scholarly journals Real-time measurements of ammonia, acidic trace gases and water-soluble inorganic aerosol species at a rural site in the Amazon Basin

2004 ◽  
Vol 4 (4) ◽  
pp. 967-987 ◽  
Author(s):  
I. Trebs ◽  
F. X. Meixner ◽  
J. Slanina ◽  
R. Otjes ◽  
P. Jongejan ◽  
...  

Abstract. We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2 and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3-), nitrite (NO2-), chloride (Cl- and sulfate (SO42-), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia - Smoke Aerosols, Clouds, Rainfall and Climate: Aerosols from Biomass Burning Perturb Global and Regional Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder (WAD) in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015ppb for acidic trace gases and aerosol anions and ≤0.118ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative humidity and temperature variations between day and night as well as to changing photochemistry and stability conditions of the planetary boundary layer. HONO exhibited a characteristic diel cycle with high mixing ratios at nighttime and was not completely depleted by photolysis during daylight hours.

2004 ◽  
Vol 4 (1) ◽  
pp. 1203-1246 ◽  
Author(s):  
I. Trebs ◽  
F. X. Meixner ◽  
J. Slanina ◽  
R. Otjes ◽  
P. Jongejan ◽  
...  

Abstract. We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2) and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3−), nitrite (NO2−), chloride (Cl−) and sulfate (SO42−), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia Smoke Aerosols, Clouds, Rainfall and Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015 ppb for acidic trace gases and aerosol anions and ≤0.118 ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative humidity and temperature variations between day and night as well as to changing photochemistry and stability conditions of the planetary boundary layer. HONO exhibited a characteristic diel cycle with high mixing ratios at nighttime and was not completely depleted by photolysis during daylight hours.


2021 ◽  
Author(s):  
Simone M. Pieber ◽  
Dac-Loc Nguyen ◽  
Hendryk Czech ◽  
Stephan Henne ◽  
Nicolas Bukowiecki ◽  
...  

<p>Open biomass burning (BB) is a globally widespread phenomenon. The fires release pollutants, which are harmful for human and ecosystem health and alter the Earth's radiative balance. Yet, the impact of various types of BB on the global radiative forcing remains poorly constrained concerning greenhouse gas emissions, BB organic aerosol (OA) chemical composition and related light absorbing properties. Fire emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation-type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. Here we investigate the influence of seasonally recurring BB on trace gas concentration and air quality at the regional Global Atmosphere Watch (GAW) station Pha Din (PDI) in rural Northwestern Vietnam. PDI is located in a sparsely populated area on the top of a hill (1466 m a.s.l.) and is well suited to study the large-scale fires on the Indochinese Peninsula, whose pollution plumes are frequently transported towards the site [1]. We present continuous trace gas observations of CO<sub>2</sub>, CH<sub>4</sub>, CO, and O<sub>3</sub> conducted at PDI since 2014 and interpret the data with atmospheric transport simulations. Annually recurrent large scale BB leads to hourly time-scale peaks CO mixing ratios at PDI of 1000 to 1500 ppb around every April since the start of data collection in 2014. We complement this analysis with carbonaceous PM<sub>2.5 </sub>chemical composition analyzed during an intensive campaign in March-April 2015. This includes measurements of elemental and organic carbon (EC/OC) and more than 50 organic markers, such as sugars, PAHs, fatty acids and nitro-aromatics [2]. For the intensive campaign, we linked CO, CO<sub>2</sub>, CH<sub>4</sub> and O<sub>3</sub> mixing ratios to a statistical classification of BB events, which is based on OA composition. We found increased CO and O<sub>3</sub> levels during medium and high BB influence during the intensive campaign. A backward trajectory analysis confirmed different source regions for the identified periods based on the OA cluster. Typically, cleaner air masses arrived from northeast, i.e., mainland China and Yellow sea during the intensive campaign. The more polluted periods were characterized by trajectories from southwest, with more continental recirculation of the medium cluster, and more westerly advection for the high cluster. These findings highlight that BB activities in Northern Southeast Asia significantly enhances the regional OA loading, chemical PM<sub>2.5 </sub>composition and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on air quality in a region of scarce data availability.</p><p> </p><p><strong>REFERENCES</strong></p><p>[1] Bukowiecki, N. et al. Effect of Large-scale Biomass Burning on Aerosol Optical Properties at the GAW Regional Station Pha Din, Vietnam. AAQR. 19, 1172–1187 (2019).</p><p>[2] Nguyen, D. L, et al. Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case-study in Northwestern Vietnam. ACPD., https://doi.org/10.5194/acp-2020-1027, in review, 2020.</p>


