Joanne H. Shorter

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.

Development of atmospheric tracer methods to measure methane emissions from natural gas facilities and urban areas.

Environ. Sci. Techno/. 1995, 29, 1468-1 479 Introduction Tracer -Methods To Measure Downloaded by UNIV OF CALIFORNIA IRVINE on August 26, 2015 | http://pubs.acs.org Publication Date: June 1, 1995 | doi: 10.1021/es00006a007 Gas Faciliies and U h n Areas BRIAN K. LAMB,*,’ J. BARRY MCMANUS,* JOANNE H. SHORTER,* CHARLES E . KOLB,* BYARD MOSHER,

Methane emission measurements in urban areas in eastern Germany

R O B E R T C . HARRISS,§ EUGENE ALLWINE,’ DENISE BLAHA,

An estimate of the uptake of atmospheric methyl bromide by agricultural soils

T O U C H E H O W A R D , ” A L E X GUENTHER,l ROBERT A. LOTT,A ROBERT SIVERSON,’ HAL WESTBERG,’ AND PAT ZIMMERMAN- Laboratory for Atmospheric Research, Department of Civil & Environmental Engineering, Washington State University, Pullman, WA 99164-2910, Center for Chemical and Environmental Physics, Aerodyne Research, Inc., Billerica, Massachusetts 01821, Institute for the Study of Earth, Oceans and Space, University of New Hampshire, Durham, New Hampshire 03824, Indaco Air Quality Services, Inc., Pullman, Washington 99163, National Center for Atmospheric Research, Boulder, Colorado 80303, and Gas Research Institute, Chicago, Illinois 60631 -3562 A new, integrated methodologyto locate and measure methane emissions from natural gas systems has been developed. Atmospheric methane sources are identified by elevated ambient CH4 concentrations measured with a mobile laser-based methane analyzer. The total methane emission rate from a source is obtained by simulating the source with a sulfur hexafluoride (SFS) tracer gas release and by measuring methane and tracer concentrations along downwind sampling paths using mobile, real-time analyzers. Combustion sources of methane are dis- tinguished from noncombustion sources by concur- rent ambient carbon dioxide measurements. Three variations on the tracer ratio method are described for application to (1) small underground vaults, (2) above- ground natural gas facilities, and (3) diffuse methane emissions from an entire town. Results from controlled releases and from replicate tests demonstrate thatthe tracer ratio approach can yield total emission rates to within approximately &15%. The estimated accuracy of emission estimates for urban areas with a variety of diffuse emissions is &50%. Methane (CH4) has been a contributor to the increasing burden of greenhouse gases in the earth’s atmosphere for more than a century (1). Faced with significant risks identified in scenarios of increasing greenhouse gas con- centrations, many countries are developing plans to reduce emissions. However, uncertainties in specific source emission rates for CH4 and other non-COz greenhouse gases currently limit the quantitative risk-benefit analysis needed to answer key policy questions related to the socioeconomic impacts of large-scale mitigation actions (2, 3 ) . Initial attempts to estimate CH4 losses to the atmosphere from natural gas production and use assumed that emis- sions could be approximated by industry reports of “unac- counted for” gas (e.g., ref 4). Unaccounted for gas, defined as the difference between the amount of natural gas metered into a system and the amount of gas metered out of a system, does not account for gas losses from wells to the processing plant, gas used as fuel in facilities, theft of gas, meter inaccuracies, and differences in accounting procedures between companies (4,5). Thus, the unaccounted for gas estimates cannot unambiguously be considered an upper or lower bound on emissions (5). Extrapolation of engi- neering estimates or data obtained from component by component sniffing methods also leads to large uncertain- ties in estimated emissions. In the United Kingdom, the British Gas Company estimates CH4 emissions from gas distribution system components to be less than 1% of throughput, while others estimate losses as high as 11% of gas throughput (6). A recent estimate of CH4 leakage from the natural gas system in the former Soviet Union, which was characterized as “tentative and highly conditional” suggested a range of total losses from 3.3% to 7% of gas production ( 7 ) . The U.S. Environmental Protection Agency (EPA) and the Gas Research Institute (GRI) have recently sponsored an integrated field measurement and analysis program to better define methane emissions from the U.S. natural gas system. Drawing on initial measurements using some of the techniques reported here as weil as engineering estimates, GRI has developed a preliminary estimate of methane emissions from the gas industry that equals approximately 1.5 i 0.5% of annual throughput (8). In the case of CH4 emissions due to the use of natural gas, there is an added motivation for correctly prescribing the methane source strength. Since natural gas typically produces 32-45% less COz per unit of thermal output compared to coal and 30% less compared to fuel oil, switching from coal and fuel oil to natural gas has the potential to reduce carbon dioxide emissions and reduce global warming (5). However, CH4 is a more potent greenhouse gas than CO2 on a molecule for molecule basis (9- 1 I). As a result, increasing the usage of natural gas may * To whom correspondence should be addressed: e-mail address: blamb@wsu.edu. + Washington State University. Aerodyne Research, Inc. 5 University of New Hampshire. I’ Indaco Air Quality Services, Inc. National Center for Atmospheric Research. A Gas Research Institute. 1468 ENVIRONMENTAL SCIENCE &TECHNOLOGY / VOL. 29, NO. 6, 1995 0013-936)(/95/0929-1468

