scholarly journals Molecular Distributions and Compound-Specific Stable Carbon Isotopic Compositions of Plant Wax n-Alkanes in Marine Aerosols along a North–South Transect in the Arctic–Northwest Pacific Region

Atmosphere ◽  
2020 ◽  
Vol 11 (5) ◽  
pp. 499
Author(s):  
Jung-Hyun Kim ◽  
Jiyeon Park ◽  
Sol-Bin Kim ◽  
Kyung-Hoon Shin ◽  
Sookwan Kim ◽  
...  

A geographical source of n-alkanes in marine aerosols was assessed along a North–South transect in the Arctic–Northwest Pacific region. Marine aerosol samples were collected during the ARA08 cruise with the R/V Araon between 28 August and 28 September 2017. We investigated molecular distributions of n-alkanes (homologous series of C16 to C34) and compound-specific stable carbon isotopes (δ13C) of n-C27, n-C29, and n-C31. Unresolved complex mixtures (UCM) showed a latitudinal trend from the Arctic Ocean to the northwest Pacific Ocean, highlighting an increasing influence of the plume of polluted air exported from East Asian countries. The anthropogenic input was further evidenced by high U/R ratios (>5) and low CPI17–23 (0.6–1.4). The occurrence of high molecular weight (HMW) n-alkanes with high CPI27–31 (>3) indicated the biogenic input of terrestrial higher plant leaf waxes in all studied samples. The δ13C of HMW n-alkanes was influenced by both the relative contributions from the C3/C4 plant sources and from fossil fuel combustions. The back-trajectory analyses provided evidence that changes in molecular distributions and δ13C of n-alkanes were due to the long-range atmospheric transport of anthropogenic and biogenic organic materials from North American and East Asian countries to the Arctic Ocean and the remote northwest Pacific Ocean, respectively.

2012 ◽  
Vol 9 (8) ◽  
pp. 10429-10465
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
J. Chen ◽  
B. Charrière ◽  
R. Sempéré

Abstract. Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m−3 (mean 47.6 ng m−3), accounting for 1.8–11.0% (4.8%) of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA) tracers formed from the oxidation of biogenic volatile organic compounds (VOCs) such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m−3 (9.2 ng m−3), followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 10.7% (up to 26.2%) of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8%) and α-pinene SOC (2.9%). In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.


2012 ◽  
Vol 9 (11) ◽  
pp. 4725-4737 ◽  
Author(s):  
K. Kawamura ◽  
K. Ono ◽  
E. Tachibana ◽  
B. Charriére ◽  
R. Sempéré

Abstract. Oxalic and other small dicarboxylic acids have been reported as important water-soluble organic constituents of atmospheric aerosols from different environments. Their molecular distributions are generally characterized by the predominance of oxalic acid (C2) followed by malonic (C3) and/or succinic (C4) acids. In this study, we collected marine aerosols from the Arctic Ocean during late summer in 2009 when sea ice was retreating. The marine aerosols were analyzed for the molecular distributions of dicarboxylic acids as well as ketocarboxylic acids and α-dicarbonyls to better understand the source of water-soluble organics and their photochemical processes in the high Arctic marine atmosphere. We found that diacids are more abundant than ketoacids and α-dicarbonyls, but their concentrations are generally low (< 30 ng m−3), except for one sample (up to 70 ng m−3) that was collected near the mouth of Mackenzie River during clear sky condition. Although the molecular compositions of diacids are in general characterized by the predominance of oxalic acid, a depletion of C2 was found in two samples in which C4 became the most abundant. Similar depletion of oxalic acid has previously been reported in the Arctic aerosols collected at Alert after polar sunrise and in the summer aerosols from the coast of Antarctica. Because the marine aerosols that showed a depletion of C2 were collected under the overcast and/or foggy conditions, we suggest that a photochemical decomposition of oxalic acid may have occurred in aqueous phase of aerosols over the Arctic Ocean via the photo dissociation of oxalate-Fe (III) complex. We also determined stable carbon isotopic compositions (δ13C) of bulk aerosol carbon and individual diacids. The δ13C of bulk aerosols showed −26.5‰ (range: −29.7 to −24.7‰, suggesting that marine aerosol carbon is derived from both terrestrial and marine organic materials. In contrast, oxalic acid showed much larger δ13C values (average: −20.9‰, range: −24.7‰ to −17.0‰) than those of bulk aerosol carbon. Interestingly, δ13C values of oxalic acid were higher than C3 (av. −26.6‰) and C4 (−25.8‰) diacids, suggesting that oxalic acid is enriched with 13C due to its photochemical processing (aging) in the marine atmosphere.


2013 ◽  
Vol 10 (2) ◽  
pp. 653-667 ◽  
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
J. Chen ◽  
B. Charrière ◽  
R. Sempéré

Abstract. Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m−3 (mean 47.6 ng m−3), accounting for 1.8–11.0% (4.8%) of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA) tracers formed from the oxidation of biogenic volatile organic compounds (VOCs) such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m−3 (9.2 ng m−3), followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 10.7% (up to 26.2%) of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8%) and α-pinene SOC (2.9%). In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.