2012 ◽  
Vol 12 (11) ◽  
pp. 28661-28703 ◽  
Author(s):  
S. L. Mkoma ◽  
K. Kawamura ◽  
P. Fu

Abstract. Atmospheric aerosol samples of PM2.5 and PM10 were collected at a rural site in Tanzania in 2011 during wet and dry seasons and they were analysed for carbonaceous components, levoglucosan and water-soluble inorganic ions. The mean mass concentrations of PM2.5 and PM10 were 28.2±6.4 μg m−3 and 47±8.2 μg m−3 in wet season, and 39.1±9.8 μg m−3 and 61.4±19.2 μg m−3 in dry season, respectively. Total carbon (TC) accounted for 16–19% of the PM2.5 mass and 13–15% of the PM10 mass. On average, 85.9 to 88.7% of TC in PM2.5 and 87.2 to 90.1% in PM10 was organic carbon (OC), of which 67–72% and 63% was found to be water-soluble organic carbon (WSOC) in PM2.5 and PM10, respectively. Water-soluble potassium (K+) and sulphate (SO42−) in PM2.5 and, sodium (Na+) and SO42− in PM10 were the dominant ionic species. We found, that concentrations of biomass burning tracers (levoglucosan and mannosan) well correlated with non-sea-salt-K+, WSOC and OC in the aerosols from Tanzania, East Africa. Mean contributions of levoglucosan to OC ranged between 3.9–4.2% for PM2.5 and 3.5–3.8% for PM10. This study demonstrates that emissions from biomass- and biofuel-burning activities followed by atmospheric photochemical processes mainly control the air quality in Tanzania.


2012 ◽  
Vol 12 (13) ◽  
pp. 6041-6065 ◽  
Author(s):  
M. O. Andreae ◽  
P. Artaxo ◽  
V. Beck ◽  
M. Bela ◽  
S. Freitas ◽  
...  

Abstract. We present the results of airborne measurements of carbon monoxide (CO) and aerosol particle number concentration (CN) made during the Balanço Atmosférico Regional de Carbono na Amazônia (BARCA) program. The primary goal of BARCA is to address the question of basin-scale sources and sinks of CO2 and other atmospheric carbon species, a central issue of the Large-scale Biosphere-Atmosphere (LBA) program. The experiment consisted of two aircraft campaigns during November–December 2008 (BARCA-A) and May–June 2009 (BARCA-B), which covered the altitude range from the surface up to about 4500 m, and spanned most of the Amazon Basin. Based on meteorological analysis and measurements of the tracer, SF6, we found that airmasses over the Amazon Basin during the late dry season (BARCA-A, November 2008) originated predominantly from the Southern Hemisphere, while during the late wet season (BARCA-B, May 2009) low-level airmasses were dominated by northern-hemispheric inflow and mid-tropospheric airmasses were of mixed origin. In BARCA-A we found strong influence of biomass burning emissions on the composition of the atmosphere over much of the Amazon Basin, with CO enhancements up to 300 ppb and CN concentrations approaching 10 000 cm−3; the highest values were in the southern part of the Basin at altitudes of 1–3 km. The ΔCN/ΔCO ratios were diagnostic for biomass burning emissions, and were lower in aged than in fresh smoke. Fresh emissions indicated CO/CO2 and CN/CO emission ratios in good agreement with previous work, but our results also highlight the need to consider the residual smoldering combustion that takes place after the active flaming phase of deforestation fires. During the late wet season, in contrast, there was little evidence for a significant presence of biomass smoke. Low CN concentrations (300–500 cm−3) prevailed basinwide, and CO mixing ratios were enhanced by only ~10 ppb above the mixing line between Northern and Southern Hemisphere air. There was no detectable trend in CO with distance from the coast, but there was a small enhancement of CO in the boundary layer suggesting diffuse biogenic sources from photochemical degradation of biogenic volatile organic compounds or direct biological emission. Simulations of CO distributions during BARCA-A using a range of models yielded general agreement in spatial distribution and confirm the important contribution from biomass burning emissions, but the models evidence some systematic quantitative differences compared to observed CO concentrations. These mismatches appear to be related to problems with the accuracy of the global background fields, the role of vertical transport and biomass smoke injection height, the choice of model resolution, and reliability and temporal resolution of the emissions data base.


