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Description
Currently, approximately 40% of the world’s electricity is generated from coal and coal power plants are one of the major sources of greenhouse gases accounting for a third of all CO2 emissions. The Integrated Gasification Combined Cycle (IGCC) has been shown to provide an increase in plant efficiency compared to traditional coal-based power generation processes resulting in a reduction of greenhouse gas emissions. The goal of this project was to analyze the performance of a new SNDC ceramic-carbonate dual-phase membrane for CO2 separation. The chemical formula for the SNDC-carbonate membrane was Sm0.075Nd0.075Ce0.85O1.925. This project also focused on the use of this membrane for pre-combustion CO2 capture coupled with a water gas shift (WGS) reaction for a 1000 MW power plant. The addition of this membrane to the traditional IGCC process provides a purer H2 stream for combustion in the gas turbine and results in lower operating costs and increased efficiencies for the plant. At 900 °C the CO2 flux and permeance of the SNDC-carbonate membrane were 0.65 mL/cm2•min and 1.0×10-7 mol/m2•s•Pa, respectively. Detailed in this report are the following: background regarding CO2 separation membranes and IGCC power plants, SNDC tubular membrane preparation and characterization, IGCC with membrane reactor plant design, process heat and mass balance, and plant cost estimations.
ContributorsDunteman, Nicholas Powell (Author) / Lin, Jerry (Thesis director) / Dong, Xueliang (Committee member) / Barrett, The Honors College (Contributor) / Chemical Engineering Program (Contributor) / School of Sustainability (Contributor)
Created2014-05
Description
There are three known materials that readily undergo fission, allowing their use as a base for nuclear fuel: uranium-235, a naturally-occurring but uncommon isotope; plutonium, created from irradiated natural uranium; and uranium-233, produced from thorium. Of the three, uranium-235 and plutonium feature heavily in the modern nuclear industry, while uranium-233 and the thorium fuel cycle have failed to have significant presence in the field. Historically, nuclear energy development in the United States, and thorium development in particular, has been tied to the predominant societal outlook on the field, and thorium was only pursued seriously as an option during a period when nuclear energy was heavily favored, and resources seemed scarce. Recently, thorium-based energy has been experiencing a revival in interest in response to pollution concerns regarding fossil fuels. While public opinion is still wary of uranium, thorium-based designs could reduce reliance on fossil fuels while avoiding traditional drawbacks of nuclear energy. The thorium fuel cycle is more protected against proliferation, but is also much more expensive than the uranium-plutonium cycle in a typical reactor setup. Liquid-fueled molten salt reactor designs, however, bypass the prohibitive expense of U-233 refabrication by avoiding the stage entirely, keeping the chain reaction running with nothing but thorium input required. MSRs can use any fissile material as fuel, and are relatively safe to operate, due to passive features inherent to the design.
ContributorsGalbiati, Joseph Nicco (Author) / Martin, Thomas (Thesis director) / Foy, Joseph (Committee member) / Barrett, The Honors College (Contributor) / School of Sustainability (Contributor)
Created2014-05
Description
This paper seeks to analyze the relationship between energy subsidies on fossil fuels by countries and corresponding energy consumption, specifically electricity, by its citizens and occupants. The purpose of this was to determine whether pre-tax subsidies and post-tax subsidies have an effect on that consumption. This paper will discuss the prospect of accounting for post-tax subsidies as a method to curb rampant energy consumption throughout the world, with the focus being on residential electricity use. The two case studies, the Netherlands and Saudi Arabia, will illustrate the consumption patterns in relatively similar economic societies with different subsidy policies. Saudi Arabia will be a high pre-tax subsidy example while the Netherlands will be shown to account for some of the post-tax subsidies through an externality tax system. At the end of this analysis, this paper will show that the heavy subsidization of electricity production is strongly correlated to residential electricity consumption at levels that many officials would deem unsustainable, and that as such, subsidy reform is both beneficial and necessary.
