Determination of emission factors from a landfill through an inverse methodology: Experimental determination of ambient air concentrations and use of numerical modelling.

The application of numeric modelling for determining the impact of landfills needs for reliable emission source data. In this study, a methodology for the characterization of the emission profiles of the different sources present in landfills for emission factors determination, applying an indirect methodology, is presented. Ambient air concentrations of volatile organic compounds (VOCs), hydrogen sulphide (H2S) and ammonia (NH3) were determined in three potentially emission sources in Can Mata landfill (Hostalets de Pierola, Catalonia, Spain): dumping areas, pre-closed zone and leachate reservoir as well as in biogas, for the determination of emission factors. Multi-sorbent bed and Tenax TA tubes were used for a wide range of VOCs sampling, and analysis was conducted through TD-GC/MS. H2S and NH3 were sampled and analysed using Radiello passive samplers. The highest total VOC (TVOC) concentrations were found in dumping areas (0.7-3.5 mg m-3), followed by leachate reservoir (0.3-0.6 mg m-3) and pre-closed area (77-165 µg m-3). On the other hand, the highest H2S and NH3 concentrations were found in leachate reservoir, presenting values of 0.8-1.1 mg m-3 and 1.7-1.8 mg m-3, respectively. With the application of odour thresholds to the concentrations obtained, the most critical compounds regarding odour annoyances were determined. The highest odour units (O.U.) were found in leachate reservoir due to H2S concentrations, whereas VOCs contributed mainly to O.U. in the dumping areas. The obtained ambient air concentrations were used for the indirect determination of the emission factors through numerical modelling using a Eulerian dispersion model. The emission factors obtained for the landfill for TVOC, H2S and NH3 were in the range of 0.44-10.9 g s-1, 0.16-1.02 g s-1 and 0.23-1.82 g s-1, respectively, depending on the emission source. Reliable emission factors are crucial to obtain landfill impact maps, which are essential for the correct management of these facilities.

Air quality impacts of landfill fires: A case study from the Brahmapuram Municipal Solid Waste Treatment Plant in Kochi, India.

The occurrence of waste fires in unscientifically managed landfill sites has become a pressing environmental issue in the urban centers of developing economies. In the present work, an investigation was carried out to evaluate the air quality implications of three major fire events that occurred at the Brahmapuram Municipal Solid Waste Treatment Plant (BMSWTP) in Kochi, India. Initially, Landsat-based surface temperature monitoring was conducted to identify the thermal hotspots within the landfill. The emissions of different pollutants during waste fires were quantified and compared between satellite-based ex-situ and field-based in-situ methods. The dispersion patterns of PM2.5 particles released during the fires were visualised using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) particle dispersion model. The Landfill Gas Emissions Model (LandGEM) was employed to quantify the greenhouse gases (GHGs) released during waste storage, which was then compared with the GHGs emissions during waste fires. In-situ emission estimates showed that the combustion of waste at BMSWTP led to the release of 909.3 MT of PM10, 938.8 MT of PM2.5, 5832.9 MT of CO, 43.6 MT of SOx, 284.2 MT of NOx, 138,941.9 MT of CO2, 426.8 MT of CH4, and 2665.1 MT of VOC. However, a noticeable disparity was observed between the in-situ and ex-situ emission estimates, wherein the latter underestimated the actual emissions. Most of the emitted PM2.5 particles propagated oceanward under the influence of prevailing winds, covering the densely populated areas of Kochi municipal corporation. The amount of CH4 and CO2 emitted during the waste fires was on par with the emissions from 159 days of waste storage for CH4 and 51.8 years of waste storage for CO2, with a cumulative global warming potential of 147.9 Gg CO2-e.

Real-time air concentrations and turbulent fluxes of volatile organic compounds (VOCs) over historic closed landfills to assess their potential environmental impact.