2018 ◽  
Author(s):  
Yang Wang ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Sebastian Böhnke ◽  
Isabelle De Smedt ◽  
...  

Abstract. A Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18° N, 114.36° E) in the suburban area of Xingtai (one of the most polluted cities in China) during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ~ 3.5 ppb. Underestimates of MAX-DOAS results compared to in situ measurements of NO2 (~ 60 %), SO2 (~ 20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2, SO2 are reasonably consistent with those measured by a collocated Raman Lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO, and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ~ 1.4 km) than did NO2, SO2, and HONO (with 75 % integrated column below ~ 0.5 km) under polluted condition. Lifted layers were systematically observed for all species, (except HONO), indicating accumulation, secondary formation, or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2, SO2, and HONO, but around noon for aerosols, HCHO, and CHOCHO, mainly dominated by photochemistry, characteristic upslope/downslope circulation and PBL dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution from the southern areas such as industrialized Wuan. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases, and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations of HCHO, CHOCHO and aerosols.


2006 ◽  
Vol 6 (10) ◽  
pp. 2911-2925 ◽  
Author(s):  
D. Chand ◽  
P. Guyon ◽  
P. Artaxo ◽  
O. Schmid ◽  
G. P. Frank ◽  
...  

Abstract. As part of the Large Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) campaign, detailed surface and airborne aerosol measurements were performed over the Amazon Basin during the dry to wet season from 16 September to 14 November 2002. Optical and physical properties of aerosols at the surface, and in the boundary layer (BL) and free troposphere (FT) during the dry season are discussed in this article. Carbon monoxide (CO) is used as a tracer for biomass burning emissions. At the surface, good correlation among the light scattering coefficient (σs at 545 nm), PM2.5, and CO indicates that biomass burning is the main source of aerosols. Accumulation of haze during some of the large-scale biomass burning events led to high PM2.5 (225 μg m−3), σs (1435 Mm−1), aerosol optical depth at 500 nm (3.0), and CO (3000 ppb). A few rainy episodes reduced the PM2.5, number concentration (CN) and CO concentration by two orders of magnitude. The correlation analysis between σs and aerosol optical thickness shows that most of the optically active aerosols are confined to a layer with a scale height of 1617 m during the burning season. This is confirmed by aircraft profiles. The average mass scattering and absorption efficiencies (545 nm) for small particles (diameter Dp<1.5 μm) at surface level are found to be 5.0 and 0.33 m2 g−1, respectively, when relating the aerosol optical properties to PM2.5 aerosols. The observed mean single scattering albedo (ωo at 545 nm) for submicron aerosols at the surface is 0.92±0.02. The light scattering by particles (Δσs/Δ CN) increase 2–10 times from the surface to the FT, most probably due to the combined affects of coagulation and condensation.


2010 ◽  
Vol 10 (12) ◽  
pp. 5625-5639 ◽  
Author(s):  
E. O. Fors ◽  
J. Rissler ◽  
A. Massling ◽  
B. Svenningsson ◽  
M. O. Andreae ◽  
...  