2012 ◽  
Vol 9 (8) ◽  
pp. 10121-10148
Author(s):  
K. Kawamura ◽  
K. Ono ◽  
E. Tachibana ◽  
B. Charriére ◽  
R. Sempéré

Abstract. Oxalic and other small dicarboxylic acids have been reported as important water-soluble organic constituents of atmospheric aerosols from different environments. Their molecular distributions are generally characterized by the predominance of oxalic acid (C2) followed by malonic (C3) and/or succinic (C4) acids. In this study, we collected marine aerosols from the Arctic Ocean during late summer in 2009 when sea ice is retreated. The marine aerosols were analyzed for the molecular distributions of dicarboxylic acids as well as ketocarboxylic acids and α-dicarbonyls to better understand the source of water-soluble organics and their photochemical processes in the high Arctic marine atmosphere. We found that diacids are more abundant than ketoacids and α-dicarbonyls, but their concentrations are generally low (< 30 ng m−3), except for one sample (up to 70 ng m−3) that was collected near the mouth of Mackenzie River during clear sky condition. Although the molecular compositions of diacids are in general characterized by the predominance of oxalic acid, a depletion of C2 was found in two samples in which C4 became the most abundant. Similar depletion of oxalic acid has previously been reported in the Arctic aerosols collected at Alert after polar sunrise and in the summer aerosols from the coastal Antarctica. Because the marine aerosols that showed a depletion of C2 were observed under the overcast and/or foggy conditions, we suggest that a photochemical decomposition of oxalic acid may have occurred in aqueous phase of aerosols over the Arctic Ocean via the photo dissociation of oxalate-Fe (III) complex. We also determined stable carbon isotopic compositions (δ13C) of bulk aerosol carbon and individual diacids. The δ13C of bulk aerosols showed −26.5‰ (range: −29.7‰ to −24.7‰), suggesting that marine aerosol carbon is derived from both terrestrial and marine organic materials. In contrast, oxalic acid showed much larger δ13C values (average: −20.9‰, range: −24.7‰ to −17.0‰) than those of bulk aerosol carbon. Interestingly, δ13C values of oxalic acid were higher than C3 (av. −26.6‰) and C4 (−25.8‰) diacids, suggesting that oxalic acid is enriched with 13C due to its photochemical processing (aging) in the marine atmosphere.


2020 ◽  
Author(s):  
Xiaole Pan ◽  
Yu Tian ◽  
Jinpei Yan ◽  
Qi Lin ◽  
Yele Sun ◽  
...  

&lt;p&gt;Atmospheric aerosols over polar regions have attracted considerable attention for their pivotal effects on climate change. In this study, temporospatial variations in single-particle-based depolarization ratios (&amp;#948;: s-polarized component divided by the total backward scattering intensity) were studied over the Northwest Pacific and the Arctic Ocean using an optical particle counter with a depolarization module. The &amp;#948; value of aerosols was 0.06 &amp;#177; 0.01 for the entire observation period, 61 &amp;#177; 10% lower than the observations for coastal Japan (0.12 &amp;#177; 0.02) (Pan et al. Atmos. Chem. Phys. 2016, 16, 9863&amp;#8722;9873) and inland China (0.19 &amp;#177; 0.02) (Tian et al. Atmos. Chem. Phys. 2018, 18, 18203&amp;#8722;18217) in summer. The volume concentration showed two dominant size modes at 0.9 and 2 &amp;#956;m. The super-micrometer particles were mostly related to sea-salt aerosols with a &amp;#948; value of 0.09 over marine polar areas, &amp;#8764;22% larger than in the low-latitude region because of differences in chemical composition and dry air conditions. The &amp;#948; values for fine particles (&lt;1 &amp;#956;m) were 0.05 &amp;#177; 0.1, 50% lower than inland anthropogenic pollutants, mainly because of the complex mixtures of sub-micrometer sea salts. High particle concentrations in the Arctic Ocean could mostly be attributed to the strong marine emission of sea salt associated with deep oceanic cyclones, whereas long-range transport pollutants from the continent were among the primary causes of high particle concentrations in the Northwest Pacific region.&lt;/p&gt;


2010 ◽  
Vol 7 (5) ◽  
pp. 406 ◽  
Author(s):  
Siqi Xu ◽  
Zhouqing Xie ◽  
Bing Li ◽  
Wei Liu ◽  
Liguang Sun ◽  
...  

Environmental context.Iodine in the atmosphere plays an important role in troposphere ozone destruction and climate change. However, cycling of atmospheric iodine is still poorly understood because of uncertainties in iodine speciation in aerosols. Here we report iodine levels and speciation in marine aerosols collected along a cruise path from Shanghai to the Arctic Ocean. Abstract.Total iodine (TI) and water-soluble iodine species in the total suspended particle samples collected onboard a round-trip cruise from Shanghai, China to the Arctic Ocean were measured using inductively coupled plasma mass spectrometry and ion chromatography–inductively coupled plasma mass spectrometry respectively. TI and total soluble iodine (TSI) levels varied considerably both spatially and temporally over the length of the voyage. The maximum iodine levels occurred in the Arctic Ocean in September, whereas the minimum levels occurred in the Western and Northern Pacific Ocean in July. Iodate (IO3 –) was found to be the dominant species in most samples, accounting for 57.8% of TSI on average, whereas iodide and soluble organic iodine only accounted for 16.8% of TSI on average. There was also a significant fraction of insoluble iodine. This finding confirms model predictions of atmospheric iodine speciation, i.e. the predominant iodine species is iodate rather than iodide.


2011 ◽  
Vol 26 (3) ◽  
pp. n/a-n/a ◽  
Author(s):  
Petra L. Schoon ◽  
Appy Sluijs ◽  
Jaap S. Sinninghe Damsté ◽  
Stefan Schouten

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