skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Effect of Thermodenuding on the Structure of Nascent Flame Soot Aggregates

Abstract

The optical properties (absorption and scattering) of soot particles depend on soot size and index of refraction, but also on the soot complex morphology and the internal mixing with materials that can condense on a freshly emitted (nascent) soot particle and coat it. This coating can affect the soot optical properties by refracting light, or by changing the soot aggregate structure. A common approach to studying the effect of coating on soot optical properties is to measure the absorption and scattering coefficients in ambient air, and then measure them again after removing the coating using a thermodenuder. In this approach, it is assumed that: (1) most of the coating material is removed; (2) charred organic coating does not add to the refractory carbon; (3) oxidation of soot is negligible; and, (4) the structure of the pre-existing soot core is left unaltered, despite the potential oxidation of the core at elevated temperatures. In this study, we investigated the validity of the last assumption, by studying the effect of thermodenuding on the morphology of nascent soot. To this end, we analyzed the morphological properties of laboratory generated nascent soot, before and after thermodenuding. Our investigation shows that there is only minor restructuringmore » of nascent soot by thermodenuding« less

Authors:
 [1];  [1];  [2];  [3];  [2];  [3];  [4];  [5];  [6];  [7];  [1]
  1. Michigan Technological Univ., Houghton, MI (United States)
  2. Aerodyne Research, Inc., Billerica, MA (United States); Boston College, Chestnut Hill, MA (United States)
  3. Boston College, Chestnut Hill, MA (United States)
  4. Aerodyne Research, Inc., Billerica, MA (United States)
  5. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  6. Univ. of Alberta, Edmonton, AB (Canada)
  7. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC). Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1463510
Report Number(s):
LA-UR-18-26271
Journal ID: ISSN 2073-4433; ATMOCZ
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Atmosphere (Basel)
Additional Journal Information:
Journal Name: Atmosphere (Basel); Journal Volume: 8; Journal Issue: 12; Journal ID: ISSN 2073-4433
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Earth Sciences; Aerosols, Soot, Optical properties, Climate, Microscopy

Citation Formats

Bhandari, Janarjan, China, Swarup, Onasch, Timothy, Wolff, Lindsay, Lambe, Andrew, Davidovits, Paul, Cross, Eben, Ahern, Adam, Olfert, Jason, Dubey, Manvendra, and Mazzoleni, Claudio. Effect of Thermodenuding on the Structure of Nascent Flame Soot Aggregates. United States: N. p., 2017. Web. doi:10.3390/atmos8090166.
Bhandari, Janarjan, China, Swarup, Onasch, Timothy, Wolff, Lindsay, Lambe, Andrew, Davidovits, Paul, Cross, Eben, Ahern, Adam, Olfert, Jason, Dubey, Manvendra, & Mazzoleni, Claudio. Effect of Thermodenuding on the Structure of Nascent Flame Soot Aggregates. United States. doi:10.3390/atmos8090166.
Bhandari, Janarjan, China, Swarup, Onasch, Timothy, Wolff, Lindsay, Lambe, Andrew, Davidovits, Paul, Cross, Eben, Ahern, Adam, Olfert, Jason, Dubey, Manvendra, and Mazzoleni, Claudio. Wed . "Effect of Thermodenuding on the Structure of Nascent Flame Soot Aggregates". United States. doi:10.3390/atmos8090166. https://www.osti.gov/servlets/purl/1463510.
@article{osti_1463510,
title = {Effect of Thermodenuding on the Structure of Nascent Flame Soot Aggregates},
author = {Bhandari, Janarjan and China, Swarup and Onasch, Timothy and Wolff, Lindsay and Lambe, Andrew and Davidovits, Paul and Cross, Eben and Ahern, Adam and Olfert, Jason and Dubey, Manvendra and Mazzoleni, Claudio},
abstractNote = {The optical properties (absorption and scattering) of soot particles depend on soot size and index of refraction, but also on the soot complex morphology and the internal mixing with materials that can condense on a freshly emitted (nascent) soot particle and coat it. This coating can affect the soot optical properties by refracting light, or by changing the soot aggregate structure. A common approach to studying the effect of coating on soot optical properties is to measure the absorption and scattering coefficients in ambient air, and then measure them again after removing the coating using a thermodenuder. In this approach, it is assumed that: (1) most of the coating material is removed; (2) charred organic coating does not add to the refractory carbon; (3) oxidation of soot is negligible; and, (4) the structure of the pre-existing soot core is left unaltered, despite the potential oxidation of the core at elevated temperatures. In this study, we investigated the validity of the last assumption, by studying the effect of thermodenuding on the morphology of nascent soot. To this end, we analyzed the morphological properties of laboratory generated nascent soot, before and after thermodenuding. Our investigation shows that there is only minor restructuring of nascent soot by thermodenuding},
doi = {10.3390/atmos8090166},
journal = {Atmosphere (Basel)},
number = 12,
volume = 8,
place = {United States},
year = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Structural Properties of Diesel Exhaust Particles Measured by Transmission Electron Microscopy (TEM): Relationships to Particle Mass and Mobility
journal, September 2004

