scholarly journals Identification of an organic coating on marine aerosol particles by TOF-SIMS

Author(s):  
Heikki Tervahattu
1999 ◽  
Vol 30 ◽  
pp. S13-S14
Author(s):  
C.R. Zeisse ◽  
S.G. Gathman ◽  
D.R. Jensen ◽  
K.M. Littfin ◽  
W.K. Moision ◽  
...  

2019 ◽  
Vol 53 (16) ◽  
pp. 9407-9417 ◽  
Author(s):  
Amanda A. Frossard ◽  
Violaine Gérard ◽  
Patrick Duplessis ◽  
Joanna D. Kinsey ◽  
Xi Lu ◽  
...  

2013 ◽  
Vol 13 (23) ◽  
pp. 11791-11802 ◽  
Author(s):  
M. van Pinxteren ◽  
H. Herrmann

Abstract. An analytical method for the determination of the alpha dicarbonyls glyoxal (GLY) and methylglyoxal (MGLY) from seawater and marine aerosol particles is presented. The method is based on derivatization with o-(2,3,4,5,6-Pentafluorobenzyl)-hydroxylamine (PFBHA) reagent, solvent extraction and GC-MS (SIM) analysis. The method showed good precision (RSD < 10%), sensitivity (detection limits in the low ng L−1 range), and accuracy (good agreement between external calibration and standard addition). The method was applied to determine GLY and MGLY in oceanic water sampled during the Polarstern cruise ANT XXVII/4 from Capetown to Bremerhaven in spring 2011. GLY and MGLY were determined in the sea surface microlayer (SML) of the ocean and corresponding bulk water (BW) with average concentrations of 228 ng L−1 (GLY) and 196 ng L−1 (MGLY). The results show a significant enrichment (factor of 4) of GLY and MGLY in the SML. Furthermore, marine aerosol particles (PM1) were sampled during the cruise and analyzed for GLY (average concentration 0.19 ng m−3) and MGLY (average concentration 0.15 ng m−3). On aerosol particles, both carbonyls show a very good correlation with oxalate, supporting the idea of a secondary formation of oxalic acid via GLY and MGLY. Concentrations of GLY and MGLY in seawater and on aerosol particles were correlated to environmental parameters such as global radiation, temperature, distance to the coastline and biological activity. There are slight hints for a photochemical production of GLY and MGLY in the SML (significant enrichment in the SML, higher enrichment at higher temperature). However, a clear connection of GLY and MGLY to global radiation as well as to biological activity cannot be concluded from the data. A slight correlation between GLY and MGLY in the SML and in aerosol particles could be a hint for interactions, in particular of GLY, between seawater and the atmosphere.


2020 ◽  
Vol 20 (11) ◽  
pp. 6921-6951 ◽  
Author(s):  
Manuela van Pinxteren ◽  
Khanneh Wadinga Fomba ◽  
Nadja Triesch ◽  
Christian Stolle ◽  
Oliver Wurl ◽  
...  