ContributorsCorona, Kyle (Author) / Kelman, Jonathan (Thesis director) / Breetz, Hanna (Committee member) / School of Sustainability (Contributor, Contributor) / Economics Program in CLAS (Contributor) / Barrett, The Honors College (Contributor)
Created2016-12
Description
This honors thesis is focused on two separate catalysis projects conducted under the mentorship of Dr. Javier Pérez-Ramírez at ETH Zürich. The first project explored ethylene oxychlorination over supported europium oxychloride catalysts. The second project investigated alkyne semihydrogenation over nickel phosphide catalysts. This work is the subject of a publication of which I am a co-author, as cited below.
Project 1 Abstract: Ethylene Oxychlorination
The current two-step process for the industrial process of vinyl chloride production involves CuCl2 catalyzed ethylene oxychlorination to ethylene dichloride followed by thermal cracking of the latter to vinyl chloride. To date, no industrial application of a one-step process is available. To close this gap, this work evaluates a wide range of self-prepared supported CeO2 and EuOCl catalysts for one-step production of vinyl chloride from ethylene in a fixed-bed reactor at 623 773 K and 1 bar using feed ratios of C2H4:HCl:O2:Ar:He = 3:3 6:1.5 6:3:82 89.5. Among all studied systems, CeO2/ZrO2 and CeO2/Zeolite MS show the highest activity but suffer from severe combustion of ethylene, forming COx, while 20 wt.% EuOCl/γ-Al2O3 leads to the best vinyl chloride selectivity of 87% at 15.6% C2H4 conversion with complete suppression of CO2 formation and only 4% selectivity to CO conversion for over 100 h on stream. Characterization by XRD and EDX mapping reveals that much of the Eu is present in non-active phases such as Al2Eu or EuAl4, indicating that alternative synthesis methods could be employed to better utilize the metal. A linear relationship between conversion and metal loading is found for this catalyst, indicating that always part of the used Eu is available as EuOCl, while the rest forms inactive europium aluminate species. Zeolite-supported EuOCl slightly outperforms EuOCl/γ Al2O3 in terms of total yield, but is prone to significant coking and is unstable. Even though a lot of Eu seems locked in inactive species on EuOCl/γ Al2O3, these results indicate possible savings of nearly 16,000 USD per kg of catalyst compared to a bulk EuOCl catalyst. These very promising findings constitute a crucial step for process intensification of polyvinyl chloride production and exploring the potential of supported EuOCl catalysts in industrially-relevant reactions.
Project 2 Abstract: Alkyne Semihydrogenation
Despite strongly suffering from poor noble metal utilization and a highly toxic selectivity modifier (Pb), the archetypal catalyst applied for the three-phase alkyne semihydrogenation, the Pb-doped Pd/CaCO3 (Lindlar catalyst), is still being utilized at industrial level. Inspired by the very recent strategies involving the modification of Pd with p-block elements (i.e., S), this work extrapolates the concept by preparing crystalline metal phosphides with controlled stoichiometry. To develop an affordable and environmentally-friendly alternative to traditional hydrogenation catalysts, nickel, a metal belonging to the same group as Pd and capable of splitting molecular hydrogen has been selected. Herein, a simple two-step synthesis procedure involving nontoxic precursors was used to synthesize bulk nickel phosphides with different stoichiometries (Ni2P, Ni5P4, and Ni12P5) by controlling the P:Ni ratios. To uncover structural and surface features, this catalyst family is characterized with an array of methods including X-ray diffraction (XRD), 31P magic-angle nuclear magnetic resonance (MAS-NMR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). Bulk-sensitive techniques prove the successful preparation of pure phases while XPS analysis unravels the facile passivation occurring at the NixPy surface that persists even after reductive treatment. To assess the characteristic surface fingerprints of these materials, Ar sputtering was carried out at different penetration depths, reveling the presence of Ni+ and P-species. Continuous-flow three-phase hydrogenations of short-chain acetylenic compounds display that the oxidized layer covering the surface is reduced under reaction conditions, as evidenced by the induction period before reaching the steady state performance. To assess the impact of the phosphidation treatment on catalytic performance, the catalysts were benchmarked against a commercial Ni/SiO2-Al2O3 sample. While Ni/SiO2-Al2O3 presents very low selectivity to the alkene (the selectivity is about 10% at full conversion) attributed to the well-known tendency of naked nickel nanoparticles to form hydrides, the performance of nickel phosphides is highly selective and independent of P:Ni ratio. In line with previous findings on PdxS, kinetic tests indicate the occurrence of a dual-site mechanism where the alkyne and hydrogen do not compete for the same site.
