scholarly journals Oxygenated organic functional groups and their sources in single and submicron organic particles in MILAGRO 2006 campaign

2009 ◽  
Vol 9 (1) ◽  
pp. 4567-4607 ◽  
Author(s):  
S. Liu ◽  
S. Takahama ◽  
L. M. Russell ◽  
S. Gilardoni ◽  
D. Baumgardner
Keyword(s):  
Functional Groups ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Sampling Period ◽  
Fuel Combustion ◽  
Ftir Spectra ◽  
Submicron Particles ◽  
Fossil Fuel Combustion ◽  
X Ray ◽  
Organic Functional Groups

Abstract. Fourier Transform Infrared (FTIR) and X-ray Fluorescence (XRF) were used to measure organic functional groups and elements of submicron particles collected during MILAGRO in March 2006 on three platforms: the Mexico City urban area (SIMAT), the high altitude site at 4010 m (Altzomoni), and the NCAR C130 aircraft. Scanning transmission X-ray Microscopy (STXM) and Near-Edge X-ray Absorption Fine Structure (NEXAFS) were applied to single particle organic functional group abundance analysis of particles simultaneously collected at SIMAT and C130. Correlations of elemental concentrations showed different groups of source related elements at SIMAT, Altzomoni, and C130, suggesting different processes affecting the air masses sampled at the three platforms. Cluster analysis resulted in seven distinct Clusters of FTIR spectra, with the last three clusters consisting of spectra collected almost exclusively on the C130 platform, reflecting the variety of sources contributing to C130 samples. Positive Matrix Factorization (PMF) of NEXAFS-STXM spectra identified three main factors representing soot, secondary, and biomass burning type spectra. PMF of FTIR spectra resulted in three fossil fuel combustion type factors, one biomass burning factor, and one mixed or processed factor. The fossil fuel combustion type factors were found to have the largest contributions to OM, while the processed factor has the largest O/C among all factors. Alkane, carboxylic acid, and amine functional groups were mainly associated with combustion related sources, while alcohol groups were likely from atmospheric processing of mixed sources. While the processed factor has the highest O/C, half of the OM and O/C measured could be attributed directly to fossil fuel combustion sources. Both PMF of NEXAFS-STXM spectra and PMF of FTIR spectra indicate that the combustion type factors are more affected by fluctuations in local sources, while the processed factors are more consistent during the sampling period.

scholarly journals Oxygenated organic functional groups and their sources in single and submicron organic particles in MILAGRO 2006 campaign

2009 ◽  
Vol 9 (18) ◽  
pp. 6849-6863 ◽  
Author(s):  
S. Liu ◽  
S. Takahama ◽  
L. M. Russell ◽  
S. Gilardoni ◽  
D. Baumgardner
Keyword(s):  
Functional Groups ◽  
Biomass Burning ◽  
Ftir Spectra ◽  
Submicron Particles ◽  
Air Masses ◽  
X Ray ◽  
Source Regions ◽  
Organic Functional Groups ◽  
Scanning Transmission ◽  
Organic Particles

Abstract. Fourier Transform Infrared (FTIR) and X-ray Fluorescence (XRF) were used to measure organic functional groups and elements of submicron particles collected during MILAGRO in March 2006 on three platforms: the Mexico City urban area (SIMAT), the high altitude site at 4010 m (Altzomoni), and the NCAR C130 aircraft. Scanning Transmission X-ray Microscopy (STXM) and Near-Edge X-ray Absorption Fine Structure (NEXAFS) were applied to single particle organic functional group abundance analysis of particles simultaneously collected at SIMAT and C130. Correlations of elemental concentrations showed different groups of source-related elements at SIMAT, Altzomoni, and C130, suggesting different processes affecting the air masses sampled at the three platforms. Cluster analysis resulted in seven distinct clusters of FTIR spectra, with the last three clusters consisting of spectra collected almost exclusively on the C130 platform, reflecting the variety of sources contributing to C130 samples. Positive Matrix Factorization (PMF) of STXM-NEXAFS spectra identified three main factors representing soot, secondary, and biomass burning type spectra. PMF of FTIR spectra resulted in two fossil fuel combustion factors and one biomass burning factor, the former representative of source regions to the northeast and southwest of SIMAT. Alkane, carboxylic acid, amine, and alcohol functional groups were mainly associated with combustion related sources, while non-acid carbonyl groups were likely from biomass burning events. The majority of OM and O/C was attributed to combustion sources, although no distinction between direct emissions and atmospherically processed OM could be identified.

