Temporal Trends in Ambient SO₂ at a High Altitude Site in Semi-Arid Western India: Observations versus Chemical Transport Modeling

Timmy Francis

Physical Research Laboratory, Ahmedabad, India.

DOI: 10.4236/jep.2012.37079                

Abstract

Ambient sulphur dioxide (SO₂) measurements have been performed at a high altitude site in the semi arid region of western India, Gurushikhar, Mt. Abu (24.6°N, 72.7°E, 1680 m ASL), during different sampling periods span over Sep-Dec 2009 and Feb-Mar 2010. A global three dimensional chemical transport Model, GEOS-Chem, (v8-03-01) is employed to generate the SO₂ profile for the entire region for the different sampling months which in turn is used to explain the major features in the measured SO₂ spectra via correlating with HYSPLIT generated wind back trajectories. The mean SO₂ concentrations recorded at the sampling site varied for the different sampling periods (4.3 ppbv in Sep-Oct 2009, 3.4 ppbv in Nov 2009, 3.5 ppbv in Dec 2009, 7.7 ppbv in Feb 2010 and 9.2 ppbv in Mar 2010) which were found to be strongly influenced by long range transport from a source region surrounding 30°N, 75°E—the one projected with the highest SO₂ concentration in the GEOS-Chem generated profiles for the region—lying only a few co-ordinates away. A diurnal cycle of SO₂ concentration exists throughout the sampling periods, with the greatest day-night changes observed during Feb and Mar 2010, barely detectable during Sep-Oct 2009, and intermediate values for Nov and Dec 2009 which are systematically studied using the time series PBL height and OH radical values from the GEOS-Chem model. During the sampling period in Nov 2009, a plume transport to the sampling site also was detected when a major fire erupted at an oil depot in Jaipur (26.92°N, 75.82°E), located few co-ordinates away. Separate runs of the model, performed to study the long range transport effects, show a drop in the SO₂ levels over the sampling region in the absence of transport, throughout the year with Jan to Apr seen to be influenced the lowest by long range transport while Jul and Dec influenced the highest.

