scholarly journals Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain

2018 ◽  
Vol 18 (20) ◽  
pp. 15069-15086 ◽  
Author(s):  
Jingjing Meng ◽  
Gehui Wang ◽  
Zhanfang Hou ◽  
Xiaodi Liu ◽  
Benjie Wei ◽  
...  
Keyword(s):  
Azelaic Acid ◽  
North China Plain ◽  
North China ◽  
Organic Aerosols ◽  
Dicarboxylic Acids ◽  
Stable Carbon ◽  
Δ13c Values ◽  
Carbon Isotopic ◽  
The North ◽  
The North China Plain

Abstract. Molecular distributions and stable carbon isotopic (δ13C values) compositions of dicarboxylic acids and related secondary organic aerosols (SOA) in PM2.5 aerosols collected on a day/night basis at the summit of Mt. Tai (1534 m a.s.l.) in the summer of 2016 were analyzed to investigate the sources and photochemical aging process of organic aerosols in the forested highland region of the North China Plain. The molecular distributions of dicarboxylic acids and related SOA are characterized by the dominance of oxalic acid (C2), followed by malonic (C3), succinic (C4) and azelaic (C9) acids. The concentration ratios of C2 ∕ C4, diacid-C ∕ OC and C2 ∕ total diacids are larger in the daytime than in the nighttime, suggesting that the daytime aerosols are more photochemically aged than those in the nighttime due to the higher temperature and stronger solar radiation. Both ratios of C2 ∕ C4 (R2>0.5) and C3 ∕ C4 (R2>0.5) correlated strongly with the ambient temperatures, indicating that SOA in the mountaintop atmosphere are mainly derived from the photochemical oxidation of local emissions rather than long-range transport. The mass ratios of azelaic acid to adipic acid (C9 ∕ C6), azelaic acid to phthalic aid (C9 ∕ Ph) and glyoxal to methylglyoxal (Gly ∕ mGly) and the strong linear correlations of major dicarboxylic acids and related SOA (i.e., C2, C3, C4, ωC2, Pyr, Gly and mGly) with biogenic precursors (SOA tracers derived from isoprene, α/β-pinene and β-caryophyllene) further suggest that aerosols in this region are mainly originated from biogenic sources (i.e., tree emissions). C2 concentrations correlated well with aerosol pH, indicating that particle acidity favors the organic acid formation. The stable carbon isotopic compositions (δ13C) of the dicarboxylic acids are higher in the daytime than in the nighttime, with the highest value (-16.5±1.9 ‰) found for C2 and the lowest value (-25.2±2.7 ‰) found for C9. An increase in δ13C values of C2 along with increases in C2 ∕ Gly and C2 ∕ mGly ratios was observed, largely due to the isotopic fractionation effect during the precursor oxidation process.

scholarly journals Diurnal variations of organic molecular tracers and stable carbon isotopic composition in atmospheric aerosols over Mt. Tai in the North China Plain: an influence of biomass burning

2012 ◽  
Vol 12 (18) ◽  
pp. 8359-8375 ◽  
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
J. Chen ◽  
J. Li ◽  
Y. L. Sun ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
North China Plain ◽  
North China ◽  
Carbon Isotopic Composition ◽  
Organic Aerosol ◽  
Stable Carbon ◽  
Carbon Isotopic ◽  
The North ◽  
The North China Plain

Abstract. Organic tracer compounds, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated in aerosol samples collected during early and late periods of the Mount Tai eXperiment 2006 (MTX2006) field campaign in the North China Plain. Total solvent-extractable fractions were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in the North China Plain were very active, the total identified organics (2090 ± 1170 ng m−3) were double those in late June (926 ± 574 ng m−3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88–1210 ng m−3, mean 403 ng m−3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude, which could be further transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the OC in the Mt. Tai aerosols was due to biomass burning in early June, followed by the contribution of isoprene SOC (mean 4.3%). In contrast, isoprene SOC was the main contributor (6.6%) to OC, and only 3.0% of the OC was due to biomass burning in late June. In early June, δ13C of TC (−26.6 to −23.2‰, mean −25.0‰) were lower than those (−23.9 to −21.9‰, mean −22.9‰) in late June. In addition, a strong anti-correlation was found between levoglucosan and δ13C values. This study demonstrates that crop-residue burning activities can significantly enhance the organic aerosol loading and alter the organic composition and stable carbon isotopic composition of aerosol particles in the troposphere over the North China Plain.

scholarly journals Molecular distribution and stable carbon isotopic compositions of dicarboxylic acids and related SOA from biogenic sources in the summertime atmosphere of Mt. Tai in the North China Plain

2018 ◽  
Author(s):  
Jingjing Meng ◽  
Gehui Wang ◽  
Zhanfang Hou ◽  
Xiaodi Liu ◽  
Benjie Wei ◽  
...  
Keyword(s):  
North China Plain ◽  
North China ◽  
Isotopic Fractionation ◽  
Dicarboxylic Acids ◽  
Photochemical Oxidation ◽  
Photochemical Degradation ◽  
Stable Carbon ◽  
Δ13c Values ◽  
Isotopic Compositions ◽  
Carbon Isotopic