scholarly journals Seasonal changes in Fe species and soluble Fe concentration in the atmosphere in the Northwest Pacific region based on the analysis of aerosols collected in Tsukuba, Japan

2013 ◽  
Vol 13 (15) ◽  
pp. 7695-7710 ◽  
Author(s):  
Y. Takahashi ◽  
T. Furukawa ◽  
Y. Kanai ◽  
M. Uematsu ◽  
G. Zheng ◽  
...  
Keyword(s):  
Fossil Fuel ◽  
Fuel Combustion ◽  
Anthropogenic Sources ◽  
Anthropogenic Activity ◽  
Northwest Pacific ◽  
Pacific Region ◽  
Fossil Fuel Combustion ◽  
Factors Affecting ◽  
X Ray ◽  
Fe Species

Abstract. Atmospheric iron (Fe) can be a significant source of nutrition for phytoplankton inhabiting remote oceans, which in turn has a large influence on the Earth's climate. The bioavailability of Fe in aerosols depends mainly on the fraction of soluble Fe (= [FeSol]/[FeTotal], where [FeSol] and [FeTotal] are the atmospheric concentrations of soluble and total Fe, respectively). However, the numerous factors affecting the soluble Fe fraction have not been fully understood. In this study, the Fe species, chemical composition, and soluble Fe concentrations in aerosols collected in Tsukuba, Japan were investigated over a year (nine samples from December 2002 to October 2003) to identify the factors affecting the amount of soluble Fe supplied into the ocean. The soluble Fe concentration in aerosols is correlated with those of sulfate and oxalate originated from anthropogenic sources, suggesting that soluble Fe is mainly derived from anthropogenic sources. Moreover, the soluble Fe concentration is also correlated with the enrichment factors of vanadium and nickel emitted by fossil fuel combustion. These results suggest that the degree of Fe dissolution is influenced by the magnitude of anthropogenic activity, such as fossil fuel combustion. X-ray absorption fine structure (XAFS) spectroscopy was performed in order to identify the Fe species in aerosols. Fitting of XAFS spectra coupled with micro X-ray fluorescence analysis (μ-XRF) showed the main Fe species in aerosols in Tsukuba to be illite, ferrihydrite, hornblende, and Fe(III) sulfate. Moreover, the soluble Fe fraction in each sample measured by leaching experiments is closely correlated with the Fe(III) sulfate fraction determined by the XAFS spectrum fitting, suggesting that Fe(III) sulfate is the main soluble Fe in the ocean. Another possible factor that can control the amount of soluble Fe supplied into the ocean is the total Fe(III) concentration in the atmosphere, which was high in spring due to the high mineral dust concentrations during spring in East Asia. However, this factor does not contribute to the amount of soluble Fe to a larger degree than the effect of Fe speciation, or more strictly speaking the presence of Fe(III) sulfate. Therefore, based on these results, the most significant factor influencing the amount of soluble Fe in the North Pacific region is the concentration of anthropogenic Fe species such as Fe(III) sulfate that can be emitted from megacities in Eastern Asia.

scholarly journals Sources and formation of carbonaceous aerosols in Xi'an, China: primary emissions and secondary formation constrained by radiocarbon

2020 ◽  
Author(s):  
Haiyan Ni ◽  
Ru-Jin Huang ◽  
Ulrike Dusek
Keyword(s):  
Biomass Burning ◽  
Coal Combustion ◽  
Vehicle Emissions ◽  
Fossil Fuel ◽  
Fuel Combustion ◽  
Warm Period ◽  
Water Soluble ◽  
Formation Mechanisms ◽  
Carbonaceous Aerosols ◽  
Fossil Fuel Combustion

