and band structure alternation were further investigated by density functional theory (DFT) calculations. The DFT results confirm the high capability of the GCN-NC hybrids to activate the electron-hole pairs by reducing the band gap energy and efficiently separating electron/hole pairs. Superoxide and hydroxyl radicals are subsequently produced, leading to the efficient SCP removal.

| S-EPMC7770884 | biostudies-literature

Highly Crystalline K-Intercalated Polymeric Carbon Nitride for Visible-Light Photocatalytic Alkenes and Alkynes Deuterations.

Project description:In addition to the significance of photocatalytic hydrogen evolution, the utilization of the in situ generated H/D (deuterium) active species from water splitting for artificial photosynthesis of high value-added chemicals is very attractive and promising. Herein, photocatalytic water splitting technology is utilized to generate D-active species (i.e., Dad) that can be stabilized on anchored 2nd metal catalyst and are readily for tandem controllable deuterations of carbon-carbon multibonds to produce high value-added D-labeled chemicals/pharmaceuticals. A highly crystalline K cations intercalated polymeric carbon nitride (KPCN), rationally designed, and fabricated by a solid-template induced growth, is served as an ultraefficient photocatalyst, which shows a greater than 18-fold enhancement in the photocatalytic hydrogen evolution over the bulk PCN. The photocatalytic in situ generated D-species by superior KPCN are utilized for selective deuteration of a variety of alkenes and alkynes by anchored 2nd catalyst, Pd nanoparticles, to produce the corresponding D-labeled chemicals and pharmaceuticals with high yields and D-incorporation. This work highlights the great potential of developing photocatalytic water splitting technology for artificial photosynthesis of value-added chemicals instead of H2 evolution.

| S-EPMC6325627 | biostudies-literature

Tailoring TiO2 Nanotube-Interlaced Graphite Carbon Nitride Nanosheets for Improving Visible-Light-Driven Photocatalytic Performance.

Project description:Rapid recombination of photoinduced electron-hole pairs is one of the major defects in graphitic carbon nitride (g-C3N4)-based photocatalysts. To address this issue, perforated ultralong TiO2 nanotube-interlaced g-C3N4 nanosheets (PGCN/TNTs) are prepared via a template-based process by treating g-C3N4 and TiO2 nanotubes polymerized hybrids in alkali solution. Shortened migration distance of charge transfer is achieved from perforated PGCN/TNTs on account of cutting redundant g-C3N4 nanosheets, leading to subdued electron-hole recombination. When PGCN/TNTs are employed as photocatalysts for H2 generation, their in-plane holes and high hydrophilicity accelerate cross-plane diffusion to dramatically promote the photocatalytic reaction in kinetics and supply plentiful catalytic active centers. By having these unique features, PGCN/TNTs exhibit superb visible-light H2-generation activity of 1364 µmol h-1 g-1 (λ > 400 nm) and a notable quantum yield of 6.32% at 420 nm, which are much higher than that of bulk g-C3N4 photocatalysts. This study demonstrates an ingenious design to weaken the electron recombination in g-C3N4 for significantly enhancing its photocatalytic capability.

| S-EPMC6010724 | biostudies-literature

Photocatalytic Generation of Singlet Oxygen by Graphitic Carbon Nitride for Antibacterial Applications.

Project description:Carbon-based functional nanocomposites have emerged as potent antimicrobial agents and can be exploited as a viable option to overcome antibiotic resistance of bacterial strains. In the present study, graphitic carbon nitride nanosheets are prepared by controlled calcination of urea. Spectroscopic measurements show that the nanosheets consist of abundant carbonyl groups and exhibit apparent photocatalytic activity under UV photoirradiation towards the selective production of singlet oxygen. Therefore, the nanosheets can effectively damage the bacterial cell membranes and inhibit the growth of bacterial cells, such as Gram-negative Escherichia coli, as confirmed in photodynamic, fluorescence microscopy, and scanning electron microscopy measurements. The results from this research highlight the unique potential of carbon nitride derivatives as potent antimicrobial agents.

| S-EPMC11313655 | biostudies-literature

Biogenic Synthesis of Graphitic Carbon Nitride for Photocatalytic Degradation of Organic Dyes.

Project description:A simple approach of template growth of graphitic-carbon nitride (g-CN), a polymeric unit consisting of C, N, O, and H elements derived from extracts of green plant Aloe vera, which are rich in several chemical constituents, has been successfully experimented in this work. Comparing several other methods used for synthesizing g-CN involving a large amount of toxic components, here, we propose the simplest route economically and environmentally highly viable for near future. Green plants are highly rich in natural carbon and nitrogen compounds, such as acemannan, glucose, aloin, protein, etc. Way before g-CN research, many carbon-based materials have been synthesized for multifunctional properties, but g-CN has much benefit over them due to the presence of elements such as C, N, O, and H, thus making it electron-rich. Multifunctional properties of graphitic-carbon nitride interface bonding as a supercapacitor or as a metal-free catalyst thus help degrade dyes. Violet-blue broad band emission was even noticed when excited at 240 nm via C-C bonding (π-π* transition) in the absorption band with an extinction coefficient of ∼104 M-1 cm-1. With our research, we want to pave new ways of synthesizing such materials present in our nature in a biological form, which can protect our environment, thus causing less harm to mankind.

| S-EPMC6648270 | biostudies-literature

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