Sulfur dioxide (SO₂), a well-known pollutant emitted from fossil fuel combustion, has major adverse health and environmental impacts. It is harmful at low concentration with a permissible exposure limit of two ppm for the eight-hour time-weighted average (TWA) value. Fortunately, its atmospheric concentration, like other air pollutants, has gradually reduced in Canada in the past years. However, despite the well-established flue gas desulfurization technologies, they have the disadvantages of being energy-intensive, not very efficient to achieve very low concentrations (at ppm level) and they operate at high temperatures. Moreover, emission standards are becoming more stringent.
Novel methods are therefore investigated to capture SO₂, such as adsorption processes using zeolites and metal oxides (e.g., Iron (Fe) and Vanadium (V) based) which tend to sustain wide ranges of temperatures and pressures. Graphene oxide (GO) was also shown to physisorb SO₂ at low temperatures. In this work, we propose to metal functionalize GO as a step forward on the path for efficient SO₂ capture, by promoting the SO₂ oxidation reaction into sulfur trioxide (SO₃) for increased capacity due to a possible higher affinity with the surface. The GO has a high surface area, high porosity, and controllable surface chemistry. The aim is to achieve outlet concentration of SO₂ as low as 1 ppm through combined physisorption and reaction promoted that the presence of GO and metal, at low operating temperature.
Iron oxide functionalized GO was synthesized using two different techniques: a polyol process (GO-FeₓOᵧ-P) and using a hydrolysis method (GO-FeₓOᵧ-H). The characterization analysis, scanning electron microscopy (SEM) and transmission electron microscopy (TEM), performed on the materials before and after SO₂ reaction show changes on the surface due to metal adding and to the sulfur capture. The breakthrough curves and the capacity calculations of the performed experiments have shown that with the addition of FeₓOᵧ on the surface of GO, the capturing capacity increases by a factor of three to four, indicating a possible change in the capturing mechanism. The evaluation of the temperature effect (from room temperature to 100℃) showed an increasing trend in the capture capacity for SO₂ with an increase in temperature, for both functionalized and non-functionalized GO, indicating it is not driven only by surface adsorption. The presence of sulfur species captured from the gas stream has been confirmed by energy-dispersive X-ray (EDXS) analysis. The future work would be focused on the investigation of the mechanisms and capturing phenomenon and the regeneration step for the materials in order to further improve the capturing capacity and process applicability.
| Identifer | oai:union.ndltd.org:uottawa.ca/oai:ruor.uottawa.ca:10393/41945 |
| Date | 31 March 2021 |
| Creators | Sanyal, Tanushree Sankar |
| Contributors | Fauteux-Lefebvre, Clémence, Sowinski, Andrew |
| Publisher | Université d'Ottawa / University of Ottawa |
| Source Sets | Université d’Ottawa |
| Language | English |
| Detected Language | English |
| Type | Thesis |
| Format | application/pdf |
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