To better understand the origins of aerosol nitrogen, we measured concentrations of total nitrogen (TN) and its isotope ratios (δ15N) in tropical Indian aerosols (PM10) collected from Chennai (13.04°N; 80.17°E) on day- and night-time basis in winter and summer 2007. We found high δ15N values (+15.7 to +31.2‰) of aerosol N (0.3-3.8 μg m-3), in which NH4+ is the major species (78%) with lesser contribution from NO3- (6%). Based on the comparison of δ15N in Chennai aerosols with those reported for atmospheric aerosols from mid-latitudes and for the particles emitted from point sources (including a laboratory study), as well as the δ15N ratios of cow-dung samples (this study), we found that the atmospheric aerosol N in Chennai has two major sources; animal excreta and bio-fuel/biomass burning from South and Southeast Asia. We demonstrate that a gas-to-particle conversion of NH3 to NH4HSO4 and (NH4)2SO4 and the subsequent exchange reaction between NH3 and NH4+ are responsible for the isotopic enrichment of 15N in aerosol nitrogen. © 2010 Elsevier Ltd.

Thiyagarajan R. Swaminathan

COW-DUNG SAMPLES

NITROGEN ISOTOPE RATIO

NITROGEN ISOTOPE RATIOS

SOURCE OF AEROSOL NITROGEN

South Asia

Atmospheric thermodynamics

Isotopes

nitrogen

Tropics

Atmospheric aerosols

Ammonia

ammonium sulfate

Biofuel

LEVOGLUCOSAN

aerosol

biomass burning

Concentration (composition)

ISOTOPIC RATIO

Manure

Nitrate

nitrogen isotope

Point source

Seasonal variation

TROPICAL ENVIRONMENT

article

Biomass

controlled study

FECES

India

LABORATORY

NIGHT

Particulate Matter

priority journal

SOUTHEAST ASIA

summer

winter

Asia

Animalia

Fulltext

IIT Madras is a public technical and research university located in Chennai, Tamil Nadu. Founded in 1959, it is recognised as an Institute of National Importance.

IIT Madras has been ranked as the top engineering institute in India for four years in a row by the National Institutional Ranking Framework of the MHRD

It currently offers undergraduate, postgraduate and research degrees across 16 disciplines in Engineering, Sciences, Humanities and Management. About 596 faculty belonging to science and engineering departments and centres of the Institute are engaged in teaching, research and industrial consultancy.

IIT Madras

Atmospheric Environment

To better understand the photochemical production and diurnal distributions of organic and inorganic aerosols in the tropical coastal Indian atmosphere, the aerosol (TSP) samples were collected every 3h during 30-31 January, 14-15 February and 28-29 May 2007 from Chennai and studied for total carbon (TC) and nitrogen (TN) and their stable isotope ratios (δ13CTC and δ15NTN), carbonaceous components, inorganic ions, diacids, ketoacids and α-dicarbonyls. Time-resolved distributions of bulk parameters, inorganic ions, and diacids and related compounds, except for few species, did not show any clear diurnal trend but showed peaks at 6-9h during all the study periods, except for the peak at 15-18h on 28 May. SO42-, C2-C6 diacids, ketoacids and α-dicarbonyls in February and on 29 May showed a diurnal trend. δ13CTC and δ15NTN stayed relatively constant during the study periods but showed 13C depletion (in January) and 15N enrichment when TC and TN peaked. Based on these results together with air mass trajectories, we found that the diurnal distributions of Chennai aerosols are mainly influenced by land/sea breeze and the aged (photochemically processed) air masses, although in situ photochemical production and nighttime chemistry of secondary aerosol species, particularly C2-C4 diacids and SO42-, are significant. The characteristics of seasonal variations of carbonaceous components, and diacids and related compounds and comparisons of δ13CTC and δ15NTN of Chennai aerosols with the isotopic signatures of the point sources inferred that biofuel/biomass burning in South and Southeast Asia are the major sources of aerosols (TSP). © 2014 Elsevier B.V.

Atmospheric Research

Time-resolved distributions of bulk parameters, diacids, ketoacids and α-dicarbonyls and stable carbon and nitrogen isotope ratios of TC and TN in tropical Indian aerosols: Influence of land/sea breeze and secondary processes

To better understand the sources of PM10 samples in Mumbai, India, aerosol chemical composition, i.e., total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4 ‰, also suggests that biofuel/biomass burning is a predominate source in both the summer and winter seasons. Aerosol mass concentrations of major species increased 3-4 times in winter compared to summer, indicating enhanced emission from these sources in the winter season. Photochemical production tracers, C2 diacid and nssSO42-, do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for daytime (0.37 ± 0.06 (0.28 ± 0.04)) and nighttime (0.38 ± 0.07 (0.28 ± 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant and the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r 2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from -27.0 to -25.4‰, with slightly lower average (-26.5 ± 0.3 ‰) in summer than in winter (-25.9 ± 0.3 ‰). Positive correlation between WSOC/TC ratios and δ13C values suggested that the relative increment in 13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests that in winter, the tropical aerosols are more aged due to longer residence time in the atmosphere than in summer aerosols. However, these conclusions are based on the analysis of a limited number of samples (n = 25) and more information on this topic may be needed from other similar coastal sites in future. © Author(s) 2013.

