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- All Subjects: Environmental engineering
- Creators: Westerhoff, Paul
- Resource Type: Text
Description
Limited access to clean water due to natural or municipal disasters, drought, or contaminated wells is driving demand for point-of-use and humanitarian drinking water technologies. Atmospheric water capture (AWC) can provide water off the centralized grid by capturing water vapor in ambient air and condensing it to a liquid. The overarching goal of this dissertation was to define geographic and thermodynamic design boundary conditions for AWC and develop nanotechnology-enabled AWC technologies to produce clean drinking water.
Widespread application of AWC is currently limited because water production, energy requirement, best technology, and water quality are not parameterized. I developed a geospatial climatic model for classical passive solar desiccant-driven AWC, where water vapor is adsorbed onto a desiccant bed at night, desorbed by solar heat during the day, and condensed. I concluded passive systems can capture 0.25–8 L/m2/day as a function of material properties and climate, and are limited because they only operate one adsorption-desorption-condensation cycle per day. I developed a thermodynamic model for large-scale AWC systems and concluded that the thermodynamic limit for energy to saturate and condense water vapor can vary up to 2-fold as a function of climate and mode of saturation.
Thermodynamic and geospatial models indicate opportunity space to develop AWC technologies for arid regions where solar radiation is abundant. I synthesized photothermal desiccants by optimizing surface loading of carbon black nanoparticles on micron-sized silica gel desiccants (CB-SiO2). Surface temperature of CB-SiO2 increased to 60oC under solar radiation and water vapor desorption rate was 4-fold faster than bare silica. CB-SiO2 could operate >10 AWC cycles per day to produce 2.5 L/m2/day at 40% relative humidity, 3-fold more water than a conventional passive system.
Models and bench-scale experiments were paired with pilot-scale experiments operating electrical desiccant and compressor dehumidifiers outdoors in a semi-arid climate to benchmark temporal water production, water quality and energy efficiency. Water quality varied temporally, e.g, dissolved organic carbon concentration was 3 – 12 mg/L in the summer and <1 mg/L in the winter. Collected water from desiccant systems met all Environmental Protection Agency standards, while compressor systems may require further purification for metals and turbidity.
Widespread application of AWC is currently limited because water production, energy requirement, best technology, and water quality are not parameterized. I developed a geospatial climatic model for classical passive solar desiccant-driven AWC, where water vapor is adsorbed onto a desiccant bed at night, desorbed by solar heat during the day, and condensed. I concluded passive systems can capture 0.25–8 L/m2/day as a function of material properties and climate, and are limited because they only operate one adsorption-desorption-condensation cycle per day. I developed a thermodynamic model for large-scale AWC systems and concluded that the thermodynamic limit for energy to saturate and condense water vapor can vary up to 2-fold as a function of climate and mode of saturation.
Thermodynamic and geospatial models indicate opportunity space to develop AWC technologies for arid regions where solar radiation is abundant. I synthesized photothermal desiccants by optimizing surface loading of carbon black nanoparticles on micron-sized silica gel desiccants (CB-SiO2). Surface temperature of CB-SiO2 increased to 60oC under solar radiation and water vapor desorption rate was 4-fold faster than bare silica. CB-SiO2 could operate >10 AWC cycles per day to produce 2.5 L/m2/day at 40% relative humidity, 3-fold more water than a conventional passive system.
Models and bench-scale experiments were paired with pilot-scale experiments operating electrical desiccant and compressor dehumidifiers outdoors in a semi-arid climate to benchmark temporal water production, water quality and energy efficiency. Water quality varied temporally, e.g, dissolved organic carbon concentration was 3 – 12 mg/L in the summer and <1 mg/L in the winter. Collected water from desiccant systems met all Environmental Protection Agency standards, while compressor systems may require further purification for metals and turbidity.
