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Atmospheric Environment 74 (2013) 422E431 Atmospheric Environment 74 (2013) 422e431 Contents lists available at SciVerse ScienceDirect Atmospheric Environment journal homepage: www.elsevier.com/locate/atmosenv Transcontinental methane measurements: Part 1. A mobile surface platform for source investigations Paige Farrell, Daniel Culling, Ira Leifer* Marine Science Institute, University of California, Santa Barbara, CA 93106, United States highlights < First-ever cross-country continent scale methane measurements. < First quantification of methane emissions from the La Brea tar pit/seepage area geologic source. < Desert background methane measurements. < Lower atmospheric vertical profiling using a mountain descending road. article info abstract Article history: The potent greenhouse gas, methane, CH4, originates from a wide range of anthropogenic and natural Received 24 March 2012 sources. A ground-based, satellite-scale, transcontinental (Florida to California) survey was conducted to Received in revised form understand better emissions from key sources including wetlands, forest fire, and geologic sources, as 12 July 2012 well as to acquire desert background values and lower atmosphere vertical profiling in the San Ber- Accepted 5 February 2013 nardino Mountains. A total of 6600 measurements along 7020 km of roadways were made by flame ion detection, gas chromatography (GC) onboard a recreational vehicle in 2010, and during a second survey Keywords: with a cavity ring-down spectrometer system in Southern California in 2012. Significant vibration Methane Gas chromatography reduction efforts allowed near continuous mobile GC measurements. fi Wetlands Nocturnal CH4 measurements tended to be higher compared to daytime values, sometime signi - Greenhouse gas cantly, for similar sources and were concluded due to day/night meteorological differences. The lowest Fire GC observations were 1.80 ppm, observed in the California desert, w60 ppb less than minimum desert Geologic methane CH4 observed in 2012. Thanks to smoke visualization of a brush fire plume, the flux from the fire was 1 Seepage estimated at 0.15 kiloton dayÀ . Geologic CH4 emissions from the La Brea tar pit and surrounding areas La Brea tar pits were surprisingly strong, with peak concentrations of nearly 50 ppm and highly elevated CH4 concen- Southern California trations extending over at least w100 km2, and accounting potentially for a significant fraction of the LA Emission basin CH emissions. Geologic CO emissions also were observed. South US 4 2 Ó 2013 Elsevier Ltd. All rights reserved. 1. Introduction concentrations nearly stabilizing in the last decade. These changes may have resulted from anthropogenic emissions (Aydin et al., 1.1. Atmospheric methane 2011), primarily related to Fossil Fuel Industrial emissions mask- ing wetlands increases (Bousquet et al., 2006), although decreased CH4 has a greenhouse warming potential 26 times that of carbon microbial emission have been proposed (Kai et al., 2011). Since dioxide, CO2, on a per molecule basis and century timescale; 2008, strong CH4 growth has resumed (Heimann, 2011), high- however, on a 20-year timescale its radiative contribution is greater lighting the need for better understanding of sources and trends. than that of CO2 (IPCC, 2007), due in part to its shorter lifetime (8e Atmospheric CH4 concentration depends on the balance between 10 years). Since the industrial revolution, CH4 concentrations have sources and sinks, which primarily is governed by hydroxyl radical, nearly tripled, although growth slowed in the 1990s with CH4 OH, oxidation. Other losses include escape to the stratosphere, soil, and shallow sediment microbial degradation, and chlorine oxidation. The latter three account for w5% each. Atmospheric CH4 isotopic * Corresponding author. Tel.: 1 805 893 4931; fax: 1 805 893 4927. modeling suggests OH oxidation has increased w5% since 1980, þ þ E-mail addresses: [email protected], [email protected] (I. Leifer). decreasing CH4 lifetimes (Lassey and Ragnauth, 2010). 1352-2310/$ e see front matter Ó 2013 Elsevier Ltd. All rights reserved. http://dx.doi.org/10.1016/j.atmosenv.2013.02.014 P. Farrell et al. / Atmospheric Environment 74 (2013) 422e431 423 1 Natural (145e260 Tg yrÀ ) and anthropogenic (264e (Yokota et al., 2009). However, satellite footprints are large, 30 27e 1 1 Â 428 Tg yrÀ )CH sources release a combined w582 87 Tg yrÀ , 30 240 km and 10.5 10.5 km for SCIAMACHY and GOSAT, 4 Æ Â Â but uncertainties are large (Denman et al., 2007). Natural and respectively, limiting direct source interpretation to large-scale anthropogenic microbial sources contribute an estimated w69% to features hundreds of kilometers in size (Bergamaschi et al., 2007). atmospheric budgets (Conrad, 2009). Important natural sources include wetlands, whose emissions are driven by anaerobic mi- 1.3. Study motivation crobial oxidation and contribute w23% of the global CH4 budget. Microbial production underlies most anthropogenic CH4 emissions, Global satellite data are critical to understanding global budgets, such as from landfills, rice, and ruminants. Natural fossil CH4 but current spatial and temporal resolutions are too coarse to eval- emissions generally are estimated at w20% of the global budget uate most sources directly, thus source assessment primarily is from (Etiope et al., 2008), although Lassey et al. (2007) suggest global and continental inversion modeling (Bousquet et al., 2006). 