Matching Items (4)
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- Creators: Nielsen, David
- Creators: Phelan, Patrick
Description
Post-combustion carbon capture is a viable option for reducing CO2 greenhouse gas emissions, and one potentially promising technology for this route is adsorption using chemically and physically based sorbents. A number of exceptional CO2 sorbents materials have been prepared including metal organic frameworks, zeolites, and carbon based materials. One particular group of capable materials are amine based solid sorbents that has shown to possess high adsorption capacities and favorable adsorption kinetics. A key variable in the synthesis of an amine based sorbent is the support which acts as the platform for the amine modification. Aerogels, due to their high porosities and surface areas, appear to be a promising support for an amine modified CO2 sorbent. Therefore, in order to develop a commercially viable CO2 sorbent, particulate aerogels manufactured by Cabot Corporation through an economical and proprietary ambient drying process were modified with amines using a variety of functionalization methods. Two methods of physical impregnation of the amino polymer TEPA were performed in order to observe the performance as well as understand the effects of how the TEPA distribution is affected by the method of introduction. Both samples showed excellent adsorption capacities but poor cyclic stability for lack of any covalent attachment. Furthermore the method of TEPA impregnation seems to be independent on how the polymer will be distributed in the pore space of aerogel. The last two methods utilized involved covalently attaching amino silanes to the surface silanols of the aerogel. One method was performed in the liquid phase under anhydrous and hydrous conditions. The materials developed through the hydrous method have much greater adsorption capacities relative to the anhydrous sample as a result of the greater amine content present in the hydrous sample. Water is another source of silylation where additional silanes can attach and polymerize. These samples also possessed stable cyclic stability after 100 adsorption/regeneration cycles. The other method of grafting was performed in the gas phase through ALD. These samples possessed exceptionally high amine efficiencies and levels of N content without damaging the microstructure of the aerogel in contrast to the liquid phase grafted sorbents.
ContributorsLinneen, Nick (Author) / Lin, Jerry (Thesis advisor) / Pfeffer, Robert (Thesis advisor) / Lind, Mary (Committee member) / Rege, Kaushal (Committee member) / Nielsen, David (Committee member) / Anderson, James (Committee member) / Arizona State University (Publisher)
Created2014
Description
One the major problems of this modern industrialized world is its dependence on fossil fuels for its energy needs. Burning of fossils fuels generates green-house gases which have adverse effects on global climate contributing to global warming. According to Environmental Protection Agency (EPA), carbon dioxide makes up 80 percent of green-house gases emitted in USA. Electrochemical reduction of carbon dioxide is an approach which uses CO2 emissions to produce other useful hydrocarbons which can be used in many ways.
In this study, primary focus was on optimizing the operating conditions, determining the better catalyst material, and analyzing the reaction products for the process of electrochemical reduction of carbon dioxide (ERC). Membrane electrode assemblies (MEA’s) are developed by air bushing the metal particles with a spray gun on to Nafion-212 which is a solid polymer based electrolyte (SPE), to support the electrodes in the electrochemical reactor gas diffusion layers (GDL) are developed using porous carbon paper. Anode was always made using the same material which is platinum but cathode material was changed as it is the working electrode.
The membrane electrode assembly (MEA) is then placed into the electrochemical reactor along with gas diffusion layer (GDL) to assess the performance of the catalyst material by techniques like linear sweep voltammetry and chronoamperometry. Performance of MEA was analyzed at 4 different potentials, 2 different temperatures and for 2 different cathode catalyst materials. The reaction products of the process are analyzed using gas chromatography (GC) which has thermal conductivity detector (TCD) used for detecting hydrogen (H2), carbon monoxide (CO) and flame ionization detector (FID) used for detecting hydrocarbons. The experiments performed at 40o C gave the better results when compared with the experiments performed at ambient temperature. Also results suggested that copper oxide cathode catalyst has better durability than platinum-carbon. Maximum faradaic efficiency for methane was 5.3% it was obtained at 2.25V using copper oxide catalyst. Furthermore, experiments must be carried out to make the electrochemical reactor more robust to withstand all the operating conditions like higher potentials and to make it a solar powered reactor.
In this study, primary focus was on optimizing the operating conditions, determining the better catalyst material, and analyzing the reaction products for the process of electrochemical reduction of carbon dioxide (ERC). Membrane electrode assemblies (MEA’s) are developed by air bushing the metal particles with a spray gun on to Nafion-212 which is a solid polymer based electrolyte (SPE), to support the electrodes in the electrochemical reactor gas diffusion layers (GDL) are developed using porous carbon paper. Anode was always made using the same material which is platinum but cathode material was changed as it is the working electrode.
