P. Czepiel

Quantifying the effect of oxidation on landfill methane emissions

Field, laboratory, and computer modeling methods were utilized to quantitatively assess the capability of aerobic microorganisms to oxidize landfill-derived methane (CH4) in cover soils. The investigated municipal landfill, located in Nashua, New Hampshire, was operating without gas controls of any type at the time of sample collection. Soil samples from locations of CH4 flux to the atmosphere were returned to the laboratory and subjected to incubation experiments to quantify the response of oxidation in these soils to temperature, soil moisture, in situ CH4 mixing ratio, soil depth, and oxygen. The mathematical representations of the observed oxidation reponses were combined with measured and predicted soil characteristics in a computer model to predict the rate of CH4 oxidation in the soils at the locations of the measured fluxes described by Czepiel et al. [this issue]. The estimated whole landfill oxidation rate at the time of the flux measurements in October 1994 was 20%. Local air temperature and precipitation data were then used in conjunction with an existing soil climate model to estimate an annual whole landfill oxidation rate in 1994 of 10%.

Nitrous Oxide Emissions from Municipal Wastewater Treatment

Nitrous oxide (N 2 0) emissions from primary and secondary wastewater treatment processes were measured during spring and summer 1993 in Durham, NH. The most significant emissions occurred during secondary aeration. Dissolved N 2 0 generated as a result of denitrification during primary settling was stripped from the liquid during mechanical aeration. Emission factors derived from our field measurements included per capita emissions of 3.2 g of N 2 0 person -1 yr -1 and flow based emissions of 1.6 x 10 -6 of N 2 0 (L of wastewater) -1 .

Landfill methane emissions measured by enclosure and atmospheric tracer methods

Methane (CH4) emissions were measured from the Nashua, New Hampshire municipal landfill using static enclosure and atmospheric tracer methods. The spatial variability of emissions was also examined using geostatistical methods. One hundred and thirty nine enclosure measurements were performed on a regular grid pattern over the emitting surface of the landfill resulting in an estimate of whole landfill emissions of 15,800 L CH4 min−1. Omnidirectional variograms displayed spatial correlation among CH4 fluxes below a separation distance of 7 m. Eleven tracer tests, using sulfur hexafluoride (SF6) as a tracer gas, resulted in a mean emissions estimate of 17,750 L CH4 min−1. The favorable agreement between the emission estimates was further refined using the observed relationship between atmospheric pressure and CH4 flux. This resulted in a pressure-corrected tracer flux estimate of whole landfill emissions of 16,740 L CH4 min−1.

The influence of atmospheric pressure on landfill methane emissions.

Landfills are the largest source of anthropogenic methane (CH4) emissions to the atmosphere in the United States. However, few measurements of whole landfill CH4 emissions have been reported. Here, we present the results of a multi-season study of whole landfill CH4 emissions using atmospheric tracer methods at the Nashua, New Hampshire Municipal landfill in the northeastern United States. The measurement data include 12 individual emission tests, each test consisting of 5-8 plume measurements. Measured emissions were negatively correlated with surface atmospheric pressure and ranged from 7.3 to 26.5 m3 CH4 min(-1). A simple regression model of our results was used to calculate an annual emission rate of 8.4 x 10(6) m3 CH4 year(-1). These data, along with CH4 oxidation estimates based on emitted landfill gas isotopic characteristics and gas collection data, were used to estimate annual CH4 generation at this landfill. A reported gas collection rate of 7.1 x 10(6) m3 CH4 year(-1) and an estimated annual rate of CH4 oxidation by cover soils of 1.2 x 10(6) m3 CH4 year(-1) resulted in a calculated annual CH4 generation rate of 16.7 x 10(6) m3 CH4 year(-1). These results underscore the necessity of understanding a landfills dynamic environment before assessing long-term emissions potential.

