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Algal Fuels: A Future Less Green than the Plant

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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

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.

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2019-05

Heterogeneous Catalysis for Organic Reactions

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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

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

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2019-05

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Temperature dependency on baseline of polymer modified Tuning Forks

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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

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.

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2017-05

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Converting Combustion By-Products to Useful Chemicals and Fuels

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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

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.

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2018-05

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Carbon Dioxide Separation by Ceramic-Carbonate Dual-Phase Membranes and Process Design for Membrane Reactor in IGCC Power Plant

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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

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.

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2014-05

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Design of an Ethanol Fermentation Plant

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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

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.

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2015-05

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Sustainable Soil Improvement via Abiotic Carbon Dioxide Sequestration

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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

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.

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2015-05

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Engineering High Yield Production of L-Serine in Cyanobacterium Synechococcus sp. PCC 7002

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Cyanobacteria have the potential to efficiently produce L-serine, an industrially important amino acid, directly from CO2 and sunlight, which is a more sustainable and inexpensive source of energy as compared to current methods. The research aims to engineer a strain

Cyanobacteria have the potential to efficiently produce L-serine, an industrially important amino acid, directly from CO2 and sunlight, which is a more sustainable and inexpensive source of energy as compared to current methods. The research aims to engineer a strain of Cyanobacterium Synechococcus sp. PCC 7002 that increases L-serine production by mutating regulatory mechanisms that natively inhibit its production and encoding an exporter. While an excess of L-serine was not found in the supernatant of the cell cultures, with further fine tuning of the metabolic pathway and culture conditions, high titers of L-serine can be found. With the base strain engineered, the work can be extended and optimized by deleting degradation pathways, tuning gene expression levels, optimizing growth conditions, and investigating the effects of nitrogen supplementation for the strain.

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2020-05

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Plastics and Environmental Health: The Road Ahead

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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

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.

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2013-05

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Engineering a Co-Culture of Bacteria and Yeast for the Production of Renewable p-Coumaric Acid

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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.

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.

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2016-12