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Oxidation dehydrogenation of n-butane over chromium and vanadium supported catalysts with CO2 as mild oxidant: Synthesis, characterization and kinetics
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Oxidation dehydrogenation of n-butane over chromium and vanadium supported catalysts with CO2 as mild oxidant: Synthesis, characterization and kinetics
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Oxidation dehydrogenation of n-butane over chromium and vanadium supported catalysts with CO2 as mild oxidant: Synthesis, characterization and kinetics
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Dissertation
Oxidation dehydrogenation of n-butane over chromium and vanadium supported catalysts with CO2 as mild oxidant: Synthesis, characterization and kinetics
2013
Overview
The study investigates the simple dehydrogenation of n-butane over mono (Cr or V) and bimetal (Cr-V) loaded MCM-41 catalysts. Wet impregnation technique was used, where the metal content maintained around 4wt.%. The unique properties of bimetal supported catalysts were evaluated by means of XRD, N2 adsorption, pyridine FT-IR, Raman spectroscopy, SEM-EDX, temperature programmed analysis (H2-TPR, NH3-TPD, CO2-TPD). The catalytic evaluation shows that Cr content of 1.2wt% and V content of 2.8wt% over MCM-41 designated as 1.2Cr2.8V/M-41 exhibited the highest butane conversion of 20.1% and butenes selectivity of 88.5% at 600 °C. In the presence of CO2, the stability of 1.2Cr2.8V/M-41catalyst was quite improved. The improved performance of bimetal catalysts can be correlated to synergetic effect of uniformly dispersed Cr-V-O mixed oxides over MCM-41, high reducibility and surface acidity. Oxidative dehydrogenation of n-butane was tested using CO2 as a mild oxidant over bimetallic Cr-V supported catalysts (MCM-41, ZSM-5, MCM-22 and mesoZSM-5). The metal content of Cr and V was maintained around 1.2wt.% and 2.8wt.% for the catalytic test in packed bed reactor at different temperatures (525–600°C) for 180 min. 1.2Cr2.8V/MCM-41 and 1.2Cr2.8V/ZSM-5 exhibited maximum conversion of 14 % and 13.1%, respectively at 10 min and 600 °C. Significantly, high butenes selectivity was observed over MCM-41 (86.27%) than ZSM-5 support (58.1%). The mesoporousity in ZSM-5 had a negative impact on conversion level (7.1%) but improved the butenes selectivity slightly. 1.2Cr2.8V/M-22 showed the highest cracking ability leading to overall reduced butenes selectivity (57.9%). The study shows that over all catalysts, n-butane conversion is independent of CO2 conversion. 1.2Cr2.8V/M-22 showed highest CO2 conversion in the range 2.35–2.2% between 525–550°C. The kinetics of n-butane dehydrogenation over 1.2Cr2.8V/M-41 catalyst was studied. The models were developed based on the catalyst tests carried out in a fixed bed reactor at reaction temperature varied from 525–575°C. Based on the experimental observations, power law type models were formulated and parameters were estimated by fitting the experimental data implemented in MATLAB.
Publisher
ProQuest Dissertations & Theses
Subject
ISBN
9781369525441, 1369525443
