Environmental assessment of landfill gas mitigation using biocover and gas collection with energy utilisation at aging landfills.

A life cycle-based environmental assessment was conducted on the mitigation of landfill gas emissions, by implementing biocover and gas collection along with energy utilisation at aging landfills. Based on recent studies about gas generation at Danish landfills, the efficiency of the mitigation technologies involved and the composition of substituted energy production, 15 scenarios were modelled using the EASETECH life cycle assessment model, through which potential environmental impacts in the category "Climate change" were calculated. In all scenarios, biocover and gas collection systems with energy utilisation led to significant environmental improvements compared to the baseline scenario with no emission mitigation action. Scenarios representing biocovers with methane oxidation efficiencies between 70 and 90 % were environmentally superior in terms of climate change impact - in comparison to scenarios with 20-30 years of gas collection and energy utilisation (collection efficiencies between 40 and 80 %). Combining gas collection with energy utilisation and the subsequent installation of a biocover saw major improvements in comparison to where only gas collection and energy utilisation were in effect. Overall, it can be concluded that a biocover under the given assumptions is environmentally more appropriate than gas collection and utilisation at aging landfills, mainly due to methane emissions escaping through the landfill cover during and after the gas collection period playing a crucial role in the latter situation. Maintaining high methane oxidation efficiency for a biocover throughout the lifetime of a landfill is vital for reducing environmental impacts.

The effect of barometric pressure changes on the performance of a passive biocover system, Skellingsted landfill, Denmark.

This study investigated the performance of a passive biocover system at a Danish landfill. The overall methane oxidation efficiency of the system was assessed by comparing annual whole-site methane emissions before and after biocover installation. Annual whole-site methane emission predictions were calculated based on empirical models developed by a discrete number of tracer gas dispersion measurements. Moreover, a series of field campaigns and continuous flux measurements was carried out to evaluate the functionality of an individual biowindow. The results indicated that biocover system performance highly depended on barometric pressure variations. Under decreasing barometric pressure, estimated efficiency declined to 20%, while under increasing barometric pressure, nearly 100% oxidation was achieved. In-situ measurements on a specific biowindow showed a similar oxidation efficiency pattern in respect to barometric pressure changes despite the difference in spatial representation. Eddy covariance results revealed pronounced seasonal variability in the investigated biowindow, measuring higher methane fluxes during the cold period compared to the warm period. Results from the in-situ campaigns confirmed this finding, reporting a threefold increase in the biowindow's methane oxidation capacity from April to May. The annual average oxidation efficiency of the system was estimated to range between 51% and 65%, taking into consideration the impact of changes in barometric pressure and seasonal variability. This indicated an annual reduction in landfill's methane emissions between 24 and 35 tonnes. This study revealed the challenge facing current approaches in documenting accurately the performance of a passive biocover system, due to the short-term variability of oxidation efficiency, which is influenced by barometric pressure changes.

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.

Methane emission dynamics from a Danish landfill: The effect of changes in barometric pressure.

This study investigates temporal variability on landfill methane (CH4) emissions from an old abandoned Danish landfill, caused by the rate of changes in barometric pressure. Two different emission quantification techniques, namely the dynamic tracer dispersion method (TDM) and the eddy covariance method (EC), were applied simultaneously and their results compared. The results showed a large spatial and temporal CH4 emission variation ranging from 0 to 100 kg h-1 and 0 to 12 µmol m-2 s-1, respectively. Landfill CH4 emissions dynamics were influenced by two environmental factors: the rate of change in barometric pressure (a strong negative correlation) and wind speed (a weak positive correlation). The relationship between CH4 emissions and the rate of change in barometric pressure was more complicated than a linear one, thereby making it difficult to estimate accurately annual CH4 emissions from a landfill based on discrete measurements. Furthermore, the results did not show any clear relationship between CH4 emissions and ambient temperature. Large seasonal variations were identified by the two methods, whereas no diurnal variability was observed throughout the investigated period. CH4 fluxes measured with the EC method were strongly correlated with emissions from the TDM method, even though no direct relationship could be established, due to the different sampling ranges of the two methods and the spatial heterogeneity of CH4 emissions.

Closing the methane mass balance for an old closed Danish landfill.

