Stable isotopic determination of methane oxidation: When smaller scales are better.

Stable isotope measurements are an effective tool for evaluating methane (CH4) consumption in landfill soils. However, determining the extent of CH4 oxidation in soils using this approach can be inherently biased, depending on characteristics of the study site and the sampling strategy that is employed. In this study, we establish the unusual case that sampling at smaller scales captures a better representation of the degree of oxidation occurring in landfill cover soils. We did this by comparing three techniques (Plume, Probe, and Transect) that vary in the location of sampling within a site and in the areal footprint of each sample. The Plume method yielded estimates of CH4 oxidation that were 13-16% lower than the Transect and Probe methods, respectively. The Probe and Transect methods, two relatively small-scale and high resolution methods, the latter of which has not been previously described, are best suited to quantify CH4 oxidation in landfill soils as they demonstrably overcome the tendency of stable isotope methods to underestimate CH4 oxidation at the landfill scale. We recommend the use of these two sampling methods for monitoring the efficacy of landfill CH4 reduction strategies that are desired to help meet the goals of the Paris Agreement.

Comparison of Field Measurements to Methane Emissions Models at a New Landfill.

Estimates of methane emissions from landfills rely primarily on models due to both technical and economic limitations. While models are easy to implement, there is uncertainty due to the use of parameters that are difficult to validate. The objective of this research was to compare modeled emissions using several greenhouse gas (GHG) emissions reporting protocols including: (1) Intergovernmental Panel on Climate Change (IPCC); (2) U.S. Environmental Protection Agency Greenhouse Gas Reporting Program (EPA GHGRP); (3) California Air Resources Board (CARB); and (4) Solid Waste Industry for Climate Solutions (SWICS), with measured emissions data collected over three calendar years from a young landfill with no gas collection system. By working with whole landfill measurements of fugitive methane emissions and methane oxidation, the collection efficiency could be set to zero, thus eliminating one source of parameter uncertainty. The models consistently overestimated annual methane emissions by a factor ranging from 4-31. Varying input parameters over reasonable ranges reduced this range to 1.3-8. Waste age at the studied landfill was less than four years and the results suggest the need for measurements at additional landfills to evaluate the accuracy of the tested models to young landfills.

Liquid balance monitoring inside conventional, Retrofit, and bio-reactor landfill cells.

The Outer Loop landfill bioreactor (OLLB) in Louisville, KY, USA has been the site of a study to evaluate long-term bioreactor performance at a full-scale operational landfill. Three types of landfill units were studied including a conventional landfill (Control cell), a new landfill area that had an air addition and recirculation piping network installed as waste was being placed (As-Built cell), and a conventional landfill that was modified to allow for liquids recirculation (Retrofit cell). During the monitoring period, the Retrofit, Control, and As-Built cells received 48, 14, and 213LMg(-1) (liters of liquids per metric ton of waste), respectively. The leachate collection system yielded 60, 57 and 198LMg(-1) from the Retrofit, Control, and As-Built cells, respectively. The head on liner in all cells was below regulatory limits. In the Control and As-Built cells, leachate head on liner decreased once waste placement stopped. The measured moisture content of the waste samples was consistent with that calculated from the estimate of accumulated liquid by the liquid balance. Additionally, measurements on excavated solid waste samples revealed large spatial variability in waste moisture content. The degree of saturation in the Control cells decreased from 85% to 75%. The degree of saturation increased from 82% to 83% due to liquids addition in the Retrofit cells and decreased back to 80% once liquid addition stopped. In the As-Built cells, the degree of saturation increased from 87% to 97% during filling activities and then started to decrease soon after filling activities stopped to reach 92% at the end of the monitoring period. The measured leachate generation rates were used to estimate an in-place saturated hydraulic conductivity of the MSW in the range of 10(-8) to 10(-7)ms(-1) which is lower than previous reports. In the Control and Retrofit cells, the net loss in liquids, 43 and 12LMg(-1), respectively, was similar to the measured settlement of 15% and 5-8% strain, respectively (Abichou et al., 2013). The increase in net liquid volume in the As-Built cells indicates that the 37% (average) measured settlement strain in these cells cannot be due to consolidation as the waste mass did not lose any moisture but rather suggests that settlement was attributable to lubrication of waste particle contacts, softening of flexible porous materials, and additional biological degradation.

