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Description
Life Cycle Assessment (LCA) is used in the chemical process sector to compare the environmental merits of different product or process alternatives. One of the tasks that involves much time and cost in LCA studies is the specification of the exact materials and processes modeled which has limited its widespread application. To overcome this, researchers have recently created probabilistic underspecification as an LCA streamlining method, which uses a structured data classification system to enable an LCA modeler to specify materials and processes in a less precise manner. This study presents a statistical procedure to understand when streamlined LCA methods can be used, and what their impact on overall model uncertainty is. Petrochemicals and polymer product systems were chosen to examine the impacts of underspecification and mis-specification applied to LCA modeling. Ecoinvent database, extracted using GaBi software, was used for data pertaining to generic crude oil refining and polymer manufacturing modules. By assessing the variation in LCA results arising out of streamlined materials classification, the developed statistics estimate the amount of overall error incurred by underspecifying and mis-specifying material impact data in streamlined LCA. To test the impact of underspecification and mis-specification at the level of a product footprint, case studies of HDPE containers and aerosol air fresheners were conducted. Results indicate that the variation in LCA results decreases as the specificity of materials increases. For the product systems examined, results show that most of the variability in impact assessment is due to the differences in the regions from which the environmental impact datasets were collected; the lower levels of categorization of materials have relatively smaller influence on the variance. Analyses further signify that only certain environmental impact categories viz. global warming potential, freshwater eutrophication, freshwater ecotoxicity, human toxicity and terrestrial ecotoxicity are affected by geographic variations. Outcomes for the case studies point out that the error in the estimation of global warming potential increases as the specificity of a component of the product decreases. Fossil depletion impact estimates remain relatively robust to underspecification. Further, the results of LCA are much more sensitive to underspecification of materials and processes than mis-specification.
ContributorsMurali, Ashwin Krishna (Author) / Dooley, Kevin (Thesis advisor) / Dai, Lenore (Thesis advisor) / Nielsen, David (Committee member) / Arizona State University (Publisher)
Created2014
Description
Ethanol is a widely used biofuel in the United States that is typically produced through the fermentation of biomass feedstocks. Demand for ethanol has grown significantly from 2000 to 2015 chiefly due to a desire to increase energy independence and reduce the emissions of greenhouse gases associated with transportation. As demand grows, new ethanol plants must be developed in order for supply to meet demand. This report covers some of the major considerations in developing these new plants such as the type of biomass used, feed treatment process, and product separation and investigates their effect on the economic viability and environmental benefits of the ethanol produced. The dry grind process for producing ethanol from corn, the most common method of production, is examined in greater detail. Analysis indicates that this process currently has the highest capacity for production and profitability but limited effect on greenhouse gas emissions compared to less common alternatives.
ContributorsSchrilla, John Paul (Author) / Kashiwagi, Dean (Thesis director) / Kashiwagi, Jacob (Committee member) / Barrett, The Honors College (Contributor) / Chemical Engineering Program (Contributor)
Created2015-05
Description
Calcium hydroxide carbonation processes were studied to investigate the potential for abiotic soil improvement. Different mixtures of common soil constituents such as sand, clay, and granite were mixed with a calcium hydroxide slurry and carbonated at approximately 860 psi. While the carbonation was successful and calcite formation was strong on sample exteriors, a 4 mm passivating boundary layer effect was observed, impeding the carbonation process at the center. XRD analysis was used to characterize the extent of carbonation, indicating extremely poor carbonation and therefore CO2 penetration inside the visible boundary. The depth of the passivating layer was found to be independent of both time and choice of aggregate. Less than adequate strength was developed in carbonated trials due to formation of small, weakly-connected crystals, shown with SEM analysis. Additional research, especially in situ analysis with thermogravimetric analysis would be useful to determine the causation of poor carbonation performance. This technology has great potential to substitute for certain Portland cement applications if these issues can be addressed.
ContributorsHermens, Stephen Edward (Author) / Bearat, Hamdallah (Thesis director) / Dai, Lenore (Committee member) / Mobasher, Barzin (Committee member) / Barrett, The Honors College (Contributor) / Chemical Engineering Program (Contributor)
Created2015-05
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
Hydrothermal Liquefaction of Algae represents one of many pathways for the sustainable replacement of fossil fuels in transportation. When processing and researching algal biofuel, determination of the higher heating value (HHV) is paramount. Bomb calorimetry represents to current method for direct determination of HHV. When determining HHV’s indirectly, the industry standard is using one of many linear correlations relating elemental composition to HHV. Most of these correlations were developed from coal industry data, meaning that they do not necessarily fit algal product data well. In this study bomb calorimetry data and CHNS/O elemental composition data were collected for Chlorella, Micract, GS 5587.1, Kirchnella, and Gal 87.1 MM8 algae species. This data was added to CHNS/O and HHV values for other algal products in literature, and utilized to test the accuracy of the Dulong, Gumz, Vandralek and Boie correlations for algae products. Several preliminary algae specific correlations were proposed through a linear regression model of the data. Of the 5 samples tested, Kirchnella exhibited the highest HHV (23.2405 ± 0.0216 MJ/kg) and Chlorella exhibited the lowest (20.2055 ± 0.0484 MJ/kg). For both the experimental, and literature CHNS/O vs HHV data, the Vandralek and Boie correlations provided the best approximations in this study. For the totality of the data collected and researched in this study, 6 of 8 proposed correlations outperformed the Vandralek equation for HHV approximation. The most promising proposed correlations incorporated multiple linear regressions for elemental fractions of CHS, CHSO and CHNSO. Being that only 20 distinct algal product samples were regressed to create the proposed correlations, more data should be incorporated before publication of a final correlation. This study should serve as a starting point for the compilation of an exhaustive database for algal product assay and HHV data.