In this study, a methane (CH4) mass balance was established for Hedeland landfill. CH4 generation rates were modelled using a multiphase first-order decay model (The Afvalzorg model) and determined at between 57 and 79 kg h-1. The CH4 emission rate was quantified at between 2 and 14 kg h-1, using the tracer gas dispersion method and the CH4 gas recovery efficiency was between 8 and 21%. At three places along the perimeter of the landfill, gas remediation systems have been installed to protect the residential houses from any risk of migrating landfill gas. About 0.76 kg h-1 of CH4 was extracted from these three remediation systems. Using a carbon mass balance for the lateral migrating landfill gas showed a fractional oxidation of about 78%, which corresponded to a CH4 flux of 3.5 kg h-1 from the three remediation systems, including the oxidised CH4. The total lateral CH4 flux (un-oxidised) from the total landfill perimeter was estimated at between 6.9 and 10.4 kg h-1. CH4 oxidation efficiency in the landfill cover soil, determined from stable carbon isotope analyses, was found to be between 12% and 92%. This resulted in an average CH4 oxidation rate of 32 kg h-1, using an average CH4 emission rate of 8 kg h-1. CH4 surface screenings and surface flux measurements supported the hypothesis that oxidation efficiency was in the higher range and that oxidation could close the CH4 mass balance.

Biofiltration of diluted landfill gas in an active loaded open-bed compost filter.

Microbial oxidation in a biofilter is a treatment solution for diluted landfill gas (LFG), for instance at old landfills, where LFG recovery is no longer feasible, or from remediation systems designed to cut off laterally migrating LFG. In this study, an actively loaded open-bed compost filter, designed for the treatment of diluted LFG, was tested at an old landfill in Denmark. An 18 m3 biofilter was constructed in a 30 m3 container loaded with LFG mixed with air, in order to obtain diluted LFG. The inlet concentration of methane (CH4) fluctuated between 4.4 and 9.2 vol% during the five tested flow campaigns, resulting in CH4 loads of 106-794 g CH4 m-2 d-1. The maximum identified CH4 oxidation rate was 460 g m-2 d-1, with an overall CH4 oxidation efficiency of 58%. Due to preferential flows, especially along the edges of the filter at the transition points between the compost and the container wall, an overall CH4 oxidation efficiency of 100% was never achieved. However, pore gas profiles in selected areas in the filter material showed oxidation efficiencies close to 100%. The results were supported by tracer gas tests showing average oxidation efficiency in the nine measuring points of 89% at a CH4 load of 487 ± 64 g CH4 m-2 d-1.

Assessment of a landfill methane emission screening method using an unmanned aerial vehicle mounted thermal infrared camera - A field study.

An unmanned aerial vehicle (UAV)-mounted thermal infrared (TIR) camera's ability to delineate landfill gas (LFG) emission hotspots was evaluated in a field test at two Danish landfills (Hedeland landfill and Audebo landfill). At both sites, a test area of 100 m2 was established and divided into about 100 measuring points. The relationship between LFG emissions and soil surface temperatures were investigated through four to five measuring campaigns, in order to cover different atmospheric conditions along with increasing, decreasing and stable barometric pressure. For each measuring campaign, a TIR image of the test area was obtained followed by the measurement of methane (CH4) and carbon dioxide (CO2) emissions at each measuring point, using a static flux chamber. At the same time, soil temperatures measured on the surface, at 5 cm and 10 cm depths, were registered. At the Hedeland landfill, no relationship was found between LFG emissions and surface temperatures. In addition, CH4 emissions were very limited, on average 0.92-4.52 g CH4 m-2 d-1, and only measureable on the two days with decreasing barometric pressure. TIR images from Hedeland did not show any significant temperature differences in the test area. At the Audebo landfill, an area with slightly higher surface temperatures was found in the TIR images, and the same pattern with slightly higher temperatures was found at a depth of 10 cm. The main LFG emissions were found in the area with the higher surface temperatures. LFG emissions at Audebo were influenced significantly by changes in barometric pressure, and the average CH4 emissions varied between 111 g m-2 d-1 and 314 g m-2 d-1, depending on whether the barometric pressure gradient had increased or decreased, respectively. The temperature differences observed in the TIR images from both landfills were limited to between 0.7 °C and 1.2 °C. The minimum observable CH4 emission for the TIR camera to identify an emission hotspot was 150 g CH4 m-2 d-1 from an area of more than 1 m2.

