Ozone variability and halogen oxidation within the Arctic and sub-Arctic springtime boundary layer

Gilman, J. B.; Burkhart, John F.; Lerner, B. M.; Williams, E. J.; Kuster, W. C.; Murphy, P. C.; Warneke, C.; Fowler, Charles W.; Montzka, S. A.; Miller, Benjamin R.; Miller, Lisa A.; Oltmans, S. J.; Ryerson, Thomas B.; Cooper, O. R.; Stohl, Andreas; Gouw, J. A. de

doi:10.5194/acp-10-10223-2010

Cited by 108 publications

(88 citation statements)

References 62 publications

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“…The reasons for this difference are unknown; calibration standards were not compared for the purpose of this study. Our GC measurements in the Arctic in 2008 were systematically higher than canister samples analyzed by the NOAA Global Monitoring Division (Gilman, et al, 2010). As reported in previous work (Apel et al, 1994), it appears that the accuracy of the measurement of acetylene is considerably outside the 10% calibration uncertainty estimated for other species.…”

Section: Noaa Gc-fid Versus Uci Canisterssupporting

confidence: 60%

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Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution

et al. 2011

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Abstract. Volatile organic compound (VOC) mixing ratios were measured with two different instruments at the T1 ground site in Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO) campaign in March of 2006. A gas chromatograph with flame ionization detector (GC-FID) quantified 18 light alkanes, alkenes and acetylene while a proton-transfer-reaction iontrap mass spectrometer (PIT-MS) quantified 12 VOC species including oxygenated VOCs (OVOCs) and aromatics. A GC separation system was used in conjunction with the PIT-MS (GC-PIT-MS) to evaluate PIT-MS measurements and to aid in the identification of unknown VOCs. The VOC measurements are also compared to simultaneous canister samples and to two independent proton-transfer-reaction mass spectrometers (PTR-MS) deployed on a mobile and an airborne platform during MILAGRO. VOC diurnal cycles demonstrate the large influence of vehicle traffic and liquid propane gas (LPG) emissions during the night and photochemical processing during the afternoon. Emission ratios for VOCs and OVOCs relative to CO are derived from early-morning Correspondence to: J. A. de Gouw (joost.degouw@noaa.gov) measurements. Average emission ratios for non-oxygenated species relative to CO are on average a factor of ∼2 higher than measured for US cities. Emission ratios for OVOCs are estimated and compared to literature values the northeastern US and to tunnel studies in California. Positive matrix factorization analysis (PMF) is used to provide insight into VOC sources and processing. Three PMF factors were distinguished by the analysis including the emissions from vehicles, the use of liquid propane gas and the production of secondary VOCs + long-lived species. Emission ratios to CO calculated from the results of PMF analysis are compared to emission ratios calculated directly from measurements. The total PIT-MS signal is summed to estimate the fraction of identified versus unidentified VOC species.

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Section: Noaa Gc-fid Versus Uci Canisterssupporting

confidence: 60%

“…Calibrations were made 1-2 times per day from a gas standard. A detailed description of this instrument is given elsewhere (Goldan et al, 2000). Samples were collected from an air intake approximately 6 m above ground level that was shared with the PIT-MS system described below.…”

Section: Noaa Gc-fidmentioning

confidence: 99%

Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution

et al. 2011

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“…Additionally, ipentane and n-pentane have similar physical and chemical characteristics (i.e., boiling point and reaction rate coefficients with hydroxyl radical), which result in less susceptibility of the i-pentane / n-pentane ratio in source identification (Gilman et al, 2013). The pentanes are always from NG emissions, vehicle emissions, liquid gasoline and fuel evaporation, with the i-pentane / n-pentane ratios ranging between 0.82 and 0.89 (Gilman et al, 2010(Gilman et al, , 2013, ∼ 2.2 and 3.8 (Conner et al, 1995;McGaughey et al, 2004), 1.5 and 3.0, and 1.8 and 4.6 (Watson et al, 2001), respectively. As shown in Fig.…”

