Assessment of biogenic secondary organic aerosol in the Himalayas

Article

<< Previous

Next >>

Contents Vol 9(3)

doi:10.1071/EN12002

Environmental problems - Chemical approaches

	Search




	Advanced Search



	Journal Home

	About the Journal

	Editorial Boards

	Contacts



	Content

	Online Early

	Current Issue

	Just Accepted

	All Issues

	Special Issues

	Research Fronts

	Sample Issue



	For Authors

	General Information

	Notice to Authors

	Submit Article

	Open Access



	For Referees

	Referee Guidelines

	Review Article



	For Subscribers

	Subscription Prices

	Customer Service

e-Alerts

Subscribe to our Email Alert or

feeds for the latest journal papers.

Connect with us

Assessment of biogenic secondary organic aerosol in the Himalayas

Elizabeth A. Stone ^A ^C, Tony T. Nguyen ^A, Bidya Banmali Pradhan ^B and Pradeep Man Dangol ^B

^A Department of Chemistry, University of Iowa, Iowa City, IA 52246, USA.
^B International Centre for Integrated Mountain Development, Kathmandu, Nepal.
^C Corresponding author. Email: betsy-stone@uiowa.edu

Environmental Chemistry 9(3) 263-272 http://dx.doi.org/10.1071/EN12002
Submitted: 3 January 2012 Accepted: 10 April 2012 Published: 26 June 2012





	PDF (319 KB) $25



	Export Citation

Print

Environmental context. Secondary organic aerosols derived from biogenic gases are ubiquitous in the atmosphere. We found that biogenic secondary organic aerosol in Nepal accounted for 6 to 23 % of organic carbon. Primary and secondary biogenic sources combined accounted for approximately half of the observed organic aerosol, suggesting that additional aerosol sources or precursors are significant in this region of the Himalayas.

Abstract. Biogenic contributions to secondary organic aerosol (SOA) in the South-East Asian regional haze were assessed by measurement of isoprene, monoterpene and sesquiterpene photooxidation products in fine particles (PM_2.5) at a mid-latitude site in the Himalayas. Organic species were measured in solvent extracts of filter samples using gas chromatography–mass spectrometry (GCMS) and chemical derivatisation; this analysis was used to quantify molecular markers for primary aerosol sources – including motor vehicles, biomass burning and detritus – and SOA tracers. Authentic standards of most SOA products were not commercially available at the time of this study, so surrogate standards were used for semiquantitation. Using an empirical approach to uncertainty estimation based on homologous series of atmospherically relevant model compounds, analytical uncertainties ranged from 32 % for SOA tracers with structurally similar surrogates to more than 100 % for tracers with a poorly matched surrogate. Biogenic SOA contributions to PM_2.5 organic carbon content in the 2005 monsoon and post-monsoon season ranged from 2–19 % for isoprene, 1–5 % for monoterpenes and 1–4 % for sesquiterpenes. High concentrations of isoprene derivatives in aerosol, particularly in the late summer months, point to biogenic SOA as a significant source of organic carbon in the Himalayan region.

References

[1] K. L. Denman, G. Brasseur, A. Chidthaisong, P. Ciais, P. M. Cox, R. E. Dickinson, D. Hauglustaine, C. Heinze, E. Holland, D. Jacob, U. Lohmann, S. Ramachandran, P. L. da Silva Dias, S. C. Wofsey, X. Zhang, Chapter 7: Couplings Between Changes in the Climate System and Biogeochemistry, in Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change (Eds S. Solomon, D. Qin, M. Manning, Z. Chen, M. Marquis, K. B. Averyt, M. Tignor, H. L. Miller) 2007, pp. 555–565 (Cambridge University Press: Cambridge, UK, and New York).

[2] P. Saxena, L. M. Hildemann, Water-soluble organics in atmospheric particles: a critical review of the literature and application of thermodynamics to identify candidate compounds J. Atmos. Chem. 1996, 24, 57.
| CrossRef | CAS |

[3] S. N. Pandis, R. H. Harley, G. R. Cass, J. H. Seinfeld, Secondary organic aerosol formation and transport. Atmos. Environ. 1992, 26A, 2269.
| CAS |

[4] T. Hoffmann, J. R. Odum, F. Bowman, D. Collins, D. Klockow, R. C. Flagan, J. H. Seinfeld, Formation of organic aerosols from the oxidation of biogenic hydrocarbons. J. Atmos. Chem. 1997, 26, 189.
| CrossRef | CAS |