This work is the subject of a publication of which I am a co-author, as cited below.
D. Albani; K. Karajovic; B. Tata; Q. Li; S. Mitchell; N. López; J. Pérez-Ramírez. Ensemble Design in Nickel Phosphide Catalysts for Alkyne Semi-Hydrogenation. ChemCatChem 2019. doi.org/10.1002/cctc.201801430
Project 1 Abstract: Ethylene Oxychlorination
The current two-step process for the industrial process of vinyl chloride production involves CuCl2 catalyzed ethylene oxychlorination to ethylene dichloride followed by thermal cracking of the latter to vinyl chloride. To date, no industrial application of a one-step process is available. To close this gap, this work evaluates a wide range of self-prepared supported CeO2 and EuOCl catalysts for one-step production of vinyl chloride from ethylene in a fixed-bed reactor at 623 773 K and 1 bar using feed ratios of C2H4:HCl:O2:Ar:He = 3:3 6:1.5 6:3:82 89.5. Among all studied systems, CeO2/ZrO2 and CeO2/Zeolite MS show the highest activity but suffer from severe combustion of ethylene, forming COx, while 20 wt.% EuOCl/γ-Al2O3 leads to the best vinyl chloride selectivity of 87% at 15.6% C2H4 conversion with complete suppression of CO2 formation and only 4% selectivity to CO conversion for over 100 h on stream. Characterization by XRD and EDX mapping reveals that much of the Eu is present in non-active phases such as Al2Eu or EuAl4, indicating that alternative synthesis methods could be employed to better utilize the metal. A linear relationship between conversion and metal loading is found for this catalyst, indicating that always part of the used Eu is available as EuOCl, while the rest forms inactive europium aluminate species. Zeolite-supported EuOCl slightly outperforms EuOCl/γ Al2O3 in terms of total yield, but is prone to significant coking and is unstable. Even though a lot of Eu seems locked in inactive species on EuOCl/γ Al2O3, these results indicate possible savings of nearly 16,000 USD per kg of catalyst compared to a bulk EuOCl catalyst. These very promising findings constitute a crucial step for process intensification of polyvinyl chloride production and exploring the potential of supported EuOCl catalysts in industrially-relevant reactions.
Project 2 Abstract: Alkyne Semihydrogenation
Despite strongly suffering from poor noble metal utilization and a highly toxic selectivity modifier (Pb), the archetypal catalyst applied for the three-phase alkyne semihydrogenation, the Pb-doped Pd/CaCO3 (Lindlar catalyst), is still being utilized at industrial level. Inspired by the very recent strategies involving the modification of Pd with p-block elements (i.e., S), this work extrapolates the concept by preparing crystalline metal phosphides with controlled stoichiometry. To develop an affordable and environmentally-friendly alternative to traditional hydrogenation catalysts, nickel, a metal belonging to the same group as Pd and capable of splitting molecular hydrogen has been selected. Herein, a simple two-step synthesis procedure involving nontoxic precursors was used to synthesize bulk nickel phosphides with different stoichiometries (Ni2P, Ni5P4, and Ni12P5) by controlling the P:Ni ratios. To uncover structural and surface features, this catalyst family is characterized with an array of methods including X-ray diffraction (XRD), 31P magic-angle nuclear magnetic resonance (MAS-NMR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). Bulk-sensitive techniques prove the successful preparation of pure phases while XPS analysis unravels the facile passivation occurring at the NixPy surface that persists even after reductive treatment. To assess the characteristic surface fingerprints of these materials, Ar sputtering was carried out at different penetration depths, reveling the presence of Ni+ and P-species. Continuous-flow three-phase hydrogenations of short-chain acetylenic compounds display that the oxidized layer covering the surface is reduced under reaction conditions, as evidenced by the induction period before reaching the steady state performance. To assess the impact of the phosphidation treatment on catalytic performance, the catalysts were benchmarked against a commercial Ni/SiO2-Al2O3 sample. While Ni/SiO2-Al2O3 presents very low selectivity to the alkene (the selectivity is about 10% at full conversion) attributed to the well-known tendency of naked nickel nanoparticles to form hydrides, the performance of nickel phosphides is highly selective and independent of P:Ni ratio. In line with previous findings on PdxS, kinetic tests indicate the occurrence of a dual-site mechanism where the alkyne and hydrogen do not compete for the same site.