Amendment of arsenic and chromium polluted soil from wood preservation by iron residues from water treatment.

An iron-rich water treatment residue (WTR) consisting mainly of ferrihydrite was used for immobilization of arsenic and chromium in a soil contaminated by wood preservatives. A leaching batch experiment was conducted using two soils, a highly contaminated soil (1033 mg kg(-1) As and 371 mg kg(-1) Cr) and slightly contaminated soil (22 5mg kg(-1) As and 27 mg kg(-1) Cr). Compared to an untreated reference soil, amendment with 5% WTR reduced leaching in the highly contaminated soil by 91% for Cr and 98% for As. No aging effect was observed after 103 d. In a small field experiment, soil was mixed with 2.5% WTR in situ. Pore water was extracted during 3 years from the amended soil and a control site. Pore water arsenic concentrations in the amended soil were more than two orders of magnitude lower than in the control for the upper samplers. An increased release of arsenic was observed during winter in both fields, mostly in the deepest samplers. This is likely due to the formation of a pseudo-gley because of precipitation surplus. Stabilization of arsenic and chromium contaminated soil using WTR is a promising method but the transformation of ferrihydrite in soil proves a concern in case of waterlogged soils. Still the amendment minimized the leaching of arsenic, even in cases of seasonal releases.

Quantification of multiple methane emission sources at landfills using a double tracer technique.

A double tracer technique was used successfully to quantify whole-site methane (CH(4)) emissions from Fakse Landfill. Emissions from different sections of the landfill were quantified by using two different tracers. A scaled-down version of the tracer technique measuring close-by to localized sources having limited areal extent was also used to quantify emissions from on-site sources at the landfill facility, including a composting area and a sewage sludge storage pit. Three field campaigns were performed. At all three field campaigns an overall leak search showed that the CH(4) emissions from the old landfill section were localized to the leachate collection wells and slope areas. The average CH(4) emissions from the old landfill section were quantified to be 32.6 ± 7.4 kg CH(4)h(-1), whereas the source at the new section was quantified to be 10.3 ± 5.3 kg CH(4)h(-1). The CH(4) emission from the compost area was 0.5 ± 0.25 kg CH(4)h(-1), whereas the carbon dioxide (CO(2)) and nitrous oxide (N(2)O) flux was quantified to be in the order of 332 ± 166 kg CO(2)h(-1) and 0.06 ± 0.03 kg N(2)Oh(-1), respectively. The sludge pit located west of the compost material was quantified to have an emission of 2.4 ± 0.63 kg h(-1) CH(4), and 0.03 ± 0.01 kg h(-1) N(2)O.

Transport and reaction processes affecting the attenuation of landfill gas in cover soils.

Methane and trace organic gases produced in landfill waste are partly oxidized in the top 40 cm of landfill cover soils under aerobic conditions. The balance between the oxidation of landfill gases and the ingress of atmospheric oxygen into the soil cover determines the attenuation of emissions of methane, chlorofluorocarbons, and hydrochlorofluorocarbons to the atmosphere. This study was conducted to investigate the effect of oxidation reactions on the overall gas transport regime and to evaluate the contributions of various gas transport processes on methane attenuation in landfill cover soils. For this purpose, a reactive transport model that includes advection and the Dusty Gas Model for simulation of multicomponent gas diffusion was used. The simulations are constrained by data from a series of counter-gradient laboratory experiments. Diffusion typically accounts for over 99% of methane emission to the atmosphere. Oxygen supply into the soil column is driven exclusively by diffusion, whereas advection outward offsets part of the diffusive contribution. In the reaction zone, methane consumption reduces the pressure gradient, further decreasing the significance of advection near the top of the column. Simulations suggest that production of water or accumulation of exopolymeric substances due to microbially mediated methane oxidation can significantly reduce diffusive fluxes. Assuming a constant rate of methane production within a landfill, reduction of the diffusive transport properties, primarily due to exopolymeric substance production, may result in reduced methane attenuation due to limited O(2) -ingress.

