Matching Items (5)
Filtering by
- All Subjects: Carbon, Activated
- Creators: Fox, Peter
- Resource Type: Text
- Status: Published
Description
Granular activated carbon (GAC) filters are final polishing step in the drinking water treatment systems for removal of dissolved organic carbon fractions. Generally filters are colonized by bacterial communities and their activity reduces biodegradable solutes allowing partial regeneration of GAC's adsorptive capacity. When the bacteria pass into the filtrate due to increased growth, microbiological quality of drinking water is compromised and regrowth in the distribution system occurs. Bacteria attached to carbon particles as biofilms or in conjugation with other bacteria were observed to be highly resistant to post filtration microbial mitigation techniques. Some of these bacteria were identified as pathogenic.
This study focuses on one such pathogen Legionella pneumophila which is resistant to environmental stressors and treatment conditions. It is also responsible for Legionnaires' disease outbreak through drinking water thus attracting attention of regulatory agencies. The work assessed the attachment and colonization of Legionella and heterotrophic bacteria in lab scale GAC media column filters. Quantification of Legionella and HPC in the influent, effluent, column's biofilms and on the GAC particles was performed over time using fluorescent microscopy and culture based techniques.
The results indicated gradual increase in the colonization of the GAC particles with HPC bacteria. Initially high number of Legionella cells were detected in the column effluent and were not detected on GAC suggesting low attachment of the cells to the particles potentially due to lack of any previous biofilms. With the initial colonization of the filter media by other bacteria the number of Legionella cells on the GAC particles and biofilms also increased. Presence of Legionella was confirmed in all the samples collected from the columns spiked with Legionella. Significant increase in the Legionella was observed in column's inner surface biofilm (0.25 logs up to 0.52 logs) and on GAC particles (0.42 logs up to 0.63 logs) after 2 months. Legionella and HPC attached to column's biofilm were higher than that on GAC particles indicating the strong association with biofilms. The bacterial concentration slowly increased in the effluent. This may be due to column's wall effect decreasing filter efficiency, possible exhaustion of GAC capacity over time and potential bacterial growth.
This study focuses on one such pathogen Legionella pneumophila which is resistant to environmental stressors and treatment conditions. It is also responsible for Legionnaires' disease outbreak through drinking water thus attracting attention of regulatory agencies. The work assessed the attachment and colonization of Legionella and heterotrophic bacteria in lab scale GAC media column filters. Quantification of Legionella and HPC in the influent, effluent, column's biofilms and on the GAC particles was performed over time using fluorescent microscopy and culture based techniques.
The results indicated gradual increase in the colonization of the GAC particles with HPC bacteria. Initially high number of Legionella cells were detected in the column effluent and were not detected on GAC suggesting low attachment of the cells to the particles potentially due to lack of any previous biofilms. With the initial colonization of the filter media by other bacteria the number of Legionella cells on the GAC particles and biofilms also increased. Presence of Legionella was confirmed in all the samples collected from the columns spiked with Legionella. Significant increase in the Legionella was observed in column's inner surface biofilm (0.25 logs up to 0.52 logs) and on GAC particles (0.42 logs up to 0.63 logs) after 2 months. Legionella and HPC attached to column's biofilm were higher than that on GAC particles indicating the strong association with biofilms. The bacterial concentration slowly increased in the effluent. This may be due to column's wall effect decreasing filter efficiency, possible exhaustion of GAC capacity over time and potential bacterial growth.