[5] E. O. Edney, T. E. Kleindienst, M. Jaoui, M. Lewandowski, J. H. Offenberg, W. Wang, M. Claeys, Formation of 2-methyl tetrols and 2-methylglyceric acid in secondary organic aerosol from laboratory irradiated isoprene/NO_X/SO₂/air mixtures and their detection in ambient PM_2.5 samples collected in the eastern United States. Atmos. Environ. 2005, 39, 5281.
| CrossRef | CAS |

[6] R. Atkinson, J. Arey, Gas-phase tropospheric chemistry of biogenic volatile organic compounds: a review. Atmos. Environ. 2003, 37, 197.
| CrossRef |

[7] J. Kesselmeier, M. Staudt, Biogenic volatile organic compounds (VOC): an overview on emission, physiology and ecology. J. Atmos. Chem. 1999, 33, 23.
| CrossRef | CAS |

[8] A. Guenther, C. N. Hewitt, D. Erickson, R. Fall, C. Geron, T. Graedel, P. Harley, L. Klinger, M. Lerdau, W. A. McKay, T. Pierce, B. Scholes, R. Steinbrecher, R. Tallamraju, J. Taylor, P. Zimmerman, A global-model of natural volatile organic-compound emissions. J. Geophys. Res. – Atmos. 1995, 100, 8873.
| CrossRef | CAS |

[9] M. Jaoui, M. Lewandowski, T. E. Kleindienst, J. H. Offenberg, E. O. Edney, β-caryophyllinic acid: an atmospheric tracer for β-caryophyllene secondary organic aerosol. Geophys. Res. Lett. 2007, 34, L05816.
| CrossRef |

[10] M. Jaoui, T. E. Kleindienst, M. Lewandowski, J. H. Offenberg, E. O. Edney, Identification and quantification of aerosol polar oxygenated compounds bearing carboxylic or hydroxyl groups. 2. Organic tracer compounds from monoterpenes. Environ. Sci. Technol. 2005, 39, 5661.
| CrossRef | CAS |

[11] T. E. Kleindienst, T. S. Conver, C. D. McIver, E. O. Edney, Determination of secondary organic aerosol products from the photooxidation of toluene and their implications in ambient PM_2.5. J. Atmos. Chem. 2004, 47, 79.
| CrossRef | CAS |

[12] R. Szmigielski, J. D. Surratt, Y. Gomez-Gonzalez, P. Van der Veken, I. Kourtchev, R. Vermeylen, F. Blockhuys, M. Jaoui, T. E. Kleindienst, M. Lewandowski, J. H. Offenberg, E. O. Edney, J. H. Seinfeld, W. Maenhaut, M. Claeys, 3-methyl-1,2,3-butanetricarboxylic acid: an atmospheric tracer for terpene secondary organic aerosol. Geophys. Res. Lett. 2007, 34, L24811.
| CrossRef |

[13] T. E. Kleindienst, M. Jaoui, M. Lewandowski, J. H. Offenberg, C. W. Lewis, P. V. Bhave, E. O. Edney, Estimates of the contributions of biogenic and anthropogenic hydrocarbons to secondary organic aerosol at a southeastern US location. Atmos. Environ. 2007, 41, 8288.
| CrossRef | CAS |

[14] J. D. Surratt, J. H. Kroll, T. E. Kleindienst, E. O. Edney, M. Claeys, A. Sorooshian, N. L. Ng, J. H. Offenberg, M. Lewandowski, M. Jaoui, R. C. Flagan, J. H. Seinfeld, Evidence for organosulfates in secondary organic aerosol. Environ. Sci. Technol. 2007, 41, 517.
| CrossRef | CAS |

[15] J. J. Schauer, W. F. Rogge, L. M. Hildemann, M. A. Mazurek, G. R. Cass, Source apportionment of airborne particulate matter using organic compounds as tracers. Atmos. Environ. 1996, 30, 3837.
| CrossRef | CAS |

[16] M. Lewandowski, M. Jaoui, J. H. Offenberg, E. O. Edney, R. J. Sheesley, J. J. Schauer, Primary and secondary contributions to ambient PM in the Midwestern United States. Environ. Sci. Technol. 2008, 42, 3303.
| CrossRef | CAS |

[17] E. A. Stone, C. J. Hedman, J. B. Zhou, M. Mieritz, J. J. Schauer, Insights into the nature of secondary organic aerosol in Mexico City during the MILAGRO experiment 2006. Atmos. Environ. 2010, 44, 312.
| CrossRef | CAS |

