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Title: Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures

Abstract

Typical tropospheric temperatures render possible phase states of amorphous organic aerosol (OA) particles of solid, semisolid, and liquid. This will affect the multiphase oxidation kinetics involving the organic condensed-phase and gaseous oxidants and radicals. To quantify this effect, we determined the reactive uptake coefficients (γ) of O3, NO3, and OH by substrate films composed of single and binary OA surrogate species under dry conditions for temperatures from 213 to 313 K. A temperature-controlled coated-wall flow reactor coupled to a chemical ionization mass spectrometer was applied to determine γ with consideration of gas diffusion transport limitation and gas flow entrance effects, which can impact heterogeneous reaction kinetics. The phase state of the organic substrates was probed via the poke-flow technique, allowing the estimation of the substrates' glass transition temperatures. γ values for O3 and OH uptake to a canola oil substrate, NO3 uptake to a levoglucosan and a levoglucosan / xylitol substrate, and OH uptake to a glucose and glucose / 1,2,6-hexanetriol substrate have been determined as a function of temperature. We observed the greatest changes in γ with temperature for substrates that experienced the largest changes in viscosity as a result of a solid-to-liquid phase transition. Organic substrates that maintainmore » a semisolid or solid phase state and as such a relatively higher viscosity do not display large variations in heterogeneous reactivity. From 213 to 293 K, γ values of O3 with canola oil, of NO3 with a levoglucosan / xylitol mixture, and of OH with a glucose / 1,2,6-hexanetriol mixture and canola oil, increase by about a factor of 34, 3, 2, and 5, respectively, due to a solid-to-liquid phase transition of the substrate. These results demonstrate that the surface and bulk lifetime of the OA surrogate species can significantly increase due to the slowed heterogeneous kinetics when OA species are solid or highly viscous in the middle and upper troposphere. This experimental study will further our understanding of the chemical evolution of OA particles with subsequent important consequences for source apportionment, air quality, and climate.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]
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  1. Stony Brook Univ., NY (United States). School of Marine and Atmospheric Sciences
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Biological and Environmental Research (BER). Earth and Environmental Systems Science Division
OSTI Identifier:
1802962
Alternate Identifier(s):
OSTI ID: 1832476
Grant/Contract Number:  
SC0016370
Resource Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 20; Journal Issue: 10; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Environmental Sciences & Ecology; Meteorology & Atmospheric Sciences; organic aerosol, multiphase chemical kinetics, oxidation reaction, atmospheric oxidants

Citation Formats

Li, Jienan, Forrester, Seanna M., and Knopf, Daniel A. Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures. United States: N. p., 2020. Web. doi:10.5194/acp-20-6055-2020.
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Li, Jienan, Forrester, Seanna M., & Knopf, Daniel A. Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures. United States. https://doi.org/10.5194/acp-20-6055-2020
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Li, Jienan, Forrester, Seanna M., and Knopf, Daniel A. Mon . "Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures". United States. https://doi.org/10.5194/acp-20-6055-2020. https://www.osti.gov/servlets/purl/1802962.
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@article{osti_1802962,
title = {Heterogeneous oxidation of amorphous organic aerosol surrogates by O3, NO3, and OH at typical tropospheric temperatures},
author = {Li, Jienan and Forrester, Seanna M. and Knopf, Daniel A.},
abstractNote = {Typical tropospheric temperatures render possible phase states of amorphous organic aerosol (OA) particles of solid, semisolid, and liquid. This will affect the multiphase oxidation kinetics involving the organic condensed-phase and gaseous oxidants and radicals. To quantify this effect, we determined the reactive uptake coefficients (γ) of O3, NO3, and OH by substrate films composed of single and binary OA surrogate species under dry conditions for temperatures from 213 to 313 K. A temperature-controlled coated-wall flow reactor coupled to a chemical ionization mass spectrometer was applied to determine γ with consideration of gas diffusion transport limitation and gas flow entrance effects, which can impact heterogeneous reaction kinetics. The phase state of the organic substrates was probed via the poke-flow technique, allowing the estimation of the substrates' glass transition temperatures. γ values for O3 and OH uptake to a canola oil substrate, NO3 uptake to a levoglucosan and a levoglucosan / xylitol substrate, and OH uptake to a glucose and glucose / 1,2,6-hexanetriol substrate have been determined as a function of temperature. We observed the greatest changes in γ with temperature for substrates that experienced the largest changes in viscosity as a result of a solid-to-liquid phase transition. Organic substrates that maintain a semisolid or solid phase state and as such a relatively higher viscosity do not display large variations in heterogeneous reactivity. From 213 to 293 K, γ values of O3 with canola oil, of NO3 with a levoglucosan / xylitol mixture, and of OH with a glucose / 1,2,6-hexanetriol mixture and canola oil, increase by about a factor of 34, 3, 2, and 5, respectively, due to a solid-to-liquid phase transition of the substrate. These results demonstrate that the surface and bulk lifetime of the OA surrogate species can significantly increase due to the slowed heterogeneous kinetics when OA species are solid or highly viscous in the middle and upper troposphere. This experimental study will further our understanding of the chemical evolution of OA particles with subsequent important consequences for source apportionment, air quality, and climate.},
doi = {10.5194/acp-20-6055-2020},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 10,
volume = 20,
place = {United States},
year = {Mon May 25 00:00:00 EDT 2020},
month = {Mon May 25 00:00:00 EDT 2020}
}
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  • DOI: 10.1039/c1cp22478f

