Julia Gebert

Microbial methane oxidation processes and technologies for mitigation of landfill gas emissions

Landfill gas containing methane is produced by anaerobic degradation of organic waste. Methane is a strong greenhouse gas and landfills are one of the major anthropogenic sources of atmospheric methane. Landfill methane may be oxidized by methanotrophic microorganisms in soils or waste materials utilizing oxygen that diffuses into the cover layer from the atmosphere. The methane oxidation process, which is governed by several environmental factors, can be exploited in engineered systems developed for methane emission mitigation. Mathematical models that account for methane oxidation can be used to predict methane emissions from landfills. Additional research and technology development is needed before methane mitigation technologies utilizing microbial methane oxidation processes can become commercially viable and widely deployed.

Kinetics of microbial landfill methane oxidation in biofilters

A methane oxidizing biofilter system fitted to the passive venting system of a harbor sludge landfill in Germany was characterized with respect to the the methanotrophic population, methane oxidizing capacity, and reaction kinetics. Methanotrophic cell counts stabilized on a high level with 1.3 x 10(8) to 7.1 x 10(9) cells g dw(-1) about one year after first biofilter operation, and a maximum of 1.2 x 10(11) cells g dw(-1). Potential methane oxidizing activity varied between 5.3 and 10.7 microg h(-1) g dw(-1). Cell numbers correlated well with methane oxidation activities. Extrapolation of potential activities gave methane removal rates between 35 and 109 g CH4 h(-1) m(-3), calculated for 30 degrees C. Optimum temperature was 38 degrees C for freshly sampled biofilter material and 22 degrees C for a methanotrophic enrichment culture grown at 10 degrees C incubation temperature. Substrate kinetics revealed the presence of a low-affinity methane oxidizing community with a high Vmax of 1.78 micromol CH4 h(-1) g ww(-1) and a high K(M) of 15.1 microM. K(MO2) for methane oxidation was 58 microM. No substantial methane oxidizing activity was detected below 1.7-2.6 vol.-% O2 in the gaseous phase. Methane deprivation led to a decrease in methane oxidation activity within 5-9 weeks but could still be detected after 25 weeks of substrate deprivation and was fully restored within 3 weeks of continuous methane supply. Very high salt loads are leached from the novel biofilter material, expanded clay, yielding electric conductivity values of up to 15 mS cm(-1) in the leachate. Values > 6 mS cm(-1) were shown to depress methane consumption. Water retention characteristics of the material proved to be favourable for methane oxidizing systems with a gas permeable volume of 78% of bulk volume at field capacity water content. Correspondingly, no influence of water content on methane oxidation activity could be detected at water contents between 2.5 and 20 vol.-%.

Biotic systems to mitigate landfill methane emissions

Landfill gases produced during biological degradation of buried organic wastes include methane, which when released to the atmosphere, can contribute to global climate change. Increasing use of gas collection systems has reduced the risk of escaping methane emissions entering the atmosphere, but gas capture is not 100% efficient, and further, there are still many instances when gas collection systems are not used. Biotic methane mitigation systems exploit the propensity of some naturally occurring bacteria to oxidize methane. By providing optimum conditions for microbial habitation and efficiently routing landfill gases to where they are cultivated, a number of bio-based systems, such as interim or long-term biocovers, passively or actively vented biofilters, biowindows and daily-used biotarps, have been developed that can alone, or with gas collection, mitigate landfill methane emissions. This paper reviews the science that guides bio-based designs; summarizes experiences with the diverse natural or engineered substrates used in such systems; describes some of the studies and field trials being used to evaluate them; and discusses how they can be used for better landfill operation, capping, and aftercare.

Analysis of methanotrophic communities in landfill biofilters using diagnostic microarray.

Biofilters operated for the microbial oxidation of landfill methane at two sites in Northern Germany were analysed for the composition of their methanotrophic community by means of diagnostic microarray targeting the pmoA gene of methanotrophs. The gas emitted from site Francop (FR) contained the typical principal components (CH4, CO2, N2) only, while the gas at the second site Müggenburger Strasse (MU) was additionally charged with non-methane volatile organic compounds (NMVOCs). Methane oxidation activity measured at 22 degrees C varied between 7 and 103 microg CH4 (g dw)(-1) h(-1) at site FR and between 0.9 and 21 microg CH4 (g dw)(-1) h(-1) at site MU, depending on the depth considered. The calculated size of the active methanotrophic population varied between 3 x 10(9) and 5 x 10(11) cells (g dw)(-1) for biofilter FR and 4 x 10(8) to 1 x 10(10) cells (g dw)(-1) for biofilter MU. The methanotrophic community in both biofilters as well as the methanotrophs present in the landfill gas at site FR was strongly dominated by type II organisms, presumably as a result of high methane loads, low copper concentration and low nitrogen availability. Within each biofilter, community composition differed markedly with depth, reflecting either the different conditions of diffusive oxygen supply or the properties of the two layers of materials used in the filters or both. The two biofilter communities differed significantly. Type I methanotrophs were detected in biofilter FR but not in biofilter MU. The type II community in biofilter FR was dominated by Methylocystis species, whereas the biofilter at site MU hosted a high abundance of Methylosinus species while showing less overall methanotroph diversity. It is speculated that the differing composition of the type II population at site MU is driven by the presence of NMVOCs in the landfill gas fed to the biofilter, selecting for organisms capable of co-oxidative degradation of these compounds.