Abstract. The project MarParCloud (Marine biological production, organic aerosol Particles and marine Clouds: a process chain) aims to improve our understanding of the genesis, modification and impact of marine organic matter (OM) from its biological production, to its export to marine aerosol particles and, finally, to its ability to act as ice-nucleating particles (INPs) and cloud condensation nuclei (CCN). A field campaign at the Cape Verde Atmospheric Observatory (CVAO) in the tropics in September–October 2017 formed the core of this project that was jointly performed with the project MARSU (MARine atmospheric Science Unravelled). A suite of chemical, physical, biological and meteorological techniques was applied, and comprehensive measurements of bulk water, the sea surface microlayer (SML), cloud water and ambient aerosol particles collected at a ground-based and a mountain station took place. Key variables comprised the chemical characterization of the atmospherically relevant OM components in the ocean and the atmosphere as well as measurements of INPs and CCN. Moreover, bacterial cell counts, mercury species and trace gases were analyzed. To interpret the results, the measurements were accompanied by various auxiliary parameters such as air mass back-trajectory analysis, vertical atmospheric profile analysis, cloud observations and pigment measurements in seawater. Additional modeling studies supported the experimental analysis. During the campaign, the CVAO exhibited marine air masses with low and partly moderate dust influences. The marine boundary layer was well mixed as indicated by an almost uniform particle number size distribution within the boundary layer. Lipid biomarkers were present in the aerosol particles in typical concentrations of marine background conditions. Accumulation- and coarse-mode particles served as CCN and were efficiently transferred to the cloud water. The ascent of ocean-derived compounds, such as sea salt and sugar-like compounds, to the cloud level, as derived from chemical analysis and atmospheric transfer modeling results, denotes an influence of marine emissions on cloud formation. Organic nitrogen compounds (free amino acids) were enriched by several orders of magnitude in submicron aerosol particles and in cloud water compared to seawater. However, INP measurements also indicated a significant contribution of other non-marine sources to the local INP concentration, as (biologically active) INPs were mainly present in supermicron aerosol particles that are not suggested to undergo strong enrichment during ocean–atmosphere transfer. In addition, the number of CCN at the supersaturation of 0.30 % was about 2.5 times higher during dust periods compared to marine periods. Lipids, sugar-like compounds, UV-absorbing (UV: ultraviolet) humic-like substances and low-molecular-weight neutral components were important organic compounds in the seawater, and highly surface-active lipids were enriched within the SML. The selective enrichment of specific organic compounds in the SML needs to be studied in further detail and implemented in an OM source function for emission modeling to better understand transfer patterns, the mechanisms of marine OM transformation in the atmosphere and the role of additional sources. In summary, when looking at particulate mass, we see oceanic compounds transferred to the atmospheric aerosol and to the cloud level, while from a perspective of particle number concentrations, sea spray aerosol (i.e., primary marine aerosol) contributions to both CCN and INPs are rather limited.


2015 ◽  
Vol 15 (15) ◽  
pp. 8847-8869 ◽  
Author(s):  
E. F. Mikhailov ◽  
G. N. Mironov ◽  
C. Pöhlker ◽  
X. Chi ◽  
M. L. Krüger ◽  
...  

Abstract. In this study we describe the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the Zotino Tall Tower Observatory (ZOTTO) in central Siberia (61° N, 89° E) from 16 to 21 June 2013. The hygroscopic growth measurements were supplemented with chemical analyses of the samples, including inorganic ions and organic/elemental carbon. In addition, the microstructure and chemical compositions of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM). A mass closure analysis indicates that organic carbon accounted for 61 and 38 % of particulate matter (PM) in the accumulation mode and coarse mode, respectively. The water-soluble fraction of organic matter was estimated to be 52 and 8 % of PM in these modes. Sulfate, predominantly in the form of ammoniated sulfate, was the dominant inorganic component in both size modes: ~ 34 % in the accumulation mode vs. ~ 47 % in the coarse mode. The hygroscopic growth measurements were conducted with a filter-based differential hygroscopicity analyzer (FDHA) over the range of 5–99.4 % RH in the hydration and dehydration operation modes. The FDHA study indicates that both accumulation and coarse modes exhibit pronounced water uptake approximately at the same relative humidity (RH), starting at ~ 70 %, while efflorescence occurred at different humidities, i.e., at ~ 35 % RH for submicron particles vs. ~ 50 % RH for supermicron particles. This ~ 15 % RH difference was attributed to higher content of organic material in the submicron particles, which suppresses water release in the dehydration experiments. The kappa mass interaction model (KIM) was applied to characterize and parameterize non-ideal solution behavior and concentration-dependent water uptake by atmospheric aerosol samples in the 5–99.4 % RH range. Based on KIM, the volume-based hygroscopicity parameter, κv, was calculated. The κv,ws value related to the water-soluble (ws) fraction was estimated to be ~ 0.15 for the accumulation mode and ~ 0.36 for the coarse mode, respectively. The obtained κv,ws for the accumulation mode is in good agreement with earlier data reported for remote sites in the Amazon rain forest (κv &amp;approx; 0.15) and a Colorado mountain forest (κv &amp;approx; 0.16 ). We used the Zdanovskii–Stokes–Robinson (ZSR) mixing rule to predict the chemical composition dependent hygroscopicity, κv,p. The obtained κv,p values overestimate the experimental FDHA-KIM-derived κv,ws by factors of 1.8 and 1.5 for the accumulation and coarse modes, respectively. This divergence can be explained by incomplete dissolution of the hygroscopic inorganic compounds resulting from kinetic limitations due to a sparingly soluble organic coating. The TEM and STXM-NEXAFS results indicate that aged submicron (> 300 nm) and supermicron aerosol particles possess core–shell structures with an inorganic core, and are enriched in organic carbon at the mixed particle surface. The direct FDHA kinetic studies provide a bulk diffusion coefficient of water of ~ 10−12 cm2 s−1 indicating a semi-solid state of the organic-rich phase leading to kinetic limitations of water uptake and release during hydration and dehydration cycles. Overall, the present ZOTTO data set, obtained in the growing season, has revealed a strong influence of organic carbon on the hygroscopic properties of the ambient aerosols. The sparingly soluble organic coating controls hygroscopic growth, phase transitions, and microstructural rearrangement processes. The observed kinetic limitations can strongly influence the outcome of experiments performed on multi-second timescales, such as the commonly applied HTDMA (Hygroscopicity Tandem Differential Mobility Analyzer) and CCNC (Cloud Condensation Nuclei Counter) measurements.


