Low molecular weight organic acids in aerosol particles from Rondônia, Brazil, during the biomass-burning, transition and wet periods

Abstract. Particles from biomass burning and regional haze were sampled in Rondonia, Brazil, during dry, transition and wet periods from September to November 2002, as part of the LBA-SMOCC (Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall, and Climate) field campaign. Water soluble organic and inorganic compounds in bulk (High Volume and Stacked Filter Unit sampler) and size-resolved (Micro Orifice Uniform Deposit Impactor – MOUDI) smoke samples were determined by ion chromatography. It was found that low molecular weight polar organic acids account for a significant fraction of the water soluble organic carbon (WSOC) in biomass burning aerosols (C2-C6 dicarboxylic acids reached up to 3.7% and one-ring aromatic acids reached up to 2% of fine fraction WSOC during burning period). Short dicarboxylic (C2-C6) acids are dominated by oxalic acid followed by malonic and succinic acids. The largest ionic species is ammonium sulfate (60–70% of ionic mass). It was found that most of the ionic mass is concentrated in submicrometer-sized particles. Based on the size distribution and correlations with K+, a known biomass burning tracer, it is suggested that many of the organic acids are directly emitted by vegetation fires. Concentrations of dicarboxylic acids in the front and back filters of high volume sampler were determined. Based on these measurements, it was concluded that in the neutral or slightly basic smoke particles typical of this region, dicarboxylic acids are mostly confined to the particulate phase. Finally, it is shown that the distribution of water soluble species shifts to larger aerosols sizes as the aerosol population ages and mixes with other aerosol types in the atmosphere.

[1]  A. Limbeck,et al.  Gas to particle distribution of low molecular weight dicarboxylic acids at two different sites in central Europe (Austria) , 2005 .

[2]  Y. Rudich,et al.  New analytical method for the determination of levoglucosan, polyhydroxy compounds, and 2-methylerythritol and its application to smoke and rainwater samples. , 2005, Environmental science & technology.

[3]  Timo Mäkelä,et al.  Intercomparison of methods to measure the mass concentration of the atmospheric aerosol during INTERCOMP2000: influence of instrumentation and size cuts , 2004 .

[4]  Franz X. Meixner,et al.  Real-time measurements of ammonia, acidic trace gases and water-soluble inorganic aerosol species at a rural site in the Amazon Basin , 2004 .

[5]  N. Kubilay,et al.  Ionic composition of lower tropospheric aerosols at a Northeastern Mediterranean site: implications regarding sources and long-range transport , 2004 .

[6]  J. Seinfeld,et al.  Molecular composition of the water-soluble fraction of atmospheric carbonaceous aerosols collected during ACE-Asia: ACE-ASIA CARBONACEOUS AEROSOLS , 2004 .

[7]  M. Andreae,et al.  Sources of optically active aerosol particles over the Amazon forest , 2004 .

[8]  G. Kiss,et al.  Chemical characterization of humic‐like substances (HULIS) formed from a lignin‐type precursor in model cloud water , 2004 .

[9]  M. Andreae,et al.  Smoking Rain Clouds over the Amazon , 2004, Science.

[10]  Y. Rudich,et al.  Adsorption of organic compounds pertinent to urban environments onto mineral dust particles , 2004 .

[11]  T. Bates,et al.  Spatial distributions of oxygenated organic compounds (dicarboxylic acids, fatty acids, and levoglucosan) in marine aerosols over the western Pacific and off the coast of East Asia: Continental outflow of organic aerosols during the ACE-Asia campaign , 2003 .

[12]  Shao-Meng Li,et al.  Size distributions of ionic aerosols measured at Waliguan Observatory: Implication for nitrate gas‐to‐particle transfer processes in the free troposphere , 2003 .

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

[14]  P. Formenti,et al.  Inorganic and carbonaceous aerosols during the Southern African Regional Science Initiative (SAFARI 2000) experiment: Chemical characteristics, physical properties, and emission data for smoke from African biomass burning , 2003 .

[15]  J. Seinfeld,et al.  Sampling methods used for the collection of particle-phase organic and elemental carbon during ACE-Asia , 2003 .

[16]  J. Seinfeld,et al.  Impact of biomass burning on cloud properties in the Amazon Basin , 2003 .

[17]  M. Facchini,et al.  Water‐soluble organic compounds in biomass burning aerosols over Amazonia 2. Apportionment of the chemical composition and importance of the polyacidic fraction , 2002 .

[18]  M. Andreae,et al.  Surface exchange of nitric oxide, nitrogen dioxide, and ozone at a cattle pasture in Rondônia, Brazil , 2002 .

[19]  M. Facchini,et al.  Water‐soluble organic compounds in biomass burning aerosols over Amazonia 1. Characterization by NMR and GC‐MS , 2002 .

[20]  P. Quinn,et al.  Carbonaceous aerosol over the Indian Ocean: OC/EC fractions and selected specifications from size‐segregated onboard samples , 2002 .