Section: Ambient Ratios: Sources and Photochemical Removalmentioning

confidence: 99%

Monitoring of volatile organic compounds (VOCs) from an oil and gas station in northwest China for 1 year

et al. 2018

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Abstract. Oil and natural gas are important for energy supply around the world. The exploring, drilling, transportation and processing in oil and gas regions can release a lot of volatile organic compounds (VOCs). To understand the VOC levels, compositions and sources in such regions, an oil and gas station in northwest China was chosen as the research site and 57 VOCs designated as the photochemical precursors were continuously measured for an entire year (September 2014-August 2015) using an online monitoring system. The average concentration of total VOCs was 297 ± 372 ppbv and the main contributor was alkanes, accounting for 87.5 % of the total VOCs. According to the propylene-equivalent concentration and maximum incremental reactivity methods, alkanes were identified as the most important VOC groups for the ozone formation potential. Positive matrix factorization (PMF) analysis showed that the annual average contributions from natural gas, fuel evaporation, combustion sources, oil refining processes and asphalt (anthropogenic and natural sources) to the total VOCs were 62.6 ± 3.04, 21.5 ± .99, 10.9 ± 1.57, 3.8 ± 0.50 and 1.3 ± 0.69 %, respectively. The five identified VOC sources exhibited various diurnal patterns due to their different emission patterns and the impact of meteorological parameters. Potential source contribution function (PSCF) and concentration-weighted trajectory (CWT) models based on backward trajectory analysis indicated that the five identified sources had similar geographic origins. Raster analysis based on CWT analysis indicated that the local emissions contributed 48.4-74.6 % to the total VOCs. Based on the high-resolution observation data, this study clearly described and analyzed the temporal variation in VOC emission characteristics at a typical oil and gas field, which exhibited different VOC levels, compositions and origins compared with those in urban and industrial areas.

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“…Uncertainties were about 15-25 % for hydrocarbons (HCs) and 20-25 % for oxygenates compounds. A detailed description of the instrument is given in the work of Gilman et al (2010) and Goldan et al (2004).…”

Section: Carbon Monoxide (Co) and Volatile Organic Compound (Voc) Meamentioning

confidence: 99%

Nitrous acid formation in a snow-free wintertime polluted rural area

et al. 2018

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Abstract. Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH) in the lower atmosphere, in particular in winter when other OH sources are less efficient. The nighttime formation of HONO and its photolysis in the early morning have long been recognized as an important contributor to the OH budget in polluted environments. Over the past few decades it has become clear that the formation of HONO during the day is an even larger contributor to the OH budget and additionally provides a pathway to recycle NO x . Despite the recognition of this unidentified HONO daytime source, the precise chemical mechanism remains elusive. A number of mechanisms have been proposed, including gas-phase, aerosol, and ground surface processes, to explain the elevated levels of daytime HONO. To identify the likely HONO formation mechanisms in a wintertime polluted rural environment we present LP-DOAS observations of HONO, NO 2 , and O 3 on three absorption paths that cover altitude intervals from 2 to 31, 45, and 68 m above ground level (a.g.l.) during the UBWOS 2012 experiment in the Uintah Basin, Utah, USA. Daytime HONO mixing ratios in the 2-31 m height interval were, on average, 78 ppt, which is lower than HONO levels measured in most polluted urban environments with similar NO 2 mixing ratios of 1-2 ppb. HONO surface fluxes at 19 m a.g.l., calculated using the HONO gradients from the LP-DOAS and measured eddy diffusivity coefficient, show clear upward fluxes. The hourly average vertical HONO flux during sunny days followed solar irradiance, with a maximum of (4.9 ± 0.2) × 10 10 molec. cm −2 s −1 at noontime. A photostationary state analysis of the HONO budget shows that the surface flux closes the HONO budget, accounting for 63 ± 32 % of the unidentified HONO daytime source throughout the day and 90 ± 30 % near noontime. This is also supported by 1-D chemistry and transport model calculations that include the measured surface flux, thus clearly identifying chemistry at the ground as the missing daytime HONO source in this environment. Comparison between HONO surface flux, solar radiation, NO 2 and HNO 3 mixing ratios, and results from 1-D model runs suggest that, under high NO x conditions, HONO formation mechanisms related to solar radiation and NO 2 mixing ratios, such as photo-enhanced conversion of NO 2 on the ground, are most likely the source of daytime HONO. Under moderate to low NO 2 conditions, photolysis of HNO 3 on the ground seems to be the main source of HONO.

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Ozone variability and halogen oxidation within the Arctic and sub-Arctic springtime boundary layer

Cited by 108 publications

References 62 publications

Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution

Measurements of volatile organic compounds at a suburban ground site (T1) in Mexico City during the MILAGRO 2006 campaign: measurement comparison, emission ratios, and source attribution

Monitoring of volatile organic compounds (VOCs) from an oil and gas station in northwest China for 1 year

Nitrous acid formation in a snow-free wintertime polluted rural area

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