Search results for: Deoxygenation

Authors: Tossaporn Jindarat, Siriporn Jongpatiwut, Somchai Osuwan, Suchada Butnark

Abstract:

Deoxygenation of beef fat for the production of hydrogenated biodiesel is investigated in a high pressure continuous flow fixed bed reactor over palladium-supported mesoporous titania catalyst synthesized via a combined single-step sol-gel process with surfactant-assisted templating method (SATM). The catalyst possessed a mesoporous charactheristic with high surface area and narrow pore size distribution. The main products of all Pd/TiO2 catalysts are n-heptadecane (n-C17) and n-pentadecane (n-C15) resulting from decarbonylation reaction. Pd/TiO2 catalyst synthesized via a combined single-step sol-gel process with SATM (SSSG) gave higher activity and selectivity to the desired products when compared to IWI/SG-TiO2 and IWI/P25-TiO2, respectively. SSSG catalyst gave the average conversion up to 80-90 % and 80 % for the selectivity in diesel range hydrocarbons. This result may cause by the higher surface area and the ability in dispersion of palladium ion in mesoporous of TiO2 during sol-gel process.

Keywords: Beef fat, Deoxygenation, Hydrogenated biodiesel, Pd/TiO2

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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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Authors: A. Pruna, D. Pullini, D. Busquets

Abstract:

Graphene-based materials were prepared by chemical reduction of covalently functionalized graphene oxide with environmentally friendly agents. Two varying stoichiometry of graphene oxide (GO) induced by using different chemical preparation conditions, further covalent functionalization of the GO materials with 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide hydrochloride / N-hydroxysuccinimide and ascorbic acid and sodium bisulfite as reducing agents were exploited in order to obtain controllable properties of the final solution-based graphene materials. The obtained materials were characterized by thermo-gravimetric analysis, Fourier transform infrared and Raman spectroscopy and X-ray diffraction. The results showed successful functionalization of the GO materials, while a comparison of the deoxygenation efficiency of the two-type functionalized graphene oxide suspensions by the different reducing agents has been made, revealing the strong dependence of their properties on the GO structure and reducing agents.

Keywords: Graphene oxide, covalent functionalization, reduction, ascorbic acid, sodium bisulfate.

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Authors: Panatcha Bovornseripatai, Siriporn Jongpatiwut, Somchai Osuwan, Suchada Butnark

Abstract:

Hydrogenated biodiesel is one of the most promising renewable fuels. It has many advantages over conventional biodiesel, including higher cetane number, higher heating value, lower viscosity, and lower corrosiveness due to its absence of oxygen. From previous work, Pd/TiO2 gave high conversion and selectivity in hydrogenated biodiesel. In this work, the effect of biomass feedstocks (i.e. beef fat, chicken fat, pork fat, and jatropha oil) on the production of hydrogenated biodiesel over Pd/TiO2 has been studied. Biomass feedstocks were analyzed by ICP-OES (inductively coupled plasma optical emission spectrometry) to identify the content of impurities (i.e. P, K, Ca, Na, and Mg). The deoxygenation catalyst, Pd/TiO2, was prepared by incipient wetness impregnation (IWI) and tested in a continuous flow packed-bed reactor at 500 psig, 325°C, H2/feed molar ratio of 30, and LHSV of 4 h-1 for its catalytic activity and selectivity in hydrodeoxygenation. All feedstocks gave high selectivity in diesel specification range hydrocarbons and the main hydrocarbons were n-pentadecane (n-C15) and n-heptadecane (n- C17), resulting from the decarbonylation/decarboxylation reaction. Intermediates such as oleic acid, stearic acid, palmitic acid, and esters were also detected in minor amount. The conversion of triglycerides in jatropha oil is higher than those of chicken fat, pork fat, and beef fat, respectively. The higher concentration of metal impurities in feedstock, the lower conversion of feedstock.

Keywords: Hydrogenated biodiesel, hydrodeoxygenation, Pd/TiO2, biomass feedstock

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