Activity and structure of methanotrophic communities in landfill cover soils.

The composition of the methanotrophic community in soil covers on five landfills in Northern and Eastern Germany was investigated by means of diagnostic microarray and terminal restriction fragment length polymorphism (T-RFLP), both targeting the pmoA gene of methanotrophs. Physical and chemical properties of the 15 sampled soil profiles varied greatly, thus providing for very different environmental conditions. The potential methane oxidation activity, assessed using undisturbed soil cores, varied between 0.2 and 28 µg CH4 gdw (-1)  h(-1) , the latter amounting to 426 g CH4 m(-2)  h(-1) . Total nitrogen was found to be the soil variable correlating most strongly with methanotrophic activity. Explaining close to 50% of the observed variability, this indicates that on the investigated sites activity and thus abundance of methanotrophs may have been nitrogen-limited. Variables that enhance organic matter and thus nitrogen accumulation, such as field capacity, also positively impacted methanotrophic activity. In spite of the great variability of soil properties and different geographic landfill location, both microarray and T-RFLP analysis suggested that the composition of the methanotrophic community on all five sites, in all profiles and across all depths was similar. Methylocystis, Methylobacter and Methylococcus species, including Methylococcus-related uncultivated methanotrophs, were predominantly detected among type II, Ia and Ib methanotrophs, respectively. This indicates that the high methane fluxes typical for landfill environments may be the most influential driver governing the community composition, or other variables not analysed in this study. Principal component analysis suggested that community diversity is most influenced by the site from which the samples were taken and second, from the location on the individual sites, i.e. the soil profile. Landfill and individual profiles reflect the combined impact of all effective variables, including those that were not measured in this study.

Can soil gas profiles be used to assess microbial CH4 oxidation in landfill covers

A method is proposed to estimate CH(4) oxidation efficiency in landfill covers, biowindows or biofilters from soil gas profile data. The approach assumes that the shift in the ratio of CO(2) to CH(4) in the gas profile, compared to the ratio in the raw landfill gas, is a result of the oxidation process and thus allows the calculation of the cumulative share of CH(4) oxidized up to a particular depth. The approach was validated using mass balance data from two independent laboratory column experiments. Values corresponded well over a wide range of oxidation efficiencies from less than 10% to nearly total oxidation. An incubation experiment on 40 samples from the cover soil of an old landfill showed that the share of CO(2) from respiration falls below 10% of the total CO(2) production when the methane oxidation capacity is 3.8 μg CH(4)g(dw)(-1)h(-1) or higher, a rate that is often exceeded in landfill covers and biofilters. The method is mainly suitable in settings where the CO(2) concentrations are not significantly influenced by processes such as respiration or where CH(4) loadings and oxidation rates are high enough so that CO(2) generated from CH(4) oxidation outweighs other sources of CO(2). The latter can be expected for most biofilters, biowindows and biocovers on landfills. This simple method constitutes an inexpensive complementary tool for studies that require an estimation of the CH(4) oxidation efficiency values in methane oxidation systems, such as landfill biocovers and biowindows.

Spatial variability of soil gas concentration and methane oxidation capacity in landfill covers

In order to devise design criteria for biocovers intended to enhance the microbial oxidation of landfill methane it is critical to understand the factors influencing gas migration and methane oxidation in landfill cover soils. On an old municipal solid waste landfill in north-western Germany soil gas concentrations (10, 40, 90 cm depth), topsoil methane oxidation capacity and soil properties were surveyed at 40 locations along a 16 m grid. As soil properties determine gas flow patterns it was hypothesized that the variability in soil gas composition and the subsequent methanotrophic activity would correspond to the variability of soil properties. Methanotrophic activity was found to be subject to high spatial variability, with values ranging between 0.17 and 9.80 g CH(4)m(-2)h(-1)(.) Considering the current gas production rate of 0.03 g CH(4)m(-2)h(-1), the oxidation capacity at all sampled locations clearly exceeded the flux to the cover, and can be regarded as an effective instrument for mitigating methane fluxes. The methane concentration in the cover showed a high spatial heterogeneity with values between 0.01 and 0.32 vol.% (10 cm depth), 22.52 vol.% (40 cm), and 36.85 vol.% (90 cm). The exposure to methane raised the oxidation capacity, suggested by a statistical correlation to an increase in methane concentration at 90 cm depth. Methane oxidation capacity was further affected by the methanotroph bacteria pH optimum and nutrient availability, and increased with decreasing pH towards neutrality, and increased with soluble ion concentration). Soil methane and carbon dioxide concentration increased with lower flow resistance of the cover, as represented by the soil properties of a reduced bulk density, increase in air capacity and in relative ground level.

Assessment of the methane oxidation capacity of compacted soils intended for use as landfill cover materials.