Keywords

SO₂; GEOS-Chem; HYSPLIT; IOCL Oil Fire; PBL Height; OH Radical

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1]	J. Crawford, J. Olson, D. Davis, et al., “Clouds and Trace Gas Distributions during TRACE-P,” Journal of Geophysical Research, Vol. 108, No. D21, 2003, pp. 8818-8830. doi:10.1029/2002JD003177
[2]	T. Larssen, E. Lydersen, D. Tang, et al., “Acid Rain in China,” Environmental Science & Technology, Vol. 40, No. D2, 2006, pp. 418-425.
[3]	T. Ohara, H. Akimoto, J. Kurokawa, et al., “An Asian Emission Inventory of Anthropogenic Emission Sources for the Period 1980-2020,” Atmospheric Chemistry and Physics Discuss, Vol. 7, 2007, pp. 4419-4444. doi:10.5194/acpd-7-6843-2007
[4]	D. G. Streets, T. C. Bond, G. R. Carmichael, et al., “An Inventory of Gaseous and Primary Aerosol Emissions in Asia in the Year 2000,” Journal of Geophysical Research, Vol. 108, No. D21, 2003, pp. 8809-8831. doi:10.1029/2002JD003093
[5]	D. G. Streets and S. T. Waldhoff, “Present and Future Emissions of Air Pollutants in China: SO2, NOX, and CO,” Atmospheric Environment, Vol. 34, No. 3, 2000, pp. 363-374. doi:10.1016/S1352-2310(99)00167-3
[6]	T. Francis, “Effect of Asian Dust Storms on the Ambient SO2 Concentration over North-East India: A Case Study,” Journal of Environmental Protection, Vol. 2, No. 6, 2011, pp. 778-795. doi:10.4236/jep.2011.26090
[7]	D. C. Thornton, A. R. Bandy, B. W. Blomquist, et al., “Sulfur Dioxide as a Source of Condensation Nuclei in the Upper Troposphere of the Pacific Ocean,” Journal of Geophysical Research, Vol. 101, No. D1, 1996, pp. 1883 -1890. doi:10.1029/95JD02273
[8]	D. C. Thornton, A. R. Bandy, B. W. Blomquist, et al., “Transport of Sulfur Dioxide from the Asian Pacific Rim to the North Pacific Troposphere,” Journal of Geophysical Research, Vol. 102, No. D23, 1997, pp. 28489-28499. doi:10.1029/97JD01818
[9]	C. M. Benkovitz, M. T. Scholtz, J. Pacyna, et al., “Global gridded Inventories of Anthropogenic Emissions of Sulfur and Nitrogen,” Journal of Geophysical Research, Vol. 101, No. D22, 1996, pp. 29239-29253. doi:10.1029/96JD00126
[10]	P. A. Spiro, D. J. Jacob and J. A. Logan, “Global Inventory of Sulfur Emissions with 1? × 1? Resolution,” Journal of Geophysical Research, Vol. 97, No. D5, 1992, pp. 6023-6036. doi:10.1029/91JD03139
[11]	M. O. Andreae, “Ocean-Atmosphere Interactions in the Global Biogeochemical Sulfur Cycle,” Marine Chemistry, Vol. 30, 1990, pp. 1-29. doi:10.1016/0304-4203(90)90059-L
[12]	M. O. Andreae and W. A. Jaeschke, “Exchange of Sulfur between Biosphere and Atmosphere over Temperate and Tropical Regions,” In: R. W. Howarth and J. W. B. Stewart, Eds., Sulfur Cycling in Terrestrial Systems and Wetlands, John Wiley, New York, 1992.
[13]	T. S. Bates, J. D. Cline, R. H. Gammon, et al., “Regional and Seasonal Variations in the Flux of Oceanic Dimethyl Sulfide to the Atmosphere,” Journal of Geophysical Research, Vol. 92, No. C3, 1987, pp. 2930-2938. doi:10.1029/JC092iC03p02930
[14]	C. F. Cullis and M. M. Hirschler, “Atmospheric Sulphur: Natural and Man-Made Sources,” Atmospheric Environment, Vol. 14, No. 11, 1980, pp. 1263-1278.
[15]	J. R. Freney, M. V. Ivanov and H. Rhodhe, “The Sulphur Cycle, in the Major Biogeochemical Cycles and Their Interactions, SCOPE 24,” John Wiley, New York, 1983.
[16]	H. Rodhe and I. Isaksen, “Global Distribution of Sulfur Compounds in the Troposphere Estimated in a Height/Latitude Transport Model,” Journal of Geophysical Research, Vol. 85, No. C12, 1980, pp. 7401-7409. doi:10.1029/JC085iC12p07401
[17]	E. S. Saltzman and D. J. Cooper, “Shipboard Measurements of Atmospheric Dimethyl Sulfide and Hydrogen Sulfide in the Caribbean and Gulf of Mexico,” Journal of Atmospheric Chemistry, Vol. 7, No. 2, 1988, pp. 191-209. doi:10.1007/BF00048046
[18]	O. B. Toon, et al., “The Sulfur Cycle in the Marine Atmosphere,” Journal of Geophysical Research, Vol. 92, No. D1, 1987, pp. 943-963. doi:10.1029/JD092iD01p00943
[19]	L. Gerhardsson, A. Oskarsson and S. Skerfving, “Acid Precipitation—Effects on Trace Elements and Human Health,” The Science of the Total Environment, Vol. 153, No. 3, 1994, pp. 237-245. doi:10.1016/0048-9697(94)90203-8
[20]	D. W. Schindler, “Effects of Acid Rain on Freshwater Ecosystems,” Science, Vol. 239, No. 4836, 1988, pp. 149-157.
[21]	Y. Igarashi, Y. Sawa, K. Yoshioka, et al., “Monitoring the SO2 Concentration at the Summit of Mt. Fuji and a Comparison with Other Trace Gases during Winter,” Journal of Geophysical Research, Vol. 109, No. D17, 2004, Article ID: D17304. doi:10.1029/2003JD004428
[22]	W. T. Luke, “Evaluation of a Commercial Pulsed Fluorescence Detector for the Measurement of Low-Level SO2 Concentrations during the Gas-Phase Sulfur Intercomparison Experiment,” Journal of Geophysical Research, Vol. 102, No. D13, 1997, pp. 16255-16265. doi:10.1029/96JD03347
[23]	M. Luria, J. F. Boatman, J. Harris, et al., “Atmospheric Sulfur Dioxide at Mauna Loa, Hawaii,” Journal of Geophysical Research, Vol. 97, No. D5, 1992, pp. 6011-6022. doi:10.1029/91JD03126
[24]	I. Bey, D. J. Jacob, R. M. Yantosca, et al., “Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation,” Journal of Geophysical Research, Vol. 106, No. D19, 2001, pp. 23073-23095. doi:10.1029/2001JD000807
[25]	R. J. Park, D. J. Jacob, B. D. Field, et al., “Natural and Transboundary Pollution Influences on Sulfate-Nitrate-Ammonium Aerosols in the United States: Implications for Policy,” Journal of Geophysical Research, Vol. 109, No. D15, 2004, Article ID: D15204. doi:10.1029/2003JD004473
[26]	J. Wang, D. J. Jacob and S. T. Martin, “Sensitivity of Sulfate Direct Climate Forcing to the Hysteresis of Particle Phase Transitions,” Journal of Geophysical Research, Vol. 113, No. D11, 2008, Article ID: D11207. doi:10.1029/2007JD009368
[27]	T. Duncan Fairlie, D. J. Jacob and R. J. Park, “The Impact of Transpacific Transport of Mineral Dust in the United States,” Atmospheric Environment, Vol. 41, No. 6, 2007, pp. 1251-1266. doi:10.1016/j.atmosenv.2006.09.048
[28]	D. Chen, Y. Wang, M. B. McElroy, et al., “Regional CO Pollution and Export in China Simulated by the High-Resolution Nested-Grid GEOS-Chem Model,” Atmospheric Chemistry and Physics, Vol. 9, No. 11, 2009, pp. 3825-3839. doi:10.5194/acp-9-3825-2009
[29]	V. Vestreng and H. Klein, “Emission Data Reported to UNECE/EMEP. Quality Assurance 769 and Trend Analysis and Presentation of WebDab,” MSC-W Status Report, Norwegian Meteorological Institute, 2002.
[30]	H. Kuhns, M. Green and V. Etyemezian, “Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study Emissions Inventory,” Desert Research Institute, 2003.
[31]	J. G. J. Olivier and J. J. M. Berdowski, “Global Emissions Sources and Sinks, in the Climate System,” The Netherlands A.A. Balkema Publishers/Swets & Zeitlinger Publishers, 2001.
[32]	D. G. Streets, Q. Zhang, L. Wang, et al., “Revisiting China’s CO Emissions after the Transport and Chemical Evolution over the Pacific (TRACE-P) Mission: Synthesis of Inventories, Atmospheric Modeling, and Observations,” Journal of Geophysical Research, Vol. 111, No. D14, 2006, Article ID: D14306. doi:10.1029/2006JD007118
[33]	R. R. Draxler and G. D. Rolph, “HYSPLIT—HYbrid Single-Particle Lagrangian Integrated Trajectory Model,” 2012. http://www.arl.noaa.gov/ready/hysplit4.html
[34]	G. D. Rolph, “Real-Time Environmental Applications and Display System (READY),” 2003.