Abstract:Abstract. From about 1500 measurements of ethane in the remote troposphere the longitudinally and vertically averaged latitudinal and seasonal variability of ethane was derived. To improve the data coverage, several data sets from literature were included. There are only very few data sets available for the southern hemisphere. Nevertheless, the uncertainty of the average seasonal/latitudinal ethane profile is estimated to less than 30%. The global annually averaged ethane mixing ratio is 860 ppt. There is a s… Show more
“…Using similar conditions to the CH 4 calculations, an emission rate of 0.3-0.5 Tg per year is calculated for ethane. By comparison, global natural gas emissions are believed to release 6 Tg of ethane yr Ϫ1 out of a global ethane budget of 13-15.5 Tg per year (17,18).…”
Light alkane hydrocarbons are present in major quantities in the near-surface atmosphere of Texas, Oklahoma, and Kansas during both autumn and spring seasons. In spring 2002, maximum mixing ratios of ethane [34 parts per 10 9 by volume (ppbv)], propane (20 ppbv), and n-butane (13 ppbv) were observed in north-central Texas. The elevated alkane mixing ratios are attributed to emissions from the oil and natural gas industry. Measured alkyl nitrate mixing ratios were comparable to urban smog values, indicating active photochemistry in the presence of nitrogen oxides, and therefore with abundant formation of tropospheric ozone. We estimate that 4 -6 teragrams of methane are released annually within the region and represents a significant fraction of the estimated total U.S. emissions. This result suggests that total U.S. natural gas emissions may have been underestimated. Annual ethane emissions from the study region are estimated to be 0.3-0.5 teragrams.W e have performed two regional studies in different seasons of hydrocarbon and halocarbon mixing ratios in surfacelevel air sampled within the southwestern United States. Elevated atmospheric mixing ratios of C 1 -C 4 alkanes and C 2 -C 4 alkyl nitrates (RONO 2 ) were measured over much of the region during both studies. The alkyl nitrate enhancements show that significant photochemistry analogous to urban smog formation is occurring within the source region. The release of hydrocarbons into the atmosphere contributes to photochemical ozone (O 3 ) production, with related adverse health effects, reduction in plant growth, and climate change (1-3). The production, storage, and transport of oil and natural gas are a major global source of hydrocarbons into the atmosphere (4), and the southwestern states have some of the largest oil and natural gas reserves in the United States. Although the U.S. natural gas industry has been estimated to account for Ϸ20% of the total U.S. anthropogenic methane (CH 4 ) emissions (5), the global budgets of light (C 2 -C 4 ) alkanes, including their emissions from the oil and natural gas industry, are more poorly assessed.The C 2 -C 4 alkanes have globally averaged lifetimes ranging from Ϸ2 months for ethane to several days for the butanes (6). Because of their short lifetimes, the atmospheric concentrations of light alkanes are variable and depend on the number and strength of nearby emission sources. By contrast, CH 4 is by far the most abundant hydrocarbon in the atmosphere, in part because of its 8-year atmospheric lifetime (7), which allows it to be widely distributed throughout both the northern and southern hemispheres. The greater reactivity of C 2 -C 4 alkanes relative to CH 4 ensures that a much larger fraction of the former will react in the area where the emissions occur, making the combined C 2 -C 4 alkane contributions more important for local and regional O 3 formation than the influence of the incremental local increases in CH 4 .In the troposphere, photochemical O 3 production begins with the attack of parent hydrocarbon...
“…Using similar conditions to the CH 4 calculations, an emission rate of 0.3-0.5 Tg per year is calculated for ethane. By comparison, global natural gas emissions are believed to release 6 Tg of ethane yr Ϫ1 out of a global ethane budget of 13-15.5 Tg per year (17,18).…”
Light alkane hydrocarbons are present in major quantities in the near-surface atmosphere of Texas, Oklahoma, and Kansas during both autumn and spring seasons. In spring 2002, maximum mixing ratios of ethane [34 parts per 10 9 by volume (ppbv)], propane (20 ppbv), and n-butane (13 ppbv) were observed in north-central Texas. The elevated alkane mixing ratios are attributed to emissions from the oil and natural gas industry. Measured alkyl nitrate mixing ratios were comparable to urban smog values, indicating active photochemistry in the presence of nitrogen oxides, and therefore with abundant formation of tropospheric ozone. We estimate that 4 -6 teragrams of methane are released annually within the region and represents a significant fraction of the estimated total U.S. emissions. This result suggests that total U.S. natural gas emissions may have been underestimated. Annual ethane emissions from the study region are estimated to be 0.3-0.5 teragrams.W e have performed two regional studies in different seasons of hydrocarbon and halocarbon mixing ratios in surfacelevel air sampled within the southwestern United States. Elevated atmospheric mixing ratios of C 1 -C 4 alkanes and C 2 -C 4 alkyl nitrates (RONO 2 ) were measured over much of the region during both studies. The alkyl nitrate enhancements show that significant photochemistry analogous to urban smog formation is occurring within the source region. The release of hydrocarbons into the atmosphere contributes to photochemical ozone (O 3 ) production, with related adverse health effects, reduction in plant growth, and climate change (1-3). The production, storage, and transport of oil and natural gas are a major global source of hydrocarbons into the atmosphere (4), and the southwestern states have some of the largest oil and natural gas reserves in the United States. Although the U.S. natural gas industry has been estimated to account for Ϸ20% of the total U.S. anthropogenic methane (CH 4 ) emissions (5), the global budgets of light (C 2 -C 4 ) alkanes, including their emissions from the oil and natural gas industry, are more poorly assessed.The C 2 -C 4 alkanes have globally averaged lifetimes ranging from Ϸ2 months for ethane to several days for the butanes (6). Because of their short lifetimes, the atmospheric concentrations of light alkanes are variable and depend on the number and strength of nearby emission sources. By contrast, CH 4 is by far the most abundant hydrocarbon in the atmosphere, in part because of its 8-year atmospheric lifetime (7), which allows it to be widely distributed throughout both the northern and southern hemispheres. The greater reactivity of C 2 -C 4 alkanes relative to CH 4 ensures that a much larger fraction of the former will react in the area where the emissions occur, making the combined C 2 -C 4 alkane contributions more important for local and regional O 3 formation than the influence of the incremental local increases in CH 4 .In the troposphere, photochemical O 3 production begins with the attack of parent hydrocarbon...