ContributorsSharma, Harsha (Author) / Abbaszadegan, Morteza (Thesis advisor) / Alum, Absar (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2014
Description
Increasing concentrations of carbon dioxide in the atmosphere will inevitably lead to long-term changes in climate that can have serious consequences. Controlling anthropogenic emission of carbon dioxide into the atmosphere, however, represents a significant technological challenge. Various chemical approaches have been suggested, perhaps the most promising of these is based on electrochemical trapping of carbon dioxide using pyridine and derivatives. Optimization of this process requires a detailed understanding of the mechanisms of the reactions of reduced pyridines with carbon dioxide, which are not currently well known. This thesis describes a detailed mechanistic study of the nucleophilic and Bronsted basic properties of the radical anion of bipyridine as a model pyridine derivative, formed by one-electron reduction, with particular emphasis on the reactions with carbon dioxide. A time-resolved spectroscopic method was used to characterize the key intermediates and determine the kinetics of the reactions of the radical anion and its protonated radical form. Using a pulsed nanosecond laser, the bipyridine radical anion could be generated in-situ in less than 100 ns, which allows fast reactions to be monitored in real time. The bipyridine radical anion was found to be a very powerful one-electron donor, Bronsted base and nucleophile. It reacts by addition to the C=O bonds of ketones with a bimolecular rate constant around 1* 107 M-1 s-1. These are among the fastest nucleophilic additions that have been reported in literature. Temperature dependence studies demonstrate very low activation energies and large Arrhenius pre-exponential parameters, consistent with very high reactivity. The kinetics of E2 elimination, where the radical anion acts as a base, and SN2 substitution, where the radical anion acts as a nucleophile, are also characterized by large bimolecular rate constants in the range ca. 106 - 107 M-1 s-1. The pKa of the bipyridine radical anion was measured using a kinetic method and analysis of the data using a Marcus theory model for proton transfer. The bipyridine radical anion is found to have a pKa of 40±5 in DMSO. The reorganization energy for the proton transfer reaction was found to be 70±5 kJ/mol. The bipyridine radical anion was found to react very rapidly with carbon dioxide, with a bimolecular rate constant of 1* 108 M-1 s-1 and a small activation energy, whereas the protonated radical reacted with carbon dioxide with a rate constant that was too small to measure. The kinetic and thermodynamic data obtained in this work can be used to understand the mechanisms of the reactions of pyridines with carbon dioxide under reducing conditions.
ContributorsRanjan, Rajeev (Author) / Gould, Ian R (Thesis advisor) / Buttry, Daniel A (Thesis advisor) / Yarger, Jeff (Committee member) / Seo, Dong-Kyun (Committee member) / Arizona State University (Publisher)
Created2015
Description
Granular activated carbon (GAC) is effectively used to remove natural organic matter (NOM) and to assist in the removal of disinfection byproducts (DBPs) and their precursors. However, operation of GAC is cost- and labor-intensive due to frequent media replacement. Optimizing the use of GAC is necessary to ensure treatment efficiency while reducing costs. This dissertation presents four strategies to reduce improve GAC usage while reducing formation of DBPs. The first part of this work adopts Rapid Small Scale Tests (RSSCTs) to evaluate removal of molecular weight fractions of NOM, characterized using size exclusion chromatography (SECDOC). Total trihalomethanes (TTHM), haloacetic acids (HAA5) and haloacetonitriles (HAN) formation were quantified after treatment with GAC. Low MW NOM was removed preferentially in the early bed volumes, up until exhaustion of available adsorption sites. DBP formation potential lowered with DOC removal. Chlorination prior to GAC is investigated in the second part of this work as a strategy to increase removal of NOM and DBP precursors. Results showed lower TTHM formation in the effluent of the GAC treatment when pre-chlorination was adopted, meaning this strategy could help optimize and extend the bed life if GAC filters. The third part of this work investigates in-situ GAC regeneration as an alternative to recover adsorption capacity of field-spent GAC that could potentially offer new modes of operation for water treatment facilities while savng costs with reactivation of spent GAC in an external facility. Field-spent GACs were treated with different oxidant solutions and recovery in adsorption capacity was evaluated for NOM and for two micro pollutants. Recovery of GAC adsorption capacity was not satisfactory for most of conditions evaluated. This indicates that in-situ GAC regeneration could be more effective when the adsorbates are present at high concentrations. Lastly, this work investigates the impact of low molecular weight polyDADMAC on N-nitrosodimethylamine (NDMA) formation. Water treatment facilities rely on polyDADMAC as a coagulant aid to comply with NOM removal and turbidity requirements. Since polymer-derived NDMA precursors are not removed by GAC, it is essential to optimize the use and synthesis of polyDADMAC to reduce NDMA precursors during water treatment.
ContributorsFischer, Natalia (Author) / Westerhoff, Paul (Thesis advisor) / Hristovski, Kiril (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2017
Description
Specific inorganic and organic pollutants in water (As(V), Cr(VI), THMs, and hardness) cause health concerns or aesthetic problems. The goal of this dissertation is to demonstrate novel approaches to improve the performance of point of use and municipal activated carbon processes to provide safe and reliable water to the public at distributed centralized locations.
Template Assisted Crystallization system would adjust saturation index (SI) value of TAC treated water to zero when SI value of influent water was in the range at 0.08~0.3. However, the reduction in SI when SI values were higher (e.g. 0.7~1.3) was similar to the reduction at lower SI values which could be due to limitations in kinetics or mass transfer with the template on TAC media.