  • Park, Kihong; Kittelson, David B.; McMurry, Peter H.
  • Aerosol Science and Technology, Vol. 38, Issue 9
  • DOI: 10.1080/027868290505189

Light-absorbing properties of ambient black carbon and brown carbon from fossil fuel and biomass burning sources: LIGHT-ABSORBING PROPERTIES OF BC
journal, July 2015

  • Healy, R. M.; Wang, J. M.; Jeong, C. -H.
  • Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 13
  • DOI: 10.1002/2015JD023382

Effect of Engine Load on Diesel Soot Particles
journal, May 2004

  • Virtanen, Annele K. K.; Ristimäki, Jyrki M.; Vaaraslahti, Kati M.
  • Environmental Science & Technology, Vol. 38, Issue 9
  • DOI: 10.1021/es035139z

Relative Humidity Dependence of Soot Aggregate Restructuring Induced by Secondary Organic Aerosol: Effects of Water on Coating Viscosity and Surface Tension
journal, July 2017

  • Leung, Kaiser K.; Schnitzler, Elijah G.; Jäger, Wolfgang
  • Environmental Science & Technology Letters, Vol. 4, Issue 9
  • DOI: 10.1021/acs.estlett.7b00298

Changes of hygroscopicity and morphology during ageing of diesel soot
journal, July 2011


Electron tomography of nanoparticle clusters: Implications for atmospheric lifetimes and radiative forcing of soot
journal, January 2005

  • van Poppel, Laura H.; Friedrich, Heiner; Spinsby, Jacob
  • Geophysical Research Letters, Vol. 32, Issue 24
  • DOI: 10.1029/2005GL024461

Broadband optical absorbance spectroscopy using a whispering gallery mode microsphere resonator
journal, March 2008

  • Westcott, Sarah L.; Zhang, Jiangquan; Shelton, Robert K.
  • Review of Scientific Instruments, Vol. 79, Issue 3
  • DOI: 10.1063/1.2894307

Mass Absorption Cross-Section of Ambient Black Carbon Aerosol in Relation to Chemical Age
journal, May 2009


Effect of Traffic and Driving Characteristics on Morphology of Atmospheric Soot Particles at Freeway On-Ramps
journal, March 2014

  • China, Swarup; Salvadori, Neila; Mazzoleni, Claudio
  • Environmental Science & Technology, Vol. 48, Issue 6
  • DOI: 10.1021/es405178n

Effects of mixing on extinction by carbonaceous particles
journal, July 1999

  • Fuller, Kirk A.; Malm, William C.; Kreidenweis, Sonia M.
  • Journal of Geophysical Research: Atmospheres, Vol. 104, Issue D13
  • DOI: 10.1029/1998JD100069

Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols
journal, February 2001


Effects of volatile coatings and coating removal mechanisms on the morphology of graphitic soot
journal, September 2013


Soot aggregate restructuring during water processing
journal, December 2013


In situ determination of the activation energy for restructuring of nanometer aerosol agglomerates
journal, March 1997


Structure–property relationship in nanostructures of young and mature soot in premixed flames
journal, January 2009


Examination of the oxidation behavior of biodiesel soot
journal, September 2006


Universality in colloid aggregation
journal, June 1989

  • Lin, M. Y.; Lindsay, H. M.; Weitz, D. A.
  • Nature, Vol. 339, Issue 6223
  • DOI: 10.1038/339360a0

Ns-Soot: A Material-Based Term for Strongly Light-Absorbing Carbonaceous Particles
journal, May 2014


Thermal fragmentation and deactivation of combustion-generated soot particles
journal, September 2014


Coating Mass Dependence of Soot Aggregate Restructuring due to Coatings of Oleic Acid and Dioctyl Sebacate
journal, February 2013


Intercomparison of Thermal–Optical Methods for the Determination of Organic and Elemental Carbon: Influences of Aerosol Composition and Implications
journal, December 2011

