The density of humic acids and humic like substances ( HULIS ) from fresh and aged wood burning and pollution aerosol particles

Atmospheric aerosols play significant roles in cli- matic related phenomena. Size, density and shape of par- ticles affect their fluid-dynamic parameters which in turn dictate their transport and lifecycle. Moreover, density and shape are also related to particles' optical properties, influ- encing their regional and global radiative effects. In the present study we have measured and compared the effective densities of humic like substances (HULIS) extracted from smoke and pollution aerosol particles to those of molecu- lar weight-fractionated aquatic and terrestrial Humic Sub- stances (HS). The effective density was measured by compar- ing the electro mobility and vacuum aerodynamic diameter of aerosol particles composed of these compounds. Charac- terization of chemical parameters such as molecular weight, aromaticity and elemental composition allow us to test how they affect the effective density of these important environ- mental macromolecules. It is suggested that atmospheric ag- ing processes increase the effective density of HULIS due to oxidation, while packing due to the aromatic moieties plays important role in determining the density of the aquatic HS substances.

[1]  M. Facchini,et al.  A simplified model of the water soluble organic component of atmospheric aerosols , 2001 .

[2]  Hans-Christen Hansson,et al.  Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility , 1999 .

[3]  H. Hansson,et al.  Organic atmospheric aerosols: Review and state of the science , 2000 .

[4]  J. Lead,et al.  Experimental determination of partial specific volumes of humic substances in aqueous solutions , 1995 .

[5]  A. Zelenyuk,et al.  High Precision Density Measurements of Single Particles: The Density of Metastable Phases , 2005 .

[6]  Y. Kaufman,et al.  Aerosol invigoration and restructuring of Atlantic convective clouds , 2005 .

[7]  D. Worsnop,et al.  Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 2: Application to Combustion-Generated Soot Aerosols as a Function of Fuel Equivalence Ratio , 2004 .

[8]  Remo Guidieri Res , 1995, RES: Anthropology and Aesthetics.

[9]  H. Hasan,et al.  Apportioning light extinction coefficients to chemical species in atmospheric aerosol , 1983 .

[10]  J. Hansen,et al.  Efficacy of climate forcings , 2005 .

[11]  Xin Wang,et al.  The Relationship between Mass and Mobility for Atmospheric Particles: A New Technique for Measuring Particle Density , 2002 .

[12]  S. Ghan,et al.  Parameterization of the influence of organic surfactants on aerosol activation , 2004 .

[13]  D. Huffman,et al.  Experimental determinations of Mueller scattering matrices for nonspherical particles. , 1978, Applied optics.

[14]  P. Ziemann,et al.  Optical shape fraction measurements of submicrometre laboratory and atmospheric aerosols , 1998 .

[15]  Peter Höppe,et al.  Health effects of particles in ambient air. , 2004, International journal of hygiene and environmental health.

[16]  Renato Zenobi,et al.  Characterization of high molecular weight compounds in urban atmospheric particles , 2005 .

[17]  Y. Tsai,et al.  Characterization of visibility and atmospheric aerosols in urban, suburban, and remote areas. , 2000, The Science of the total environment.

[18]  G. Kiss,et al.  Characterization of water-soluble organic matter isolated from atmospheric fine aerosol , 2002 .

[19]  Kenneth A. Smith,et al.  Development of an Aerosol Mass Spectrometer for Size and Composition Analysis of Submicron Particles , 2000 .

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

[21]  Alla Zelenyuk,et al.  From Agglomerates of Spheres to Irregularly Shaped Particles: Determination of Dynamic Shape Factors from Measurements of Mobility and Vacuum Aerodynamic Diameters , 2006 .

[22]  E. Tipping,et al.  Determination of molecular weights of humic substances by analytical (UV scanning) ultracentrifugation , 1990 .

[23]  R. A. Cox,et al.  Phase transitions and hygroscopic growth of aerosol particles containing humic acid and mixtures of humic acid and ammonium sulphate , 2005 .

[24]  G. Kiss,et al.  Structural Characterisation of Organic Matter in Fine Tropospheric Aerosol by Pyrolysis-Gas Chromatography-Mass Spectrometry , 2000 .

[25]  M. Facchini,et al.  The influence of the organic aerosol component on CCN supersaturation spectra for different aerosol types , 2002 .

[26]  Douglas R. Worsnop,et al.  Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 1: Theory , 2004 .

[27]  J. Thudium,et al.  Mean bulk densities of samples of dry atmospheric aerosol particles: A summary of measured data , 1977 .

[28]  Erik Swietlicki,et al.  Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance , 2005 .

[29]  D. Sparks,et al.  Methods of soil analysis. Part 3 - chemical methods. , 1996 .

[30]  W. Goddard,et al.  3-D structural modeling of humic acids through experimental characterization, computer assisted structure elucidation and atomistic simulations. 1. Chelsea soil humic acid. , 2003, Environmental science & technology.

[31]  M. Benedetti,et al.  Humic Substances Considered as a Heterogeneous Donnan Gel Phase , 1996 .

[32]  Ulrich Pöschl,et al.  Atmospheric aerosols: composition, transformation, climate and health effects. , 2005, Angewandte Chemie.

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

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

[35]  G. Kiss,et al.  Isolation of water-soluble organic matter from atmospheric aerosol. , 2001, Talanta.

[36]  I. Tang,et al.  Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance , 1994 .

[37]  M. Andreae,et al.  Constraining the density and complex refractive index of elemental and organic carbon in biomass burning aerosol using optical and chemical measurements , 2007 .

[38]  Alfred Wiedensohler,et al.  Variability of apparent particle density of an urban aerosol. , 2003, Environmental science & technology.