Abstract. HUmic-LIke Substances (HULIS) have been identified as major contributors to the organic carbon in atmospheric aerosol. The term "HULIS" is used to describe the organic material found in aerosol particles that resembles the humic organic material in rivers and sea water and in soils. In this study, two sets of filter samples from atmospheric aerosols were collected at different sites. One set of samples was collected at the K-puszta rural site in Hungary, about 80 km SE of Budapest, and a second was collected at a site in Rondônia, Amazonia, Brazil, during the Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) biomass burning season experiment. HULIS were extracted from the samples and their hygroscopic properties were studied using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) at relative humidity (RH) <100%, and a cloud condensation nucleus counter (CCNC) at RH >100%. The H-TDMA measurements were carried out at a dry diameter of 100 nm and for RH ranging from 30 to 98%. At 90% RH the HULIS samples showed diameter growth factors between 1.04 and 1.07, reaching values of 1.4 at 98% RH. The cloud nucleating properties of the two sets of aerosol samples were analysed using two types of thermal static cloud condensation nucleus counters. Two different parameterization models were applied to investigate the potential effect of HULIS surface activity, both yielding similar results. For the K-puszta winter HULIS sample, the surface tension at the point of activation was estimated to be lowered by between 34% (47.7 mN/m) and 31% (50.3 mN/m) for dry sizes between 50 and 120 nm in comparison to pure water. A moderate lowering was also observed for the entire water soluble aerosol sample, including both organic and inorganic compounds, where the surface tension was decreased by between 2% (71.2 mN/m) and 13% (63.3 mN/m).


2005 ◽  
Vol 5 (4) ◽  
pp. 4373-4406 ◽  
Author(s):  
D. Chand ◽  
P. Guyon ◽  
P. Artaxo ◽  
O. Schmid ◽  
G. P. Frank ◽  
...  

Abstract. As part of the Large Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) campaign, detailed surface and airborne aerosol measurements were performed over the Amazon Basin during the dry to wet season from 16 September to 14 November 2002. Optical and physical properties of aerosols at the surface, boundary layer (BL) and free troposphere (FT) during the dry season are discussed in this article. Carbon monoxide (CO) is used as a tracer for biomass burning emissions. At the surface, good correlation among the light scattering coefficient (σs at 550 nm), PM2.5, and CO indicates that biomass burning is the main source of aerosols. Accumulation of haze during some of the large-scale biomass burning events led to high mass loadings (PM2.5=200 µgm−3), σs (1400 Mm−1), aerosol optical depth at 500 nm (3.0), and CO (3000 ppb). A few rainy episodes reduced the aerosol mass loading, number concentration (CN) and CO concentration by two orders of magnitude. The correlation analysis between σs and aerosol optical thickness shows that most of the optically active aerosols are confined to a layer with a scale height of 1660 m during the burning season. The average mass scattering and absorption efficiencies (532 nm) for small particles (diameter Dp<1.5 µm) at surface level are found to be 5.3 and 0.42 m2 g−1, respectively, when relating the aerosol optical properties to PM2.5 aerosols. The observed mean single scattering albedo (ωo at ~540 nm) for submicron aerosols at the surface (0.92±0.02) is significantly higher than reported previously. The scattering efficiency (dσs/dCN) of particles increases 2–10 times from the surface to the FT, most probably due to the combined affects of coagulation and condensation.


2021 ◽  
Vol 21 (15) ◽  
pp. 11815-11828
Author(s):  
Nana Suto ◽  
Hiroto Kawashima

Abstract. The sources and seasonal trends of water-soluble organic carbon (WSOC) in carbonaceous aerosols are of significant interest. From July 2017 to July 2019, we collected samples of PM2.5 (particulate matter, aerodynamic diameter<2.5 µm) from one suburban and one rural site in Japan. The average δ13CWSOC was -25.2±1.1 ‰ and -24.6±2.4 ‰ at the suburban site and rural site, respectively. At the suburban site, the δ13CWSOC was consistent with the δ13C of burned C3 plants, and a high correlation was found between WSOC concentrations and non-sea-salt potassium concentrations; these results suggest that the main source of WSOC at this site was biomass burning of rice straw. At the rural site, the average δ13CWSOC was significantly heavier from autumn to spring (-23.9±2.1 ‰) than in summer (-27.4±0.7 ‰) (p<0.01). The δ13CWSOC from autumn to spring was consistent with that of biomass burning of rice straw, whereas that in summer was considered to reflect mainly the formation of secondary organic aerosols from biogenic volatile organic compounds (VOCs). The heaviest δ13CWSOC (-21.3±1.9 ‰) was observed from February to April 2019, which may be explained by long-range transport of C4 plant burning such as corn from overseas. Thus, the present study indicates that δ13CWSOC is potentially useful for elucidating the sources and atmospheric processes that contribute to seasonal variations of WSOC concentration.


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