30.0 2.3% from fossil sources. Often, satellite-scale data are ground-referenced by airborne (Kort Æ Fires release anthropogenic and natural CH4 and contribute et al., 2008) or ground station measurements (Bergamaschi et al., significantly to inter-annual variability in CH4 growth (NRC, 2010) 2007; Pétron et al., 2012). However, airborne data can be of limited 1 contributing an estimated 14e88 Tg yrÀ (Fletcher et al., 2004). use as high airspeeds prevent resolving finer scale plumes with the Anthropogenic biomass burning in residential settings (open fire- required accuracy, and flight paths may be restricted over urban and 1 places, cooking, etc.) is estimated to contribute 8e12 Tg yrÀ (Piccot industrial areas. Ground measurements from fixed locations near et al., 1996). Wildfires can be significant, for example, 1998 arctic emission sources can investigate nearby individual sources (Bradley 1 wildfires (a very active year) released an estimated 2.9e4.7 Tg yrÀ , et al., 2010; Pétron et al., 2012), as can typical mobile ground mea- or 12% of global fire CH4 emissions (Kasischke and Bruhwiler, surements (Herndon et al., 2005; Pétron et al., 2012; Shorter et al., 2002). Emission rates depend on the fuel type consumed and the 1996); however, such data lack satellite spatial-scales. combustion mode - burning versus smoldering (Lobert and To address this need, a surface expedition was conducted 6e12 Warnatz, 1991). Koppmann et al. (2005) recommended between Oct. 2009 to acquire satellite-scale CH4 data at high spatial reso- 1 3 and 10 g kgÀ biomass for flaming and smoldering combustion, lution to allow source identification and comparison (Fig. 1B) and a respectively, although these values are highly variable. second survey in southern California on 21e22 Feb. 2012. The ex- peditions focused on important CH4 sources with significant 1.2. Atmospheric methane budget estimation growth potential, such as wetlands under warmer climate sce- narios. Data were collected almost entirely while in motion. Herein Source strengths for global CH4 budgets are derived in two we present the detailed approach and application to several natural manners; from top-down estimates based on atmospheric mea- sources including wetlands, a forest fire, a major geologic source, surements and inversion modeling and from bottom-up inventory and the California desert (no source), summarized in Table 1. estimates of individual sources (NRC, 2010). Comparison of top- down and bottom-up estimates can indicate under and over- 2. Methods inventoried sources or un-inventoried CH4 sources, e.g., Hsu et al. (2010) for the Los Angeles Basin. On a global scale, satellite- 2.1. Study area derived, top-down CH4 budgets, such as from SCIAMACHY (Scan- ning Imaging Absorption Spectrometer for Atmospheric Cartog- The 2010 expedition focused on key natural and anthropogenic raphy) have the best global coverage for such budgets (Schneising CH4 sources to characterize better their relative importance and et al., 2011); GOSAT (Greenhouse gases Observing SATellite) being understand better CH4 spatial distribution on a transcontinental the other currently orbiting, tropospheric CH4 observing satellite scale spanning the south United States. In situ CH4 measurements Fig. 1. A) Map showing survey path (yellow day, blue night) including major urban centers for 2010 and 2012. City population key on figure. B) Measured survey methane, CH4, values for 2010. Note truncated color scale to emphasize near background variations. Surface image from GoogleEarth. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.) 424 P. Farrell et al. / Atmospheric Environment 74 (2013) 422e431 Table 1 Summary characteristics of survey study areas. Area Type Location Span (km) Starta lengthb Maxc (ppm) Meanc (ppm) California (2010) Sonora Desert 33.42282N,112.60754We33.92035N, 116.54893W 370 11:10 12/10 04:05 2.27 1.91 0.12 Æ California (2012) Mojave Desert 34.99527N,117.54140We35.00681N,117.69483W 15 17:47 21/02 00:15 n/a 1.8639 0.0038 Æ La Brea Geology 34.03500N,118.37500We34.07833N,118.35167W 5.6 03:00 21/02 01:00 47.975 5.0627 4.25 Æ S. Bernadino Mtns. 34.31321N,116.80953We34.33486N,116.83340W 4.0 09:10 21/02 00:14 1.8638 1.8584 0.0016 Æ Florida (2010) Paynes Park Wetland 29.55474N,82.34157We29.58828N,82.36136W 3.8 02:49 10/10 00:07 2.9 2.61 0.2 Æ Panhandle Wetland 30.48551N,85.21087We30.46404N,88.38193W 300 19:20 07/10 05:58 9.06 1.95 0.22 Æ Louisiana (2010) Raceland Fire 29.78582N,90.51951We29.77079N,90.53828W 2.3 18:23 03/10 00:57 4.48 2.58 0.59 Æ a Local Time.
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