Environmental factors influencing the variability of methane oxidation in temperate zone soils

The influence of organic matter and soil moisture on the spatial distribution of methane (CH4) oxidation was examined in temperate zone soils by laboratory incubations. CH4 oxidation in soil cores exhibited distinct vertical zonation with maxima at 3 to 6 cm. The kinetic parameters of CH4 oxidation were measured in soil composites. The maximum rate of CH4 uptake, Vmax, ranged from 6.8 to 7.4 nmol hr−1 g dry soil−1 and the apparent half saturation constant, Km, ranged from 17.4 to 19.9 (parts per million by volume) ppmv. Oxidation in random samples was observed to be influenced by both soil moisture and organic matter contents. The rate of oxidation in each sample increased to a maximum with increasing water content and decreased with additional water. Maximum oxidation rates ranged from 2.2 to 9.0 nmol hr−1 g dry soil−1 at sample moisture contents of 18 to 51%. Organic matter content appears to explain the spatial variability of methane oxidation at optimal soil moisture contents. The oxidation maximum at this site was coincident with an organic matter content of 14% by weight and a gravimetric moisture content of 33%.

Natural and anthropogenic methane sources in New England

We have recently completed a methane emissions inventory for the New England region. Methane emissions were calculated to be 0.91 Tg yr-1, with wetlands and landfills dominating all other sources. Wetlands are estimated to produce 0.33 Tg CH4 yr-1, of which 74% come from Maine. Active landfills emit an estimated 0.28 Tg CH4 yr-1, 60% of which are generated from twelve landfills. Although uncertainty in the estimate is greater, emissions from closed landfills are on the same order of magnitude as active landfills and wetlands; 0.25 Tg CH4 yr-1. Sources of moderate magnitude include ruminant animals (0.05 Tg CH4 yr-1) and residential wood combustion (0.03 Tg CH4 yr-1). Motor vehicles, natural gas, and wastewater treatment make only minor contributions. New England is heavily forested and the soil uptake of atmospheric methane in upland forests, 0.06 Tg CH4 yr-1, decreases emissions from soils by about 18%. Although uncertainties remain, our estimates indicate that even in a highly urbanized region such as New England, natural sources of methane make the single greatest contribution to total emissions, with state totals varying between 8% (Massachusetts) and 92% (Maine). Because emissions from only a few large landfills dominate anthropogenic sources, mitigation strategies focused on these discrete point sources should result in significant improvements in regional air quality. Current federal regulations mandate landfill gas collection at only the largest sites. Expanding recovery efforts to moderately sized landfills through either voluntary compliance or further regulations offers the best opportunity to substantially reduce atmospheric methane in New England. In the short term, however, the large contribution from closed, poorly regulated landfills may make the attribution of air quality improvements difficult. Mitigation efforts toward these landfills should also be a priority.

Methane measurements in central New England: An assessment of regional transport from surrounding sources

The Harvard Forest research site located in central New England is influenced by numerous anthropogenic methane sources on a year-round basis. Methane is strongly correlated to other chemical species that have an anthropogenic component, including acetylene, propane, ethane, hexane, and additional short-lived nonmethane hydrocarbons. The correlation between methane and acetylene is due to the colocation of landfills and cities. The correlation between methane and other short-lived species implies that emissions from local and regional rather than distant sources are the primary cause of elevated events. Wind roses of chemical species are examined for annual and seasonal time periods with enhancements in anthropogenic species corresponding to the location of large cities and landfills. The southwest quadrant is subjected to the most severe pollution events and is impacted by outflow from nearby cities in that sector, including Northampton and Springfield, Massachusetts. Emissions from cities in other quadrants, including Boston and Worcester, Massachusetts, Providence, Rhode Island, and the close-by town of Petersham, Massachusetts, also affect the site, but to a lesser degree. Case studies are used to identify atmospheric conditions that lead to high concentrations of methane and other species. The co-occurrence of a persistent wind direction, light wind speed, and stable atmospheric conditions is the ideal scenario in which emissions from nearby cities and landfills are advected to the site. Emissions from local and regional, rather than distant sources, are the primary cause of elevated events.