Atmospheric emissions and attenuation of non-methane organic compounds in cover soils at a French landfill.

In addition to methane (CH(4)) and carbon dioxide (CO(2)), landfill gas may contain more than 200 non-methane organic compounds (NMOCs) including C(2+)-alkanes, aromatics, and halogenated hydrocarbons. Although the trace components make up less than 1% v/v of typical landfill gas, they may exert a disproportionate environmental burden. The objective of this work was to study the dynamics of CH(4) and NMOCs in the landfill cover soils overlying two types of gas collection systems: a conventional gas collection system with vertical wells and an innovative horizontal gas collection layer consisting of permeable gravel with a geomembrane above it. The 47 NMOCs quantified in the landfill gas samples included primarily alkanes (C(2)-C(10)), alkenes (C(2)-C(4)), halogenated hydrocarbons (including (hydro)chlorofluorocarbons ((H)CFCs)), and aromatic hydrocarbons (BTEXs). In general, both CH(4) and NMOC fluxes were all very small with positive and negative fluxes. The highest percentages of positive fluxes in this study (considering all quantified species) were observed at the hotspots, located mainly along cell perimeters of the conventional cell. The capacity of the cover soil for NMOC oxidation was investigated in microcosms incubated with CH(4) and oxygen (O(2)). The cover soil showed a relatively high capacity for CH(4) oxidation and simultaneous co-oxidation of the halogenated aliphatic compounds, especially at the conventional cell. Fully substituted carbons (TeCM, PCE, CFC-11, CFC-12, CFC-113, HFC-134a, and HCFC-141b) were not degraded in the presence of CH(4) and O(2). Benzene and toluene were also degraded with relative high rates. This study demonstrates that landfill soil covers show a significant potential for CH(4) oxidation and co-oxidation of NMOCs.

A simple model for the distribution and fate of organic chemicals in a landfill: MOCLA.

A simple mathematical model (MOCLA: Model for Organic Chemicals in Landfills) is presented, describing the distribution of organic chemicals between leachate, gas and solid waste. The model also predicts the fate of the chemicals in terms of emissions with leachate and landfill gas and in terms of degradation and transformation in the landfill. Local equilibrium is assumed for the distribution of the chemicals in the landfill as expressed by Henry's Law for the leachate-gas interface, and by the linear partition coefficient based on the waste solid organic carbon content for the waste-leachate interface. Degradation of the chemicals is expressed as a first order reaction. Annual specific leachate and gas generation data in combination with data on landfill area and volume allow for prediction of main emission routes. Model simulations involving two landfill scenarios for a number of chemicals with different physico-chemical characteristics indicate that volatilisation is a likely route for some chemicals (e.g. vinyl chloride, and some of the freons), while other chemicals (e.g. phenol, lower chlorinated aliphatic compounds) more likely will appear as dissolved in the leachate. However, many chemicals will be strongly associated with the solid waste (e.g. dichlorobenzene, naphthalene, and higher Polycyclic Aromatic Hydrocarbons (PAHs), and the pool available will be able to supply the landfill gas and leachate with organic trace components for decades unless these are degraded in the landfill. The model suggests that, in addition to the physico-chemical characteristics of the organic chemical, the presence of free phases of organic chemicals and the degradability of the chemicals are the main factors controlling the fate and emissions of organic chemicals in the landfill environment.

Composition of leachate from old landfills in Denmark.

The Danish counties have performed numerous investigations of old landfills. These investigations have been presented in several reports, but no comprehensive summary of the findings has been carried out. The objective of this study was to evaluate the typical composition of leachates from old smaller landfills by a comprehensive review of the investigations carried out by the counties. In total 106 landfills were selected by criteria avoiding dilution effects. A database was constructed using a standard program. Statistical evaluations showed that the leachate concentrations in general decreased with the age of the landfill, and that the leachate concentrations were lower than found in other similar studies.

Lateral gas transport in soil adjacent to an old landfill: factors governing emissions and methane oxidation.

