Faculté des Sciences Fondamentales et Appliquées (UFR SFA), Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP, CNRS), University of Poitiers, France
Dr. Prince Nana Amaniampong
Faculté des Sciences Fondamentales et Appliquées (UFR SFA), Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP, CNRS), University of Poitiers, France
Nanostructured mesoporous titanium dioxide (TiO2) particles with high specific surface area and average crystallite domain sizes within 2 nm and 30 nm have been prepared via the sol-gel and hydrothermal procedures. The characteristics of produced nanoparticles have been tested using X-Ray Diffraction (XRD), Brunauer-Emmett-Teller (BET) surface area analysis, Scanning Electron Microscopy (SEM), Fourier Transform Infra-Red (FTIR), and Raman Spectroscopy as a function of temperature for their microstructural, porosity, morphological, structural and absorption properties. The as-synthesized TiO2 nanostructures were attempted as catalysts in Rhodamine B and Sudan III dyes' photocatalytic decomposition in a batch reactor with the assistance of Ultra Violet (UV) light. The results show that for catalysts calcined at 300 °C, ∼100 % decomposition of Sudan III dye was observed when Hydrothermal based catalyst was used whiles ∼94 % decomposition of Rhodamine B dye was observed using the sol-gel based catalysts. These synthesized TiO2 nanoparticles have promising potential applications in the light aided decomposition of a wide range of dye pollutants.
In this study, a Pd-based catalytic model over a nitrogen enriched fibrous Porous-Organic-Polymer (POP) is established to execute hydrodeoxygenation of various vegetable oils in producing potential large-scale renewable diesel. Here we report a cost-effective synthesis strategy for a new microporous hypercrosslinked POP through the FeCl3 assisted Friedel–Crafts alkylation reaction, followed by fabrication of Pd0-NPs (2–3 nm) using a solid gas phase hydrogenation route to deliver a novel catalytic system. This catalyst (called Pd@PPN) exhibits versatile catalytic performance for different types of vegetable oils including palm oil, soybean oil, sunflower oil and rapeseed oil to furnish long chain diesel range alkanes. The catalyst is comprehensively characterized using various spectroscopic tools and it shows high stability during five runs of recycling without leaching of Pd. Our results further reveal that a direct decarbonylation (DCN) pathway of fatty acids to produce alkanes with one fewer carbon is the dominant mechanism. Under optimized conditions, using stearic acid to represent the long linear carboxylic acids in the vegetable oils, up to 90% conversion with 83% selectivity of C17-alkane has been achieved on our fabricated catalyst. Density functional theory (DFT) calculations are performed to provide insights into the electronic properties of the catalyst, the mechanistic reaction pathway, the crucial role of the catalyst surface and the product selectivity trend. The strong interaction between the corrugated polymer-frame-structure and the Pd-NPs suggests the presence of high density step sites on the fabricated Pd-NP anchored within the cage of the polymer structure. DFT calculations also reveal the strong promotional effect of step sites and charge transfer in facilitating rate-limiting steps during the decarbonylation (DCN) pathway and removal of strongly bound intermediates formed during the process, therefore explaining the high activity of the fabricated Pd@PPN catayst for the hydrodeoxygenation (HDO) conversion to produce bio-based alkane diesel.
The integration of nanostructured catalytic cavitation agents, microfluidic solutions, and computational molecular modelling forms a trilateral synergistic platform that unlocks new potential of sonocatalysis in green and sustainable chemistry.
We demonstrate a catalytic base-free strategy for the selective oxidation of microcrystalline cellulose to oxalic acid (OA) by combining low frequency ultrasound as an unconventional activation technique and Au/Fe2O3 as a catalyst.
Ultrasonic irradiation of cellulose at a high frequency induces its selective depolymerization to glucose at room temperature and atmospheric pressure within only a few minutes.
16 November 2024 in Angewandte Chemie International Edition
Efficient energy transfer management in catalytic processes is crucial for overcoming activation energy barriers while minimizing costs and CO2 emissions. We exploit here a concept of CuO particle design with multiple gas‐stabilizing sites, engineered to function as cavitation nuclei and catalysts. This concept facilitates the selective and efficient acoustic energy transfer directly to the catalyst surface, avoiding the undesired dissipation of acoustic energy into the bulk solution while demonstrating superior cavitation properties at lower acoustic pressure amplitudes. Utilizing a chemical thermometric approach, we demonstrate that the local temperature on the surface of our CuO particles during cavitation bubble implosions can create an effective equivalent temperature of about 360 °C. This temperature effect facilitates the efficient catalysis of oxidative reactions using an organic pollutant probe molecule. Density functional theory (DFT) calculations were used to assess the decomposition of H2O2 and of pollutant probe molecule on CuO (111). Our work represents a significant advance in sonocatalytic systems, promising efficient energy use in catalytic reactions.