The Outer Loop bioreactor: a case study of settlement monitoring and solids decomposition.

The Outer Loop landfill bioreactor (OLLB) located in Louisville, KY, USA has been in operation since 2000 and represents an opportunity to evaluate long-term bioreactor monitoring data at a full-scale operational landfill. Three types of landfill units were studied including a Control cell, a new landfill area that had a piping network installed as waste was being placed to support leachate recirculation (As-Built cell), and a conventional landfill that was modified to allow for liquid recirculation (Retrofit cell). The objective of this study is to summarize the results of settlement data and assess how these data relate to solids decomposition monitoring at the OLLB. The Retrofit cells started to settle as soon as liquids were introduced. The cumulative settlement during the 8years of monitoring varied from 60 to 100cm. These results suggest that liquid recirculation in the Retrofit cells caused a 5-8% reduction in the thickness of the waste column. The average long-term settlement in the As-Built and Control Cells was about 37% and 19%, respectively. The modified compression index (Cα(')) was 0.17 for the Control cells and 0.2-0.48 for the As-Built cells. While the As-Built cells exhibited greater settlement than the Control cells, the data do not support biodegradation as the only explanation. The increased settlement in the As-Built bioreactor cell appeared to be associated with liquid movement and not with biodegradation because both chemical (biochemical methane potential) and physical (moisture content) indicators of decomposition were similar in the Control and As-Built cells. The solids data are consistent with the concept that bioreactor operations accelerate the rate of decomposition, but not necessarily the cumulative loss of anaerobically degradable solids.

A new approach to characterize emission contributions from area sources during optical remote sensing technique testing.

UNLABELLED: In the method termed "Other Test Method-10," the U.S. Environmental Protection Agency has proposed a method to quantify emissions from nonpoint sources by the use of vertical radial plume mapping (VRPM) technique. The surface area of the emitting source and the degree to which the different zones of the emitting source are contributing to the VRPM computed emissions are often unknown. The objective of this study was to investigate and present an approach to quantify the unknown emitting surface area that is contributing to VRPM measured emissions. Currently a preexisting model known as the "multiple linear regression model," which is described in Thoma et al. (2009), is used for quantifying the unknown surface area. The method investigated and presented in this paper utilized tracer tests to collect data and develop a model much like that described in Thoma et al. (2009). However unlike the study used for development of the multiple linear regression model, this study is considered a very limited study due to the low number of pollutant releases performed (seven total releases). It was found through this limited study that the location of an emitting source impacts VRPM computed emissions exponentially, rather than linearly (i.e., the impact that an emitting source has on VRPM measurements decreases exponentially with increasing distances between the emitting source and the VRPM plane). The data from the field tracer tests were used to suggest a multiple exponential regression model. The findings of this study, however, are based on a very small number of tracer tests. More tracer tests performed during all types of climatic conditions, terrain conditions, and different emissions geometries are still needed to better understand the variation of capture efficiency with emitting source location. This study provides a step toward such an objective. IMPLICATIONS: The findings of this study will aid in the advancement of the VRPM technique. In particular, the contribution of this study is to propose a slight improvement in how the area contributing to flux is determined during VRPM campaigns. This will reduce some of the technique's inherent uncertainties when it is employed to estimate emissions from an area source under nonideal conditions.

Landfill methane oxidation across climate types in the U.S.

Methane oxidation in landfill covers was determined by stable isotope analyses over 37 seasonal sampling events at 20 landfills with intermediate covers over four years. Values were calculated two ways: by assuming no isotopic fractionation during gas transport, which produces a conservative or minimum estimate, and by assuming limited isotopic fractionation with gas transport producing a higher estimate. Thus bracketed, the best assessment of mean oxidation within the soil covers from chamber captured emitted CH(4) was 37.5 ± 3.5%. The fraction of CH(4) oxidized refers to the fraction of CH(4) delivered to the base of the cover that was oxidized to CO(2) and partitioned to microbial biomass instead of being emitted to the atmosphere as CH(4) expressed as a percentage. Air samples were also collected at the surface of the landfill, and represent CH(4) from soil, from leaking infrastructure, and from cover defects. A similar assessment of this data set yields 36.1 ± 7.2% oxidation. Landfills in five climate types were investigated. The fraction oxidized in arid sites was significantly greater than oxidation in mediterranean sites, or cool and warm continental sites. Sub tropical sites had significantly lower CH(4) oxidation than the other types of sites. This relationship may be explained by the observed inverse relationship between cover loading and fractional CH(4) oxidation.

