scholarly journals Observations of volatile organic compounds during ARCTAS – Part 1: Biomass burning emissions and plume enhancements

2011 ◽  
Vol 11 (5) ◽  
pp. 14127-14182 ◽  
Author(s):  
R. S. Hornbrook ◽  
D. R. Blake ◽  
G. S. Diskin ◽  
H. E. Fuelberg ◽  
S. Meinardi ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Biomass Burning ◽  
Time Of Day ◽  
The Arctic ◽  
Fire Emissions ◽  
Mixing Ratios ◽  
Significant Difference ◽  
Volatile Organic ◽  
Good Agreement

Abstract. Mixing ratios of a large number of volatile organic compounds (VOCs) were observed by the Trace Organic Gas Analyzer (TOGA) on board the NASA DC-8 as part of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. Many of these VOCs were observed concurrently by one or both of two other VOC measurement techniques on board the DC-8: proton-transfer-reaction mass spectrometry (PTR-MS) and whole air canister sampling (WAS). A comparison of these measurements to the data from TOGA indicates good agreement for the majority of co-measured VOCs. The ARCTAS study, which included both spring and summer deployments, provided opportunities to sample a large number of biomass burning (BB) plumes with origins in Asia, California and Central Canada, ranging from very recent emissions to plumes aged one week or more. For this analysis, identified BB plumes were grouped by flight, source region and, in some cases, time of day, generating 40 individual plume groups, each consisting of one or more BB plume interceptions. Normalized excess mixing ratios (EMRs) to CO were determined for each of the 40 plume groups for up to 19 different VOCs or VOC groups, many of which show significant variability, even within relatively fresh plumes. This variability demonstrates the importance of assessing BB plumes both regionally and temporally, as emissions can vary from region to region, and even within a fire over time. Comparisons with literature confirm that variability of EMRs to CO over an order of magnitude for many VOCs is consistent with previous observations. However, this variability is often diluted in the literature when individual observations are averaged to generate an overall regional EMR from a particular study. Previous studies give the impression that emission ratios are generally consistent within a given region, and this is not necessarily the case, as our results show. For some VOCs, earlier assumptions may lead to significant under-prediction of emissions in fire emissions inventories. Notably, though variable between plumes, observed EMRs of individual light alkanes are highly correlated within BB emissions. Using the NCAR master mechanism chemical box model initialized with concentrations based on two observed scenarios, i.e., fresh Canadian BB and fresh Californian BB, both plumes are expected to experience primarily decreases in oxygenated VOCs during the first 2.5 days, such that any production in the plumes of these compounds is less than the chemical loss. Comparisons of the modeled EMRs to the observed EMRs from BB plumes estimated to be three days in age or less indicate overall good agreement and, for most compounds, no significant difference between BB plumes in these two regions.

scholarly journals Observations of nonmethane organic compounds during ARCTAS − Part 1: Biomass burning emissions and plume enhancements

2011 ◽  
Vol 11 (21) ◽  
pp. 11103-11130 ◽  
Author(s):  
R. S. Hornbrook ◽  
D. R. Blake ◽  
G. S. Diskin ◽  
A. Fried ◽  
H. E. Fuelberg ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Biomass Burning ◽  
Source Region ◽  
Measurement Techniques ◽  
Proton Transfer Reaction ◽  
Time Of Day ◽  
The Arctic ◽  
Mixing Ratios ◽  
Order Of Magnitude ◽  
Good Agreement

Abstract. Mixing ratios of a large number of nonmethane organic compounds (NMOCs) were observed by the Trace Organic Gas Analyzer (TOGA) on board the NASA DC-8 as part of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. Many of these NMOCs were observed concurrently by one or both of two other NMOC measurement techniques on board the DC-8: proton-transfer-reaction mass spectrometry (PTR-MS) and whole air canister sampling (WAS). A comparison of these measurements to the data from TOGA indicates good agreement for the majority of co-measured NMOCs. The ARCTAS study, which included both spring and summer deployments, provided opportunities to sample a large number of biomass burning (BB) plumes with origins in Asia, California and central Canada, ranging from very recent emissions to plumes aged one week or more. For this analysis, BB smoke interceptions were grouped by flight, source region and, in some cases, time of day, generating 40 identified BB plumes for analysis. Normalized excess mixing ratios (NEMRs) to CO were determined for each of the 40 plumes for up to 19 different NMOCs or NMOC groups. Although the majority of observed NEMRs for individual NMOCs or NMOC groups were in agreement with previously-reported values, the observed NEMRs to CO for ethanol, a rarely quantified gas-phase trace gas, ranged from values similar to those previously reported, to up to an order of magnitude greater. Notably, though variable between plumes, observed NEMRs of individual light alkanes are highly correlated within BB emissions, independent of estimated plume ages. BB emissions of oxygenated NMOC were also found to be often well-correlated. Using the NCAR Master Mechanism chemical box model initialized with concentrations based on two observed scenarios, fresh Canadian BB and fresh Californian BB, decreases are predicted for the low molecular weight carbonyls (i.e. formaldehyde, acetaldehyde, acetone and methyl ethyl ketone, MEK) and alcohols (i.e. methanol and ethanol) as the plumes evolve in time, i.e. the production of these compounds is less than the chemical loss. Comparisons of the modeled NEMRs to the observed NEMRs from BB plumes estimated to be three days in age or less indicate overall good agreement.