The membrane electrode assembly (MEA) is then placed into the electrochemical reactor along with gas diffusion layer (GDL) to assess the performance of the catalyst material by techniques like linear sweep voltammetry and chronoamperometry. Performance of MEA was analyzed at 4 different potentials, 2 different temperatures and for 2 different cathode catalyst materials. The reaction products of the process are analyzed using gas chromatography (GC) which has thermal conductivity detector (TCD) used for detecting hydrogen (H2), carbon monoxide (CO) and flame ionization detector (FID) used for detecting hydrocarbons. The experiments performed at 40o C gave the better results when compared with the experiments performed at ambient temperature. Also results suggested that copper oxide cathode catalyst has better durability than platinum-carbon. Maximum faradaic efficiency for methane was 5.3% it was obtained at 2.25V using copper oxide catalyst. Furthermore, experiments must be carried out to make the electrochemical reactor more robust to withstand all the operating conditions like higher potentials and to make it a solar powered reactor.
ContributorsMudunur, Santosh shekar (Author) / Kannan, Arunachala (Thesis advisor) / Phelan, Patrick (Committee member) / Huang, Huei-Ping (Committee member) / Arizona State University (Publisher)
Created2017
Description
Amine-modified solid sorbents and membrane separation are promising technologies for separation and capture of carbon dioxide (CO2) from combustion flue gas. Amine absorption processes are mature, but still have room for improvement. This work focused on the synthesis of amine-modified aerogels and metal-organic framework-5 (MOF-5) membranes for CO2 separation. A series of solid sorbents were synthesized by functionalizing amines on the surface of silica aerogels. This was done by three coating methods: physical adsorption, magnetically assisted impact coating (MAIC) and atomic layer deposition (ALD). CO2 adsorption capacity of the sorbents was measured at room temperature in a Cahn microbalance. The sorbents synthesized by physical adsorption show the largest CO2 adsorption capacity (1.43-1.63 mmol CO2/g). An additional sorbent synthesized by ALD on hydrophilic aerogels at atmospheric pressures shows an adsorption capacity of 1.23 mmol CO2/g. Studies on one amine-modified sorbent show that the powder is of agglomerate bubbling fluidization (ABF) type. The powder is difficult to fluidize and has limited bed expansion. The ultimate goal is to configure the amine-modified sorbents in a micro-jet assisted gas fluidized bed to conduct adsorption studies. MOF-5 membranes were synthesized on α-alumina supports by two methods: in situ synthesis and secondary growth synthesis. Characterization by scanning electron microscope (SEM) imaging and X-ray diffraction (XRD) show that the membranes prepared by both methods have a thickness of 14-16 μm, and a MOF-5 crystal size of 15-25 μm with no apparent orientation. Single gas permeation results indicate that the gas transport through both membranes is determined by a combination of Knudsen diffusion and viscous flow. The contribution of viscous flow indicates that the membranes have defects.
ContributorsRosa, Teresa M (Author) / Lin, Jerry (Thesis advisor) / Pfeffer, Robert (Thesis advisor) / Dai, Lenore (Committee member) / Nielsen, David (Committee member) / Arizona State University (Publisher)
Created2010
Description
About 20-50% of industrial processes energy is lost as waste heat in their operations. The thermal hydraulic engine relies on the thermodynamic properties of supercritical carbon dioxide (CO2) to efficiently perform work. Carbon dioxide possesses great properties that makes it a safe working fluid for the engine’s applications. This research aims to preliminarily investigate the actual efficiency which can be obtained through experimental data and compare that to the Carnot or theoretical maximum efficiency. The actual efficiency is investigated through three approaches. However, only the efficiency results from the second method are validated since the other approaches are based on a complete actual cycle which was not achieved for the engine. The efficiency of the thermal hydraulic engine is found to be in the range of 0.5% to 2.2% based on the second method which relies on the boundary work by the piston. The heating and cooling phases of the engine’s operation are viewed on both the T-s (temperature-entropy) and p-v (pressure-volume) diagrams. The Carnot efficiency is also found to be 13.7% from a temperature difference of 46.20C based on the measured experimental data. It is recommended that the thermodynamic cycle and efficiency investigation be repeated using an improved heat exchanger design to reduce energy losses and gains during both the heating and cooling phases. The temperature of CO2 can be measured through direct contact with the thermocouple and pressure measurements can be improved using a digital pressure transducer for the thermodynamic cycle investigation.
ContributorsManford, David (Author) / Phelan, Patrick (Thesis advisor) / Calhoun, Ronald (Thesis advisor) / Shuaib, Abdelrahman (Committee member) / Arizona State University (Publisher)
Created2020