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Nitrogen-Rich and Porous Graphitic Carbon Nitride Nanosheet-Immobilized Palladium Nanoparticles as Highly Active and Recyclable Catalysts for the Reduction of Nitro Compounds and Degradation of Organic Dyes.

ABSTRACT: In the present study, we have successfully synthesized nitrogen-rich graphitic carbon nitride (g-C₃N₄) nanosheets by a simple direct thermal polymerization approach. The synthesized g-C₃N₄ nanosheets were exfoliated using HCl to make their surface a few nanometers thick. The ultrathin surface was achieved by simply mixing g-C₃N₄ in 3 M HCl. After that, palladium nanoparticles were uniformly immobilized on the surface of g-C₃N₄. The synthesized materials were characterized by various physiochemical techniques such as X-ray diffraction, energy-dispersive X-ray spectroscopy, and Fourier transform infrared spectroscopy. Information about morphology and size was obtained through transmission electron microscopy and scanning electron microscopy. The Brunauer-Emmett-Teller surface area, pore volume, and pore diameter were determined using nitrogen adsorption-desorption measurements. The prepared material (Pd/g-C₃N₄) was utilized as an efficient catalyst for the reduction of hazardous nitroarenes and degradation of organic dyes. The catalyst could be easily recovered through centrifugation and then could be reused multiple times for the further catalytic cycles with a little loss in its catalytic activity. The work presented here illustrates the sustainable anchoring of metal nanoparticles over the surface of nitrogen-rich g-C₃N₄ nanosheets and could be utilized for different types of catalytic reactions.

SUBMITTER: Kumar Y

PROVIDER: S-EPMC7288708 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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Nitrogen-Rich and Porous Graphitic Carbon Nitride Nanosheet-Immobilized Palladium Nanoparticles as Highly Active and Recyclable Catalysts for the Reduction of Nitro Compounds and Degradation of Organic Dyes.

Kumar Yogesh Y Rani Swati S Shabir Javaid J Kumar Lalita S LS

ACS omega 20200526 22

In the present study, we have successfully synthesized nitrogen-rich graphitic carbon nitride (g-C3N4) nanosheets by a simple direct thermal polymerization approach. The synthesized g-C3N4 nanosheets were exfoliated using HCl to make their surface a few nanometers thick. The ultrathin surface was achieved by simply mixing g-C3N4 in 3 M HCl. After that, palladium nanoparticles were uniformly immobilized on the surface of g-C3< ...[more]

PMID: 32548511

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Project description:Highlights • Nitrogen-defective porous ultrathin g-C3N4 nanosheets (DUCN) were prepared.• DUCN exhibited high photocatalytic inactivation performance toward E. coli and B. subtilis.• Ultrathin nanosheets structure enhanced the interaction between photocatalysts and bacteria.• Nitrogen defects reduced charge recombination and improved H2O2 generation.• Good stability in consecutive photocatalytic inactivation experiments. The efficient generation and utilization of ROSs is a key step in determining the achievement of safe drinking water by photocatalytic bacterial inactivation technology. Although graphitic carbon nitride (g-C3N4) serves as a green and promising photocatalyst for water disinfection, insufficient bacterial capturing capacity and serious charge recombination of pristine g-C3N4 extremely restrict its bactericidal activity. Herein, we develop a facile thermal exfoliation and thermal polymerization method to prepare the nitrogen-defective ultrathin g-C3N4 nanosheets (DUCN-500). Our results showed that ultrathin nanosheet structure greatly enhanced bacterial capturing capacity of g-C3N4 to increase the utilization efficiency of ROS, which contributed to the performance of DUCN-500 greatly outperforming bulk g-C3N4. The nitrogen defects increased ROS generation (·O2− and H2O2) by approximately 4.6 times, which was attributed to negative shift of the conduction band potential and rapid separation of charge carriers. The DUCN-500 could rapidly and completely inactivate Escherichia coli and Bacillus subtilis in real sewage under simulated solar irradiation, accompanied by good anti-interference capability and stability. Additionally, bacterial morphology destruction, the loss of antioxidant enzyme activity and the leakage of protein were proven to be the main mechanisms of photocatalytic sterilization. This study offers new insight into the rational design of efficient g-C3N4-based photocatalysts for water disinfection. Graphical abstract Image, graphical abstract

Project description:Graphitic carbon nitride (g-C3N4) is a metal-free photocatalyst used for visible-driven hydrogen production, CO2 reduction, and organic pollutant degradation. In addition to the most attractive feature of visible photoactivity, its other benefits include thermal and photochemical stability, cost-effectiveness, and simple and easy-scale-up synthesis. However, its performance is still limited due to its low absorption at longer wavelengths in the visible range, and high charge recombination. In addition, the exfoliated nanosheets easily aggregate, causing the reduction in specific surface area, and thus its photoactivity. Herein, we propose the use of ultra-thin porous g-C3N4 nanosheets to overcome these limitations and improve its photocatalytic performance. Through the optimization of a novel multi-step synthetic protocol, based on an initial thermal treatment, the use of nitric acid (HNO3), and an ultrasonication step, we were able to obtain very thin and well-tuned material that yielded exceptional photodegradation performance of methyl orange (MO) under visible light irradiation, without the need for any co-catalyst. About 96% of MO was degraded in as short as 30 min, achieving a normalized apparent reaction rate constant (k) of 1.1 × 10-2 min-1mg-1. This represents the highest k value ever reported using C3N4-based photocatalysts for MO degradation, based on our thorough literature search. Ultrasonication in acid not only prevents agglomeration of g-C3N4 nanosheets but also tunes pore size distribution and plays a key role in this achievement. We also studied their performance in a photocatalytic hydrogen evolution reaction (HER), achieving a production of 1842 µmol h-1 g-1. Through a profound analysis of all the samples' structure, morphology, and optical properties, we provide physical insight into the improved performance of our optimized porous g-C3N4 sample for both photocatalytic reactions. This research may serve as a guide for improving the photocatalytic activity of porous two-dimensional (2D) semiconductors under visible light irradiation.

Dataset Information

Nitrogen-Rich and Porous Graphitic Carbon Nitride Nanosheet-Immobilized Palladium Nanoparticles as Highly Active and Recyclable Catalysts for the Reduction of Nitro Compounds and Degradation of Organic Dyes.

Publications

Nitrogen-Rich and Porous Graphitic Carbon Nitride Nanosheet-Immobilized Palladium Nanoparticles as Highly Active and Recyclable Catalysts for the Reduction of Nitro Compounds and Degradation of Organic Dyes.

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