“…Fast response in situ measurements of CO were made spectroscopically using a folded-path, differential absorption, [Rudolph, 1995]. Figure 2 and Table I show that north of 10øN, absolute mixing ratios of ethane, ethyne, and propane, were significantly higher for the lower two altitude ranges during PEM-Tropics B compared to PEM-Tropics A. Mixing ratios of C2C14 and CH3C1 were also significantly greater during PEM-Tropics B at low altitudes, but only slightly higher at mid altitudes.…”
“…The sources of C 2 H 6 are natural gas and fossil fuel emissions (Singh and Zimmerman, 1992). C 2 H 2 main sources include natural gas, biofuel combustion products and biomass burning emissions (Gupta et al, 1998;Logan et al, 1981;Rudolph, 1995;Xiao et al, 2007;Zhao et al, 2002). CO, C 2 H 6 and C 2 H 2 are removed by oxidation via OH reaction (Logan et al, 1981), leading to atmospheric lifetimes of approximately fifty-two days (Daniel and Solomon, 1998), eighty days (Xiao et al, 2008) and two weeks in the atmosphere (Xiao et al, 2007), respectively.…”
Section: Seasonal Variabilities Of Co C 2 H 6 and C 2 Hmentioning
Abstract. We present a five-year time series of seven tropospheric species measured using a ground-based Fourier transform infrared (FTIR) spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL; Eureka, Nunavut, Canada; 80 • 05 N, 86 • 42 W) from 2007 to 2011. Total columns and temporal variabilities of carbon monoxide (CO), hydrogen cyanide (HCN) and ethane (C 2 H 6 ) as well as the first derived total columns at Eureka of acetylene (C 2 H 2 ), methanol (CH 3 OH), formic acid (HCOOH) and formaldehyde (H 2 CO) are investigated, providing a new data set in the sparsely sampled high latitudes.Total columns are obtained using the SFIT2 retrieval algorithm based on the optimal estimation method. The microwindows as well as the a priori profiles and variabilities are selected to optimize the information content of the retrievals, and error analyses are performed for all seven species. Our retrievals show good sensitivities in the troposphere. The seasonal amplitudes of the time series, ranging from 34 to 104 %, are captured while using a single a priori profile for each species. The time series of the CO, C 2 H 6 and C 2 H 2 total columns at PEARL exhibit strong seasonal cycles with maxima in winter and minima in summer, in opposite phase to the HCN, CH 3 OH, HCOOH and H 2 CO time series. These cycles result from the relative contributions of the photochemistry, oxidation and transport as well as biogenic and biomass burning emissions.Comparisons of the FTIR partial columns with coincident satellite measurements by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) show good agreement. The correlation coefficients and the slopes range from 0.56 to 0.97 and 0.50 to 3.35, respectively, for the seven target species.Our new data set is compared to previous measurements found in the literature to assess atmospheric budgets of these tropospheric species in the high Arctic. The CO and C 2 H 6 concentrations are consistent with negative trends observed over the Northern Hemisphere, attributed to fossil fuel emission decrease. The importance of poleward transport for the atmospheric budgets of HCN and C 2 H 2 is highlighted. Columns and variabilities of CH 3 OH and HCOOH at PEARL are comparable to previous measurements performed at other remote sites. However, the small columns of H 2 CO in early May might reflect its large atmospheric variability and/or the effect of the updated spectroscopic parameters used in our retrievals. Overall, emissions from biomass burning contribute to the day-to-day variabilities of the seven tropospheric species observed at Eureka.
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