Emissions of major gaseous and particulate species during experimental burns of southern African biomass

Received 2 June 2005; revised 31 October 2005; accepted 23 November 2005; published 22 February 2006. [1] Characteristic vegetation and biofuels in major ecosystems of southern Africa were sampled during summer and autumn 2000 and burned under semicontrolled conditions. Elemental compositions of fuels and ash and emissions of CO2, CO, CH3COOH, HCOOH, NOX ,N H3, HONO, HNO3, HCl, total volatile inorganic Cl and Br, SO2 and particulate C, N, and major ions were measured. Modified combustion efficiencies (MCEs, median = 0.94) were similar to those of ambient fires. Elemental emissions factors (EFel) for CH3COOH were inversely correlated with MCEs; EFels for heading and mixed grass fires were higher than those for backing fires of comparable MCEs. NOX ,N H3, HONO, and particulate N accounted for a median of 22% of emitted N; HNO3 emissions were insignificant. Grass fires with the highest EFels for NH3 corresponded to MCEs in the range of 0.93; grass fires with higher and low MCEs exhibited lower EFels. NH3 emissions for most fuels were poorly correlated with fuel N. Most Cl and Br in fuel was emitted during combustion (median for each = 73%). Inorganic gases and particulate ions accounted for medians of 53% and 30% of emitted Cl and Br, respectively. About half of volatile inorganic Cl was HCl indicating significant emissions of other gaseous inorganic Cl species. Most fuel S (median = 76%) was emitted during combustion; SO2 and particulate SO4� accounted for about half the flux. Mobilization of P by fire (median emission = 82%) implies large nutrient losses from burned regions and potentially important exogenous sources of fertilization for downwind ecosystems.

[1]  M. Andreae,et al.  An analysis of the chemical processes in the smoke plume from a savanna fire , 2005 .

[2]  A. Wall,et al.  Closure evaluation of size‐resolved aerosol pH in the New England coastal atmosphere during summer , 2004 .

[3]  P. Hobbs,et al.  Heterogeneous chemistry involving methanol in tropospheric clouds , 2004 .

[4]  J. Galloway,et al.  Phase partitioning and dry deposition of atmospheric nitrogen at the mid‐Atlantic U.S. coast , 2003 .

[5]  P. Crutzen,et al.  Inorganic bromine in the marine boundary layer: a critical review , 2003 .

[6]  P. Crutzen,et al.  Halogen cycling and aerosol pH in the Hawaiian marine boundary layer , 2003 .

[7]  W. Hao,et al.  Trace gas measurements in nascent, aged, and cloud‐processed smoke from African savanna fires by airborne Fourier transform infrared spectroscopy (AFTIR) , 2003 .

[8]  Peter V. Hobbs,et al.  Effects of humidity on aerosols in southern Africa during the biomass burning season , 2003 .

[9]  P. Buseck,et al.  Individual aerosol particles from biomass burning in southern Africa: 2, Compositions and aging of inorganic particles , 2003 .

[10]  T. Kirchstetter,et al.  Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution , 2003 .

[11]  J. Privette,et al.  Africa burning: A thematic analysis of the Southern African Regional Science Initiative (SAFARI 2000) , 2003 .

[12]  C. Justice,et al.  SAFARI-2000 characterization of fuels, fire behavior, combustion completeness, and emissions from experimental burns in infertile grass savannas in western Zambia , 2003 .

[13]  L. Radke,et al.  Mercury emissions from the August 2001 wildfires in Washington State and an agricultural waste fire in Oregon and atmospheric mercury budget estimates , 2003 .

[14]  A. Neftel,et al.  Nitrous acid formation in the urban atmosphere: Gradient measurements of NO2 and HONO over grass in Milan, Italy , 2002 .

[15]  Xianliang Zhou,et al.  Photochemical production of nitrous acid on glass sample manifold surface , 2002 .