Field investigations of lateral gas transport and subsequent emissions in soil adjacent to an old landfill in Denmark were conducted during a 1-year period. A significant seasonal variation in the emissions with high carbon dioxide and low methane fluxes in the summer (May to October) was observed. This was attributed to methane oxidation. Diurnal measurements during a drop in barometric pressure showed that the fluxes of landfill gas changed dramatically within a very short time. The concentrations and the soil moisture content in the upper part of the soil profile had significant influence on the fluxes, as did the distance from the landfill border, temperature, barometric pressure and the pressure gradient. Statistical analyses proved that soil moisture described the largest part of the variation. No methane is emitted during the summer. Calculations and isotope analyses showed that very high fractions of the laterally migrating methane were oxidised.

Lateral gas transport in soil adjacent to an old landfill: factors governing gas migration.

Field experiments investigating lateral gas transport in soil adjacent to an old landfill in Denmark during a one-year period were conducted. A significant seasonal variation, with low concentrations of methane and high concentrations of carbon dioxide in the summer, caused by methane oxidation was observed. There was a good correlation between pressure above the barometric pressure and the methane concentration in the soil, indicating that advective flow was the controlling process. This was confirmed by calculations. Diurnal measurement during a drop in barometric pressure showed that lateral migration of landfill gas was a very dynamic system and the concentrations of LFG at a specific place and depth changed dramatically within a very short time. The experiments showed that change in barometric pressure was an important factor affecting gas migration at the Skellingsted landfill in Denmark.

Release of CFC-11 from disposal of polyurethane foam waste.

The halocarbon CFC-11 has extensively been used as a blowing agent for polyurethane (PUR) insulation foams in home appliances and for residential and industrial construction. Release of CFCs is an important factor in the depletion of the ozone layer. For CFC-11 the future atmospheric concentrations will mainly depend on the continued release from PUR foams. Little is known about rates and time frames of the CFC release from foams especially after treatment and disposal of foam containing waste products. The CFC release is mainly controlled by slow diffusion out through the PUR. From the literature and by reevaluation of an old reported experiment, diffusion coefficients in the range of 0.05-1.7 x 10(-14) m2 s-1 were found reflecting differences in foam properties and experimental designs. Laboratory experiments studying the distribution of CFC in the foam and the short-term releases after shredding showed that about 40% of the CFC is solubilized in the PUR phase, and that up to 10% of the total content will be released within a few weeks if the foam is shredded down to 2-cm sized pieces. For smaller pieces the quick release will be larger. Fifty percent of residual CFC content will be released within 9-300 years from 2-cm pieces based on the range in diffusion coefficients reported. For larger pieces the initial release is insignificant, and the release time frames are much longer than for the shredded foam.

Lateral gas transport in soil adjacent to an old landfill: factors governing gas migration.

Field experiments investigating lateral gas transport in soil adjacent to an old landfill in Denmark during a one-year period were conducted. A significant seasonal variation, with low concentrations of methane and high concentrations of carbon dioxide in the summer, caused by methane oxidation was observed. There was a good correlation between pressure above the barometric pressure and the methane concentration in the soil, indicating that advective flow was the controlling process. This was confirmed by calculations. Diurnal measurement during a drop in barometric pressure showed that lateral migration of landfill gas was a very dynamic system and the concentrations of LFG at a specific place and depth changed dramatically within a very short time. The experiments showed that change in barometric pressure was an important factor affecting gas migration at the Skellingsted landfill in Denmark.

Lateral gas transport in soil adjacent to an old landfill: factors governing emissions and methane oxidation.

Field investigations of lateral gas transport and subsequent emissions in soil adjacent to an old landfill in Denmark have been conducted during a one-year period. A significant seasonal variation in the emissions with high carbon dioxide and low methane fluxes in the summer (May to October) was observed. This was attributed to methane oxidation. Diumal measurements during a drop in barometric pressure showed that the fluxes of landfill gas changed dramatically within a very short time. The concentrations and the soil moisture content in the upper part of the soil profile had significant influence on the fluxes, as did the distance from the landfill border, temperature, barometric pressure and the pressure gradient. Statistical analyses proved that soil moisture described the largest part of the variation. No methane at all emitted during the summer. Calculations and isotope analyses showed that very high fractions of the laterally migrating methane were oxidised.