[39]  J. Seinfeld,et al.  Chemical Amplification (or Dampening) of the Twomey Effect: Conditions Derived from Droplet Activation Theory , 2004 .

[40]  U. Baltensperger,et al.  Study on the Chemical Character of Water Soluble Organic Compounds in Fine Atmospheric Aerosol at the Jungfraujoch , 2001 .

[41]  Y. Rudich,et al.  Detection and quantification of levoglucosan in atmospheric aerosols: a review , 2006, Analytical and bioanalytical chemistry.

[42]  C. Barnes,et al.  5α,8β,14α,17α‐5,6,8,9,14,15,17,18‐Octahydro‐5,17:8,14‐diepoxydibenzo[e,e']benzo[1,2‐a:4,5‐a']dicyclooctene , 1993 .

[43]  Daniel M. Murphy,et al.  Particle density inferred from simultaneous optical and aerodynamic diameters sorted by composition , 2004 .

[44]  Xuedong Song,et al.  Self-Assembly of Aromatic-Functionalized Amphiphiles: The Role and Consequences of Aromatic−Aromatic Noncovalent Interactions in Building Supramolecular Aggregates and Novel Assemblies , 1998 .

[45]  D. R. Worsnop,et al.  Density changes of aerosol particles as a result of chemical reaction , 2004 .

[46]  Martin Gysel,et al.  Hygroscopic properties of water-soluble matter and humic-like organics in atmospheric fine aerosol , 2003 .

[47]  Yinon Rudich,et al.  Cloud Condensation Nuclei properties of model and atmospheric HULIS , 2006 .

[48]  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 .

[49]  W. Malm,et al.  Humidity‐dependent optical properties of fine particles during the Big Bend Regional Aerosol and Visibility Observational Study , 2003 .

[50]  P. Mcmurry,et al.  Measurement of Inherent Material Density of Nanoparticle Agglomerates , 2004 .

[51]  Erik Swietlicki,et al.  Organic aerosol and global climate modelling: a review , 2004 .

[52]  Kenneth A. Smith,et al.  Aerosol mass spectrometer for size and composition analysis of submicron particles , 1998 .

[53]  Meinrat O. Andreae,et al.  Optical properties of humic-like substances (HULIS) in biomass-burning aerosols , 2005 .

[54]  M. L. Laucks,et al.  Aerosol Technology Properties, Behavior, and Measurement of Airborne Particles , 2000 .

[55]  Ilan Koren,et al.  The effect of smoke, dust, and pollution aerosol on shallow cloud development over the Atlantic Ocean. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[56]  Ulrich Poeschl,et al.  Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects , 2006 .

[57]  S. Grambow,et al.  The Role of Soluble Components in Ambient Fine Particles-Induced Changes in Human Lungs and Blood , 2003, Inhalation toxicology.

[58]  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 .

[59]  Ehud Gazit,et al.  Analysis of the Minimal Amyloid-forming Fragment of the Islet Amyloid Polypeptide , 2001, The Journal of Biological Chemistry.

[60]  J. Penner,et al.  Large contribution of organic aerosols to cloud-condensation-nuclei concentrations , 1993, Nature.

[61]  M. Facchini,et al.  Partitioning of the organic aerosol component between fog droplets and interstitial air , 1998 .

[62]  Maria Cristina Facchini,et al.  Chemical features and seasonal variation of fine aerosol water-soluble organic compounds in the Po Valley, Italy , 2001 .

[63]  Alla Zelenyuk,et al.  Single Particle Laser Ablation Time-of-Flight Mass Spectrometer: An Introduction to SPLAT , 2005 .

[64]  D. Worsnop,et al.  Design, Modeling, Optimization, and Experimental Tests of a Particle Beam Width Probe for the Aerodyne Aerosol Mass Spectrometer , 2005 .

[65]  W. Mcdonnell,et al.  Relationships of mortality with the fine and coarse fractions of long-term ambient PM10 concentrations in nonsmokers , 2000, Journal of Exposure Analysis and Environmental Epidemiology.

[66]  Hans-Christen Hansson,et al.  Surface Tension Effects of Humic-Like Substances in the Aqueous Extract of Tropospheric Fine Aerosol , 2005 .

[67]  Charles E. Kolb,et al.  Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer , 2003 .

[68]  M. Andreae,et al.  Size Matters More Than Chemistry for Cloud-Nucleating Ability of Aerosol Particles , 2006, Science.

[69]  Yoram J. Kaufman,et al.  Disentangling the role of microphysical and dynamical effects in determining cloud properties over the Atlantic , 2006 .

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

[71]  Yinon Rudich,et al.  Atmospheric HULIS : how humic-like are they ? A comprehensive and critical review , 2005 .

[72]  C. Chan,et al.  Hygroscopic properties of two model humic-like substances and their mixtures with inorganics of atmospheric importance. , 2003, Environmental science & technology.

[73]  P. Mcmurry,et al.  Relationship between particle mass and mobility for diesel exhaust particles. , 2003, Environmental science & technology.

[74]  S. Kreidenweis,et al.  Water uptake by particles containing humic materials and mixtures of humic materials with ammonium sulfate , 2004 .

[75]  J. Lambert,et al.  Two-dimensional NMR studies of size fractionated Suwannee River fulvic and humic acid reference. , 2001, Environmental science & technology.

[76]  H. J. O H N S O N,et al.  3-D Structural Modeling of Humic Acids through Experimental Characterization, Computer Assisted Structure Elucidation and Atomistic Simulations. 1. Chelsea Soil Humic Acid , 2003 .

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