For the first time, emission/deposition fluxes of volatile organic compounds (VOCs) and H2S from a historic closed landfill site in Southern Italy were determined by Eddy Covariance (EC) using Proton Transfer Reaction Time-of-Flight Mass Spectrometry (PTR-TOF-MS). This was done in two field campaigns of one week performed in July and October 2016, where fluxes of CO2 and CH4 were also measured. Many compounds not previously identified in the biogas were detected by PTR-TOF-MS, but only in July some of them produced positive fluxes exceeding the flux limit of detection. Methanol was the most emitted compound with an average flux of 44.20 ± 4.28 µg m-2 h-1, followed by toluene with a mean flux of 18.97 ± 2.47 µg m-2 h-1. Toluene fluxes were 10 times higher than those of benzene, fitting rather well with values previously measured in the biogas. VOCs emission fluxes of monoterpenes and highly reactive arenes did not reflect, however, the biogas composition. This, combined with tiny emissions of VOC oxidation products, suggests that landfill emissions underwent some photochemical degradation before being dispersed in the atmospheric boundary layer (ABL). Deposition fluxes of some VOCs emitted from the sea was also observed in July. No relevant VOC fluxes were instead measured in October, suggesting that temperature was the variable controlling most landfill emission. Albeit small, summer landfill emissions from the investigated site can have an impact on the population living nearby, because they contain or still generate compounds that causing nuisance.

Annual upscaling of methane emission field measurements from two Danish landfills, using empirical emission models.

An empirical model was developed and employed to estimate annual methane (CH4) emissions from two Danish landfills (Skellingsted and AV Miljø). The overall aim was to provide accurate annual CH4 emission estimates based on discrete emission field measurements and to address temporal variability caused by the impact of barometric pressure. Four non-linear regression models were developed, corresponding to the two landfills as well as to the western and eastern waste sections of AV Miljø. A comparison of model predictions with on-site eddy covariance fluxes showed that the models can accurately predict short-term emission variability. Predicted annual CH4 emissions for the Skellingsted and AV Miljø landfills were 69 ± 4 and 80 ± 4 tonnes, respectively, whereas for the western and eastern sections of the AV Miljø landfill, emissions were estimated at 63 ± 3 and 19 ± 1 tonnes, respectively. The results demonstrate that even though maximum emissions from Skellingsted were approximately threefold compared to AV Miljø, annual predicted CH4 emissions for Skellingsted were lower. This was because during the most frequently occurring pressure change events, emission rates were higher at AV Miljø in comparison to Skellingsted. An optimised sampling strategy was proposed, targeting the determination of an empirical emission model though the effective use of discrete field measurements. Analysis of annual emission estimates, based on the number of the tracer dispersion method (TDM) measurements, showed that both the number as well as the distribution of performed TDM measurements across the range of expected dP/dt influence the uncertainty.

Revisiting the passive biocover system at Klintholm landfill, six years after construction.

A biocover system was established at Klintholm landfill in Denmark in 2009 to mitigate methane emissions, and the system exhibited high mitigation efficiency during the first year after implementation. The biocover system was revisited in 2016/2017, and a series of field and laboratory tests were carried out to evaluate functionality about six years after establishment. Three field campaigns were executed in three different barometric pressure conditions, namely increasing, stable and decreasing. Local surface flux measurements and gas concentration profiles in the methane oxidation layer showed that barometric pressure changes had a significant effect on gas emission and methane oxidation. Elevated concentrations of oxygen were observed in the gas distribution layer, and field data showed that significant methane oxidation took place in this location. This finding was verified in laboratory-based methane oxidation incubation tests. Temperatures higher than ambient temperature were observed throughout the methane oxidation layer, with average temperatures ranging between 13 and 27 °C, even in the coldest month of the year. Field measurements showed that total methane emissions from the whole landfill cell were at the same level or lower than measurements performed in 2009/2010 after implementation of the biocover system, and laboratory tests showed methane oxidation potential approximately equal to former tests. In spite of an inhomogeneous distribution of landfill gas load to the methane oxidation layer, the performance of the biocover system had not declined over the 6-7 years since its establishment, even though no maintenance had been carried out in the intervening years.