[18] E. A. Stone, J. B. Zhou, D. C. Snyder, A. P. Rutter, M. Mieritz, J. J. Schauer, A comparison of summertime secondary organic aerosol source contributions at contrasting urban locations. Environ. Sci. Technol. 2009, 43, 3448.
| CrossRef | CAS |

[19] D. Hu, Q. Bian, T. W. Y. Li, A. K. H. Lau, J. Z. Yu, Contributions of isoprene, monoterpenes, β-caryophyllene, and toluene to secondary organic aerosols in Hong Kong during the summer of 2006. J. Geophys. Res. – Atmos. 2008, 113, D22206.
| CrossRef |

[20] X. A. Ding, X. M. Wang, M. Zheng, The influence of temperature and aerosol acidity on biogenic secondary organic aerosol tracers: observations at a rural site in the central Pearl River Delta region, South China. Atmos. Environ. 2011, 45, 1303.
| CrossRef | CAS |

[21] A. L. Clements, J. H. Seinfeld, Detection and quantification of 2-methyltetrols in ambient aerosol in the southeastern United States. Atmos. Environ. 2007, 41, 1825.
| CrossRef | CAS |

[22] I. Kourtchev, S. Hellebust, J. M. Bell, I. P. O'Connor, R. M. Healy, A. Allanic, D. Healy, J. C. Wenger, J. R. Sodeau, The use of polar organic compounds to estimate the contribution of domestic solid fuel combustion and biogenic sources to ambient levels of organic carbon and PM_2.5 in Cork Harbour, Ireland. Sci. Total Environ. 2011, 409, 2143.
| CrossRef | CAS |

[23] I. Kourtchev, T. Ruuskanen, W. Maenhaut, M. Kulmala, M. Claeys, Observation of 2-methyltetrols and related photo-oxidation products of isoprene in boreal forest aerosols from Hyytiala, Finland. Atmos. Chem. Phys. 2005, 5, 2761.
| CrossRef | CAS |

[24] M. Claeys, I. Kourtchev, V. Pashynska, G. Vas, R. Vermeylen, W. Wang, J. Cafmeyer, X. Chi, P. Artaxo, M. O. Andreae, W. Maenhaut, Polar organic marker compounds in atmospheric aerosols during the LBA-SMOCC 2002 biomass burning experiment in Rondonia, Brazil: sources and source processes, time series, diel variations and size distributions. Atmos. Chem. Phys. 2010, 10, 9319.
| CrossRef | CAS |

[25] X. Xia, P. K. Hopke, Seasonal variation of 2-methyltetrols in ambient air samples. Environ. Sci. Technol. 2006, 40, 6934.
| CrossRef | CAS |

[26] V. Ramanathan, F. Li, M. V. Ramana, P. S. Praveen, D. Kim, C. E. Corrigan, H. Nguyen, E. A. Stone, J. J. Schauer, G. R. Carmichael, B. Adhikary, S. C. Yoon, Atmospheric brown clouds: hemispherical and regional variations in long-range transport, absorption, and radiative forcing. J. Geophys. Res. – Atmos. 2007, 112, D22S21.
| CrossRef |

[27] E. A. Stone, J. J. Schauer, B. B. Pradhan, P. M. Dangol, G. Habib, C. Venkataraman, V. Ramanathan, Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas. J. Geophys. Res. – Atmos. 2010, 115, D06301.
| CrossRef |

[28] P. M. Fine, B. Chakrabarti, M. Krudysz, J. J. Schauer, C. Sioutas, Diurnal variations of individual organic compound constituents of ultrafine and accumulation mode particulate matter in the Los Angeles basin. Environ. Sci. Technol. 2004, 38, 1296.
| CrossRef | CAS |

[29] R. B. Bhuju, P. R. Shakya, T. B. Basnet, S. Srhrestha, Nepal Biodiversity Resource Book 2007 (International Center for Integrated Mountain Development: Nepal).