scholarly journals Measurements of volatile organic compounds in the middle of Central East China during Mount Tai Experiment 2006 (MTX2006): observation of regional background and impact of biomass burning

2010 ◽  
Vol 10 (3) ◽  
pp. 1269-1285 ◽  
Author(s):  
J. Suthawaree ◽  
S. Kato ◽  
K. Okuzawa ◽  
Y. Kanaya ◽  
P. Pochanart ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Biomass Burning ◽  
Primary Source ◽  
Temporal Variations ◽  
East China ◽  
Boundary Layer Height ◽  
Mixing Ratios ◽  
Regional Background ◽  
Volatile Organic

Abstract. The measurement of volatile organic compounds (VOCs) was carried out at the summit of Mount Tai, located in the center of the Central East China (CEC) region, in June 2006 as part of the Mount Tai Experiment 2006 (MTX2006), which focused on the ozone and aerosol chemistry in the region. Temporal variations of simple VOCs between 2 June and 28 June revealed the characteristics of an aged air mass with minimum local influence. A comparison of VOCs observed at Mount Tai with other Chinese sites revealed relatively similar VOC levels to remote sites and, as expected, a lower level compared to more polluted sites. However, relatively high acetylene and benzene levels at Mount Tai were evidently indicated from comparison with normalized VOC profile by ethane suggested for Beijing. Owing to a shift in boundary layer height, we observed considerable differences between daytime and nighttime VOC mixing ratios. This suggests that the site potentially has a very useful characteristic of being able to measure regional polluted air and the free troposphere regional background air quality. Influence of emissions from biomass burning in the region was evidently found to be extensive during the first half of the campaign (2–15 June), using fire spot data coupling with backward trajectory analysis. Agricultural residue burning was suggested as the primary source of emissions elucidated by the slope of the correlation plot between CH3Cl and CO obtained during the first half of the campaign.

scholarly journals Measurement report: Source apportionment of volatile organic compounds at the remote high-altitude Maïdo observatory

2021 ◽  
Vol 21 (17) ◽  
pp. 12965-12988
Author(s):  
Bert Verreyken ◽  
Crist Amelynck ◽  
Niels Schoon ◽  
Jean-François Müller ◽  
Jérôme Brioude ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Source Apportionment ◽  
Organic Compounds ◽  
Biomass Burning ◽  
Free Troposphere ◽  
La Réunion ◽  
Air Masses ◽  
Mixing Ratios ◽  
Volatile Organic ◽  
The Impact

Abstract. We present a source apportionment study of a near-continuous 2-year dataset of volatile organic compounds (VOCs), recorded between October 2017 and November 2019 with a quadrupole-based high-sensitivity proton-transfer-reaction mass-spectrometry (hs-PTR-MS) instrument deployed at the Maïdo observatory (21.1∘ S, 55.4∘ E, 2160 m altitude). The observatory is located on La Réunion island in the southwest Indian Ocean. We discuss seasonal and diel profiles of six key VOC species unequivocally linked to specific sources – acetonitrile (CH3CN), isoprene (C5H8), isoprene oxidation products (Iox), benzene (C6H6), C8-aromatic compounds (C8H10), and dimethyl sulfide (DMS). The data are analyzed using the positive matrix factorization (PMF) method and back-trajectory calculations based on the Lagrangian mesoscale transport model FLEXPART-AROME to identify the impact of different sources on air masses sampled at the observatory. As opposed to the biomass burning tracer CH3CN, which does not exhibit a typical diel pattern consistently throughout the dataset, we identify pronounced diel profiles with a daytime maximum for the biogenic (C5H8 and Iox) and anthropogenic (C6H6, C8H10) tracers. The marine tracer DMS generally displays a daytime maximum except for the austral winter when the difference between daytime and nighttime mixing ratios vanishes. Four factors were identified by the PMF: background/biomass burning, anthropogenic, primary biogenic, and secondary biogenic. Despite human activity being concentrated in a few coastal areas, the PMF results indicate that the anthropogenic source factor is the dominant contributor to the VOC load (38 %), followed by the background/biomass burning source factor originating in the free troposphere (33 %), and by the primary (15 %) and secondary biogenic (14 %) source factors. FLEXPART-AROME simulations showed that the observatory was most sensitive to anthropogenic emissions west of Maïdo while the strongest biogenic contributions coincided with air masses passing over the northeastern part of La Réunion. At night, the observatory is often located in the free troposphere, while during the day, the measurements are influenced by mesoscale sources. Interquartile ranges of nighttime 30 min average mixing ratios of methanol (CH3OH), CH3CN, acetaldehyde (CH3CHO), formic acid (HCOOH), acetone (CH3COCH3), acetic acid (CH3COOH), and methyl ethyl ketone (MEK), representative for the atmospheric composition of the free troposphere, were found to be 525–887, 79–110, 61–101, 172–335, 259–379, 64–164, and 11–21 pptv, respectively.