<p>To investigate the sources and formation mechanisms of carbonaceous aerosols, a major contributor to severe particulate air pollution, radiocarbon (<span><sup>14</sup>C</span>) measurements were conducted on aerosols sampled from November 2015 to November 2016 in Xi'an, China. Based on the <span><sup>14</sup>C</span> content in elemental carbon (EC), organic carbon (OC) and water-insoluble OC (WIOC), contributions of major sources to carbonaceous aerosols are estimated over a whole seasonal cycle: primary and secondary fossil sources, primary biomass burning, and other non-fossil carbon formed mainly from secondary processes. Primary fossil sources of EC were further sub-divided into coal and liquid fossil fuel combustion by complementing <span><sup>14</sup>C</span> data with stable carbon isotopic signatures.</p><p>The dominant EC source was liquid fossil fuel combustion (i.e., vehicle emissions), accounting for 64 % (median; 45 %–74 %, interquartile range) of EC in autumn, 60 % (41 %–72 %) in summer, 53 % (33 %–69 %) in spring and 46 % (29 %–59 %) in winter. An increased contribution from biomass burning to EC was observed in winter (<span>∼28</span> %) compared to other seasons (warm period; <span>∼15</span> %). In winter, coal combustion (<span>∼25</span> %) and biomass burning equally contributed to EC, whereas in the warm period, coal combustion accounted for a larger fraction of EC than biomass burning. The relative contribution of fossil sources to OC was consistently lower than that to EC, with an annual average of <span>47±4</span> %. Non-fossil OC of secondary origin was an important contributor to total OC (<span>35±4</span> %) and accounted for more than half of non-fossil OC (<span>67±6</span> %) throughout the year. Secondary fossil OC (SOC<span><sub>fossil</sub></span>) concentrations were higher than primary fossil OC (POC<span><sub>fossil</sub></span>) concentrations in winter but lower than POC<span><sub>fossil</sub></span> in the warm period.</p><p>Fossil WIOC and water-soluble OC (WSOC) have been widely used as proxies for POC<span><sub>fossil</sub></span> and SOC<span><sub>fossil</sub></span>, respectively. This assumption was evaluated by (1) comparing their mass concentrations with POC<span><sub>fossil</sub></span> and SOC<span><sub>fossil</sub></span> and (2) comparing ratios of fossil WIOC to fossil EC to typical primary OC-to-EC ratios from fossil sources including both coal combustion and vehicle emissions. The results suggest that fossil WIOC and fossil WSOC are probably a better approximation for primary and secondary fossil OC, respectively, than POC<span><sub>fossil</sub></span> and SOC<span><sub>fossil</sub></span> estimated using the EC tracer method.</p>

scholarly journals Ship-borne FTIR measurements of CO and O<sub>3</sub> in the Western Pacific from 43° N to 35° S: an evaluation of the sources

2012 ◽  
Vol 12 (2) ◽  
pp. 815-828 ◽  
Author(s):  
T. Ridder ◽  
C. Gerbig ◽  
J. Notholt ◽  
M. Rex ◽  
O. Schrems ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Fuel Combustion ◽  
Western Pacific ◽  
Fossil Fuel Combustion ◽  
Source Regions ◽  
The Western Pacific

Abstract. Carbon monoxide (CO) and ozone (O3) have been measured in the Western Pacific (43° N to 35° S) during a ship campaign with Research Vessel Sonne in fall 2009. Observations have been performed using ship-based solar absorption Fourier Transform infrared spectrometry, flask sampling, balloon sounding, and in-situ Fourier Transform infrared analysis. The results obtained are compared to the GEOS-Chem global 3-D chemistry transport model for atmospheric composition. In general, a very good agreement is found between the GEOS-Chem model and all instruments. The CO and O3 distributions show a comparable variability suggesting an impact from the same source regions. Tagged-CO simulations implemented in the GEOS-Chem model make it possible to differentiate between different source processes and source regions. The source regions are verified with HYSPLIT backward trajectory calculations. In the Northern Hemisphere fossil fuel combustion in Asia is the dominant source. European and North American fossil fuel combustion also contribute to Northern Hemispheric CO pollution. In the Southern Hemisphere contributions from biomass burning and fossil fuel combustion are dominant; African biomass burning has a significant impact on Western Pacific CO pollution. Furthermore, in the tropical Western Pacific enhanced upper tropospheric CO within the tropical tropopause layer mainly originates from Indonesian fossil fuel combustion and can be transported into the stratosphere. The source regions of the measured O3 pollution are simulated with a tagged-O3 simulation implemented in the GEOS-Chem model. Similar source regions compared to the tagged-CO simulations are identified by the model. In the Northern Hemisphere contributions from Asia, Europe, and North America are significant. In the Southern Hemisphere emissions from South America, south-east Africa, and Oceania significantly contribute to the measured O3 pollution.