Quantification and control of gaseous emissions from solid waste landfill surfaces.

Landfilling is the most common option for solid waste disposal worldwide. Landfill sites can emit significant quantities of greenhouse gases (GHGs; e.g., methane, carbon dioxide, and nitrous oxide) and release toxic and odorous compounds (e.g., sulfides). Due to the complex composition and characteristics of landfill surface gas emissions, the quantification and control of landfill emissions are challenging. This review attempts to comprehensively understand landfill emission quantification and control options by primarily focusing on GHGs and odor compounds. Landfill emission quantification was highlighted by combining different emissions monitoring approaches to improve the quality of landfill emission data. Also, landfill emission control requires a specific approach that targets emission compounds or a systematic approach that reduces overall emissions by combining different control methods since the diverse factors dominate the emissions of various compounds and their transformation. This integrated knowledge of emission quantification and control options for GHGs and odor compounds is beneficial for establishing field monitoring campaigns and incorporating mitigation strategies to quantify and control multiple landfill emissions.

Locating and quantifying multiple landfills methane emissions using aircraft data.

A mass balance approach to quantify methane (CH4) emission of four co-located landfills by means of airborne measurements and dispersion modelling was proposed and assessed. By flying grids at different heights above the landfills, atmospheric CH4 densities and wind components were measured along the edges and inside the study atmospheric volume, in order to calculate mass flows in the along- and across-wind directions. A steady-state Gaussian dispersion model was applied to build the concentration fields associated to unit emission from each landfill, while the contribution of each one to the total emission was assessed using a General Linear Model approach, minimizing the difference between measured and modeled mass flows. Results showed that wind spatial and temporal variability is the main factor controlling the accuracy of the method, as a good agreement between measured and modeled mass flows was mainly found for flights made in steady wind conditions. CH4 emissions of the entire area ranged from 213.5 ±â€¯33.5 to 317.9 ±â€¯90.4 g s-1 with a mean value of 252.5 ±â€¯54.2 g s-1. Contributions from individual sources varied from 17.5 to 40.1 g m-2 day-1 indicating a substantial heterogeneity of the different landfills, which differed in age and waste composition. The proposed method was validated against tower eddy covariance flux measurements made at one of the landfills, revealing an overall agreement within 20%.

Composition and emission of VOC from biogas produced by illegally managed waste landfills in Giugliano (Campania, Italy) and potential impact on the local population.

The composition in Volatile Organic Compounds (VOC) of the biogas produced by seven landfills of Giugliano (Naples, Campania, Italy) was determined and VOC emission rates assessed to verify if these compounds represent a potential threat to the population living nearby. VOC composition in the biogas could not be predicted, as heterogeneous waste was dumped from the late 1980s to the early 2000s and then underwent biological degradation. No data are available on the amount and composition of VOC in the biogas before the landfills closure as no operational biogas collection system was present. In this study, VOC composition was determined by gas chromatography-mass spectrometry (GC-MS), after collecting samples from collection pipes and from soil fractures in cover soil or capping. Individual VOC were quantified and data compared with those collected at two landfills in Latium, when they were still in operation. Relevant differences were observed, mainly due to waste aging, but no specific VOC revealing toxic waste dumping was found, although the concurrent presence of certain compounds suggested that dumping of industrial wastes might have occurred. The average VOC emission was assessed and a dispersion model was run to find out if the emitted plume could affect the health of population. The results suggested that fugitive emissions did not represent a serious danger, since the concentrations simulated at the neighboring cities were below the threshold limits for acute and chronic diseases. However, VOC plume could cause annoyance at night when the steady state conditions of the atmosphere enhance pollutants accumulation in the lower layers. In addition, some of the emitted VOC, such as alkylbenzenes and monoterpenes, can contribute to tropospheric ozone formation.

Using multivariate regression modeling for sampling and predicting chemical characteristics of mixed waste in old landfills.