Determination of atmospheric methyl bromide by cryotrapping-gas chromatography and application to soil kinetic studies using a dynamic dilution system

09.00/0 @ 1995 American Chemical Society

Mitigation of methane emissions at landfill sites in New England, USA

We have investigated methane emissions from urban sources in the former East Germany using innovative measurement techniques including a mobile real-time methane instrument and tracer release experiments. Anthropogenic and biogenic sources were studied with the emphasis on methane emissions from gas system sources, including urban distribution facilities and a production plant. Methane fluxes from pressure regulating stations ranged from 0.006 to 24. l/min. Emissions from diffuse sources in urban areas were also measured with concentration maps and whole city flux experiments. The area fluxes of the two towns studied were 0.37 and 1.9 μg/m2/s. The emissions from individual gas system stations and total town emissions of this study are comparable to results of similar sites examined in the United States.

Rapid degradation of atmospheric methyl bromide in soils

Published estimates of removal of atmospheric methyl bromide (CH3Br) by agricultural soils are 2.7 Gg yr−1 (Gg = 109 g) [Shorter et al., 1995] and 65.8 Gg yr−1 [Serca et al., 1998]. The Serca et al. estimate, if correct, would suggest that the current value for total removal of atmospheric CH3Br by all sinks of 206 Gg yr−1 (based on Shorter et al., 1995) would be 30% too low. We have calculated a new rate of global agricultural soil uptake of atmospheric CH3Br from a larger sampling of cultivated soils collected from 40 sites located in the United States, Costa Rica, and Germany. First order reaction rates were measured during static laboratory incubations. These data were combined with uptake measurements we reported earlier based on field and laboratory experiments [Shorter et al. 1995]. Tropical (10.2°–10.4°N) and northern (45°–61°N) soils averaged lower reaction rate constants than temperate soils probably due to differing physical and chemical characteristics as well as microbial populations. Our revised global estimate for the uptake of ambient CH3Br by cultivated soils is 7.47±0.63 Gg yr−1, almost three times the value that we reported in 1995.

Methane Emissions at Nine Landfill Sites in the Northeastern United States

Methyl bromide (CH(3)Br) is considered to be a major source of stratospheric Br, which contributes to the destruction of ozone. It is therefore necessary to understand the natural sinks of this compound and to accurately measure ambient mixing ratios. Methodology is described for the measurement of atmospheric CH(3)Br by cryotrapping-gas chromatography and its application to soil kinetics. A 2-propanol/dry ice cryotrap was used to preconcentrate CH(3)Br in standard and air samples, with subsequent detection using a gas chromatograph equipped with an O(2)-doped electron capture detector (GC-ECD). The GC-ECD cryotrapping method had a detection limit of 0.23 pmol of CH(3)Br. This is equivalent to the amount of CH(3)Br in a 500 mL sample of ambient air at the estimated northern hemisphere atmospheric mixing ratio of 11 parts per trillion by volume (pptv). A dynamic dilution system was developed to produce mixing ratios of CH(3)Br ranging between 4 and 1000 pptv. Calibrated mixing ratios of CH(3)Br produced with the dilution system were used to determine soil uptake kinetics employing a dynamic soil incubation method.

Rapid Consumption of Low Concentrations of Methyl Bromide by Soil Bacteria

Field measurements of methane emissions from landfills are essential if one is to accurately constrain uncertainties in current estimates of global methane emissions from landfills and document emissions reductions realized by currently available control technology. Two experimental techniques for the measurement of methane flux from landfills, flux chamber measurements and tracer flux techniques, have been evaluated at a 24 hectare landfill site in New England. Agreement between the two techniques was quite good, with the flux chamber technique giving a landfill wide methane flux of 16.4 m 3 CH 4 min -1 while a series of seven tracer flux tests resulted in a mean flux of 17.8 m 3 CH 4 min -1 . Model estimates suggest that the installation of gas recovery measures at the five largest landfill sites in the state of New Hampshire and the ten largest sites in Massachusetts would reduce landfill emissions in each state by approximately 75%, resulting in a total emissions reduction of 65 x 10 9 g CH 4 /yr.