Given the increase in nanomaterial (NM) use in consumer products and the large fraction of waste placed in landfills worldwide, the probability of these products reaching municipal solid waste (MSW) landfills at the end of their useful life is high. Since nanotechnology use is still in its early stages, there are currently no regulations pertaining to the disposal of NMs and their fate in MSW landfills is still unknown. Understanding the fate of NMs in MSW landfills is vital to ensure the proper handling of these novel materials from cradle to grave; such research will provide information on how these NMs can be safely introduced into the environment. This research seeks to understand the fate of NMs within waste environments by examining the interactions between NMs and landfill leachate components. The primary focus of this thesis is the effect of Zinc Oxide (ZnO) on biological landfill processes, solids aggregation, and chemical speciation of Zn in landfill leachate following the addition of crystalline, nanosized ZnO coated with triethoxycaprylylsilane. This research (1) observed the effects of coated ZnO on five-day biochemical oxygen demand (BOD5) and biochemical methane potential (BMP), (2) examined effects of solids aggregation on the fate of ZnO, (3) quantified the concentration of Zinc (Zn) by size fractions, and (4) modeled the chemical speciation of Zn in landfill leachate using Visual MINTEQ. No change in dissolved Zn was observed after coated ZnO was exposed to “middle-aged” leachate. Upon exposure to “mature” leachate there was an increase in dissolved Zn assumed to be a result of the dissociation of ZnO. Solids data supported the aggregation of particles in both middle aged and mature leachate. There was an increase in the Zn concentration in leachate fractions greater than 1500 nm presumably due to the dispersion of normally insoluble ZnO ii nanoparticles (NPs) following the interaction with humic acids (HA). ZnO did not inhibit anaerobic or aerobic processes in either middle aged or mature leachate, presumably due to the relatively low concentration of dissolved ionic Zn. Despite the observation of increased dissociation upon exposure to mature leachate, the presence of dissolved organic matter (DOM) may have hindered the ability for dissolved ionic Zn to become bioavailable. Fractionation, BOD5 and BMP tests, and chemical speciation modeling provided insight on the mobility of ZnO in landfills and the absence of inhibitory effects on landfill processes. Aggregation of ZnO NPs may prevent movement through traditional containment systems (i.e. geomembrane liners) due to the increased particle size. However, the increased dispersion suggests that ZnO NPs will be transported out of the landfill in the leachate, however biological treatment of leachate should be unaffected by the presence of ZnO. The bioavailability of Zn was not substantially affected by the presence of ZnO due to affinity of dissolved Zn for DOM. However, due to the heterogeneity of landfill leachate and the utilization of different NM coatings, it is challenging to predict the overall mobility of other NMs in a landfill.

This study is an evaluation of Post Closure Care (PCC) duration of landfills using performance based methodology. The post closure care phase begins once the landfill is closed. As required by the Resource Conservation Recovery Act (RCRA) Subtitle D, PCC duration for municipal solid waste landfills is 30 years. During the PCC period, the landfill operator/owner is required to conduct monitoring for leachate, landfill gas, and ground-water and maintain the integrity of the cap so that the landfill does not impose a threat to surrounding human health and environment (HH&E). The duration of PCC can be reduced by the director of an approved State if an owner/operator of a landfill demonstrates that the landfill exhibits no threat to the surrounding HH&E or can be increased if the director of the approved State determines that an increased PCC period is required for the protection of HH&E. RCRA provides flexibility in optimizing PCC duration of landfills, although it does not identify the criteria/methodology which can be used in demonstrating the status of a landfill from the point of PCC. Researchers worldwide recognize that the threat imposed by a landfill after closure depends on the extent of degradation occurring inside the landfill. The increased functional stability of landfills reduces its risk to the surrounding HH&E. However, there is a wide range of opinions in defining functional stability of a landfill. The present thesis applies performance based methodology, developed by Environmental Research and Education Foundation (EREF), to making a decision on the PCC of landfills. Performance based methodology is a modular approach encompassing all four PCC components of landfills (Leachate, gas, groundwater and cap maintenance). This methodology was applied to Alachua County Southwest Landfill (ACSWLF) in Alachua County, Florida. Each module was analyzed individually and recommendations on the PCC monitoring at the landfill site were provided.