ContributorsCopp, Connor Joseph (Author) / Deng, Shuguang (Thesis director) / Muppaneni, Tapaswy (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2017-05
Description
p-Coumaric acid is used in the food, pharmaceutical, and cosmetic industries due to its versatile properties. While prevalent in nature, harvesting the compound from natural sources is inefficient, requiring large quantities of producing crops and numerous extraction and purification steps. Thus, the large-scale production of the compound is both difficult and costly. This research aims to produce p-coumarate directly from renewable and sustainable glucose using a co-culture of Yeast and E. Coli. Methods used in this study include: designing optimal media for mixed-species microbial growth, genetically engineering both strains to build the production pathway with maximum yield, and analyzing the presence of p-Coumarate and its pathway intermediates using High Performance Liquid Chromatography (HPLC). To date, the results of this project include successful integration of C4H activity into the yeast strain BY4741 ∆FDC1, yielding a strain that completely consumed trans-cinnamate (initial concentration of 50 mg/L) and produced ~56 mg/L p-coumarate, a resting cell assay of the co-culture that produced 0.23 mM p-coumarate from an initial L-Phenylalanine concentration of 1.14 mM, and toxicity tests that confirmed the toxicity of trans-cinnamate to yeast for concentrations above ~50 mg/L. The hope for this project is to create a feasible method for producing p-Coumarate sustainably.
ContributorsJohnson, Kaleigh Lynnae (Author) / Nielsen, David (Thesis director) / Thompson, Brian (Committee member) / Chemical Engineering Program (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
In the pursuit of sustainable sources of energy that do less harm to the environment, numerous technologies have been developed to reduce carbon emissions in the atmosphere. The implementation of carbon capture and storage systems (CCS) has played a crucial role in reducing CO2 emissions, but depleting storage reserves and ever-increasing costs of sequestrating captured CO2 has prompted the idea of utilizing CO2 as soon as it is produced (i.e. carbon capture and utilization, or CCU) and storing any remaining amounts. This project analyzes the cost of implementing a delafossite CuFeO2 backed CCU system for the average US coal-burning power plant with respect to current amounts of CO2 captured. Beyond comparing annual maintenance costs of CCU and CCS systems, the project extends previous work done on direct CO2 conversion to liquid hydrocarbons by providing a protocol for determining how the presence of NO affects the products formed during pure CO2 hydrogenation. Overall, the goal is to gauge the applicability of CCU systems to power plants with a sub 10-year lifespan left, whilst observing the potential revenue that can be potentially generated from CCU implementation. Under current energy costs ($0.12 per kWh), a delafossite CuFeO2 supported CCU system would generate over $729 thousand in profit for an average sized supercritical pulverized coal power (SCPC) plants selling diesel fuel created from CO2 hydrogenation. This amount far exceeds the cost of storing captured CO2 and suggests that CCU systems can be profitable for SCPC power plants that intend to burn coal until 2025.
ContributorsShongwe, Thembelihle Wakhile (Author) / Andino, Jean (Thesis director) / Otsengue, Thonya (Committee member) / Economics Program in CLAS (Contributor) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2018-05
Description
Polymer modified tuning fork-based sensors were fabricated to assure reproducibility. The effect of system valve switching on the modified tuning fork-based sensors was studied at the different temperature. The response to Xylene gas sample on stabilized modified tuning fork-based sensors with temperature was defined while learning about the key analytical performance for chemical sensors to be used in the real-world application.
ContributorsRohit, Riddhi S (Author) / Forzani, Erica (Thesis director) / Tsow, Francis (Committee member) / Dean, W.P. Carey School of Business (Contributor) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2017-05
Description
Plastics continue to benefit society in innumerable ways, even though recent public focus on plastics has centered mostly on human health and environmental concerns, including their endocrine-disrupting properties and the long-term pollution they represent. The benefits of plastics are particularly apparent in medicine and public health. Plastics are versatile, cost-effective, require less energy to produce than alternative materials like metal or glass, and can be manufactured to have many different properties. Due to these characteristics, polymers are used in diverse health applications like disposable syringes and intravenous bags, sterile packaging for medical instruments as well as in joint replacements, tissue engineering, etc. However, not all current uses of plastics are prudent and sustainable, as illustrated by the widespread, unwanted human exposure to endocrine-disrupting bisphenol A (BPA) and di-(2-ethylhexyl) phthalate (DEHP), problems arising from the large quantities of plastic being disposed of, and depletion of non-renewable petroleum resources as a result of the ever-increasing mass production of plastic consumer articles. Using the health-care sector as example, this review concentrates on the benefits and downsides of plastics and identifies opportunities to change the composition and disposal practices of these invaluable polymers for a more sustainable future consumption. It highlights ongoing efforts to phase out DEHP and BPA in the health-care and food industry and discusses biodegradable options for plastic packaging, opportunities for reducing plastic medical waste, and recycling in medical facilities in the quest to reap a maximum of benefits from polymers without compromising human health or the environment in the process.
ContributorsNorth, Emily Jean (Co-author) / Halden, Rolf (Co-author, Thesis director) / Mikhail, Chester (Committee member) / Hurlbut, Ben (Committee member) / Barrett, The Honors College (Contributor) / School of Mathematical and Statistical Sciences (Contributor) / Chemical Engineering Program (Contributor)
Created2013-05