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 JEP  Vol.8 No.10 , September 2017
SO2 Oxidation Efficiency Patterns during an Episode of Plume Transport over Northeast India: Implications to an OH Minimum
Abstract: Systematic monitoring of the fluctuations in atmospheric SO2 oxidation efficiency—measured as a molar ratio of SO42- to total SOx (SOx=SO2+SO42-), referred as S-ratio—have been performed during a major long range plume transport to northeast India (Shillong: 25.67°N, 91.91°E, 1064 m ASL) in March 2009. Anomalously low S-ratios (median, 0.03) were observed during the episode—associated with a cyclonic circulation—and the SO42- and SO2 exhibited unusual features in the ‘relative phase’ of their peaks. During initial days, when SO2 levels were dictated by the long range influx, the SO42- and SO2 variabilities were in anti-phase—for the differing mobility/loss mechanisms. When SO2 levels were governed by the boundary layer diurnality in the latter days, the anti-phase is explained by a ‘depleted OH level’—major portion being consumed in the initial period by the elevated SO2 and other pollutants. Simulations with a global 3D chemical transport model, GEOS-Chem (v8-03-01), also indicated ‘suppressed oxidation conditions’—with characteristic low S-ratios and poor phase agreements. The modelled OH decreased steadily from the initial days, and OH normalized to SO2—referred as OHspecific—was consistently low during the ‘suppressed S-ratio period’. Further, the geographical distribution of modelled OH showed a pronounced minimum over the region surrounding (20°N, 95°E) spanning parts of northeast India and the adjacent regions to the southeast of it—prevalent throughout the year, though the magnitude and the area of influence have a seasonality to it—with significant implications for reducing the oxidizing power of the regional atmosphere. A second set of measurements during January 2010—when prominent long range transports were absent—exhibited no anomalies, and the S-ratios were well within the acceptable limits (median, 0.32). This work highlights the GEOS-Chem model skill in simulating/detecting the ‘transient fluctuations’ in the oxidation efficiency, down to a regional scale.
Cite this paper: Francis, T. , Kundu, S. , Rengarajan, R. and Borgohain, A. (2017) SO2 Oxidation Efficiency Patterns during an Episode of Plume Transport over Northeast India: Implications to an OH Minimum. Journal of Environmental Protection, 8, 1119-1143. doi: 10.4236/jep.2017.810071.
References

[1]   Levy, H. (1971) Normal Atmosphere: Large Radical and Formaldehyde Concentrations Predicted. Science, 173, 141-143.
https://doi.org/10.1126/science.173.3992.141

[2]   Lelieveld, J., Peters, W., Dentener, F.J. and Krol, M.C. (2002) Stability of Tropospheric Hydroxyl Chemistry. Journal of Geophysical Research, 107, 4715.
https://doi.org/10.1029/2002JD002272

[3]   McConnell, J.C., McElroy, M.B. and Wofsy, S.C. (1971) Natural Sources of Atmospheric CO. Nature, 233, 187-188.
https://doi.org/10.1038/233187a0

[4]   Crutzen, P.J. (1973) A Discussion of the Chemistry of Some Minor Constituents in the Stratosphere and Troposphere. Pure and Applied Geophysics, 106-108, 1385-1399.
https://doi.org/10.1007/BF00881092

[5]   Chameides, W. and Walker, J.C.G. (1973) A Photochemical Theory of Tropospheric Ozone. Journal of Geophysical Research, 78, 8751-8760.
https://doi.org/10.1029/JC078i036p08751

[6]   Francis, T. (2011) Effect of Asian Dust Storms on the Ambient SO2 Concentration over North-East India: A Case Study. Journal of Environmental Protection, 2, 778-795.
https://doi.org/10.4236/jep.2011.26090

[7]   Kaneyasu, N., Ohta, S. and Murao, N. (1995) Seasonal Variation in the Chemical Composition of Atmospheric Aerosols and Gaseous Species in Sapporo, Japan. Atmospheric Environment, 29, 1559-1568.
https://doi.org/10.1016/1352-2310(94)00356-P

[8]   Miyakawa, T., Takegawa, N. and Kondo, Y. (2007) Removal of Sulfur Dioxide and Formation of Sulfate Aerosol in Tokyo. Journal of Geophysical Research, 112, D13209.
https://doi.org/10.1029/2006JD007896

[9]   Francis, T., Sarin, M.M. and Rengarajan, R. (2016) Atmospheric SO2 Oxidation Efficiency over a Semi-Arid Region: Seasonal Patterns from Observations and GEOS-Chem Model. Atmospheric Environment, 125, 383-395.
https://doi.org/10.1016/j.atmosenv.2015.09.021