Author(s):  
Michihiro Mochida ◽  
Chiharu Nishita-Hara ◽  
Hiroshi Furutani ◽  
Yuzo Miyazaki ◽  
Jinyoung Jung ◽  
...  

1989 ◽  
Vol 23 (2) ◽  
pp. 236-240 ◽  
Author(s):  
Leonidas N. Kolaitis ◽  
Frank J. Bruynseels ◽  
Rene E. Van Grieken ◽  
Meinrat O. Andreae

2010 ◽  
Vol 2010 ◽  
pp. 1-14 ◽  
Author(s):  
Lelia N. Hawkins ◽  
Lynn M. Russell

Carbon-containing aerosol particles collected in the Arctic and southeastern Pacific marine boundary layers show distinct chemical signatures of proteins, calcareous phytoplankton, and two types of polysaccharides in Near-Edge Absorption X-ray Fine Structure (NEXAFS) spectromicroscopy. Arctic samples contained mostly supermicron sea salt cuboids with a polysaccharide-like organic coating. Southeastern Pacific samples contained both continental and marine aerosol types; of the 28 analyzed marine particles, 19 were characterized by sharp alkane and inorganic carbonate peaks in NEXAFS spectra and are identified as fragments of calcareous phytoplankton. Submicron spherical particles with spectral similarities to carbohydrate-like marine sediments were also observed in Pacific samples. In both regions, supermicron amide and alkane-containing particles resembling marine proteinaceous material were observed. These four chemical types provide a framework that incorporates several independent reports of previous marine aerosol observations, showing the diversity of the composition and morphology of ocean-derived primary particles.


2015 ◽  
Vol 15 (17) ◽  
pp. 24369-24401 ◽  
Author(s):  
W. J. Li ◽  
S. R. Chen ◽  
Y. S. Xu ◽  
X. C. Guo ◽  
Y. L. Sun ◽  
...  

Abstract. Transmission electron microscopy (TEM) was employed to obtain morphology, size, composition, and mixing state of background fine particles with diameter less than 1 μm in the Qinghai-Tibetan Plateau (QTP) during 15 September to 15 October 2013. Individual aerosol particles mainly contained secondary inorganic aerosols (SIA-sulfate and nitrate) and organics during clean periods (PM2.5: particles less than 2.5 μg m−3). The presence of KCl-NaCl associated with organics and an increase of soot particles suggest that an intense biomass burning event caused the highest PM2.5 concentrations (> 30 μg m−3) during the study. A large number fraction of the fly ash-containing particles (21.73 %) suggests that coal combustion emissions in the QTP significantly contributed to air pollutants at the median pollution level (PM2.5: 10–30 μg m−3). We concluded that emissions from biomass burning and from coal combustion both constantly contribute to anthropogenic particles in the QTP atmosphere. Based on size distributions of individual particles in different pollution levels, we found that gas condensation on existing particles is an important chemical process for the formation of SIA with organic coating. TEM observations show that refractory aerosols (e.g., soot, fly ash, and visible organic particles) likely adhere to the surface of SIA particles larger than 200 nm due to coagulation. Organic coating and soot on surface of the aged particles likely influence their hygroscopic and optical properties in the QTP, respectively. To our knowledge, this study reports the first microscopic analysis of fine particles in the background QTP air.


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