Chemical Imaging of Atmospheric Particles
journal, November 2019

Influence of relative humidity on the heterogeneous oxidation of secondary organic aerosol
journal, January 2018

  • Li, Ziyue; Smith, Katherine A.; Cappa, Christopher D.
  • Atmospheric Chemistry and Physics, Vol. 18, Issue 19
  • DOI: 10.5194/acp-18-14585-2018

Glass formation and unusual hygroscopic growth of iodic acid solution droplets with relevance for iodine mediated particle formation in the marine boundary layer
journal, January 2012

  • Murray, B. J.; Haddrell, A. E.; Peppe, S.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 18
  • DOI: 10.5194/acp-12-8575-2012

Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species
journal, January 2006

  • Atkinson, R.; Baulch, D. L.; Cox, R. A.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 11
  • DOI: 10.5194/acp-6-3625-2006

Characterization of the temperature and humidity-dependent phase diagram of amorphous nanoscale organic aerosols
journal, January 2017

  • Rothfuss, Nicholas E.; Petters, Markus D.
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 9
  • DOI: 10.1039/C6CP08593H

Chemistry of Atmospheric Brown Carbon
journal, February 2015

  • Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.
  • Chemical Reviews, Vol. 115, Issue 10
  • DOI: 10.1021/cr5006167

Collision dynamics and reactive uptake of OH radicals at liquid surfaces of atmospheric interest
journal, January 2011

  • Waring, Carla; King, Kerry L.; Bagot, Paul A. J.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 18
  • DOI: 10.1039/c0cp02734k

Glass Formation Processes in Mixed Inorganic/Organic Aerosol Particles
journal, November 2014

  • Dette, Hans P.; Koop, Thomas
  • The Journal of Physical Chemistry A, Vol. 119, Issue 19
  • DOI: 10.1021/jp5106967

Tubular flow reactors with first-order kinetics
journal, January 1978

  • Brown, R. L.
  • Journal of Research of the National Bureau of Standards, Vol. 83, Issue 1
  • DOI: 10.6028/jres.083.001

A Novel Flow Reactor for Studying Reactions on Liquid Surfaces Coated by Organic Monolayers:  Methods, Validation, and Initial Results
journal, November 2007

  • Knopf, D. A.; Cosman, L. M.; Mousavi, P.
  • The Journal of Physical Chemistry A, Vol. 111, Issue 43
  • DOI: 10.1021/jp075724c

Ozonolysis of Mixed Oleic-Acid/Stearic-Acid Particles:  Reaction Kinetics and Chemical Morphology
journal, December 2005

  • Katrib, Y.; Biskos, G.; Buseck, P. R.
  • The Journal of Physical Chemistry A, Vol. 109, Issue 48
  • DOI: 10.1021/jp054714d

Diffusion of Organic Molecules as a Function of Temperature in a Sucrose Matrix (a Proxy for Secondary Organic Aerosol)
journal, September 2019

  • Kiland, Kristian J.; Maclean, Adrian M.; Kamal, Saeid
  • The Journal of Physical Chemistry Letters, Vol. 10, Issue 19
  • DOI: 10.1021/acs.jpclett.9b02182