[10]   Rajput, P., Sarin, M. and Kundu, S.S. (2013) Atmospheric Particulate Matter (PM2.5), EC, OC, {WSOC} and {PAHs} from NE-Himalaya: Abundances and Chemical Characteristics. Atmospheric Pollution Research, 4, 214-221.
https://doi.org/10.5094/APR.2013.022

[11]   Igarashi, Y., Sawa, Y., Yoshioka, K., Matsueda, H., Fujii, K. and Dokiya, Y. (2004) Monitoring the SO2 Concentration at the Summit of Mt. Fuji and a Comparison with Other Trace Gases during Winter. Journal of Geophysical Research, 109, D17304.
https://doi.org/10.1029/2003JD004428

[12]   Luke, W.T. (1997) 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, 102, 16255-16265.
https://doi.org/10.1029/96JD03347

[13]   Luria, M., Boatman, J.F., Harris, J., Ray, J., Straube, T., Chin, J., Gunter, R.L., Herbert, G., Gerlach, T.M. and Van Valin, C.C. (1992) Atmospheric Sulfur Dioxide at Mauna Loa, Hawaii. Journal of Geophysical Research, 97, 6011-6022.
https://doi.org/10.1029/91JD03126

[14]   Rastogi, N. and Sarin, M.M. (2005) Long-Term Characterization of Ionic Species in Aerosols from Urban and High-Altitude Sites in Western India: Role of Mineral Dust and Anthropogenic Sources. Atmospheric Environment, 39, 5541-5554.
https://doi.org/10.1016/j.atmosenv.2005.06.011

[15]   Rengarajan, R. and Sarin, M.M. (2004) Atmospheric Deposition Fluxes of 7Be, 210Pb and Chemical Species to the Arabian Sea and Bay Bengal. Indian Journal of Marine Sciences, 33, 56-64.

[16]   Bey, I., Jacob, D.J., Yantosca, R.M., Logan, J.A., Field, B.D., Fiore, A.M., Li, Q., Liu, H.Y., Mickley, L.J. and Schultz, M.G. (2001) Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation. Journal of Geophysical Research, 106, 23073-23095.
https://doi.org/10.1029/2001JD000807

[17]   Park, R.J., Jacob, D.J., Field, B.D., Yantosca, R.M. and Chin, M. (2004) Natural and Transboundary Pollution Influences on Sulfate-Nitrate-Ammonium Aerosols in the United States: Implications for Policy. Journal of Geophysical Research, 109, D15204.
https://doi.org/10.1029/2003JD004473

[18]   Wang, J., Jacob, D.J. and Martin, S.T. (2008) Sensitivity of Sulfate Direct Climate forcing to the Hysteresis of Particle Phase Transitions. Journal of Geophysical Research, 113, D11207.
https://doi.org/10.1029/2007JD009368

[19]   Fairlie, T.D., Jacob, D.J. and Park, R.J. (2007) The Impact of Transpacific Transport of Mineral Dust in the United States. Atmospheric Environment, 41, 1251-1266.
https://doi.org/10.1016/j.atmosenv.2006.09.048

[20]   Chen, D., Wang, Y., McElroy, M.B., He, K., Yantosca, R.M. and Le Sager, P. (2009) Regional CO Pollution and Export in China Simulated by the High-Resolution Nested-Grid GEOS-Chem Model. Atmospheric Chemistry and Physics, 9, 3825-3839.
https://doi.org/10.5194/acp-9-3825-2009

[21]   Park, R.J., Jacob, D.J., Kumar, N. and Yantosca, R.M. (2006) Regional Visibility Statistics in the United States: Natural and Transboundary Pollution Influences, and Implications for the Regional Haze Rule. Atmospheric Environment, 40, 5405-5423.
https://doi.org/10.1016/j.atmosenv.2006.04.059

[22]   Alexander, B., Park, R.J., Jacob, D.J., Li, Q.B., Yantosca, R.M., Savarino, J., Lee, C.C.W. and Thiemens, M.H. (2005) Sulfate Formation in Sea-Salt Aerosols: Constraints from Oxygen Isotopes. Journal of Geophysical Research, 110, D10307.
https://doi.org/10.1029/2004JD005659

[23]   Liu, H., Jacob, D.J., Bey, I. and Yantosca, R.M. (2001) Constraints from 210Pb and 7Be on Wet Deposition and Transport in a Global Three-Dimensional Chemical Tracer Model Driven by Assimilated Meteorological Fields. Journal of Geophysical Research, 106, 12109-12128.
https://doi.org/10.1029/2000JD900839

[24]   Wesely, M.L. (1989) Parameterization of Surface Resistances to Gaseous Dry Deposition in Regional-Scale Numerical Models. Atmospheric Environment, 23, 1293-1304.
https://doi.org/10.1016/0004-6981(89)90153-4

[25]   Vestreng, V. and Klein, H. (2002) Emission Data Reported to UNECE/EMEP. Quality Assurance and Trend Analysis and Presentation of WebDab, MSC-W Status Report 2002. Norwegian Meteorological Institute, Oslo.

