Molecular filtration : the study of adsorbents

Sammanfattning: Adsorbent materials for gas purification have been studied and developed for application in many areas. It is known that a single adsorbent may not adequately control multiple contaminants. Therefore, the development of adsorbent materials has accelerated over the past two decades, and is today an area attracting a lot of attention. In view of the global environmental movement for clean air, the development of improved sorbents will help address new challenges that cannot efficiently be met with the generic sorbents that are presently commercially available. On the other hand, the utilization of these new sorbents for specific applications within the area of molecular filtration remains largely unexplored. This thesis presents a synthesis of new sorbent materials, and the characterization and application of these materials for molecular filtration. Commercial adsorbents have been used for benchmarking for the pore properties, the applicability, and the performance of these new adsorbents. A double metal-silica adsorbent has been synthesized. The preparation procedure is based on the use of sodium silicate coagulated with various ratios of magnesium and calcium salts which yields micro-meso porous structures in the resulting material. The results show that molar ratios of Mg/Ca influence the pore parameters as well as the structure and morphology. The bimodal pore size can be tailored by controlling the Mg/Ca ratio. The effect of thermal treatment on pore parameters of these adsorbents has been investigated. The results show that heat treatment had a notable effect on the pore parameters, and that the pore structure was thermally stable even at 600°C.  A synthesis method has also been developed for the preparation of carbon-silica composites. The method involves a number of routes, which can be summarised as addition of activated carbon particles to (I) the paste, (II) the salt solution, or (III) with the sodium silicate solution. In route II and III the activated carbon is present also before coagulation. The routes presented here leads to carbon-silica composites possessing high micro porosity, meso porosity as well as large surface areas. The increase in micro porosity and surface areas was linear with carbon content. The results shows further that pore size distribution may be tailored based on the route of addition of the carbon particles. Following route I and III a wide pore size (1-30nm) was obtained where as by route II a narrow pore size (1-4nm) was observed. KOH or KMnO4 modified MgCa adsorbent varieties were also prepared. The impregnationwas performed by either a direct synthesis or post-synthesis procedure. Potassium hydroxide and potassium permanganate have been chosen as impregnate chemicals. Results revealed that theimpregnate amount significantly affected both the structural and the gas adsorption characteristics of the impregnated MgCa adsorbents. The properties of double- metal adsorbents, impregnated adsorbents and carbon-silica composites were characterized by various methods (X-ray diffraction, scanning electron microscopy, thermo gravimetric analysis, and nitrogen adsorption at 77K) to study the material structure and morphology, thermal stability, ignition temperature and porous parameters with regard to surface area, pore size, pore size distribution and porosity volume, which is important for optimizing their use in many practical application. The up-take performance of adsorbents for dynamic adsorption of SO2, H2S and toluene was performed in a system similar to the setup usedin ASHRAE 145.1. Finally the applicability and performance of the impregnated modified MgCa-silica adsorbents and composites have been evaluated for H2S, SO2 and toluene adsorption and compared to some commercial adsorbent materials. Results revealed that a potassium permanganate modified MgCa-adsorbent has a H2S adsorption capacity in the range of 0.08-3.19 wt % at 50% efficiency, and that the uptake capacity was relative to the amount of potassiumpermanganate loading. Moreover, KOH modified MgCa-adsorbent shows highest SO2 adsorption capacity (1.7 wt %) which is 3.47 times higher than commercial alumina impregnate with potassium permanganate (0.49 wt %). Carbon-silica composites on the other hand shows adsorption of toluene and high adsorption capacity was obtained when carbon content was 45 wt %. The results further shows that a composite with 45 wt % carbon and obtained via route I present the highest toluene adsorption capacity ( 27.6 wt % relative to carbon content) at 0% efficiency. The large uptake capacity of this composite was attributed to the presence of high microporosity volume and a wide (1-30nm) bimodal pore system consisting of extensive mesopore channels (2-30nm) as well as large surface area. These capacity values of carbon-silica composites are competitive to results obtained for commercial coconut based carbon (31 wt %), and better than commercial alumina-carbon composite.