This work is the subject of a publication of which I am a co-author, as cited below.
D. Albani; K. Karajovic; B. Tata; Q. Li; S. Mitchell; N. López; J. Pérez-Ramírez. Ensemble Design in Nickel Phosphide Catalysts for Alkyne Semi-Hydrogenation. ChemCatChem 2019. doi.org/10.1002/cctc.201801430
ContributorsTata, Bharath (Author) / Deng, Shuguang (Thesis director) / Muhich, Christopher (Committee member) / Chemical Engineering Program (Contributor, Contributor) / School of Sustainability (Contributor) / Barrett, The Honors College (Contributor)
Created2019-05
Description
Desorption processes are an important part of all processes which involve utilization of solid adsorbents such as adsorption cooling, sorption thermal energy storage, and drying and dehumidification processes and are inherently energy-intensive. Here, how those energy requirements can be reduced through the application of ultrasound for three widely used adsorbents namely zeolite 13X, activated alumina and silica gel is investigated. To determine and justify the effectiveness of incorporating ultrasound from an energy-savings point of view, an approach of constant overall input power of 20 and 25 W was adopted. To measure the extent of the effectiveness of using ultrasound, the ultrasonic-power-to-total power ratios of 0.2, 0.25, 0.4 and 0.5 were investigated and the results compared with those of no-ultrasound (heat only) at the same total power. Duplicate experiments were performed at three nominal frequencies of 28, 40 and 80 kHz to observe the influence of frequency on regeneration dynamics. Regarding moisture removal, application of ultrasound results in higher desorption rate compared to a non-ultrasound process. A nonlinear inverse proportionality was observed between the effectiveness of ultrasound and the frequency at which it is applied. Based on the variation of desorption dynamics with ultrasonic power and frequency, three mechanisms of reduced adsorbate adsorption potential, increased adsorbate surface energy and enhanced mass diffusion are proposed. Two analytical models that describe the desorption process were developed based on the experimental data from which novel efficiency metrics were proposed, which can be employed to justify incorporating ultrasound in regeneration and drying processes.
ContributorsDaghooghi Mobarakeh, Hooman (Author) / Phelan, Patrick (Thesis advisor) / Wang, Liping (Committee member) / Wang, Robert (Committee member) / Calhoun, Ronald (Committee member) / Deng, Shuguang (Committee member) / Arizona State University (Publisher)
Created2021
Description
Fossil fuels are currently the main source of energy in the world’s transportation sector. They are also the primary contributor to carbon emissions in the atmosphere, leading to adverse climate effects. The objective of the following research is to increase the yield and efficiency of algal biofuel in order to establish algal-derived fuel as a competitive alternative to predominantly used fossil fuels. Using biofuel commercially will reduce the cost of production and ultimately decrease additional carbon emissions. Experiments were performed using hydrothermal liquefaction (HTL) to determine which catalyst would enhance the algal biocrude oil and result in the highest quality biofuel product, as well as to find the optimal combination of processing temperature and manure co-liquefaction of biomass ratio. For the catalytic upgrading experiments, Micractenium Immerum algae was used in conjunction with pure H2, Pt/C, MO2C, and HZSM-5 catalysts at 350℃ and 400℃, 430 psi, and a 30-minute residence time to investigate the effects of catalyst choice and temperature on the crude oil yield. While all catalysts increased the carbon content of the crude oil, it was found that using HZSM-5 at 350℃ resulted in the greatest overall yield of about 75%. However, the Pt/C catalyst increased the HHV from 34.26 MJ/kg to 43.26 MJ/kg. Cyanidioschyzon merolae (CM) algae and swine manure were utilized in the co-liquefaction experiments, in ratios (algae to swine) of 80:20, 50:50, and 20:80 at temperatures of 300℃ and 330℃. It was found that a ratio of 80:20 at 330℃ produced the highest biocrude oil yield of 29.3%. Although the 80:20 experiments had the greatest biomass conversion and best supported the deacidification of the oil product, the biocrude oil had a HHV of 33.58 MJ/kg, the lowest between the three different ratios. However, all calorific values were relatively close to each other, suggesting that both catalytic upgrading and co-liquefaction can increase the efficiency and economic viability of algal biofuel.