ContributorsMulchandani, Anjali (Author) / Westerhoff, Paul (Thesis advisor) / Rittmann, Bruce (Committee member) / Álvarez, Pedro (Committee member) / Herckes, Pierre (Committee member) / Arizona State University (Publisher)
Created2020
Description
Engineered nanomaterials (ENMs) are added to numerous consumer products to enhance their effectiveness, whether it be for environmental remediation, mechanical properties, or as dietary supplements. Uses of ENMs include adding to enhance products, carbon for strength or dielectric properties, silver for antimicrobial properties, zinc oxide for UV sun-blocking properties, titanium dioxide for photocatalysis, or silica for desiccant properties. However, concerns arise from ENM functional properties that can impact the environment and a lack of regulation regarding ENMs leads to potential public exposure to ENMs and results in ill-informed public or manufacturer perceptions of ENMs. My dissertation evaluates the environmental, human health, and societal impacts of using ENMs, with a focus on ionic silver and nanosilver, in consumer and industrial products. Reproducible experiments served as functional assays to assess ENM distributions among various environmental matrices. Functional assay results were visualized using radar plots and aid in a framework to estimate likely ENM disposition in the environment. To assess beneficial uses of ENMs, bromide ion removal from drinking waters to limit disinfection by-product formation was studied. Silver-enabled graphene oxide materials were capable of removing bromide from water, and exhibited less competition from background solutes (e.g. natural organic matter) when compared against solely ionic silver addition to water for bromide removal. To assess complex interactions of ENMs with the microbiome, batch experiments were performed using fecal samples spiked with ionic silver or commercial dietary silver nanoparticles. Dietary nanosilver and ionic silver exposures to the fecal microbiome for 24 hours reduce short chain fatty acid (SCFA) production and changes the relative abundance of the microbiota. To understand the social perceptions of ENMS, statistically rigorous surveys were conducted to assess related perceptions related to the use of ENMs in drinking water treatment devices the general public and, separately, industrial manufacturers. These stakeholders are influenced by costs and efficiency of the technologies, consumer concerns of the safety of technologies, and environmental health and safety of the technologies. This dissertation represents novel research that took an interdisciplinary approach, spanning from wet-lab engineering bench scale testing to social science survey assessments to better understand the environmental, human health, and societal impacts of using ENMs such as nanosilver and ionic silver in industrial processes and consumer products.
ContributorsKidd, Justin (Author) / Westerhoff, Paul (Thesis advisor) / Krajmalnik-Brown, Rosa (Committee member) / Perreault, Francois (Committee member) / Maynard, Andrew (Committee member) / Arizona State University (Publisher)
Created2020
Description
Per- and polyfluoroalkyl substances (PFAS) are a group of man-made chemicals that are detected ubiquitously in the aquatic environment, biota, and humans. Human exposure and adverse health of PFAS through consuming impacted drinking water is getting regulatory attention. Adsorption using granular activated carbon (GAC) and ion exchange resin (IX) has proved to be efficient in removing PFAS from water. There is a need to study the effectiveness of commercially available sorbents in PFAS removal at the pilot-scale with real PFAS contaminated water, which would aid in efficient full-scale plant design. Additionally, there is also a need to have validated bench-scale testing techniques to aid municipalities and researchers in selecting or comparing adsorbents to remove PFAS. Rapid Small-Scale Column Tests (RSSCTs) are bench-scale testing to assess media performance and operational life to remove trace organics but have not been validated for PFAS. Different design considerations exist for RSSCTs, which rely upon either proportional diffusivity (PD) or constant diffusivity (CD) dimensionless scaling relationships.
This thesis aims to validate the use of RSSCTs to simulate PFAS breakthrough in pilot columns. First, a pilot-scale study using two GACs and an IX was conducted for five months at a wellsite in central Arizona. PFAS adsorption capacity was greatest for a commercial IX, and then two GAC sources exhibited similar performance. Second, RSSCTs scaled using PD or CD relationships, simulated the pilot columns, were designed and performed. For IX and the two types of GAC, the CD–RSSCTs simulated the PFAS breakthrough concentration, shape, and order of C8 to C4 compounds observed pilot columns better than the PD-RSSCTs. Finally, PFAS breakthrough and adsorption capacities for PD- and CD-RSSCTs were performed on multiple groundwaters (GWs) from across Arizona to assess the treatability of PFAS chain length and functional head-group moieties. PFAS breakthrough in GAC and IX was dictated by chain length (C4>C6>C8) and functional group (PFCAs>PFSAs) of the compound. Shorter-chain PFAS broke through earlier than the longer chain, and removal trends were related to the hydrophobicity of PFAS. Overall, single-use IX performed superior to any of the evaluated GACs across a range of water chemistries in Arizona GWs.
This thesis aims to validate the use of RSSCTs to simulate PFAS breakthrough in pilot columns. First, a pilot-scale study using two GACs and an IX was conducted for five months at a wellsite in central Arizona. PFAS adsorption capacity was greatest for a commercial IX, and then two GAC sources exhibited similar performance. Second, RSSCTs scaled using PD or CD relationships, simulated the pilot columns, were designed and performed. For IX and the two types of GAC, the CD–RSSCTs simulated the PFAS breakthrough concentration, shape, and order of C8 to C4 compounds observed pilot columns better than the PD-RSSCTs. Finally, PFAS breakthrough and adsorption capacities for PD- and CD-RSSCTs were performed on multiple groundwaters (GWs) from across Arizona to assess the treatability of PFAS chain length and functional head-group moieties. PFAS breakthrough in GAC and IX was dictated by chain length (C4>C6>C8) and functional group (PFCAs>PFSAs) of the compound. Shorter-chain PFAS broke through earlier than the longer chain, and removal trends were related to the hydrophobicity of PFAS. Overall, single-use IX performed superior to any of the evaluated GACs across a range of water chemistries in Arizona GWs.