[30] J. J. Schauer, B. T. Mader, J. T. Deminter, G. Heidemann, M. S. Bae, J. H. Seinfeld, R. C. Flagan, R. A. Cary, D. Smith, B. J. Huebert, T. Bertram, S. Howell, J. T. Kline, P. Quinn, T. Bates, B. Turpin, H. J. Lim, J. Z. Yu, H. Yang, M. D. Keywood, ACE-Asia intercomparison of a thermal-optical method for the determination of particle-phase organic and elemental carbon. Environ. Sci. Technol. 2003, 37, 993.
| CrossRef | CAS |

[31] C. G. Nolte, J. J. Schauer, G. R. Cass, B. R. T. Simoneit, Trimethylsilyl derivatives of organic compounds in source samples and in atmospheric fine particulate matter. Environ. Sci. Technol. 2002, 36, 4273.
| CrossRef | CAS |

[32] M. Claeys, B. Graham, G. Vas, W. Wang, R. Vermeylen, V. Pashynska, J. Cafmeyer, P. Guyon, M. O. Andreae, P. Artaxo, W. Maenhaut, Formation of secondary organic aerosols through photooxidation of isoprene. Science 2004, 303, 1173.
| CrossRef | CAS |

[33] B. J. Turpin, H. J. Lim, Species contributions to PM_2.5 mass concentrations: revisiting common assumptions for estimating organic mass. Aerosol Sci. Technol. 2001, 35, 602.
| CrossRef | CAS |

[34] B. Adhikary, G. R. Carmichael, S. Kulkarni, C. Wei, Y. Tang, A. D'Allura, M. Mena-Carrasco, D. G. Streets, Q. Zhang, R. B. Pierce, J. A. Al-Saadi, L. K. Emmons, G. G. Pfister, M. A. Avery, J. D. Barrick, D. R. Blake, W. H. Brune, R. C. Cohen, J. E. Dibb, A. Fried, B. G. Heikes, L. G. Huey, D. W. O'Sullivan, G. W. Sachse, R. E. Shetter, H. B. Singh, T. L. Campos, C. A. Cantrell, F. M. Flocke, E. J. Dunlea, J. L. Jimenez, A. J. Weinheimer, J. D. Crounse, P. O. Wennberg, J. J. Schauer, E. A. Stone, D. A. Jaffe, D. R. Reidmiller, A regional scale modeling analysis of aerosol and trace gas distributions over the eastern Pacific during the INTEX-B field campaign. Atmos. Chem. Phys. 2010, 10, 2091.
| CrossRef | CAS |

[35] A. Chatterjee, A. Adak, A. K. Singh, M. K. Srivastava, S. K. Ghosh, S. Tiwari, P. C. S. Devara, S. Raha, Aerosol chemistry over a high altitude station at northeastern Himalayas, India. PLoS ONE 2010, 5, e11122.
| CrossRef |

[36] B. Adhikary, G. R. Carmichael, Y. Tang, L. R. Leung, Y. Qian, J. J. Schauer, E. A. Stone, V. Ramanathan, M. V. Ramana, Characterization of the seasonal cycle of south Asian aerosols: a regional-scale modeling analysis. J. Geophys. Res. – Atmos. 2007, 112, D22S22.
| CrossRef |

[37] P. Bonasoni, P. Laj, F. Angelini, J. Arduini, U. Bonafe, F. Calzolari, P. Cristofanelli, S. Decesari, M. C. Facchini, S. Fuzzi, G. P. Gobbi, M. Maione, A. Marinoni, A. Petzold, F. Roccato, J. C. Roger, K. Sellegri, M. Sprenger, H. Venzac, G. P. Verza, P. Villani, E. Vuillermoz, The ABC-Pyramid Atmospheric Research Observatory in Himalaya for aerosol, ozone and halocarbon measurements. Sci. Total Environ. 2008, 391, 252.
| CrossRef | CAS |

[38] B. R. T. Simoneit, J. J. Schauer, C. G. Nolte, D. R. Oros, V. O. Elias, M. P. Fraser, W. F. Rogge, G. R. Cass, Levoglucosan, a tracer for cellulose in biomass burning and atmospheric particles. Atmos. Environ. 1999, 33, 173.
| CrossRef | CAS |

[39] C. Venkataraman, G. Habib, A. Eiguren-Fernandez, A. H. Miguel, S. K. Friedlander, Residential biofuels in south Asia: carbonaceous aerosol emissions and climate impacts. Science 2005, 307, 1454.
| CrossRef | CAS |

[40] S. Lee, K. Baumann, J. J. Schauer, R. J. Sheesley, L. P. Naeher, S. Meinardi, D. R. Blake, E. S. Edgerton, A. G. Russell, M. Clements, Gaseous and particulate emissions from prescribed burning in Georgia. Environ. Sci. Technol. 2005, 39, 9049.
| CrossRef | CAS |