ContributorsMurdock, Tessa A (Author) / Deng, Shuguang (Thesis director) / Varman, Arul (Committee member) / Chemical Engineering Program (Contributor, Contributor) / Barrett, The Honors College (Contributor)
Created2020-05
Description
Membrane-based technology for gas separations is currently at an emerging stage of advancement and adoption for environmental and industrial applications due to its substantial advantages like lower energy and operating costs over the conventional gas separation technologies. Unfortunately, the available polymeric (or organic) membranes suffer a trade-off between permeance and selectivity. Mixed matrix membranes (MMMs) containing two-dimensional (2D) metal-organic frameworks (MOFs) as fillers are a highly sought approach to redress this trade-off given their enhanced gas permeabilities and selectivities compared to the pure polymeric membrane. These MMMs are increasingly gaining attention by researchers due to their unique properties and wide small- and large-scale gas separation applications. However, straightforward and scalable methods for the synthesis of MOFs nanosheets have thus far been persistently elusive. This study reports the single-phase preparation, and characterization of MMMs with 2D MOFs nanosheets as fillers. The prepared MOF and the polymer matrix form the ‘dense’ MMMs which exhibit increased gas diffusion resistance, and thus improved separation abilities. The single-phase approach was more successful than the bi-phase at synthesizing the MOFs. The influence of sonication power and time on the characteristics and performance of the membranes are examined and discussed. Increasing the sonication power from 50% to 100% reduces the pore size. Additionally, the ultimate effect on the selectivity and permeance of the MMMs with different single gases is reported. Analysis of results with various gas mixers indicates further performance improvements in these MMMs could be achieved by increasing sonication time and tuning suitable membrane thicknesses. Reported results reveal that MMMs are excellent candidates for next-generation gas mixture separations, with potential applications in CO2 capture and storage, hydrogen recovery, alkene recovery from alkanes, and natural gas purification.
ContributorsNkuutu, John (Author) / Mu, Bin (Thesis director) / Shan, Bohan (Committee member) / Chemical Engineering Program (Contributor) / School of Sustainability (Contributor) / Barrett, The Honors College (Contributor)
Created2019-05
Description
Drilling in Section 1002 has been an ongoing debate since the region was designated as a potential area for drilling projects, pending congressional approval in 1980. In 2017, the area was officially opened up for oil and gas development through its passage in the GOP Tax Cuts and Jobs Act of 2017. This act requires 2 lease sales of 400,000 acres, with an allowed 2,000 acre physical footprint (not including pipelines, ice roads, or gravel mines). Using Social-Life Cycle Assessment methodology to assess the process of oil extraction in Section 1002, significant benefits and drawbacks of drilling in this region, with economic, cultural, and social impacts ranging from the local level to the state level to the national level were identified.
Stakeholders impacted by oil development in the Section 1002 region include the Kaktovik community who lives within the Program Area, the Gwich’in people who live south of ANWR, the corporations who will be leasing the land, as well as the employees who will be working on the projects. These stakeholders share similar values and interests, however, when it comes down to the attainment of these values, there are significant differences in opinion. This debate comes down specifically to the desire to ensure stability for one’s family and community, as this means 2 different things to the majority stakeholders on this issue: The Inupiaq and the Gwich’in. The Inupiaq ,who live in Kaktovik specifically ,are particularly keen on the idea of drilling in the Section 1002 region, because the revenues and opportunities that come with the oil and gas development provide access to better standards of living and a more westernized way of life. The Gwich’in, however, value their relationship to the land and the caribou that are at risk of significant change. These 2 groups are critical to the debate, but the state and federal governments have the final say, and a financial incentive to move forward with the lease sales.