Landfill fires are relatively common incidents that landfill operators encounter which have great impact on landfill structure and the environment. According to a U.S. Fire Administration report in 2001, an average of 8,300 landfill fires occurs each year in the United States, most of them in the spring and summer months. Subsurface spontaneous fires are considered the most dangerous and difficult to detect and extinguish among landfill fires. Few studies have been conducted on spontaneous fires in landfills. Information regarding the thermal behavior of solid waste is not available nor have measurements been made to evaluate spontaneous ignition of solid waste. The purpose of this research was to provide information concerning the initiation of spontaneous ignition incidents in landfills, and investigate the conditions favoring their occurrence. This study enabled better understanding of the self-heating process and spontaneous combustion in landfills. Effects of parameters critical to landfill operation on spontaneous combustion were determined. Spontaneous combustion occurs when materials are heated beyond the ignition temperature. Temperature rise occurs inside the landfill due to exothermic reactions which cause self-heating of the solid waste. Oxygen introduction leading to biological waste degradation and chemical oxidation is believed to be the main cause of rising solid waste temperatures to the point of ignition. A survey was distributed to landfill operators collecting information regarding spontaneous firs incidents in their landfills. Survey results raised new questions necessitating further study of subsurface fires incidents. Subsurface spontaneous fires were not restricted to any landfill geometry or type of waste (municipal, industrial, commercial, and construction and demolition). Results showed that landfill fires occur in landfills that do and do not recirculate leachate. Although new methods have been developed to detect subsurface fires, landfill operators depend primarily on visual observation of smoke or steam to detect the subsurface fires. Also, survey results indicated that excavating and covering with soil are the most widespread methods for extinguishing subsurface fires. Methane often has been suspected for initiating spontaneous subsurface firs in the landfill. However, combustible mixture of methane and oxygen requires very high temperature to ignite. In this study it was shown that spontaneous fires are initiated by solid materials with lower ignition points. Laboratory tests were conducted evaluating the effect of moisture content, oxygen concentration and leachate on spontaneous ignition of solid waste. A new procedure for testing spontaneous ignition is described based on the crossing-point method. The procedure was used to study the spontaneous combustion of solid waste and determine the auto-ignition temperature of the solid waste components and a synthesized solid waste. Correlations have been established between auto-ignition temperature, specific weight and energy content and between self-heating temperature and specific weight. Correlations indicated that compaction can help avoid spontaneous combustion in the landfill. Dense materials require higher energy to increase in temperature and limit the accessibility of oxygen. In the experimental work, moisture was found to promote both biological and chemical self-heating. Increasing moisture content lowers the solid waste permeability and absorbs more energy as it evaporates. Dissolved solids in leachate were found to promote self-heating and ignition more than distilled water. Varying oxygen concentrations indicated that heat generation occurs due to chemical oxidation even at oxygen concentration as low as 10% by volume. However, at 10% by volume oxygen, solid waste did not exhibit thermal runaway nor flammable combustion. At 0% by volume oxygen, tests results indicated occurrence of self-heating due to slow pyrolysis. A numerical one-dimensional energy model was created to simulate temperature rise in landfill for four different scenarios. Using the results from the laboratory experiment, the model estimated the heat generation in solid waste due to chemical reactions. Results from the scenario simulations indicated that moisture evaporation is the major heat sink in the landfill. The model showed that gas flow has a cooling effect due to increasing amount of evaporated water and can control the temperature inside the landfill. The model showed that a temperature higher than the biological limit can be maintained in the landfill without initiating spontaneous fire.

Per- and polyfluoroalkyl substances (PFAS) are known for their persistence as well as their hydrophobic and lipophobic nature. Widespread use has led to increasing prevalence of PFAS in the environment. Due to PFAS:s extensive spread and adverse health effects, remediation of PFAS-contaminated areas has increased in recent years, resulting in an increased demand for disposal of contaminated soil. To dispose waste at landfills in Sweden, certain criteria need to be met. However, for PFAS there are no specific guidelines and landfills therefore decide their own acceptance criteria. This can lead to varying requirements, potentially causing environmentally hazardous practices. The aim of this study was to survey the requirements applied by landfills, as well as investigate how different assessment bases affect the evaluation of PFAS-contaminated soil. The study was conducted both as a questionnaire sent to 80 landfills in Sweden, and as an analysis of test results from samples of PFAS- contaminated soil. The findings reveal varying information requirements, with common criteria including soil origin, presence of contaminants and analysis of PFAS when soil is suspected of contamination. Landfills also typically required documentation about the contaminated site, sampling plan and leachate tests when accepting PFAS-contaminated soil. Additionally, this study demonstrates that the evaluation of PFAS-contaminated soil can depend on the assessment basis used. The assessment based on toxic equivalents, may alter the risk valuation in comparison to those based on measured concentrations. To include commonly occurring PFAS, the analysis should include a minimum of PFAS11.

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