Pre-chlorination prior to municipal-scale granular activated carbon (GAC) treatment was evaluated to control THM formation in distribution systems. Pre-chlorination decreased UVA, shift the dissolved organic carbon (DOC) molecular weight distribution and pre-formed trihalomethanes (THM). GAC treatment of pre-chlorinated water achieved lower THM formation in distribution systems.
To add functionality in POU systems to remove As(V) and Cr(VI), activated carbon was nano-tized to fabricate nano-enabled carbon block (CB) by (1) impregnating iron or titanium metal oxides chemically or (2) attaching titanium based P25 through electrostatic attraction force. Nanoparticle loadings of 5 to 10 wt % with respect to activated carbon enables reduction of As(V) or Cr(VI) from levels of common occurrence to below regulatory levels across carbon block designs. Minimal impacts on As(V) and Cr(VI) sorption were observed up to a nanoparticle pre-treatment temperature of 200 C, which is the temperature for CB production. Through controlling pH at 4.5 during mixing of nanoparticles with pH IEP=6 and activated carbon with pH IEP=3, electrostatic attachment of nanoparticles to activated carbon could be achieved prior to fabricating carbon block. A mini carbon block test device was designed, fabricated, and validated to mimic performances of full-scale carbon block using less volumes of test water. As(V) removal tests showed Fe impregnated CB achieved the highest As(V) removal while P25 attached CB had the lowest among three nanoparticles loaded CBs.
Template Assisted Crystallization system would adjust saturation index (SI) value of TAC treated water to zero when SI value of influent water was in the range at 0.08~0.3. However, the reduction in SI when SI values were higher (e.g. 0.7~1.3) was similar to the reduction at lower SI values which could be due to limitations in kinetics or mass transfer with the template on TAC media.
Pre-chlorination prior to municipal-scale granular activated carbon (GAC) treatment was evaluated to control THM formation in distribution systems. Pre-chlorination decreased UVA, shift the dissolved organic carbon (DOC) molecular weight distribution and pre-formed trihalomethanes (THM). GAC treatment of pre-chlorinated water achieved lower THM formation in distribution systems.
To add functionality in POU systems to remove As(V) and Cr(VI), activated carbon was nano-tized to fabricate nano-enabled carbon block (CB) by (1) impregnating iron or titanium metal oxides chemically or (2) attaching titanium based P25 through electrostatic attraction force. Nanoparticle loadings of 5 to 10 wt % with respect to activated carbon enables reduction of As(V) or Cr(VI) from levels of common occurrence to below regulatory levels across carbon block designs. Minimal impacts on As(V) and Cr(VI) sorption were observed up to a nanoparticle pre-treatment temperature of 200 C, which is the temperature for CB production. Through controlling pH at 4.5 during mixing of nanoparticles with pH IEP=6 and activated carbon with pH IEP=3, electrostatic attachment of nanoparticles to activated carbon could be achieved prior to fabricating carbon block. A mini carbon block test device was designed, fabricated, and validated to mimic performances of full-scale carbon block using less volumes of test water. As(V) removal tests showed Fe impregnated CB achieved the highest As(V) removal while P25 attached CB had the lowest among three nanoparticles loaded CBs.
ContributorsLee, Heuidae (Author) / Westerhoff, Paul (Thesis advisor) / Fox, Peter (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2018
Description
Carbon dioxide (CO2) is one of the most dangerous greenhouse gas. Its concentration in the atmosphere has increased to very high levels since the industrial revolution. This continues to be a threat due to increasing energy demands. 60% of the worlds global emissions come from automobiles and other such moving sources. Hence, to stay within safe limits, it is extremely important to curb current emissions and remove those which have already been emitted. Out of many available technologies, one such technology is the moisture swing based air capture technology that makes use of resin material that absorbs CO2 when it is dry and releases it when it is wet. A mathematical model was developed to better understand the mechanism of this process. In order to validate this model, numerical simulation and experimentation was done. Once the mechanism was proved, it was seen that there are many factors and parameters that govern this process. Some of these do not have definite value. To find the best fit value for these parameters, an optimized fitting routine needs to be developed that can minimize the standard deviation of the error. This thesis looks into ways in which the optimization of parameters can be done and the possible future work by using substantial data.
ContributorsChopra, Vinuta (Author) / Lackner, Klaus S (Thesis advisor) / Fox, Peter (Committee member) / Wright, Allen (Committee member) / Arizona State University (Publisher)
Created2016