  • Cheng, Yuan; Duan, Feng-kui; He, Ke-bin
  • Environmental Science & Technology, Vol. 45, Issue 23
  • DOI: 10.1021/es202649g

Differences in the OC/EC Ratios that Characterize Ambient and Source Aerosols due to Thermal-Optical Analysis
journal, February 2012


Design and calibration of a thermodenuder with an improved heating unit to measure the size-dependent volatile fraction of aerosol particles
journal, July 2002


Enhanced light absorption by mixed source black and brown carbon particles in UK winter
journal, September 2015

  • Liu, Shang; Aiken, Allison C.; Gorkowski, Kyle
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9435

Fragmentation and bond strength of airborne diesel soot agglomerates
journal, January 2008

  • Rothenbacher, Sonja; Messerer, Armin; Kasper, Gerhard
  • Particle and Fibre Toxicology, Vol. 5, Issue 1
  • DOI: 10.1186/1743-8977-5-9

The oxidation of soot: a review of experiments, mechanisms and models
journal, December 2001


Soot formation
journal, January 1981


Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City
journal, January 2008


Ozone loss in soot aerosols
journal, April 2000

  • Disselkamp, R. S.; Carpenter, M. A.; Cowin, J. P.
  • Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D8
  • DOI: 10.1029/1999JD901189

Brown carbon and internal mixing in biomass burning particles
journal, August 2012

  • Lack, D. A.; Langridge, J. M.; Bahreini, R.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 37
  • DOI: 10.1073/pnas.1206575109

Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties: Morphology and mixing state of aged soot
journal, February 2015

  • China, Swarup; Scarnato, Barbara; Owen, Robert C.
  • Geophysical Research Letters, Vol. 42, Issue 4
  • DOI: 10.1002/2014GL062404

Soot Particle Studies—Instrument Inter-Comparison—Project Overview
journal, June 2010


The Effect of Overlap between Monomers on the Determination of Fractal Cluster Morphology
journal, September 1997

  • Oh, C.; Sorensen, C. M.
  • Journal of Colloid and Interface Science, Vol. 193, Issue 1
  • DOI: 10.1006/jcis.1997.5046

Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties
journal, November 2015


NIH Image to ImageJ: 25 years of image analysis
journal, June 2012

  • Schneider, Caroline A.; Rasband, Wayne S.; Eliceiri, Kevin W.
  • Nature Methods, Vol. 9, Issue 7
  • DOI: 10.1038/nmeth.2089

Shapes of soot aerosol particles and implications for their effects on climate
journal, January 2010

  • Adachi, Kouji; Chung, Serena H.; Buseck, Peter R.
  • Journal of Geophysical Research, Vol. 115, Issue D15
  • DOI: 10.1029/2009JD012868

Coating surface tension dependence of soot aggregate restructuring
journal, April 2017


Light Scattering by Fractal Aggregates: A Review
journal, January 2001


Long-range correlations in smoke-particle aggregates
journal, May 1979


The heterogeneous reaction of ozone with soot aerosol
journal, December 1999


Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing
journal, July 2008

  • Zhang, R.; Khalizov, A. F.; Pagels, J.
  • Proceedings of the National Academy of Sciences, Vol. 105, Issue 30
  • DOI: 10.1073/pnas.0804860105

Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon
journal, August 2012


In situ characterization and structure modification of agglomerated aerosol particles
journal, September 1996


Environmental scanning electron microscopy as a new technique to determine the hygroscopic behaviour of individual aerosol particles
journal, December 2002


Oxidative aging and cloud condensation nuclei activation of laboratory combustion soot
journal, January 2015


Changes to the Chemical Composition of Soot from Heterogeneous Oxidation Reactions
journal, February 2015

  • Browne, Eleanor C.; Franklin, Jonathan P.; Canagaratna, Manjula R.
  • The Journal of Physical Chemistry A, Vol. 119, Issue 7
  • DOI: 10.1021/jp511507d

Microstructural changes of diesel soot during oxidation
journal, May 1991


Soot oxidation
journal, July 2003


The effect of complex black carbon microphysics on the determination of the optical properties of brown carbon: BC morphology on BrC optical properties
journal, January 2015

  • Liu, Dantong; Taylor, Jonathan W.; Young, Dominque E.
  • Geophysical Research Letters, Vol. 42, Issue 2
  • DOI: 10.1002/2014GL062443

Fractal and projected structure properties of soot aggregates
journal, March 1995


Effects of water condensation and evaporation on diesel chain-agglomerate morphology
journal, April 1994


Hybrid superaggregate morphology as a result of aggregation in a cluster-dense aerosol
journal, January 2006