[41] Y. X. Zhang, M. Shao, Y. H. Zhang, L. M. Zeng, L. Y. He, B. Zhu, Y. J. Wei, X. L. Zhu, Source profiles of particulate organic matters emitted from cereal straw burnings. J. Environ. Sci. 2007, 19, 167.
| CrossRef | CAS |

[42] D. R. Oros, B. R. T. Simoneit, Identification and emission rates of molecular tracers in coal smoke particulate matter. Fuel 2000, 79, 515.
| CrossRef | CAS |

[43] Y. X. Zhang, J. J. Schauer, Y. H. Zhang, L. M. Zeng, Y. J. Wei, Y. Liu, M. Shao, Characteristics of particulate carbon emissions from real-world Chinese coal combustion. Environ. Sci. Technol. 2008, 42, 5068.
| CrossRef | CAS |

[44] G. C. Lough, C. C. Christenson, J. J. Schauer, J. Tortorelli, E. Bean, D. Lawson, N. N. Clark, P. A. Gabele, Development of molecular marker source profiles for emissions from on-road gasoline and diesel vehicle fleets. J. Air Waste Manage. Assoc. 2007, 57, 1190.
| CrossRef | CAS |

[45] B. R. T. Simoneit, A review of current applications of mass spectrometry for biomarker/molecular tracer elucidations. Mass Spectrom. Rev. 2005, 24, 719.
| CrossRef | CAS |

[46] B. R. T. Simoneit, M. Kobayashi, M. Mochida, K. Kawamura, M. Lee, H. J. Lim, B. J. Turpin, Y. Komazaki, Composition and major sources of organic compounds of aerosol particulate matter sampled during the ACE-Asia campaign. J. Geophys. Res. – Atmos. 2004, 109, D19S10.
| CrossRef |

[47] T. D. Sharkey, A. E. Wiberley, A. R. Donohue, Isoprene emission from plants: why and how. Ann. Bot. 2008, 101, 5.
| CAS |

[48] P. Q. Fu, K. Kawamura, J. Chen, L. A. Barrie, Isoprene, monoterpene, and sesquiterpene oxidation products in the high arctic aerosols during late winter to early summer. Environ. Sci. Technol. 2009, 43, 4022.
| CrossRef | CAS |

[49] N. J. D. González, A. K. Borg-Karlson, J. P. Redeby, B. Nozière, R. Krejci, Y. X. Pei, J. Dommen, A. S. H. Prévôt, New method for resolving the enantiomeric composition of 2-methyltetrols in atmospheric organic aerosols. J. Chromatogr. A 2011, 1218, 9288.
| CrossRef |

[50] M. Claeys, R. Szmigielski, I. Kourtchev, P. Van der Veken, R. Vermeylen, W. Maenhaut, M. Jaoui, T. E. Kleindienst, M. Lewandowski, J. H. Offenberg, E. O. Edney, Hydroxydicarboxylic acids: markers for secondary organic aerosol from the photooxidation of α-pinene. Environ. Sci. Technol. 2007, 41, 1628.
| CrossRef | CAS |

[51] Y. B. Lim, P. J. Ziemann, Products and mechanism of secondary organic aerosol formation from reactions of n-alkanes with OH radicals in the presence of NO_x. Environ. Sci. Technol. 2005, 39, 9229.
| CrossRef | CAS |

[52] T. E. Kleindienst, E. O. Edney, M. Lewandowski, J. H. Offenberg, M. Jaoui, Secondary organic carbon and aerosol yields from the irradiations of isoprene and α-pinene in the presence of NO_x and SO₂. Environ. Sci. Technol. 2006, 40, 3807.
| CrossRef | CAS |

[53] M. Jaoui, S. Leungsakul, R. M. Kamens, Gas and particle products distribution from the reaction of β-caryophyllene with ozone. J. Atmos. Chem. 2003, 45, 261.
| CrossRef | CAS |

[54] K. M. Shakya, L. D. Ziemba, R. J. Griffin, Characteristics and sources of carbonaceous, ionic, and isotopic species of wintertime atmospheric aerosols in Kathmandu Valley, Nepal. Aerosol Air. Qual. Res. 2010, 10, 219.
| CAS |

[55] X. Ding, X.-M. Wang, B. Gao, X.-X. Fu, Q.-F. He, X.-Y. Zhao, J.-Z. Yu, M. Zheng, Tracer-based estimation of secondary organic carbon in the Pearl River Delta, south China. J. Geophys. Res. – Atmos. 2012, 117, D05313.
| CrossRef |

Subscriber Login

	Username: Password:

Legal & Privacy | Contact Us | Help