Observations on the methane oxidation capacity of landfill soils.

The objective of this study was to determine the role of CH(4) loading to a landfill cover in the control of CH(4) oxidation rate (gCH(4)m(-2)d(-1)) and CH(4) oxidation efficiency (% CH(4) oxidation) in a field setting. Specifically, we wanted to assess how much CH(4) a cover soil could handle. To achieve this objective we conducted synoptic measurements of landfill CH(4) emission and CH(4) oxidation in a single season at two Southeastern USA landfills. We hypothesized that percent oxidation would be greatest at sites of low CH(4) emission and would decrease as CH(4) emission rates increased. The trends in the experimental results were then compared to the predictions of two differing numerical models designed to simulate gas transport in landfill covers, one by modeling transport by diffusion only and the second allowing both advection and diffusion. In both field measurements and in modeling, we found that percent oxidation is a decreasing exponential function of the total CH(4) flux rate (CH(4) loading) into the cover. When CH(4) is supplied, a cover's rate of CH(4) uptake (gCH(4)m(-2)d(-2)) is linear to a point, after which the system becomes saturated. Both field data and modeling results indicate that percent oxidation should not be considered as a constant value. Percent oxidation is a changing quantity and is a function of cover type, climatic conditions and CH(4) loading to the bottom of the cover. The data indicate that an effective way to increase the % oxidation of a landfill cover is to limit the amount of CH(4) delivered to it.

Uncertainties associated with the use of optical remote sensing technique to estimate surface emissions in landfill applications.

Landfills represent a source of distributed emissions source over an irregular and heterogeneous surface. In the method termed "Other Test Method-10" (OTM-10), the U.S. Environmental Protection Agency (EPA) has proposed a method to quantify emissions from such sources by the use of vertical radial plume mapping (VRPM) techniques combined with measurement of wind speed to determine the average emission flux per unit area per time from nonpoint sources. In such application, the VRPM is used as a tool to estimate the mass of the gas of interest crossing a vertical plane. This estimation is done by fitting the field-measured concentration spatial data to a Gaussian or some other distribution to define a plume crossing the vertical plane. When this technique is applied to landfill surfaces, the VRPM plane may be within the emitting source area itself. The objective of this study was to investigate uncertainties associated with using OTM-10 for landfills. The spatial variability of emission in the emitting domain can lead to uncertainties of -34 to 190% in the measured flux value when idealistic scenarios were simulated. The level of uncertainty might be higher when the number and locations of emitting sources are not known (typical field conditions). The level of uncertainty can be reduced by improving the layout of the VRPM plane in the field in accordance with an initial survey of the emission patterns. The change in wind direction during an OTM-10 testing setup can introduce an uncertainty of 20% of the measured flux value. This study also provides estimates of the area contributing to flux (ACF) to be used in conjunction with OTM-10 procedures. The estimate of ACF is a function of the atmospheric stability class and has an uncertainty of 10-30%.

Evaluation of landfill gas decay constant for municipal solid waste landfills operated as bioreactors.

Prediction of the rate of gas production from bioreactor landfills is important for the optimization of energy recovery and for estimating greenhouse gas emissions. To improve the predictability of gas production, landfill gas (LFG) composition and flow rates were monitored for 4 yr from one conventional and two bioreactor landfill cells at the Outer Loop Landfill in Louisville, KY. The ultimate methane yield (L(o)) was estimated from the biochemical methane (CH4) potential of freshly buried refuse and the decay rate constant (k) was estimated from measured CH4 collection. The site-specific L(o) was estimated to be 48.4 m3-CH4 wet Mg(-1). The estimated decay rate in the conventional cell (0.06 yr(-1)) was comparable to the AP-42 default value of 0.04 yr(-1), whereas estimates for the two bioreactor cells were substantially higher (approximately 0.11 yr(-1)). The data document the ability of the bioreactor operation to enhance landfill CH4 generation, although the estimated decay rate is sensitive to the selected L(o). The more rapid decomposition in the bioreactor cells reduces the length of time over which gas will be produced and emphasizes the importance of having a LFG collection system operational once the waste receives added moisture.