Exploring matrix effects on photochemistry of organic aerosols
journal, September 2014

  • Lignell, H.; Hinks, M. L.; Nizkorodov, S. A.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 38
  • DOI: 10.1073/pnas.1322106111

Radial Diffusion and Penetration of Gas Molecules and Aerosol Particles through Laminar Flow Reactors, Denuders, and Sampling Tubes
journal, March 2015

  • Knopf, Daniel A.; Pöschl, Ulrich; Shiraiwa, Manabu
  • Analytical Chemistry, Vol. 87, Issue 7
  • DOI: 10.1021/ac5042395

New Method for Prediction of Binary Gas-Phase Diffusion Coefficients
journal, May 1966

  • Fuller, Edward N.; Schettler, Paul D.; Giddings, J. Calvin.
  • Industrial & Engineering Chemistry, Vol. 58, Issue 5
  • DOI: 10.1021/ie50677a007

Interpretation of Uptake Coefficient Data Obtained with Flow Tubes
journal, February 2008

  • Davis, E. James
  • The Journal of Physical Chemistry A, Vol. 112, Issue 9
  • DOI: 10.1021/jp074939j

Volatility and lifetime against OH heterogeneous reaction of ambient isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA)
journal, January 2016

  • Hu, Weiwei; Palm, Brett B.; Day, Douglas A.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 18
  • DOI: 10.5194/acp-16-11563-2016

Phase state of ambient aerosol linked with water uptake and chemical aging in the southeastern US
journal, January 2016

  • Pajunoja, Aki; Hu, Weiwei; Leong, Yu J.
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 17
  • DOI: 10.5194/acp-16-11163-2016

Does atmospheric processing of saturated hydrocarbon surfaces by NO 3 lead to volatilization?
journal, January 2006

  • Knopf, D. A.; Mak, J.; Gross, S.
  • Geophysical Research Letters, Vol. 33, Issue 17
  • DOI: 10.1029/2006GL026884

Shikimic acid ozonolysis kinetics of the transition from liquid aqueous solution to highly viscous glass
journal, January 2015

  • Steimer, Sarah S.; Berkemeier, Thomas; Gilgen, Anina
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 46
  • DOI: 10.1039/C5CP04544D

Gas uptake and chemical aging of semisolid organic aerosol particles
journal, June 2011

  • Shiraiwa, M.; Ammann, M.; Koop, T.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 27
  • DOI: 10.1073/pnas.1103045108

Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere
journal, January 2011

  • Koop, Thomas; Bookhold, Johannes; Shiraiwa, Manabu
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 43
  • DOI: 10.1039/c1cp22617g

Multiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in the Anthropocene
journal, February 2015

  • Pöschl, Ulrich; Shiraiwa, Manabu
  • Chemical Reviews, Vol. 115, Issue 10
  • DOI: 10.1021/cr500487s

Products and kinetics of the reactions of an alkane monolayer and a terminal alkene monolayer with NO 3 radicals
journal, January 2009

  • Gross, Simone; Bertram, Allan K.
  • Journal of Geophysical Research, Vol. 114, Issue D2
  • DOI: 10.1029/2008JD010987

The effect of varying levels of surfactant on the reactive uptake of N<sub>2</sub>O<sub>5</sub> to aqueous aerosol
journal, January 2006

  • McNeill, V. F.; Patterson, J.; Wolfe, G. M.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 6
  • DOI: 10.5194/acp-6-1635-2006

Organic tracers of primary biological aerosol particles at subtropical Okinawa Island in the western North Pacific Rim
journal, June 2015

  • Zhu, Chunmao; Kawamura, Kimitaka; Kunwar, Bhagawati
  • Journal of Geophysical Research: Atmospheres, Vol. 120, Issue 11
  • DOI: 10.1002/2015JD023611

Organic aerosol and global climate modelling: a review
journal, January 2005

  • Kanakidou, M.; Seinfeld, J. H.; Pandis, S. N.
  • Atmospheric Chemistry and Physics, Vol. 5, Issue 4
  • DOI: 10.5194/acp-5-1053-2005

Reactive intermediates revealed in secondary organic aerosol formation from isoprene
journal, December 2009

  • Surratt, J. D.; Chan, A. W. H.; Eddingsaas, N. C.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0911114107

Reference Correlation of the Viscosity of Squalane from 273 to 373 K at 0.1 MPa
journal, September 2013