Atmospheric Chemistry and Physics

Organic and inorganic markers and stable C-, N-isotopic compositions of tropical coastal aerosols from megacity Mumbai: Sources of organic aerosols and atmospheric processing

Organic molecular composition of PM10 samples, collected at Chennai in tropical India, was studied using capillary gas chromatography/mass spectrometry. Fourteen organic compound classes were detected in the aerosols, including aliphatic lipids, sugar compounds, lignin products, terpenoid biomarkers, sterols, aromatic acids, hydroxy-/polyacids, phthalate esters, hopanes, Polycyclic Aromatic Hydrocarbons (PAHs), and photooxidation products from biogenic Volatile Organic Compounds (VOCs). At daytime, phthalate esters were found to be the most abundant compound class; however, at nighttime, fatty acids were the dominant one. Di-(2-ethylhexyl) phthalate, C16 fatty acid, and levoglucosan were identified as the most abundant single compounds. The nighttime maxima of most organics in the aerosols indicate a land/sea breeze effect in tropical India, although some other factors such as local emissions and long-range transport may also influence the composition of organic aerosols. However, biogenic VOC oxidation products (e.g., 2-methyltetrols, pinic acid, 3-hydroxyglutaric acid and β-caryophyllinic acid) showed diurnal patterns with daytime maxima. Interestingly, terephthalic acid was maximized at nighttime, which is different from those of phthalic and isophthalic acids. A positive relation was found between 1,3,5-triphenylbenzene (a tracer for plastic burning) and terephthalic acid, suggesting that the field burningof municipal solid wastes including plastics is a significant source of terephthalic acid. Organic compounds were further categorized into several groups to clarify their sources. Fossil fuel combustion (24-43%) was recognized as the most significant source for the total identified compounds, followed by plastic emission (16-33%), secondary oxidation (8.6- 23%), and microbial/marine sources (7.2-17%). In contrast, the contributions of terrestrial plant waxes (5.9-11%) and biomass burning (4.2-6.4%) were relatively small. This study demonstrates that, in addition to fossil fuel combustion and biomass burning, the open-burning of plastics in urban area also contributes to the organic aerosols in South Asia. © 2010 Author(s).

Molecular characterization of urban organic aerosol in tropical India: Contributions of primary emissions and secondary photooxidation

Tropical aerosol (PM<inf>10</inf>) samples (n = 49) collected from southeast coast of India were studied for water-soluble dicarboxylic acids (C<inf>2</inf>-C<inf>12</inf>), ketocarboxylic acids (C<inf>2</inf>-C <inf>9</inf>), and -dicarbonyls (glyoxal and methylglyoxal), together with analyses of total carbon (TC) and water-soluble organic carbon (WSOC). Their distributions were characterized by a predominance of oxalic acid followed by terephthalic (t-Ph), malonic, and succinic acids. Total concentrations of diacids (227-1030 ng m-3), ketoacids (16-105 ng m-3), and dicarbonyls (4-23 ng m-3) are comparative to those from other Asian megacities such as Tokyo and Hong Kong. t-Ph acid was found as the second most abundant diacid in the Chennai aerosols. This feature has not been reported previously in atmospheric aerosols. t-Ph acid is most likely derived from the field burning of plastics. Water-soluble diacids were found to contribute 0.4%-3% of TC and 4%-11% of WSOC. Based on molecular distributions and backward air mass trajectories, we found that diacids and related compounds in coastal South Indian aerosols are influenced by South Asian and Indian Ocean monsoons. Organic aerosols are also suggested to be significantly transported long distances from North India and the Middle East in early winter and from Southeast Asia in late winter, but some originate from photochemical reactions over the Bay of Bengal. In contrast, the Arabian Sea, Indian Ocean, and South Indian continent are suggested as major source regions in summer. We also found daytime maxima of most diacids, except for C<inf>9</inf> and t-Ph acids, which showed nighttime maxima in summer. Emissions from marine and terrestrial plants, combined with land/sea breezes and in situ photochemical oxidation, are suggested especially in summer as an important factor that controls the composition of water-soluble organic aerosols over the southeast coast of India. Regional emissions from anthropogenic sources are also important in megacity Chennai, but their influence is weakened due to the dispersion caused by dynamic land/sea breeze on the coast. Copyright 2010 by the American Geophysical Union.

Journal of Geophysical Research Atmospheres

Water-soluble organic carbon, dicarboxylic acids, ketoacids, and α-dicarbonyls in the tropical Indian aerosols

Journal of Geophysical Research

Seasonal variation of the concentrations of nitrogenous species and their nitrogen isotopic ratios in aerosols at Gosan, Jeju Island: Implications for atmospheric processing and source changes of aerosols

Nature Geoscience

Global ammonia distribution derived from infrared satellite observations

Science

Transformation of the Nitrogen Cycle: Recent Trends, Questions, and Potential Solutions

Elevated nitrogen isotope ratios of tropical Indian aerosols from Chennai: Implication for the origins of aerosol nitrogen in South and Southeast Asia

Journal	Atmospheric Environment
ISSN	13522310
Open Access	Yes