Effect of an acidic and readily-biodegradable non-hazardous industrial process waste on refuse decomposition.

Non-hazardous industrial process wastes are receiving increased interest from landfill owners, especially with respect to bioreactor operation. These wastes could benefit bioreactors as they represent sources of liquid, nutrients, and/or substrate as well as revenue. However, landfill operators should exercise caution in accepting these wastes, as some could have detrimental effects on refuse decomposition. In this research, the use of laboratory-scale tests to evaluate the effect of one such waste on refuse decomposition is demonstrated. The waste evaluated, referred to as burnt sugar, is an acidic byproduct of corn-based polylactic acid production and represents a source of readily-biodegradable carbon. Lactic acid was the primary constituent of the BS at 0.73 g/g and the COD was measured at 1230 mg COD/g. Testing protocols were adapted to address the specific concerns surrounding the material. Abiotic dissolution tests conducted at mesophilic temperatures indicated that the majority of the waste dissolved into leachate recirculated over a layer of the waste within several days. Abiotic mixing tests suggested that the waste would acidify refuse to pH 6.41 at a loading of 21.9 g/dry kg refuse. However, in biologically active tests, the refuse was able to convert loadings as high as 196.7 g/dry kg refuse to methane. As the loadings increased toward and beyond this level, pronounced detrimental effects to the refuse ecosystem were observed, including a decrease in pH, accumulation of volatile fatty acids and COD, and lag in methane production. The results suggested that actively decomposing refuse has the potential to attenuate relatively high loading of a rapidly degradable but acidic substrate. Nonetheless, caution in the implementation of a field program to accept rapidly biodegradable acidic wastes is critical.

Effect of biosolids on refuse decomposition and phosphorus cycling.

Laboratory-scale reactors containing mixtures of municipal solid waste and wastewater treatment biosolids were monitored to assess the effect of biosolids on refuse decomposition and on phosphorus (P) cycling and speciation among orthophosphate, acid-hydrolysable P, and organic P. The co-disposal of 10 to 20% (by wet weight) aerobically-digested biosolids with residential refuse was compatible with refuse decomposition although the biosolids did not increase either the maximum methane production rate or the cumulative yield, and did not reduce lag times to the onset of methane production. The results of this study indicated that dissolved reactive phosphorus (DRP) was the dominant dissolved P fraction throughout refuse decomposition and that it was negatively correlated with the methane production rate and pH (r² = 0.35 for both). P was not found to limit methane production. Biosolids increased dissolved P as well as ammonia-N in some reactors, but this did not have a significant impact on maximum methane production rates. The maximum tolerated Na+ and K+ concentrations during active methane production were at least 4100 mg Na+ L⁻¹ and 800 mg K+ L⁻¹, respectively.

Effects of compost biocovers on gas flow and methane oxidation in a landfill cover.

Previous publications described the performance of biocovers constructed with a compost layer placed on select areas of a landfill surface characterized by high emissions from March 2004 to April 2005. The biocovers reduced CH(4) emissions 10-fold by hydration of underlying clay soils, thus reducing the overall amount of CH(4) entering them from below, and by oxidation of a greater portion of that CH(4). This paper examines in detail the field observations made on a control cell and a biocover cell from January 1, 2005 to December 31, 2005. Field observations were coupled to a numerical model to contrast the transport and attenuation of CH(4) emissions from these two cells. The model partitioned the biocover's attenuation of CH(4) emission into blockage of landfill gas flow from the underlying waste and from biological oxidation of CH(4). Model inputs were daily water content and temperature collected at different depths using thermocouples and calibrated TDR probes. Simulations of CH(4) transport through the two soil columns depicted lower CH(4) emissions from the biocover relative to the control. Simulated CH(4) emissions averaged 0.0gm(-2)d(-1) in the biocover and 10.25gm(-2)d(-1) in the control, while measured values averaged 0.04gm(-2)d(-1) in the biocover and 14gm(-2)d(-1) in the control. The simulated influx of CH(4) into the biocover (2.7gm(-2)d(-1)) was lower than the simulated value passing into the control cell (29.4gm(-2)d(-1)), confirming that lower emissions from the biocover were caused by blockage of the gas stream. The simulated average rate of biological oxidation predicted by the model was 19.2gm(-2)d(-1) for the control cell as compared to 2.7gm(-2)d(-1) biocover. Even though its V(max) was significantly greater, the biocover oxidized less CH(4) than the control cell because less CH(4) was supplied to it.