Utilizing the S-LCA framework, life cycle impacts of drilling on society are found using indicators that are identified and assessed using both qualitative and quantitative means. Although some conclusions are uncertain due to the forward-looking nature of this S-LCA, the Increasing/Decreasing trends can be identified and confidently attributed to the specific indicators.
Significant Results:
Significant issues this study has highlighted include the resulting impacts, both positive and negative, on the communities affected by oil and gas development in Section 1002. Significant stakeholders include the Kaktovik community, the Gwich’in people, the oil and gas workers in the state of Alaska, and the oil and gas companies themselves. The local residents are the most affected by the impacts of development, with significant issues pertaining to potential for significant lifestyle change, the increased risk of impact on subsistence species, the risks associated with pollution, and the effect on the economy through revenues and job availability.
Stakeholders impacted by oil development in the Section 1002 region include the Kaktovik community who lives within the Program Area, the Gwich’in people who live south of ANWR, the corporations who will be leasing the land, as well as the employees who will be working on the projects. These stakeholders share similar values and interests, however, when it comes down to the attainment of these values, there are significant differences in opinion. This debate comes down specifically to the desire to ensure stability for one’s family and community, as this means 2 different things to the majority stakeholders on this issue: The Inupiaq and the Gwich’in. The Inupiaq ,who live in Kaktovik specifically ,are particularly keen on the idea of drilling in the Section 1002 region, because the revenues and opportunities that come with the oil and gas development provide access to better standards of living and a more westernized way of life. The Gwich’in, however, value their relationship to the land and the caribou that are at risk of significant change. These 2 groups are critical to the debate, but the state and federal governments have the final say, and a financial incentive to move forward with the lease sales.
Utilizing the S-LCA framework, life cycle impacts of drilling on society are found using indicators that are identified and assessed using both qualitative and quantitative means. Although some conclusions are uncertain due to the forward-looking nature of this S-LCA, the Increasing/Decreasing trends can be identified and confidently attributed to the specific indicators.
Significant Results:
Significant issues this study has highlighted include the resulting impacts, both positive and negative, on the communities affected by oil and gas development in Section 1002. Significant stakeholders include the Kaktovik community, the Gwich’in people, the oil and gas workers in the state of Alaska, and the oil and gas companies themselves. The local residents are the most affected by the impacts of development, with significant issues pertaining to potential for significant lifestyle change, the increased risk of impact on subsistence species, the risks associated with pollution, and the effect on the economy through revenues and job availability.
ContributorsJunglas, Hillary L (Author) / Pasqualetti, Martin (Thesis director) / Breetz, Hanna (Committee member) / Department of Supply Chain Management (Contributor) / School of Sustainability (Contributor) / Barrett, The Honors College (Contributor)
Created2019-05
Description
The algal fuel industry has existed since the 1980s without fully commercializing a product. Algal fuels are potentially viable replacements for fossil fuels due to their fast cultivation, high oil content, carbon dioxide sequestration during growth, and ability to be grown on non-arable land. For this thesis, six companies from 61 investigated were interviewed about their history with biofuels, technological changes they have gone through, and views for the future of the industry. All companies interviewed have moved away from fuel production largely due to high production costs and have moved primarily toward pharmaceuticals and animal feed production as well as wastewater treatment. While most do not plan to return to the biofuel industry in the near future, a return would likely require additional legislation, increased technological innovation, and coproduction of multiple products.
ContributorsMassey, Alexandria Rae (Author) / Parker, Nathan (Thesis director) / Agusdinata, Buyung (Committee member) / Chemical Engineering Program (Contributor, Contributor) / School of Sustainability (Contributor) / Barrett, The Honors College (Contributor)
Created2019-05