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- All Subjects: Environmental engineering
- Genre: Academic theses
- Status: Published
Description
The large-scale anthropogenic emission of carbon dioxide into the atmosphere leads to many unintended consequences, from rising sea levels to ocean acidification. While a clean energy infrastructure is growing, mid-term strategies that are compatible with the current infrastructure should be developed. Carbon capture and storage in fossil-fuel power plants is one way to avoid our current gigaton-scale emission of carbon dioxide into the atmosphere. However, for this to be possible, separation techniques are necessary to remove the nitrogen from air before combustion or from the flue gas after combustion. Metal-organic frameworks (MOFs) are a relatively new class of porous material that show great promise for adsorptive separation processes. Here, potential mechanisms of O2/N2 separation and CO2/N2 separation are explored.
First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
ContributorsMcIntyre, Sean (Author) / Mu, Bin (Thesis advisor) / Green, Matthew (Committee member) / Lind, Marylaura (Committee member) / Arizona State University (Publisher)
Created2019
Description
Plastic pollution has become a global threat to ecosystems worldwide, with microplastics now representing contaminants reported to occur in ambient air, fresh water, seawater, soils, fauna and people. Over time, larger macro-plastics are subject to weathering and fragmentation, resulting in smaller particles, termed ‘microplastics’ (measuring < 5 mm in diameter), which have been found to pollute virtually every marine and terrestrial ecosystem on the planet. This thesis explored the transfer of plastic pollutants from consumer products into the built water environment and ultimately into global aquatic and terrestrial ecosystems.
A literature review demonstrated that municipal sewage sludge produced by wastewater treatment plants around the world contains detectable quantities of microplastics. Application of sewage sludge on land was shown to represent a mechanism for transfer of microplastics from wastewater into terrestrial environments, with some countries reporting as high as 113 ± 57 microplastic particles per gram of dry sludge.
To address the notable shortcoming of inconsistent reporting practices for microplastic pollution, this thesis introduced a novel, online calculator that converts the number of plastic particles into the unambiguous metric of mass, thereby making global studies on microplastic pollution directly comparable.
This thesis concludes with an investigation of a previously unexplored and more personal source of plastic pollution, namely the disposal of single-use contact lenses and an assessment of the magnitude of this emerging source of environmental pollution. Using an online survey aimed at quantifying trends with the disposal of lenses in the US, it was discovered that 20 ± 0.8% of contact lens wearers flushed their used lenses down the drain, amounting to 44,000 ± 1,700 kg y-1 of lens dry mass discharged into US wastewater.
From the results it is concluded that conventional and medical microplastics represent a significant global source of pollution and a long-term threat to ecosystems around the world. Recommendations are provided on how to limit the entry of medical microplastics into the built water environment to limit damage to ecosystems worldwide.
A literature review demonstrated that municipal sewage sludge produced by wastewater treatment plants around the world contains detectable quantities of microplastics. Application of sewage sludge on land was shown to represent a mechanism for transfer of microplastics from wastewater into terrestrial environments, with some countries reporting as high as 113 ± 57 microplastic particles per gram of dry sludge.
To address the notable shortcoming of inconsistent reporting practices for microplastic pollution, this thesis introduced a novel, online calculator that converts the number of plastic particles into the unambiguous metric of mass, thereby making global studies on microplastic pollution directly comparable.
This thesis concludes with an investigation of a previously unexplored and more personal source of plastic pollution, namely the disposal of single-use contact lenses and an assessment of the magnitude of this emerging source of environmental pollution. Using an online survey aimed at quantifying trends with the disposal of lenses in the US, it was discovered that 20 ± 0.8% of contact lens wearers flushed their used lenses down the drain, amounting to 44,000 ± 1,700 kg y-1 of lens dry mass discharged into US wastewater.
From the results it is concluded that conventional and medical microplastics represent a significant global source of pollution and a long-term threat to ecosystems around the world. Recommendations are provided on how to limit the entry of medical microplastics into the built water environment to limit damage to ecosystems worldwide.
ContributorsRolsky, Charles (Author) / Halden, Rolf (Thesis advisor) / Green, Matthew (Committee member) / Neuer, Susanne (Committee member) / Polidoro, Beth (Committee member) / Smith, Andrew (Committee member) / Arizona State University (Publisher)
Created2020
Description
Per- and polyfluoroalkyl substances (PFAS) are anthropogenic chemicals used for a wide variety of products and industrial processes, including being an essential class of chemicals in the fabrication of semiconductors. Proven concerns related to bioaccumulation and toxicity across multiple species have resulted in health advisory and regulatory initiatives for PFAS in drinking and wastewaters. Among impacted users of PFAS, the semiconductor industry is in urgent need of technologies to remove PFAS from water. Specifically, they prefer technologies capable of mineralizing PFAS into inorganic fluoride (F-). The goal of this thesis is to compare the effectiveness of photo- versus electrocatalytic treatment in benchtop reactor systems PFAS in industrial wastewater before selecting one technology to investigate comprehensively. First, a model wastewater was developed based upon semiconductor samples to represent water matrices near where PFAS are used and the aggregate Fab effluent, which were then used in batch catalytic experiments. Second, batch experiments with homogenous photocatalysis (UV/SO32-) were found to be more energy-intensive than heterogeneous catalysis using boron-doped diamond (BDD) electrodes, and the latter approach was then studied in-depth.
During electrocatalysis, longer chain PFAS (C8; PFOA & PFOS) were observed to degrade faster than C6 and C4 PFAS. This study is the first to report near-complete defluorination of not only C8- and C6- PFAS, but also C4-PFAS, in model wastewaters using BDD electrocatalysis, and the first to report such degradation in real Fab wastewater effluents. Based upon differences in PFAS degradation rates observed in single-solute systems containing only C4 PFAS versus multi-solute systems including C4, C6, and C8 PFAS, it was concluded that the surfactant properties of the longer-chain PFAS created surface films on the BDD electrode surface which synergistically enhanced removal of shorter-chain PFAS. The results from batch experiments that serve as the basis of this thesis will be used to assess the chemical byproducts and their associated bioaccumulation and toxicity. This thesis was aimed at developing an efficient method for the degradation of perfluoroalkyl substances from industrial process waters at realistic concentrations.
ContributorsNienhauser, Alec Brockway (Author) / Westerhoff, Paul (Thesis advisor) / Garcia-Segura, Sergi (Committee member) / Thomas, Marylaura (Committee member) / Green, Matthew (Committee member) / Arizona State University (Publisher)
Created2021