[26]   Kuhns, H., Green, M. and Etyemezian, V. (2003) Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study Emissions Inventory. Desert Research Institute, Las Vegas, Nevada.

[27]   Olivier, J.G.J. and Berdowski, J.J.M. (2001) Global Emissions Sources and Sinks, in the Climate System. In: Berdowski, J., Guicherit, R., Heij, B.J. and Lisse, Eds., The Climate System, A.A. Balkema Publishers/Swets and Zeitlinger Publishers, The Netherlands, 33-78.

[28]   Streets, D.G., Zhang, Q., Wang, L., He, K., Hao, J., Wu, Y., Tang, Y. and Carmichael, G.R. (2006) 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, 111, D14306.
https://doi.org/10.1029/2006JD007118

[29]   Li, X. and Song, W. (2009) Dust Storm Detection Based on Modis Data. Conference International Conference on Geo-Spatial Solutions for Emergency Management and the 50th Anniversary of the Chinese Academy of Surveying and Mapping, Beijing, 14-16 September 2009.

[30]   Draxler, R.R. and Hess, G.D. (1998) An Overview of the HYSPLIT_4 Modeling System of Trajectories, Dispersion, and Deposition. Australian Meteorological Magazine, 47, 295-308.

[31]   Francis, T. (2012) Temporal Trends in Ambient SO2 at a High Altitude Site in Semi-Arid Western India: Observations versus Chemical Transport Modeling. Journal of Environmental Protection, 3, 657-680.
https://doi.org/10.4236/jep.2012.37079

[32]   Daum, P.H., Al-Sunaid, A., Busness, K.M., Hales, J.M. and Mazurek, M. (1993) Studies of the Kuwait Oil Fire Plume during Midsummer 1991. Journal of Geophysical Research, 98, 16809-16827.
https://doi.org/10.1029/93JD01204

[33]   Sharma, A.R., Kharol, S.K. and Badarinath, K.V.S. (2010) An Unusual Dust Event over North-Eastern India and Its Association with Extreme Climatic Conditions—A Study Using Satellite Data. Conference Paper: Aerosols & Clouds: Climate Change Perspectives. IASTABulletin, 2000, 214-217.

[34]   Erisman, J.W., Vermeulen, A., Hensen, A., Flechard, C., Dämmgen, U., Fowler, D. and Tuovinen, J.-P. (2005) Monitoring and Modelling of Biosphere/Atmosphere Exchange of Gases and Aerosols in Europe. Environmental Pollution, 133, 403-413.
https://doi.org/10.1016/j.envpol.2004.07.004

[35]   Gupta, A., Kumar, R., Kumari, K.M. and Srivastava, S.S. (2004) Atmospheric Dry Deposition to Leaf Surfaces at a Rural Site of India. Chemosphere, 55, 1097-1107.
https://doi.org/10.1016/j.chemosphere.2003.08.035

[36]   Lee, B.-K. and Lee, C.-B. (2004) Development of an Improved Dry and Wet Deposition Collector and the Atmospheric Deposition of {PAHs} onto Ulsan Bay, Korea. Atmospheric Environment, 38, 863-871.
https://doi.org/10.1016/j.atmosenv.2003.10.047

[37]   Edwards, P.J., Gregory, J.D. and Allen, H.L. (1999) Seasonal Sulfate Deposition and Export Patterns for a Small Appalachian Watershed. Water, Air, and Soil Pollution, 110, 137-155.
https://doi.org/10.1023/A:1005087421791

[38]   Yi, S.-M., Holsen, T.M. and Noll, K.E. (1997) Comparison of Dry Deposition Predicted from Models and Measured with a Water Surface Sampler. Environmental Science & Technology, 31, 272-278.
https://doi.org/10.1021/es960410g

[39]   Bidleman, T.F. (1988) Atmospheric Processes. Environmental Science & Technology, 22, 361-367.
https://doi.org/10.1021/es00169a002

[40]   Zeller, K., Donev, E., Bojinov, H. and Nikolov, N. (1997) Air Pollution Status of the Bulgarian Govedartsi Ecosystem. Environmental Pollution, 98, 281-289.
https://doi.org/10.1016/S0269-7491(97)00144-9

[41]   Raymond, H.A., Yi, S.-M., Moumen, N., Han, Y. and Holsen, T.M. (2004) Quantifying the Dry Deposition of Reactive Nitrogen and Sulfur Containing Species in Remote Areas Using a Surrogate Surface Analysis Approach. Atmospheric Environment, 38, 2687-2697.
https://doi.org/10.1016/j.atmosenv.2004.02.011