The microbial oxidation of methane in engineered cover soils is considered a potent option for the mitigation of emissions from old landfills or sites containing wastes of low methane generation rates. A laboratory column study was conducted in order to derive design criteria that enable construction of an effective methane oxidising cover from the range of soils that are available to the landfill operator. Therefore, the methane oxidation capacity of different soils was assessed under simulated landfill conditions. Five sandy potential landfill top cover materials with varying contents of silt and clay were investigated with respect to methane oxidation and corresponding soil gas composition over a period of four months. The soils were compacted to 95% of their specific proctor density, resulting in bulk densities of 1.4-1.7 g cm(-3), reflecting considerably unfavourable conditions for methane oxidation due to reduced air-filled porosity. The soil water content was adjusted to field capacity, resulting in water contents ranging from 16.2 to 48.5 vol.%. The investigated inlet fluxes ranged from 25 to about 100g CH(4)m(-2)d(-1), covering the methane load proposed to allow for complete oxidation in landfill covers under Western European climate conditions and hence being suggested as a criterion for release from aftercare. The vertical distribution of gas concentrations, methane flux balances as well as stable carbon isotope studies allowed for clear process identifications. Higher inlet fluxes led to a reduction of the aerated zone, an increase in the absolute methane oxidation rate and a decline of the relative proportion of oxidized methane. For each material, a specific maximum oxidation rate was determined, which varied between 20 and 95 g CH(4)m(-2)d(-1) and which was positively correlated to the air-filled porosity of the soil. Methane oxidation efficiencies and gas profile data imply a strong link between oxidation capacity and diffusive ingress of atmospheric air. For one material with elevated levels of fine particles and high organic matter content, methane production impeded the quantification of methane oxidation potentials. Regarding the design of landfill cover layers it was concluded that the magnitude of the expected methane load, the texture and expected compaction of the cover material are key variables that need to be known. Based on these, a column study can serve as an appropriate testing system to determine the methane oxidation capacity of a soil intended as landfill cover material.

Temporal variability of soil gas composition in landfill covers.

In order to assess the temporal variability of the conditions for the microbial oxidation of methane in landfill cover soils and their driving variables, gas composition at non-emissive and strongly emissive locations (hotspots) was monitored on a seasonal, daily and hourly time scale on an old, unlined landfill in northern Germany. Our study showed that the impact of the various environmental factors varied with the mode of gas transport and with the time scale considered. At non-emissive sites, governed by diffusive gas transport, soil gas composition was subject to a pronounced seasonal variation. A high extent of aeration, low methane concentrations and a high ratio of CO(2) to CH(4) were found across the entire depth of the soil cover during the warm and dry period, whereas in the cool and moist period aeration was less and landfill gas migrated further upward. Statistically, variation in soil gas composition was best explained by the variation in soil temperature. At locations dominated by advective gas transport and showing considerable emissions of methane, this pattern was far less pronounced with only little increase in the extent of aeration during drier periods. Here, the change of barometric pressure was found to impact soil gas composition. On a daily scale under constant conditions of temperature, gas transport at both types of locations was strongly impacted by the change in soil moisture. On an hourly scale, under constant conditions of temperature and moisture, gas migration was impacted most by the change in barometric pressure. It was shown that at diffusion-dominated sites complete methane oxidation was achieved even under adverse wintry conditions, whereas at hotspots, even under favorable dry and warm conditions, aerobic biological activity can be limited to the upper crust of the soil.

Improving the aeration of critical fine-grained landfill top cover material by vegetation to increase the microbial methane oxidation efficiency

The natural methane oxidation potential of methanotrophic bacteria in landfill top covers is a sustainable and inexpensive method to reduce methane emissions to the atmosphere. Basically, the activity of methanotrophic bacteria is limited by the availability of oxygen in the soil. A column study was carried out to determine whether and to what extent vegetation can improve soil aeration and maintain the methane oxidation process. Tested soils were clayey silt and mature compost. The first soil is critical in light of surface crusting due to vertical erosion of an integral part of fine-grained material, blocking pores required for the gas exchange. The second soil, mature compost, is known for its good methane oxidation characteristics, due to high air-filled porosity, favorable water retention capacity and high nutrient supply. The assortment of plants consisted of a grass mixture, Canadian goldenrod and a mixture of leguminous plants. The compost offered an excellent methane oxidation potential of 100% up to a CH(4)-input of 5.6l CH(4)m(-2)h(-1). Whereas the oxidation potential was strongly diminished in the bare control column filled with clayey silt even at low CH(4)-loads. By contrast the planted clayey silt showed an increased methane oxidation potential compared to the bare column. The spreading root system forms secondary macro-pores, and hence amplifies the air diffusivity and sustain the oxygen supply to the methanotrophic bacteria. Water is produced during methane oxidation, causing leachate. Vegetation reduces the leachate by evapotranspiration. Furthermore, leguminous plants support the enrichment of soil with nitrogen compounds and thus improving the methane oxidation process. In conclusion, vegetation is relevant for the increase of oxygen diffusion into the soil and subsequently enhances effective methane oxidation in landfill cover soils.