Search results for: Ugwu Elias Ikechukwu

Authors: Dionisios Panagiotaras, Elias Stathatos, Dimitrios Papoulis

Abstract:

 Sol-gel method has been used to fabricate nanocomposite films on glass substrates composed halloysite clay mineral and nanocrystalline TiO2. The methodology for the synthesis involves a simple chemistry method utilized nonionic surfactant molecule as pore directing agent along with the acetic acid-based solgel route with the absence of water molecules. The thermal treatment of composite films at 450oC ensures elimination of organic material and lead to the formation of TiO2 nanoparticles onto the surface of the halloysite nanotubes. Microscopy techniques and porosimetry methods used in order to delineate the structural characteristics of the materials. The nanocomposite films produced have no cracks and active anatase crystal phase with small crystallite size were deposited on halloysite nanotubes. The photocatalytic properties for the new materials were examined for the decomposition of the Basic Blue 41 azo dye in solution. These, nanotechnology based composite films show high efficiency for dye’s discoloration in spite of different halloysite quantities and small amount of halloysite/TiO2 catalyst immobilized onto glass substrates. Moreover, we examined the modification of the halloysite/TiO2 films with silver particles in order to improve the photocatalytic properties of the films. Indeed, the presence of silver nanoparticles enhances the discoloration rate of the Basic Blue 41 compared to the efficiencies obtained for unmodified films.

Keywords: Clay mineral, nanotubular Halloysite, Photocatalysis, Titanium Dioxide, Silver modification.

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Authors: K. Mondal, S. Talapatra, M. Terrones, S. Pokhrel, C. Frizzel, B. Sumpter, V. Meunier, A. L. Elias

Abstract:

Worldwide energy independence is reliant on the ability to leverage locally available resources for fuel production. Recently, syngas produced through gasification of carbonaceous materials provided a gateway to a host of processes for the production of various chemicals including transportation fuels. The basis of the production of gasoline and diesel-like fuels is the Fischer Tropsch Synthesis (FTS) process: A catalyzed chemical reaction that converts a mixture of carbon monoxide (CO) and hydrogen (H₂) into long chain hydrocarbons. Until now, it has been argued that only transition metal catalysts (usually Co or Fe) are active toward the CO hydrogenation and subsequent chain growth in the presence of hydrogen. In this paper, we demonstrate that carbon nanotube (CNT) surfaces are also capable of hydro-deoxygenating CO and producing long chain hydrocarbons similar to that obtained through the FTS but with orders of magnitude higher conversion efficiencies than the present state-of-the-art FTS catalysts. We have used advanced experimental tools such as XPS and microscopy techniques to characterize CNTs and identify C-O functional groups as the active sites for the enhanced catalytic activity. Furthermore, we have conducted quantum Density Functional Theory (DFT) calculations to confirm that C-O groups (inherent on CNT surfaces) could indeed be catalytically active towards reduction of CO with H₂, and capable of sustaining chain growth. The DFT calculations have shown that the kinetically and thermodynamically feasible route for CO insertion and hydro-deoxygenation are different from that on transition metal catalysts. Experiments on a continuous flow tubular reactor with various nearly metal-free CNTs have been carried out and the products have been analyzed. CNTs functionalized by various methods were evaluated under different conditions. Reactor tests revealed that the hydrogen pre-treatment reduced the activity of the catalysts to negligible levels. Without the pretreatment, the activity for CO conversion as found to be 7 µmol CO/g CNT/s. The O-functionalized samples showed very activities greater than 85 µmol CO/g CNT/s with nearly 100% conversion. Analyses show that CO hydro-deoxygenation occurred at the C-O/O-H functional groups. It was found that while the products were similar to FT products, differences in selectivities were observed which, in turn, was a result of a different catalytic mechanism. These findings now open a new paradigm for CNT-based hydrogenation catalysts and constitute a defining point for obtaining clean, earth abundant, alternative fuels through the use of efficient and renewable catalyst.

Keywords: CNT, CO hydro-deoxygenation, DFT, liquid fuels, XPS, XTL.

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