ContributorsVenkatesh, Krishishvar (Author) / Westerhoff, Paul (Thesis advisor) / Sinha, Shahnawaz (Committee member) / Lind, Marylaura (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
Description
Halogens in drinking water sources, such as bromine (Br) and iodine (I) pose no direct health risk, but are critical precursors in formation of cyto- and genotoxic brominated and iodinated (Br-/I-) DBPs. However, few spatial or historic datasets exist for bromine and iodine species in drinking water sources. This dissertation aims to quantify and understand the occurrence and speciation of Br and I in groundwater and surface water serving as source waters for drinking water treatment plants (DWTPs). Aggregation of data from >9000 non-drinking water sampling locations in USA collected from 1930-2017 on halides (bromide (Br-) and iodide (I-)) determined that Br- concentrations were 50 μg/L and 100 μg/L; and I- concentrations were 12 μg/L and 13 μg/L in surface and groundwater respectively. Although, these locations were not drinking water sources, this first of its kind analysis provides potential bounds for Br- and I-. To focus specifically on DWTP sources, a nationwide survey of >250 drinking water sources was conducted between 2018-2020. Br- ion is the only bromine specie, whereas both inorganic (iodide and iodate ions) and organic iodine occur. I- concentrations ranged from 1-250 μg/L and are 4 to 100 times lower than Br- concentrations (10-7800 μg/L, median=80 μg/L). No strong correlation exists between bromide and iodide occurrence (R<0.5, p<0.005). I- was detected in 50% of the samples (75th percentile=5 μg/L) and IO3- was detected in 40% (75th percentile=3 μg/L) of all the samples. To quantify iodine species, tandem ion chromatography and inductively coupled plasma mass spectrometry was applied for the first time in drinking water sources. I- and IO3- peaks were well resolved and have minimum detection limit of 0.4 μg/L and 0.7 μg/L respectively. Organic iodine (Org-I) peaks in select drinking water samples from the nationwide survey were partically resolved ranging from <5 to 40 μg/L. This dissertation provides updated nationwide Br- survey and first ever national I species survey. The data generated through this dissertation will be useful to further Br-/I-DBP formation and toxicity research by providing relevant drinking water sources information. Future research targeting Br- and I- removal is advocated for managing Br-/I-DBPs in watersheds.
ContributorsSharma, Naushita (Author) / Westerhoff, Paul (Thesis advisor) / Karanfil, Tanju (Committee member) / Herckes, Pierre (Committee member) / Lackner, Klaus (Committee member) / Arizona State University (Publisher)
Created2021
Description
Nearly 2.1 billion people around the world to date do not have access to safe drinking water. This study proposes a compact (2-L) upflow photoreactor that uses widely available photocatalysts material, such as titanium dioxide (TiO2) or hexagonal boron nitrate (hBN), to oxidize toxic micropollutants. Photocatalysts, such as TiO2, can create powerful hydroxyl radicals (OH•) under UV irradiation to oxidize and disinfect water with various toxic pollutants present in untreated waters. The study assesses this along with few other photoreactors in terms of their performance with an indicator dye, such as methyl orange (MO), para-chlorobenzoic acid (pCBA), as an intermediate of pesticides, and perfluorooctanoic acid (PFOA), part of the per- and polyfluoroalkyl substances (PFAS), a highly persistent organic contaminant in water. This study also describes the various stages of evolution of this 2-L photoreactor, first using TiO2 coated sand in maintaining a uniform (photocatalyst) bed in suspension along with few other modifications that resulted in a photoreactor with a 3 to 4-fold increase in contact time, is discussed. The final stage of this upflow photoreactor modification resulted in the direct use of photocatalysts as a slurry, which was critical, especially for hBN, which cannot be coated onto the sand particles. During this modification and assessment, a smaller bench-top photoreactor (i.e., collimated beam) was also built and tested. It was primarily used in screening various photocatalysts and operational conditions before assessment at this upflow photoreactor and also at a commercial photoreactor (Purifics Photo-Cat) of a larger scale. Thus, the overall goal of this study is to compare a few of these photoreactors of different designs and scales. This includes a collimated beam (at bench-scale), upflow photoreactor (at testbed scale), and a commercial photoreactor, Photo-Cat (at pilot-scale). This study also discusses the performance of these photoreactors under different operating conditions, which includes evaluating two different photocatalyst types (TiO2 and hBN), variable loading rates, applied UV doses, environment pH, and supplemental peroxide addition (as AOP) and with corresponding EEO values.
