Low Temperature DeNOx Technologies for Power and Waste Incineration Plants

Peter Westergaard Jakobsen

Research output: Book/ReportPh.D. thesis

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Formation of NOx is inevitable during high temperature combustion processes in air. NOx is of increasing environmental concern due to its participation in detrimental photochemical reactions, which lead to ozone layer depletion. NOx emissions also cause acid rain, contributes to smog formation and induces respiratory diseases in humans. There is no doubt that anthropogenic effects are contributing to the global climate change. The largest contributor to anthropogenic greenhouse gas emissions is CO2. been of great interest as a method to decrease global CO2 emissions. Some of the fuels that have drawn particular interest over the past decade is biomass and municipal waste. While the CO2 emissions are decreased by a transition to these fuels, other problems are caused by it. Potassium present in many of the alternative fuels lead to severe deactivation of the catalyst used for NOx abatement. Consequently, NOx abatement is currently not possible when these are used exclusively. Since NOx gasses are strong pollutants, the increased emission caused by using these alternative fuels is highly undesirable and hinders a more widespread use of alternative fuels. The work presented here has primarily been concerned with finding an alternative solution to NOx abatement for biomass and waste incineration. The optimal solution to this would be a tail-end deNOx unit, which operates at low temperatures (60-140°C). Previous work has shown that ionic liquids (ILs) are promising absorbers and can selectively absorb flue gas constituents such as CO2, SO2 and NO. Utilisation of ILs is severely limited by high viscosities, which hinders mass transfer across phase boundary layers. Dispersion of the IL onto a porous support has been suggested as a possible solution to this problem. In the present work, a vast variety of supported ionic liquid phase (SILP) materials have been tested in NO breakthrough experiments. Based on the obtained results, an attempt was made to understand the chemical and physical properties governing the SILP performance. Based on these investigations, characteristics of the optimal
support were suggested. It was found that hollow-sphere silica (HS) had properties close to what was considered optimal, therefore it was decided to investigate this support material further. Synthesis of the support material and subsequently SILP formulations utilising the HS-support material were carried out in collaboration with Prof. Dai at Oak Ridge National Laboratory. The resulting HS-SILP performed significantly better than any other SILP formulation tested in NO breakthrough experiments. Based on this performance, it was suggested that the HS-support could be ideal for selective absorption of other gasses using SILP absorbers. Some SILP formulations were found to have significant oxidative capabilities, willingly oxidising NO to higher NOx species. It was found that the observed effect was due to alcohol residuals in the SILP material from the impregnation process, despite careful evaporation and drying. In order to investigate this effect further, the effect of several alcohols were screened and showed promising results. Therefore, an experimental setup was built to investigate if the oxidation would occur under continuous flow conditions, and to determine the steady state oxidation rates. Significant steady state conversions were found under continuous flow conditions, with a high turn over number for methanol. The reaction proceeded over all porous surfaces, but the use of a SILP material seemed to increase the rate of oxidation significantly. 
Original languageEnglish
PublisherDTU Chemistry
Number of pages235
Publication statusPublished - 2017


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