scholarly journals Measurement Report: Aircraft Observations of Ozone, Nitrogen Oxides, and Volatile Organic Compounds over Hebei Province, China

2020 ◽  
Author(s):  
Sarah E. Benish ◽  
Hao He ◽  
Xinrong Ren ◽  
Sandra J. Roberts ◽  
Ross J. Salawitch ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Nitrogen Oxides ◽  
Organic Compounds ◽  
Biomass Burning ◽  
Hebei Province ◽  
Model Calculations ◽  
Mixing Ratios ◽  
Chemistry Research ◽  
Volatile Organic ◽  
Low Efficiency

Abstract. To provide insight into the planetary boundary layer (PBL) production of ozone (O3) over the North China Plain, the Air chemistry Research in Asia (ARIAs) campaign conducted aircraft measurements of air pollutants over Hebei Province, China between May and June 2016. We evaluate vertical profiles of trace gas species including O3, nitrogen oxides (NOx), carbon monoxide (CO), and volatile organic compounds (VOCs) and relate to rates of O3 production. This analysis shows measured O3 levels ranged from 52 to 142 ppbv, with the peak median concentration (~ 94 ppbv) occurring between 1000 and 1500 m. The NOx concentrations exhibited strong spatial and altitudinal variations, ranging from 0.15 to 49 ppbv. Ratios of CO / NOy and CO / CO2 indicate the prevalence of low efficiency combustion from biomass burning and residential coal burning. Concentrations of total measured VOCs from 26 whole air canisters reveals alkanes dominate the total measured volume mixing ratio of VOCs (68 %) and we see evidence of vehicular emissions, fuel and solvent evaporation, and biomass burning sources. Alkanes and alkenes/alkynes are responsible for 74 % of the total VOC reactivity assessed by calculating the OH loss rates, while aromatics contribute the most to the total Ozone Formation Potential (OFP) (43 %) with toluene, m/p-xylene, ethylene, propylene, and i-pentane playing significant roles in the aloft production of O3 in this region. In the PBL below 500 m, box model calculations constrained by measured precursors indicate the peak rate of mean O3 production was ~ 7 ppbv/hour. Pollution frequently extended above the PBL into the lower free troposphere around 3000 m, where NO2 mixing ratios (~ 400 pptv) led to net production rates of O3 up to ~ 3 ppbv/hour; this pollution can travel substantial distances downwind. The O3 sensitivity regime is determined to be NOx-limited throughout the PBL, while more VOC-limited at low altitudes near urban centres, demonstrating both VOCs and NOx need further control to reduce aloft O3 over Hebei.

scholarly journals Measurement report: Aircraft observations of ozone, nitrogen oxides, and volatile organic compounds over Hebei Province, China

2020 ◽  
Vol 20 (23) ◽  
pp. 14523-14545
Author(s):  
Sarah E. Benish ◽  
Hao He ◽  
Xinrong Ren ◽  
Sandra J. Roberts ◽  
Ross J. Salawitch ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Nitrogen Oxides ◽  
Organic Compounds ◽  
Biomass Burning ◽  
Hebei Province ◽  
Model Calculations ◽  
Mixing Ratios ◽  
Chemistry Research ◽  
Volatile Organic ◽  
Low Efficiency