Abstract. Abstract: Molecular distributions and stable carbon isotopic (δ13C values) compositions of dicarboxylic acids and related SOA in PM2.5 aerosols collected on a day/night basis at the summit of Mt. Tai (1534 m  a.s.l.) in the summer of 2016 were analyzed to investigate the sources and photochemical aging process of organic aerosols in the forested highland region of North China Plain. The molecular distributions of dicarboxylic acids and related SOA are characterized by the dominance of oxalic acid (C2), followed by malonic (C3), succinic (C4) and azelaic (C9) acids. The concentration ratios of C2/C4, diacid-C/OC and C2/total diacids are larger in daytime than in nighttime, suggesting that the daytime aerosols are more photochemically aged than those in nighttime due to the higher temperatures and stronger solar radiation. Both ratios of C2/C4 (R2 > 0.5) and C3/C4 (R2 > 0.5) correlated strongly with the ambient temperature, indicating that SOA in the mountaintop atmosphere are mainly derived from the photochemical oxidation of local emissions rather than long-range transport. The mass ratios of C9/C6, C9/Ph, Gly/mGly and the strong linear correlation of major dicarboxylic acids and related SOA with biogenic precursors further suggest that aerosols in this region are mainly originated from biogenic sources (i.e., tree emissions). C2 concentrations correlated well with aerosol pH, indicating that particle acidity favors the organic acid formation. The stable carbon isotopic compositions (δ13C) of the dicarboxylic acids are higher in daytime than in nighttime with the highest value (−16.5 ± 1.9 ‰) found for C2 and the lowest value (−25.2 ± 2.7 ‰) found for C9. An increase in δ13C values of C2 along with increases in C2/Gly and C2/mGly ratios was observed, largely due to the isotopic fractionation during photochemical degradation of the precursors.

scholarly journals High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season

2013 ◽  
Vol 13 (16) ◽  
pp. 8285-8302 ◽  
Author(s):  
K. Kawamura ◽  
E. Tachibana ◽  
K. Okuzawa ◽  
S. G. Aggarwal ◽  
Y. Kanaya ◽  
...  
Keyword(s):  
Wheat Straw ◽  
North China Plain ◽  
North China ◽  
Dicarboxylic Acids ◽  
Agricultural Wastes ◽  
Water Soluble ◽  
The North ◽  
The North China Plain ◽  
Volatile Organic ◽  
Field Burning

Abstract. Aerosol (TSP) samples were collected at the summit of Mount Tai (elevation: 1534 m a.s.l., 36.25° N, 117.10° E) located in the North China Plain using a high-volume air sampler and pre-combusted quartz filters. Sampling was conducted on day/night or 3 h basis in the period from 29 May to 28 June 2006 during the field burning of wheat straw residue and the post-burning season. The filter samples were analyzed for low-molecular-weight dicarboxylic acids, ketoacids and α-dicarbonyls using capillary gas chromatography (GC) and GC-MS employing water extraction and butyl ester derivatization. Molecular distributions of dicarboxylic acids (C2-C11, 220–6070 ng m−3) were characterized by a predominance of oxalic (C2) acid (105–3920 ng m−3) followed by succinic (C4) or malonic (C3) acid. Unsaturated aliphatic diacids, including maleic (M), isomaleic (iM) and fumaric (F) acids, were also detected together with aromatic diacids (phthalic, isophthalic and terephthalic acids). ω-oxocarboxylic acids (C2-C9, 24–610 ng m−3) were detected as the second most abundant compound class with the predominance of glyoxylic acid (11–360 ng m−3), followed by α-ketoacid (pyruvic acid, 3–140 ng m−3) and α-dicarbonyls (glyoxal, 1–230 ng m−3 and methylglyoxal, 2–120 ng m−3). We found that these levels (>6000 ng m−3 for diacids) are several times higher than those reported in Chinese megacities at ground levels. The concentrations of diacids increased from late May to early June, showing a maximum on 7 June, and then significantly decreased during the period 8–11 June, when the wind direction shifted from southerly to northerly. Similar temporal trends were found for ketocarboxylic acids and α-dicarbonyls as well as total carbon (TC) and water-soluble organic carbon (WSOC). The temporal variations of water-soluble organics were interpreted by the direct emission from the field burning of agricultural wastes (wheat straw) in the North China Plain and the subsequent photochemical oxidation of volatile and semi-volatile organic precursors emitted from field burning as well as dark ozonolysis of volatile organic compounds and other organics, accretion reactions and oxidation of nonvolatile organics such as unsaturated fatty acids. This study demonstrates that the field burning of agricultural wastes in early summer strongly influenced the air quality of the free troposphere over the North China Plain.