[16]  M. Andreae,et al.  Emission of trace gases and aerosols from biomass burning , 2001 .

[17]  J. D. Neece,et al.  Anthropogenic Sources of Chlorine and Ozone Formation in Urban Atmospheres , 2000 .

[18]  L. Pirjola,et al.  Stable sulphate clusters as a source of new atmospheric particles , 2000, Nature.

[19]  J. Seinfeld,et al.  Ternary nucleation of H2SO4, NH3, and H2O in the atmosphere , 1999 .

[20]  Paul J. Crutzen,et al.  Ozone in the remote marine boundary layer: A possible role for halogens , 1999 .

[21]  J. Logan,et al.  Global chlorine emissions from biomass burning: Reactive Chlorine Emissions Inventory , 1999 .

[22]  D. Blake,et al.  Emission factors of hydrocarbons, halocarbons, trace gases and particles from biomass burning in Brazil , 1998 .

[23]  P. Crutzen,et al.  Aerosol pH in the marine boundary layer: A review and model evaluation , 1998 .

[24]  C. Justice,et al.  Effect of fuel composition on combustion efficiency and emission factors for African savanna ecosystems , 1996 .

[25]  D. Blake,et al.  Biomass burning emissions and vertical distribution of atmospheric methyl halides and other reduced carbon gases in the South Atlantic region , 1996 .

[26]  Ralf Koppmann,et al.  Methyl Halide Emissions from Savanna Fires in Southern Africa , 1996 .

[27]  Thomas E. Graedel,et al.  Tropospheric budget of reactive chlorine , 1995 .

[28]  J. Lacaux,et al.  Determination of biomass burning emission factors: Methods and results , 1995, Environmental monitoring and assessment.

[29]  P. Shepson,et al.  Organic and inorganic bromine compounds and their composition in the Arctic troposphere during polar sunrise , 1994 .

[30]  J. Galloway,et al.  Measurement technique for inorganic chlorine gases in the marine boundary layer , 1993 .

[31]  W. Hao,et al.  Emissions of N2O from the burning of biomass in an experimental system , 1991 .

[32]  P. Crutzen,et al.  Molecular nitrogen emissions from denitrification during biomass burning , 1991, Nature.

[33]  J. Levine.  Experimental Evaluation of Biomass Burning Emissions: Nitrogen and Carbon Containing Compounds , 1991 .

[34]  P. Crutzen,et al.  Importance of biomass burning in the atmospheric budgets of nitrogen-containing gases , 1990, Nature.

[35]  P. Crutzen,et al.  Biomass Burning in the Tropics: Impact on Atmospheric Chemistry and Biogeochemical Cycles , 1990, Science.

[36]  J. Levine.  Global biomass burning - Atmospheric, climatic, and biospheric implications , 1990 .

[37]  James F. Kasting,et al.  Chlorine-hydrocarbon photochemistry in the marine troposphere and lower stratosphere , 1988 .

[38]  R. Hirsch,et al.  METHODS OF FITTING A STRAIGHT LINE TO DATA: EXAMPLES IN WATER RESOURCES , 1984 .

[39]  R. Delmas.  On the emission of carbon, nitrogen and sulfur in the atmosphere during bushfires in intertropical savannah zones , 1982 .

[40]  M. Khalil,et al.  Concentration distribution of methyl chloride in the atmosphere , 1980 .

[41]  P. Crutzen,et al.  Biomass burning as a source of atmospheric gases CO, H2, N2O, NO, CH3Cl and COS , 1979, Nature.

[42]  E. Sawicki,et al.  Ion Chromatographic Analysis of Environmental Pollutants , 1978 .

[43]  A. Mcmurtrie,et al.  Ion Chromatographic determination of sulfur and chlorine using milligram and submilligram sample weights , 1977 .

[44]  R. Johnstone,et al.  The Chemical Constituents Of Tobacco And Tobacco Smoke , 1959 .