The oxidation of soot particulate in the presence of NO2
journal, September 2012


Restructuring of Chain Aggregates of Titania Nanoparticles in the Gas Phase
journal, January 1998


Interlaboratory Analyses of Carbonaceous Aerosol Samples
journal, January 1990


Structural and Fractal Properties of Particles Emitted from Spark Ignition Engines
journal, November 2006

  • Chakrabarty, Rajan K.; Moosmüller, Hans; Arnott, W. Patrick
  • Environmental Science & Technology, Vol. 40, Issue 21
  • DOI: 10.1021/es060537y

Role of OH-Initiated Oxidation of Isoprene in Aging of Combustion Soot
journal, February 2013

  • Khalizov, Alexei F.; Lin, Yun; Qiu, Chong
  • Environmental Science & Technology, Vol. 47, Issue 5
  • DOI: 10.1021/es3045339

Effect of oxidant concentration, exposure time, and seed particles on secondary organic aerosol chemical composition and yield
journal, January 2015

  • Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 6
  • DOI: 10.5194/acp-15-3063-2015

Soot Aggregate Restructuring Due to Coatings of Secondary Organic Aerosol Derived from Aromatic Precursors
journal, November 2014

  • Schnitzler, Elijah G.; Dutt, Ashneil; Charbonneau, André M.
  • Environmental Science & Technology, Vol. 48, Issue 24
  • DOI: 10.1021/es503699b

Enhanced Light Absorption and Scattering by Carbon Soot Aerosol Internally Mixed with Sulfuric Acid
journal, February 2009

  • Khalizov, Alexei F.; Xue, Huaxin; Wang, Lin
  • The Journal of Physical Chemistry A, Vol. 113, Issue 6
  • DOI: 10.1021/jp807531n

New approaches to in situ characterization of ultrafine agglomerates
journal, October 1988


Microstructure and Water Adsorbability of Aircraft Combustor Soots and Kerosene Flame Soots:  Toward an Aircraft-Generated Soot Laboratory Surrogate
journal, November 2003

  • Popovicheva, O. B.; Persiantseva, N. M.; Kuznetsov, B. V.
  • The Journal of Physical Chemistry A, Vol. 107, Issue 47
  • DOI: 10.1021/jp034402f

Dependence of Soot Optical Properties on Particle Morphology: Measurements and Model Comparisons
journal, February 2014

  • Radney, James G.; You, Rian; Ma, Xiaofei
  • Environmental Science & Technology, Vol. 48, Issue 6
  • DOI: 10.1021/es4041804

An unexpected restructuring of combustion soot aggregates by subnanometer coatings of polycyclic aromatic hydrocarbons: Restructuring of Soot Induced by PAH
journal, October 2016

  • Chen, Chao; Fan, Xiaolong; Shaltout, Tasneem
  • Geophysical Research Letters, Vol. 43, Issue 20
  • DOI: 10.1002/2016GL070877

Effects of Coating of Dicarboxylic Acids on the Mass−Mobility Relationship of Soot Particles
journal, April 2009

  • Xue, Huaxin; Khalizov, Alexei F.; Wang, Lin
  • Environmental Science & Technology, Vol. 43, Issue 8
  • DOI: 10.1021/es803287v

Development and Characterization of a Fast-Stepping/Scanning Thermodenuder for Chemically-Resolved Aerosol Volatility Measurements
journal, March 2008

  • Huffman, J. Alex; Ziemann, Paul J.; Jayne, John T.
  • Aerosol Science and Technology, Vol. 42, Issue 5
  • DOI: 10.1080/02786820802104981

Evaluation of thermal denuder and catalytic stripper methods for solid particle measurements
journal, December 2010


Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles
journal, July 2013

  • China, Swarup; Mazzoleni, Claudio; Gorkowski, Kyle
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3122

Equivalence of Elemental Carbon by Thermal/Optical Reflectance and Transmittance with Different Temperature Protocols
journal, August 2004

  • Chow, Judith C.; Watson, John G.; Chen, L. -W. Antony
  • Environmental Science & Technology, Vol. 38, Issue 16
  • DOI: 10.1021/es034936u

Light-scattering measurements of monomer size, monomers per aggregate, and fractal dimension for soot aggregates in flames
journal, January 1992


Changes of ns-soot mixing states and shapes in an urban area during CalNex: MIXING STATES AND SHAPES OF NS-SOOT
journal, May 2013

  • Adachi, Kouji; Buseck, Peter R.
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 9
  • DOI: 10.1002/jgrd.50321