1 |
Effect of Oxygen Concentration and Promoters on the Performance of Copper Catalysts During Catalytic Reduction of Nitrogen MonoxideLiu, Kai-Chung 14 September 2001 (has links)
This study utilized Cu-catalysts to catalyze a NO reduction reaction using CH4 as a reductant. Due to CH4 being a weak reductant and is easily affected by O2 concentration, we undertook a series experiments with O2 concentration and promoters, so that we could better understand their influence. The experiment conditions were as follows : reaction temperature between 150¢J- 800¢J¡Fa catalysts weight of 0.5 g¡F total gas flow rate of 1000 ml/min¡Frelative humidity at 0.9 %¡Fan O2 concentration between 0 - 6%¡Fand CH4 concentration between 1000 - 10000 ppm.
First, we sorted out the best metal carriers and calcining temperature, from this we decide to use £^-Al2O3 as a carrier with a calcining temperature under 500¢Jto produce our catalysts. During the O2 concentration experiment, when the inflow O2 concentration was below 1% (including 0% O2), Cu-catalysts reduce NO above 550¢J.The conversion reached a rate of 95 % at a temperature of 750¢J¡Fwhen the oxygen concentration was between 3% and 6% O2, catalysts reacted within 300 - 500¢J with NO converting to NO2¡Fat a concentration between 1.5% and 2% O2, NOx underwent reduction at 750¢J,and NOx conversion raised from 0 % to above 90%. Therefore in analyzing the experiment results, it shows that NOx will reduce violently when the O2 concentration is below 0.7% and while using CH4 as a reductant. This result was also apparent in O2 concentrations between 1.5 % and 2%. In the experiments of M/O ratio (the ratio of CH4 and O2 inflow), we found M/O ratio was not a deciding factor within the reaction mechanics, furthermore the limiting factor of O2 concentration decreases under 0.7%¡Fin addition it was also found that adding large amounts of CH4 could quicken the reduction process. Lastly, a mass balance was performed, which had a result over 70 %.
In the experiments where Y¡BLa¡BSr¡BCo were added as promoters to the Cu-catalysts, we found that Cu-La/£^-Al2O3¡BCu-Sr/£^-Al2O3 and Cu-Co/£^-Al2O3 can accelerate O2 depletion. Henceforth, it is possible to deduce promoters will be a useful method in solving O2 limiting. In the comparison of metals loading methods, we found no difference in activity using separate-impregnation and co-impregnation methods, whereas in the BET and SEM co-impregnation experiments, there was a larger surface-area and dispersion.
|
2 |
Catalytic Upgrading of Biogas to Fuels: Role of Reforming Temperature, Oxidation Feeds, and ContaminantsElsayed, Nada 23 January 2017 (has links)
Global energy demands are constantly increasing and fossil fuels are a finite resource. The shift towards alternative, more renewable and sustainable fuels is inevitable. Furthermore, the increased emissions of greenhouse gases have forced a pressing need to find cleaner, more environmentally friendly sources of fuel. Biomass energy is a promising alternative fuel because it offers several important advantages. It is a renewable energy form, it comes from many sources and produces biogas (CH4 and CO2). Furthermore, it can have a zero carbon footprint; this is due to the fact that the carbon produced is from the same carbon used to make the biomass. In addition, by replacing fossil fuels, the emissions of CH4 and CO2 (both greenhouse gases) is reduced. Biomass-derived syngas (H2 and CO) can be utilized as a feedstock for many important industrial processes such as methanol synthesis, ammonia synthesis and Fischer-Tropsch synthesis (FTS) to produce long chain hydrocarbon fuels.
Municipal solid waste (MSW) biomass is considered as the source of the biomass for this dissertation work. MSW accounts for 20% of man-made methane emissions making it an attractive source for utilization. However, methane reforming to synthesis gas (H2 and CO) typically occurs at temperatures higher than 600°C making it economically challenging at the smaller scale of MSW conversion processes.
This dissertation effort focused on formulating low precious metal loaded heterogeneous catalysts that can reform methane at low temperature (T<500°C) making the process more industrially viable. The effect of select contaminants (siloxanes) in the biogas on the reforming catalysts was studied through accelerated poisoning. Finally, the syngas ratio was improved by combining low temperature dry reforming with steam reforming (termed bi-reforming).
The catalyst system used for this dissertation study was comprised of 1.34wt%Ni- 1.00wt%Mg on a Ceria-Zirconia oxide support (0.6:0.4 ratio respectively). The catalysts were doped with platinum (0-0.64% by mass) and compared to palladium doped catalysts (0-0.51% by mass). The ratio chosen for the support, Ce0.6Zr0.4, was determined to be the best ratio in terms of activity and surface area by previous studies done in this group [1]. Nickel has been widely studied as methane reforming catalyst [2-6]. Alone, nickel atoms are prone to carbon deposition especially during methane decomposition, however, coupling NiO with MgO helps to reduce carbon deposition by reducing agglomeration of Ni crystallites, thereby improving catalyst lifetime [2, 7]. Furthermore, addition of small amounts of noble metals such as Pt or Pd help to drive the reduction of the catalyst to lower temperatures and enhance catalytic activity.
Different metal loadings of Pt and Pd were tested to determine the optimum catalyst that will reform methane at low temperatures, is resistant to deactivation and produces a high syngas ratio (~2:1) which is necessary for processes such as FTS. Preliminary results have shown that in general Pt is superior in this catalyst system for low temperature reforming of methane. It consistently had syngas ratios near the desired ratio compared to Pd, it did not deactivate with extended time on stream and overall had higher turnover frequencies. This catalyst system has potential to make industrial reforming of methane from biomass feedstock more economically viable.
|
Page generated in 0.0874 seconds