Release of trace organic compounds during the decomposition of municipal solid waste components.

Landfill gas contains numerous speciated organic compounds (SOCs) including alkanes, aromatics, chlorinated aliphatic hydrocarbons, alcohols, ketones, terpenes, chlorofluoro compounds, and siloxanes. The source, rate and extent of release of these compounds are poorly understood. The objective of this study was to characterize the release of SOCs and the regulated parameter, non-methane organic compounds (NMOCs) during the decomposition of residential refuse and its major biodegradable components [paper (P), yard waste (YW), food waste (FW)]. Work was conducted under anaerobic conditions in 8-L reactors operated to maximize decomposition. Refuse and YW were also tested under aerobic conditions. NMOC release during anaerobic decomposition of refuse, P, YW, and FW was 0.151, 0.016, 0.038, and 0.221 mg-C dry g(-1), respectively, while release during aerobic decomposition of refuse and YW was 0.282 and 0.236 mg-C dry g(-1), respectively. The highest NMOC release was measured under abiotic conditions (3.01 mg-C dry g(-1)), suggesting the importance of gas stripping. NMOC release was faster than CH4 production in all treatments. Terpenes and ketones accounted for 32-96% of SOC release in each treatment, while volatile fatty acids were not a significant contributor. Release in aerobic systems points to the potential importance of composting plants as an emissions source.

Relationships between analytical methods utilized as tools in the evaluation of landfill waste stability.

In this study, the refuse from 12 landfills of various ages ranging from fresh refuse to material 11 years old was collected, and changes in the bio-stability parameters were determined. The parameters measured included cellulose, lignin, biochemical methane potential (BMP) and volatile solids, along with plastics. These parameters, along with the cellulose to lignin ratio were compared to determine which were most indicative of the bio-stability of the refuse. Lignin and volatile solids measurements were affected by plastics in refuse samples. Plastics increased both lignin and volatile solids measurements by approximately 10%. Cellulose and volatile solids measurements correlated well with age, each other, and with BMP measurements and were therefore considered the best parameters to determine stability. Data for the Riverbend landfill, a landfill with a moisture content of 48%, which is similar to that of bioreactor landfills, showed that degradation was nearly complete after 5 years as indicated by low values for cellulose and BMP.

Nitrogen management in bioreactor landfills.

One scenario for long-term nitrogen management in landfills is ex situ nitrification followed by denitrification in the landfill. The objective of this research was to measure the denitrification potential of actively decomposing and well decomposed refuse. A series of 10-l reactors that were actively producing methane were fed 400 mg NO3-N /l every 48 h for periods of 19-59 days. Up to 29 nitrate additions were either completely or largely depleted within 48 h of addition and the denitrification reactions did not adversely affect the leachate pH. Nitrate did inhibit methane production, but the reactors recovered their methane-producing activity with the termination of nitrate addition. In well decomposed refuse, the nitrate consumption rate was reduced but was easily stimulated by the addition of either acetate or an overlayer of fresh refuse. Addition of acetate at five times the amount required to reduce nitrate did not lead to the production of NH4+ by dissimilatory nitrate reduction. The most probable number of denitrifying bacteria decreased by about five orders of magnitude during refuse decomposition in a reactor that did not receive nitrate. However, rapid denitrification commenced immediately with nitrate addition. This study shows that the use of a landfill as a bioreactor for the conversion of nitrate to a harmless byproduct, nitrogen gas, is technically viable.