scholarly journals Fossil fuel combustion, biomass burning and biogenic sources of fine carbonaceous aerosol in the Carpathian Basin

2019 ◽  
Author(s):  
Imre Salma ◽  
Anikó Vasanits-Zsigrai ◽  
Attila Machon ◽  
Tamás Varga ◽  
István Major ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Fossil Fuel ◽  
Fuel Combustion ◽  
Carpathian Basin ◽  
Water Soluble ◽  
Total Carbon ◽  
Carbonaceous Aerosol ◽  
City Centre ◽  
Fossil Fuel Combustion ◽  
Regional Background

Abstract. Fine-fraction aerosol samples were collected, air pollutants and meteorological properties were measured in-situ in regional background environment of the Carpathian Basin, a suburban area and central part of its largest city, Budapest in each season for 1 year-long time interval. The samples were analysed for PM2.5 mass, organic carbon (OC), elemental carbon (EC), water-soluble OC (WSOC), radiocarbon, levoglucosan (LVG) and its stereoisomers, and some chemical elements. Carbonaceous aerosol species made up 36 % of the PM2.5 mass with a modest seasonal variation and with a slightly increasing tendency from the regional background to the city centre (from 32 to 39 %). Coupled radiocarbon-LVG marker method was applied to apportion the total carbon (TC = OC + EC) into contributions of EC and OC from fossil fuel (FF) combustion (ECFF and OCFF, respectively), EC and OC from biomass burning (BB) (ECBB and OCBB, respectively) and OC from biogenic sources (OCBIO). Fossil fuel combustion showed rather constant daily or seasonal mean contributions (of 35 %) to the TC in the whole year in all atmospheric environments, while the daily contributions of BB and biogenic sources changed radically (from

scholarly journals Sources and formation of carbonaceous aerosols in Xi'an, China: primary emissions and secondary formation constrained by radiocarbon

2019 ◽  
Vol 19 (24) ◽  
pp. 15609-15628 ◽  
Author(s):  
Haiyan Ni ◽  
Ru-Jin Huang ◽  
Junji Cao ◽  
Jie Guo ◽  
Haoyue Deng ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Coal Combustion ◽  
Vehicle Emissions ◽  
Fossil Fuel ◽  
Fuel Combustion ◽  
Warm Period ◽  
Water Soluble ◽  
Formation Mechanisms ◽  
Carbonaceous Aerosols ◽  
Fossil Fuel Combustion

Abstract. To investigate the sources and formation mechanisms of carbonaceous aerosols, a major contributor to severe particulate air pollution, radiocarbon (14C) measurements were conducted on aerosols sampled from November 2015 to November 2016 in Xi'an, China. Based on the 14C content in elemental carbon (EC), organic carbon (OC) and water-insoluble OC (WIOC), contributions of major sources to carbonaceous aerosols are estimated over a whole seasonal cycle: primary and secondary fossil sources, primary biomass burning, and other non-fossil carbon formed mainly from secondary processes. Primary fossil sources of EC were further sub-divided into coal and liquid fossil fuel combustion by complementing 14C data with stable carbon isotopic signatures. The dominant EC source was liquid fossil fuel combustion (i.e., vehicle emissions), accounting for 64 % (median; 45 %–74 %, interquartile range) of EC in autumn, 60 % (41 %–72 %) in summer, 53 % (33 %–69 %) in spring and 46 % (29 %–59 %) in winter. An increased contribution from biomass burning to EC was observed in winter (∼28 %) compared to other seasons (warm period; ∼15 %). In winter, coal combustion (∼25 %) and biomass burning equally contributed to EC, whereas in the warm period, coal combustion accounted for a larger fraction of EC than biomass burning. The relative contribution of fossil sources to OC was consistently lower than that to EC, with an annual average of 47±4 %. Non-fossil OC of secondary origin was an important contributor to total OC (35±4 %) and accounted for more than half of non-fossil OC (67±6 %) throughout the year. Secondary fossil OC (SOCfossil) concentrations were higher than primary fossil OC (POCfossil) concentrations in winter but lower than POCfossil in the warm period. Fossil WIOC and water-soluble OC (WSOC) have been widely used as proxies for POCfossil and SOCfossil, respectively. This assumption was evaluated by (1) comparing their mass concentrations with POCfossil and SOCfossil and (2) comparing ratios of fossil WIOC to fossil EC to typical primary OC-to-EC ratios from fossil sources including both coal combustion and vehicle emissions. The results suggest that fossil WIOC and fossil WSOC are probably a better approximation for primary and secondary fossil OC, respectively, than POCfossil and SOCfossil estimated using the EC tracer method.