Municipal solid waste landfills pose a threat on environment and human health, especially old landfills which lack facilities for collection and treatment of landfill gas and leachate. Consequently, missing information about emission flows prevent site-specific environmental risk assessments. To overcome this gap, the combination of waste sampling and analysis with statistical modeling is one option for estimating present and future emission potentials. Optimizing the tradeoff between investigation costs and reliable results requires knowledge about both: the number of samples to be taken and variables to be analyzed. This article aims to identify the optimized number of waste samples and variables in order to predict a larger set of variables. Therefore, we introduce a multivariate linear regression model and tested the applicability by usage of two case studies. Landfill A was used to set up and calibrate the model based on 50 waste samples and twelve variables. The calibrated model was applied to Landfill B including 36 waste samples and twelve variables with four predictor variables. The case study results are twofold: first, the reliable and accurate prediction of the twelve variables can be achieved with the knowledge of four predictor variables (Loi, EC, pH and Cl). For the second Landfill B, only ten full measurements would be needed for a reliable prediction of most response variables. The four predictor variables would exhibit comparably low analytical costs in comparison to the full set of measurements. This cost reduction could be used to increase the number of samples yielding an improved understanding of the spatial waste heterogeneity in landfills. Concluding, the future application of the developed model potentially improves the reliability of predicted emission potentials. The model could become a standard screening tool for old landfills if its applicability and reliability would be tested in additional case studies.

Quantifying methane emission from fugitive sources by combining tracer release and downwind measurements - a sensitivity analysis based on multiple field surveys.

Using a dual species methane/acetylene instrument based on cavity ring down spectroscopy (CRDS), the dynamic plume tracer dispersion method for quantifying the emission rate of methane was successfully tested in four measurement campaigns: (1) controlled methane and trace gas release with different trace gas configurations, (2) landfill with unknown emission source locations, (3) landfill with closely located emission sources, and (4) comparing with an Fourier transform infrared spectroscopy (FTIR) instrument using multiple trace gasses for source separation. The new real-time, high precision instrument can measure methane plumes more than 1.2 km away from small sources (about 5 kg h(-1)) in urban areas with a measurement frequency allowing plume crossing at normal driving speed. The method can be used for quantification of total methane emissions from diffuse area sources down to 1 kg per hour and can be used to quantify individual sources with the right choice of wind direction and road distance. The placement of the trace gas is important for obtaining correct quantification and uncertainty of up to 36% can be incurred when the trace gas is not co-located with the methane source. Measurements made at greater distances are less sensitive to errors in trace gas placement and model calculations showed an uncertainty of less than 5% in both urban and open-country for placing the trace gas 100 m from the source, when measurements were done more than 3 km away. Using the ratio of the integrated plume concentrations of tracer gas and methane gives the most reliable results for measurements at various distances to the source, compared to the ratio of the highest concentration in the plume, the direct concentration ratio and using a Gaussian plume model. Under suitable weather and road conditions, the CRDS system can quantify the emission from different sources located close to each other using only one kind of trace gas due to the high time resolution, while the FTIR system can measure multiple trace gasses but with a lower time resolution.

Mitigation of methane emission from an old unlined landfill in Klintholm, Denmark using a passive biocover system.

Methane generated at landfills contributes to global warming and can be mitigated by biocover systems relying on microbial methane oxidation. As part of a closure plan for an old unlined landfill without any gas management measures, an innovative biocover system was established. The system was designed based on a conceptual model of the gas emission patterns established through an initial baseline study. The study included construction of gas collection trenches along the slopes of the landfill where the majority of the methane emissions occurred. Local compost materials were tested as to their usefulness as bioactive methane oxidizing material and a suitable compost mixture was selected. Whole site methane emission quantifications based on combined tracer release and downwind measurements in combination with several local experimental activities (gas composition within biocover layers, flux chamber based emission measurements and logging of compost temperatures) proved that the biocover system had an average mitigation efficiency of approximately 80%. The study showed that the system also had a high efficiency during winter periods with temperatures below freezing. An economic analysis indicated that the mitigation costs of the biocover system were competitive to other existing greenhouse gas mitigation options.