Abstract. To provide insight into the planetary boundary layer (PBL) production of ozone (O3) over the North China Plain, the Air chemistry Research in Asia (ARIAs) campaign conducted aircraft measurements of air pollutants over Hebei Province, China, between May and June 2016. We evaluate vertical profiles of trace gas species including O3, nitrogen oxides (NOx), carbon monoxide (CO), and volatile organic compounds (VOCs) and relate to rates of O3 production. This analysis shows measured O3 levels ranged from 45 to 146 ppbv, with the peak median concentration (∼ 92 ppbv) occurring between 1000 and 1500 m. The NOx concentrations exhibited strong spatial and altitudinal variations, with a maximum of 53 ppbv. Ratios of CO∕CO2 indicate the prevalence of low-efficiency combustion from biomass burning and residential coal burning but indicate some success of regional pollution controls compared to earlier studies in China. Concentrations of total measured VOCs reveal alkanes dominate the total measured volume mixing ratio of VOCs (68 %), and sources include vehicular emissions, fuel and solvent evaporation, and biomass burning. Alkanes and alkenes/alkynes are responsible for 74 % of the total VOC reactivity assessed by calculating the OH loss rates, while aromatics contribute the most to the total ozone formation potential (OFP) (43 %) with toluene, m/p-xylene, ethylene, propylene, and i-pentane playing significant roles in the aloft production of O3 in this region. In the PBL below 500 m, box model calculations constrained by measured precursors indicate the peak rate of mean O3 production was ∼ 7 ppbv h−1. Pollution frequently extended above the PBL into the lower free troposphere around 3000 m, where NO2 mixing ratios (∼ 400 pptv) led to net production rates of O3 up to ∼ 3 ppbv h−1; this pollution can travel substantial distances downwind. The O3 sensitivity regime is determined to be NOx-limited throughout the PBL, whereas it is more VOC-limited at low altitudes near urban centers, demonstrating that control of both VOCs and NOx is needed to reduce aloft O3 pollution over Hebei.

scholarly journals Mapping Asian anthropogenic emissions of non-methane volatile organic compounds to multiple chemical mechanisms

2013 ◽  
Vol 13 (12) ◽  
pp. 32649-32701 ◽  
Author(s):  
M. Li ◽  
Q. Zhang ◽  
D. G. Streets ◽  
K. B. He ◽  
Y. F. Cheng ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Individual Species ◽  
Chemical Mechanisms ◽  
Mixing Ratios ◽  
Wide Range ◽  
Oxygenated Volatile Organic Compounds ◽  
Volatile Organic ◽  
Species Mapping ◽  
Multiple Chemical

Abstract. An accurate speciation mapping of non-methane volatile organic compounds (NMVOC) emissions has an important impact on the performance of chemical transport models (CTMs) in simulating ozone mixing ratios and secondary organic aerosols. In this work, we developed an improved speciation framework to generate model-ready anthropogenic Asian NMVOC emissions for various gas-phase chemical mechanisms commonly used in CTMs by using an explicit assignment approach and updated NMVOC profiles, based on the total NMVOC emissions in the INTEX-B Asian inventory for the year 2006. NMVOC profiles were selected and aggregated from a wide range of new measurements and the SPECIATE database. To reduce potential uncertainty from individual measurements, composite profiles were developed by grouping and averaging source profiles from the same category. The fractions of oxygenated volatile organic compounds (OVOC) were corrected during the compositing process for those profiles which used improper sampling and analyzing methods. Emissions of individual species were then lumped into species in different chemical mechanisms used in CTMs by applying mechanism-dependent species mapping tables, which overcomes the weakness of inaccurate mapping in previous studies. Gridded emissions for eight chemical mechanisms are developed at 30 min × 30 min resolution using various spatial proxies and are provided through the website: http://mic.greenresource.cn/intex-b2006. Emission estimates for individual NMVOC species differ between one and three orders of magnitude for some species when different sets of profiles are used, indicating that source profile is the most important source of uncertainties of individual species emissions. However, those differences are diminished in lumped species as a result of the lumping in the chemical mechanisms.

scholarly journals Aerosol mass yields of selected biogenic volatile organic compounds – a theoretical study with nearly explicit gas-phase chemistry

2019 ◽  
Vol 19 (22) ◽  
pp. 13741-13758
Author(s):  
Carlton Xavier ◽  
Anton Rusanen ◽  
Putian Zhou ◽  
Chen Dean ◽  
Lukas Pichelstorfer ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Gas Phase ◽  
Organic Compounds ◽  
Chemical Mechanism ◽  
Biogenic Volatile Organic Compounds ◽  
Gas Phase Chemistry ◽  
Mass Load ◽  
Volatile Organic ◽  
Phase Chemistry ◽  
Good Agreement