scholarly journals Analysis of Four Years of Global XCO2 Anomalies as Seen by Orbiting Carbon Observatory-2

2019 ◽  
Vol 11 (7) ◽  
pp. 850 ◽  
Author(s):  
Janne Hakkarainen ◽  
Iolanda Ialongo ◽  
Shamil Maksyutov ◽  
David Crisp
Keyword(s):  
South Africa ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Global Scale ◽  
Complex Model ◽  
Fuel Combustion ◽  
Local Concentration ◽  
Fossil Fuel Combustion ◽  
Tropical Regions ◽  
Model Based

NASA’s carbon dioxide mission, Orbiting Carbon Observatory-2, began operating in September 2014. In this paper, we analyze four years (2015–2018) of global (60°S–60°N) XCO2 anomalies and their annual variations and seasonal patterns. We show that the anomaly patterns in the column-averaged CO2 dry air mole fraction, XCO2, are robust and consistent from year-to-year. We evaluate the method by comparing the anomalies to fluxes from anthropogenic, biospheric, and biomass burning and to model-simulated local concentration enhancements. We find that, despite the simplicity of the method, the anomalies describe the spatio-temporal variability of XCO2 (including anthropogenic emissions and seasonal variability related to vegetation and biomass burning) consistently with more complex model-based approaches. We see, for example, that positive anomalies correspond to fossil fuel combustion over the major industrial areas (e.g., China, eastern USA, central Europe, India, and the Highveld region in South Africa), shown as large positive XCO2 enhancements in the model simulations. We also find corresponding positive anomalies and fluxes over biomass burning areas during different fire seasons. On the other hand, the largest negative anomalies correspond to the growing season in the northern middle latitudes, characterized by negative XCO2 enhancements from simulations and high solar-induced chlorophyll fluorescence (SIF) values (indicating the occurrence of photosynthesis). The largest discrepancies between the anomaly patterns and the model-based results are observed in the tropical regions, where OCO-2 shows persistent positive anomalies over every season of every year included in this study. Finally, we demonstrate how XCO2 anomalies enable the detection of anthropogenic signatures for several local scale case studies, both in the Northern and Southern Hemisphere. In particular, we analyze the XCO2 anomalies collocated with the recent TROPOspheric Monitoring Instrument NO2 observations (used as indicator of anthropogenic fossil fuel combustion) over the Highveld region in South Africa. The results highlight the capability of satellite-based observations to monitor natural and man-made CO2 signatures on global scale.

scholarly journals Intense atmospheric pollution modifies weather: a case of mixed biomass burning with fossil fuel combustion pollution in eastern China

2013 ◽  
Vol 13 (20) ◽  
pp. 10545-10554 ◽  
Author(s):  
A. J. Ding ◽  
C. B. Fu ◽  
X. Q. Yang ◽  
J. N. Sun ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Air Pollution ◽  
Biomass Burning ◽  
Atmospheric Pollution ◽  
Fossil Fuel ◽  
Eastern China ◽  
Temperature Drop ◽  
Fuel Combustion ◽  
Climate Impacts ◽  
Fossil Fuel Combustion ◽  
Mixed Biomass

Abstract. The influence of air pollutants, especially aerosols, on regional and global climate has been widely investigated, but only a very limited number of studies report their impacts on everyday weather. In this work, we present for the first time direct (observational) evidence of a clear effect of how a mixed atmospheric pollution changes the weather with a substantial modification in the air temperature and rainfall. By using comprehensive measurements in Nanjing, China, we found that mixed agricultural burning plumes with fossil fuel combustion pollution resulted in a decrease in the solar radiation intensity by more than 70%, a decrease in the sensible heat by more than 85%, a temperature drop by almost 10 K, and a change in rainfall during both daytime and nighttime. Our results show clear air pollution–weather interactions, and quantify how air pollution affects weather via air pollution–boundary layer dynamics and aerosol–radiation–cloud feedbacks. This study highlights cross-disciplinary needs to investigate the environmental, weather and climate impacts of the mixed biomass burning and fossil fuel combustion sources in East China.

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