[21]  O. Boucher,et al.  A satellite view of aerosols in the climate system , 2002, Nature.

[22]  J. Seinfeld,et al.  Can chemical effects on cloud droplet number rival the first indirect effect? , 2002 .

[23]  B. Simoneit,et al.  Biomass burning — a review of organic tracers for smoke from incomplete combustion , 2002 .

[24]  S. Sherwood.  A Microphysical Connection Among Biomass Burning, Cumulus Clouds, and Stratospheric Moisture , 2002, Science.

[25]  V. Ramanathan,et al.  Aerosols, Climate, and the Hydrological Cycle , 2001, Science.

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

[27]  Sonia M. Kreidenweis,et al.  The effects of low molecular weight dicarboxylic acids on cloud formation , 2001 .

[28]  G. Carmichael,et al.  Gas-Particle Partitioning of Nitric Acid Modulated by Alkaline Aerosol , 2001 .

[29]  J. Seinfeld,et al.  Reshaping the Theory of Cloud Formation , 2001, Science.

[30]  M. Scholes,et al.  Semivolatile behavior of dicarboxylic acids and other polar organic species at a rural background site (Nylsvley, RSA) , 2001 .

[31]  M. Scholes,et al.  Mass balance of the atmospheric aerosol in a South African subtropical savanna (Nylsvley, May 1997) , 2000 .

[32]  N. Mihalopoulos,et al.  Carboxylic acids in gas and particulate phase above the Atlantic Ocean , 2000 .

[33]  Shaocai Yu.  Role of organic acids formic, acetic, pyruvic and / oxalic in the formation of cloud condensation / nuclei CCN : a review , 2000 .

[34]  Maria Cristina Facchini,et al.  Characterization of water‐soluble organic compounds in atmospheric aerosol: A new approach , 2000 .

[35]  J. Lacaux,et al.  Airborne aerosols over central Africa during the Experiment for Regional Sources and Sinks of Oxidants (EXPRESSO) , 1999 .

[36]  N. Takeuchi,et al.  Distribution of dicarboxylic acids and carbon isotopic compositions in aerosols from 1997 Indonesian forest fires , 1999 .

[37]  R. Hillamo,et al.  Biomass burning signatures in the atmosphere of central , 1998 .

[38]  M. Jacobson,et al.  Nitric acid scavenging by mineral and biomass burning aerosols , 1998 .

[39]  R. Charlson,et al.  Modification of the Köhler Equation to Include Soluble Trace Gases and Slightly Soluble Substances , 1998 .

[40]  P. Hobbs,et al.  Airborne measurements of carbonaceous aerosols on the East Coast of the United States , 1997 .

[41]  Y. Kaufman,et al.  The effect of smoke particles on clouds and climate forcing , 1997 .

[42]  P. Crutzen,et al.  Atmospheric aerosols: Biogeochemical sources and role in atmospheric chemistry , 1997 .

[43]  P. Carlier,et al.  Carboxylic acids in the troposphere, occurrence, sources, and sinks: A review , 1996 .

[44]  M. Hayashi,et al.  Water soluble dicarboxylic acids and related compounds in Antarctic aerosols , 1996 .

[45]  P. Saxena,et al.  Water-soluble organics in atmospheric particles: A critical review of the literature and application of thermodynamics to identify candidate compounds , 1996 .

[46]  C. Liousse,et al.  Particulate content of savanna fire emissions , 1995 .

[47]  A. G. Allen,et al.  Biomass burning in the Amazon: characterization of the ionic component of aerosols generated from flaming and smoldering rainforest and savannah. , 1995, Environmental science & technology.

[48]  K. Kawamura,et al.  Seasonal changes in the distribution of dicarboxylic acids in the urban atmosphere , 1993 .

[49]  P. Artaxo,et al.  Aerosol characteristics and sources for the Amazon Basin during the wet season , 1990 .

[50]  M. Andreae.  Soot Carbon and Excess Fine Potassium: Long-Range Transport of Combustion-Derived Aerosols , 1983, Science.

[51]  Xiaohong Yao,et al.  Sampling artifacts of acidity and ionic species in PM2.5. , 2004, Environmental science & technology.

[52]  W. Maenhaut,et al.  Elemental and organic carbon in urban canyon and background environments in Budapest, Hungary , 2004 .

[53]  P. Artaxo,et al.  Study of elemental mass size distributions in Amazonia during the LBA/CLAIRE/SMOCC 2002 campaign , 2004 .

[54]  Barbara J. Turpin,et al.  Measuring and simulating particulate organics in the atmosphere: problems and prospects , 2000 .

[55]  Paulo Artaxo,et al.  Chemical composition of aerosol particles from direct emissions of vegetation fires in the Amazon Basin: water-soluble species and trace elements , 2000 .

[56]  Christopher G. Nolte,et al.  Levoglucosan, a tracer for cellulose in biomass burning and atmospheric particles , 1999 .

[57]  B. Mason.  Principles of geochemistry , 1958 .