Abstract. In this study we modeled secondary organic aerosol (SOA) mass loadings from the oxidation (by O3, OH and NO3) of five representative biogenic volatile organic compounds (BVOCs): isoprene, endocyclic bond-containing monoterpenes (α-pinene and limonene), exocyclic double-bond compound (β-pinene) and a sesquiterpene (β-caryophyllene). The simulations were designed to replicate an idealized smog chamber and oxidative flow reactors (OFRs). The Master Chemical Mechanism (MCM) together with the peroxy radical autoxidation mechanism (PRAM) were used to simulate the gas-phase chemistry. The aim of this study was to compare the potency of MCM and MCM + PRAM in predicting SOA formation. SOA yields were in good agreement with experimental values for chamber simulations when MCM + PRAM was applied, while a stand-alone MCM underpredicted the SOA yields. Compared to experimental yields, the OFR simulations using MCM + PRAM yields were in good agreement for BVOCs oxidized by both O3 and OH. On the other hand, a stand-alone MCM underpredicted the SOA mass yields. SOA yields increased with decreasing temperatures and NO concentrations and vice versa. This highlights the limitations posed when using fixed SOA yields in a majority of global and regional models. Few compounds that play a crucial role (>95 % of mass load) in contributing to SOA mass increase (using MCM + PRAM) are identified. The results further emphasized that incorporating PRAM in conjunction with MCM does improve SOA mass yield estimation.

scholarly journals Underway seawater and atmospheric measurements of volatile organic compounds in the Southern Ocean

2020 ◽  
Vol 17 (9) ◽  
pp. 2593-2619 ◽  
Author(s):  
Charel Wohl ◽  
Ian Brown ◽  
Vassilis Kitidis ◽  
Anna E. Jones ◽  
William T. Sturges ◽  
...  
Keyword(s):  
Volatile Organic Compounds ◽  
Southern Ocean ◽  
Organic Compounds ◽  
Dimethyl Sulfide ◽  
Ambient Air ◽  
Atmospheric Measurements ◽  
Mixing Ratios ◽  
Volatile Organic ◽  
Air Mixing ◽  
Net Flux

Abstract. Dimethyl sulfide and volatile organic compounds (VOCs) are important for atmospheric chemistry. The emissions of biogenically derived organic gases, including dimethyl sulfide and especially isoprene, are not well constrained in the Southern Ocean. Due to a paucity of measurements, the role of the ocean in the atmospheric budgets of atmospheric methanol, acetone, and acetaldehyde is even more poorly known. In order to quantify the air–sea fluxes of these gases, we measured their seawater concentrations and air mixing ratios in the Atlantic sector of the Southern Ocean, along a ∼ 11 000 km long transect at approximately 60∘ S in February–April 2019. Concentrations, oceanic saturations, and estimated fluxes of five simultaneously sampled gases (dimethyl sulfide, isoprene, methanol, acetone, and acetaldehyde) are presented here. Campaign mean (±1σ) surface water concentrations of dimethyl sulfide, isoprene, methanol, acetone, and acetaldehyde were 2.60 (±3.94), 0.0133 (±0.0063), 67 (±35), 5.5 (±2.5), and 2.6 (±2.7) nmol dm−3 respectively. In this dataset, seawater isoprene and methanol concentrations correlated positively. Furthermore, seawater acetone, methanol, and isoprene concentrations were found to correlate negatively with the fugacity of carbon dioxide, possibly due to a common biological origin. Campaign mean (±1σ) air mixing ratios of dimethyl sulfide, isoprene, methanol, acetone, and acetaldehyde were 0.17 (±0.09), 0.053 (±0.034), 0.17 (±0.08), 0.081 (±0.031), and 0.049 (±0.040) ppbv. We observed diel changes in averaged acetaldehyde concentrations in seawater and ambient air (and to a lesser degree also for acetone and isoprene), which suggest light-driven production. Campaign mean (±1σ) fluxes of 4.3 (±7.4) µmol m−2 d−1 DMS and 0.028 (±0.021) µmol m−2 d−1 isoprene are determined where a positive flux indicates from the ocean to the atmosphere. Methanol was largely undersaturated in the surface ocean with a mean (±1σ) net flux of −2.4 (±4.7) µmol m−2 d−1, but it also had a few occasional episodes of outgassing. This section of the Southern Ocean was found to be a source and a sink for acetone and acetaldehyde this time of the year, depending on location, resulting in a mean net flux of −0.55 (±1.14) µmol m−2 d−1 for acetone and −0.28 (±1.22) µmol m−2 d−1 for acetaldehyde. The data collected here will be important for constraining the air–sea exchange, cycling, and atmospheric impact of these gases, especially over the Southern Ocean.

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