Quantification of known and unknown terpenoid organosulfates in PM10 using untargeted LC–HRMS/MS: contrasting summertime rural Germany and the North China Plain

2019 ◽  
Vol 16 (5) ◽  
pp. 333 ◽  
Author(s):  
Martin Brüggemann ◽  
Dominik van Pinxteren ◽  
Yuchen Wang ◽  
Jian Zhen Yu ◽  
Hartmut Herrmann
Keyword(s):  
Mass Spectrometry ◽  
Particulate Matter ◽  
North China Plain ◽  
North China ◽  
Organic Aerosols ◽  
Atmospheric Particulate Matter ◽  
Oxidation Products ◽  
The North ◽  
The North China Plain ◽  
Total Concentrations

Environmental contextSecondary organic aerosols account for a major fraction of atmospheric particulate matter, affecting both climate and human health. Organosulfates, abundant compounds in organic aerosols, are difficult to measure because of the lack of authentic standards. Here we quantify terpene-derived organosulfates in atmospheric particulate matter at a rural site in Germany and at the North China Plain using a combined target/non-target high-resolution mass spectrometry approach. AbstractOrganosulfates (OSs) are a ubiquitous class of compounds in atmospheric aerosol particles. However, a detailed quantification of OSs is commonly hampered because of missing authentic standards and the abundance of unknown OSs. Using a combined targeted and untargeted approach of high-resolution liquid chromatography–Orbitrap mass spectrometry (LC–Orbitrap MS), we quantified for the first time the total concentrations of known and unknown monoterpene (MT) and sesquiterpene (SQT) OSs in summertime PM10 particulate matter from field studies in rural Germany (MEL) and the North China Plain (NCP). At each site, we observed more than 50 MT-OSs, 13 of which were detectable at both sites. For both locations, median concentrations of MT-OSs were in the range of 10 to 40ngm−3, to which the 13 common MT-OSs contributed on average >50%. The main contributor to MT-OSs was C9H16O7S (MT-OS 267) with average mass concentrations of 2.23 and 6.38ngm−3 for MEL and NCP respectively. The concentrations of MT-OSs correlated with the concentrations of MT oxidation products only for MEL. For NCP, the low concentrations of MT oxidation products (i.e. typically <1ngm−3) suggested a suppression of carboxylic acid formation under high concentrations of NOx and particulate sulfate. Furthermore, we observed 17 SQT-OSs for the MEL samples, whereas 40 SQT-OSs were detected in the NCP samples. Only five of these SQT-OSs were detectable at both sites. Correspondingly, the total concentrations of SQT-OSs were larger for NCP than for MEL, which suggested large differences in the particle chemistry. In particular, aerosol acidity was found to be a key factor during SQT-OS formation, and was probably not sufficient in the PM10 from MEL.

scholarly journals High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountain aerosols over the North China Plain during wheat burning season

2013 ◽  
Vol 13 (2) ◽  
pp. 3695-3734 ◽  
Author(s):  
K. Kawamura ◽  
E. Tachibana ◽  
K. Okuzawa ◽  
S. G. Aggarwal ◽  
Y. Kanaya ◽  
...  
Keyword(s):  
Wheat Straw ◽  
North China Plain ◽  
North China ◽  
Dicarboxylic Acids ◽  
Agricultural Wastes ◽  
Water Soluble ◽  
Total Carbon ◽  
The North ◽  
The North China Plain ◽  
Field Burning

Abstract. Aerosol (TSP) samples were collected at the summit of Mount Tai (elevation: 1534 m a.s.l., 36.25° N; 117.10° E) located in the North China Plain using a high-volume air sampler and pre-combusted quartz filters. Sampling was conducted on day/night or 3 h basis in the period from 29 May to 28 June 2006 during the field burning of wheat straw residue and the post-burning season. The filter samples were analyzed for low molecular weight dicarboxylic acids, ketoacids and α-dicarbonyls using capillary gas chromatography (GC) and GC-MS employing water extraction and butyl ester derivatization. Dicarboxylic acids (C2–C11, 220–6070 ng m−3) were characterized by a predominance of oxalic (C2) acid (105–3920 ng m−3) followed by succinic (C4) or malonic (C3) acid. Unsaturated aliphatic diacids, including maleic (M), isomaleic (iM) and fumaric (F) acid, were also detected together with aromatic diacids (phthalic, iso-phthalic and tere-phthalic acids). ω-Oxocarboxylic acids (C2–C9, 24–610 ng m−3) were detected as the second most abundant compound class with the predominance of glyoxylic acid (11–360 ng m−3), followed by α-ketoacid (pyruvic acid, 3–140 ng m−3) and α-dicarbonyls (glyoxal, 1–230 ng m−3 and methylglyoxal, 2–120 ng m−3). We found that these levels (> 6000 ng m−3 for diacids) are several times higher than those reported in Chinese megacities at ground levels. The concentrations of diacids increased from late May to early June showing a maximum on 7 June and then significantly decreased during 8–11 June when the wind direction shifted from northeasterly to northerly. Similar temporal trends were found for ketocarboxylic acids and α-dicarbonyls as well as total carbon (TC) and water-soluble organic carbon (WSOC). The temporal variations of water-soluble organics were interpreted by the direct emission from the field burning products of agricultural wastes (wheat straw) in the North China Plain and the subsequent photochemical oxidation of volatile and semi-volatile organic precursors emitted from field burning. This study demonstrates that the field burning of agricultural wastes in early summer strongly influenced the air quality of the free troposphere over the North China Plain.

Sign in / Sign up

Export Citation Format

Share Document