ContributorsCao, Jiefei (Author) / Sinha, Shahnawaz (Thesis advisor) / Westerhoff, Paul (Committee member) / Ersan, Mahmut (Committee member) / Arizona State University (Publisher)
Created2021
Description
Global shortages of urea and unsustainable production of synthetic urea have caused concerns over the future of food production, automobile operation, and other processes. Urine is a waste product that could supplement synthetic urea production. This study utilizes polyamide reverse osmosis (RO) and nanofiltration (NF) membranes in a cross-flow orientation to selectively recover urea from fresh human urine. Urea permeation experiments were conducted to determine the effects of urea stabilization via pH adjustment and membrane type on the production of a pure urea product. Fouling mitigation experiments were then conducted to determine the efficacy of microfiltration (MF) pretreatment on the reduction of the membrane fouling layer. The results showed that the NF90 membrane had advantageous performance to the BW30 RO and NF270 membranes, permeating 76% of the urea while rejecting 68% of the conductivity. Urine stabilization via acetic acid or sodium hydroxide addition did not inhibit membrane performance, signifying the use of pH 5 as a suitable pretreatment condition. Real fresh urine had higher rejection of constituents for NF90, suggesting the reduction of flux across the membrane due to interactions with organic material. MF pretreatment reduced foulant thickness and permeate flux loss but did not change the speciation of microorganisms. Finally, different urea-based products, such as fertilizers, biocement, and synthetic polymers, were suggested to show the potential of urine-recovered urea to reduce costs. The results from this work show the efficacy of using polyamide RO and NF membranes to supplement unsustainable synthetic production of urea with sustainably sourced urea from a waste product, human urine.
ContributorsCrane, Lucas Christopher (Author) / Boyer, Treavor H (Thesis advisor) / Perreault, Francois (Committee member) / Westerhoff, Paul (Committee member) / Arizona State University (Publisher)
Created2022
Description
Bacterial biofilms exist on surfaces within pressurized water systems, posing threats to water quality and causing fouling or microbial induced corrosion. Germicidal UV irradiation has shown promise in deactivating planktonic pathogens in water but challenges in delivering light to surfaces where biofilms exist have limited advancement in understanding biofilm response to UV-C light. This dissertation aims to overcome the limitation of delivering UV-C light through use of side-emitting optical fibers (SEOFs), advance capabilities to produce SEOFs and understand if a minimum UV-C irradiance can prevent biofilm formation. Two scalable manufacturing approaches were developed for producing kilometer lengths of thin (≤500-µm) and physically flexible SEOFs. One strategy involved dip-coating amine-functionalized SiO2 nanoparticles (NPs) on bare optical fiber, followed by a coating of UV-C transparent polymer (CyTop). I showed that NPs closer to the surface achieved with higher ionic strength solutions increased side-scattering of UV-C light. This phenomenon was primarily attributed to the interaction between NPs and evanescent wave energy. The second strategy omitted NPs but utilized a post-treatment to the UV-C transparent polymer that increased surface roughness on the outer fiber surface. This modification maintained the physical flexibility of the fiber while promoting side-emission of UV-C light. The side emission was due to the enhancement of refracted light energy. Both methods were successfully scaled up for potential commercial production.
Experimental platforms were created to study biofilm responses to UV light on metal or flexible plastic pipe (1/4” ID) surfaces. Delivering UV-C light via SEOFs with irradiances >8 µW/cm2 inhibited biofilm accumulation. Neither UV-A nor UV-B light inhibited biofilm growth. At very low UV-C irradiance (<3 µW/cm2), biofilms were not inhibited. Functional genomic analysis revealed that biofilms irradiated by insufficient UV-C irradiance upregulated various essential genes related to DNA repair, energy metabolism, quorum sensing, mobility, and EPS synthesis. When net UV-C biofilm inactivation rates exceeded the biofilm growth rate, biofilms were inhibited. Insights gained from this dissertation work shed light on the prospective applications of UV-C technology in addressing biofilm challenges within water infrastructure across multiple sectors, from potable water to healthcare applications.
ContributorsZhao, Zhe (Author) / Westerhoff, Paul (Thesis advisor) / Rittmann, Bruce (Committee member) / Abbaszadegan, Morteza (Committee member) / Álvarez, Pedro (Committee member) / Arizona State University (Publisher)
Created2023