[42]   Dentener, F.J., Carmichael, G.R., Zhang, Y., Lelieveld, J. and Crutzen, P.J. (1996), Role of Mineral Aerosol as a Reactive Surface in the Global Troposphere. Journal of Geophysical Research, 101, 22869-22889.
https://doi.org/10.1029/96JD01818

[43]   Li-Jones, X. and Prospero, J.M. (1998) Variations in the Size Distribution of Non-Sea-Salt Sulfate Aerosol in the Marine Boundary Layer at Barbados: Impact of African Dust. Journal of Geophysical Research, 103, 16073-16084.
https://doi.org/10.1029/98JD00883

[44]   Zhang, Y. and Carmichael, G.R. (1999) The Role of Mineral Aerosol in Tropospheric Chemistry in East Asia—A Model Study. Journal of Applied Meteorology, 38, 353-366.
https://doi.org/10.1175/1520-0450(1999)038<0353:TROMAI>2.0.CO;2

[45]   Guthrie, P.D. (1989) The CH4-CO-OH Conundrum: A Simple Analytic Approach. Global Biogeochemical Cycles, 3, 287-298.
https://doi.org/10.1029/GB003i004p00287

[46]   Kleinman, L.I. (1994) Low and High NOx Tropospheric Photochemistry. Journal of Geophysical Research, 99, 16831-16838.
https://doi.org/10.1029/94JD01028

[47]   Prather, M.J. (1994) Lifetimes and Eigenstates in Atmospheric Chemistry. Geophysical Research Letters, 21, 801-804.
https://doi.org/10.1029/94GL00840

[48]   Stewart, R.W. (1995) Dynamics of the Low to High NOx Transition in a Simplified Tropospheric Photochemical Model. Journal of Geophysical Research, 100, 8929-8943.
https://doi.org/10.1029/95JD00691

[49]   Krol, M.C. and Poppe, D. (1998) Nonlinear Dynamics in Atmospheric Chemistry Rate Equations. Journal of Atmospheric Chemistry, 29, 1-16.
https://doi.org/10.1023/A:1005843430146

[50]   Poppe, D. and Lustfeld, H. (1996) Nonlinearities in the Gas Phase Chemistry of the Troposphere: Oscillating Concentrations in a Simplified Mechanism. Journal of Geophysical Research, 101, 14373-14380.
https://doi.org/10.1029/96JD00339

[51]   Hess, P.G. and Madronich, S. (1997) On Tropospheric Chemical Oscillations. Journal of Geophysical Research, 102, 15949-15965.
https://doi.org/10.1029/97JD00526

[52]   Hanisco, T.F., Lanzendorf, E.J., Wennberg, P.O., Perkins, K.K., Stimpfle, R.M., Voss, P.B. and Midwinter, C. (2001) Sources, Sinks, and the Distribution of OH in the Lower Stratosphere. The Journal of Physical Chemistry A, 105, 1543-1553.
https://doi.org/10.1021/jp002334g

[53]   Lelieveld, J., Dentener, F.J., Peters, W. and Krol, M.C. (2004) On the Role of Hydroxyl Radicals in the Self-Cleansing Capacity of the Troposphere, Atmos. Chemical Physics, 4, 2337-2344.

[54]   Berglen, T.F., Berntsen, T.K., Isaksen, I.S.A. and Sundet, J.K. (2004) A Global Model of the Coupled Sulfur/Oxidant Chemistry in the Troposphere: The Sulfur Cycle. Journal of Geophysical Research, 109, D19310.
https://doi.org/10.1029/2003JD003948

[55]   Manning, M.R., Lowe, D.C., Moss, R.C., Bodeker, G.E. and Allan, W. (2005) Short-Term Variations in the Oxidizing Power of the Atmosphere. Nature, 436, 1001-1004.
https://doi.org/10.1038/nature03900

[56]   Rohrer, F. and Berresheim, H. (2006) Strong Correlation between Levels of Tropospheric Hydroxyl Radicals and Solar Ultraviolet Radiation. Nature, 442, 184-187.
https://doi.org/10.1038/nature04924

[57]   Montzka, S.A., Krol, M., Dlugokencky, E., Hall, B., Jöckel, P. and Lelieveld, J. (2011) Small Interannual Variability of Global Atmospheric Hydroxyl. Science, 331, 67-69.
https://doi.org/10.1126/science.1197640

[58]   Rex, M., Wohltmann, I., Ridder, T., Lehmann, R., Rosenlof, K., Wennberg, P., Weisenstein, D., Notholt, J., Krüger, K., Mohr, V. and Tegtmeier, S. (2014) A Tropical West Pacific OH Minimum and Implications for Stratospheric Composition. Atmospheric Chemistry and Physics, 14, 4827-4841.
https://doi.org/10.5194/acp-14-4827-2014

 
 
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