  • Comuñas, M. J. P.; Paredes, X.; Gaciño, F. M.
  • Journal of Physical and Chemical Reference Data, Vol. 42, Issue 3
  • DOI: 10.1063/1.4812573

Evolution of Organic Aerosols in the Atmosphere
journal, December 2009

Heterogeneous Oxidation of Atmospheric Organic Aerosol: Kinetics of Changes to the Amount and Oxidation State of Particle-Phase Organic Carbon
journal, September 2015

  • Kroll, Jesse H.; Lim, Christopher Y.; Kessler, Sean H.
  • The Journal of Physical Chemistry A, Vol. 119, Issue 44
  • DOI: 10.1021/acs.jpca.5b06946

Diffusion coefficients of organic molecules in sucrose–water solutions and comparison with Stokes–Einstein predictions
journal, January 2017

  • Chenyakin, Yuri; Ullmann, Dagny A.; Evoy, Erin
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 3
  • DOI: 10.5194/acp-17-2423-2017

Global distribution of particle phase state in atmospheric secondary organic aerosols
journal, April 2017

  • Shiraiwa, Manabu; Li, Ying; Tsimpidi, Alexandra P.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15002

Kinetic model framework for aerosol and cloud surface chemistry and gas-particle interactions – Part 1: General equations, parameters, and terminology
journal, January 2007

  • Pöschl, U.; Rudich, Y.; Ammann, M.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 23
  • DOI: 10.5194/acp-7-5989-2007

In-situ observations of mid-latitude forest fire plumes deep in the stratosphere: FOREST FIRE PLUMES IN THE STRATOSPHERE
journal, June 2004

  • Jost, Hans-Jürg; Drdla, Katja; Stohl, Andreas
  • Geophysical Research Letters, Vol. 31, Issue 11
  • DOI: 10.1029/2003GL019253

Structure–activity relationship for the gas-phase reactions of NO3 radical with organic compounds: Update and extension to aldehydes
journal, February 2014

Trehalose + water fragile system: properties and glass transition
journal, December 1999

Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity
journal, July 2014

  • Slade, Jonathan H.; Knopf, Daniel A.
  • Geophysical Research Letters, Vol. 41, Issue 14
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Uptake of Cl and Br by organic surfaces-A perspective on organic aerosols processing by tropospheric oxidants
journal, November 2001

  • Moise, Tamar; Rudich, Yinon
  • Geophysical Research Letters, Vol. 28, Issue 21
  • DOI: 10.1029/2001GL013583

Kinetics and Mechanisms of the Oxidation of Oxygenated Organic Compounds in the Gas Phase
journal, December 2003

  • Mellouki, A.; Le Bras, G.; Sidebottom, H.
  • Chemical Reviews, Vol. 103, Issue 12
  • DOI: 10.1021/cr020526x

Reactive uptake of NO 3 by liquid and frozen organics
journal, January 2002

Reactive Uptake of N 2 O 5 on Aqueous H 2 SO 4 Solutions Coated with 1-Component and 2-Component Monolayers
journal, May 2008

  • Cosman, L. M.; Bertram, A. K.
  • The Journal of Physical Chemistry A, Vol. 112, Issue 20
  • DOI: 10.1021/jp8005469

Heterogeneous oxidation of saturated organic aerosols by hydroxyl radicals: uptake kinetics, condensed-phase products, and particle size change
journal, January 2007

  • George, I. J.; Vlasenko, A.; Slowik, J. G.
  • Atmospheric Chemistry and Physics, Vol. 7, Issue 16
  • DOI: 10.5194/acp-7-4187-2007

Reactive Uptake of O 3 by Multicomponent and Multiphase Mixtures Containing Oleic Acid
journal, June 2005

  • Knopf, Daniel A.; Anthony, Lori M.; Bertram, Allan K.
  • The Journal of Physical Chemistry A, Vol. 109, Issue 25
  • DOI: 10.1021/jp0512513

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?
journal, January 2015

  • Lienhard, D. M.; Huisman, A. J.; Krieger, U. K.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 23
  • DOI: 10.5194/acp-15-13599-2015

Ozone uptake on glassy, semi-solid and liquid organic matter and the role of reactive oxygen intermediates in atmospheric aerosol chemistry
journal, January 2016

  • Berkemeier, Thomas; Steimer, Sarah S.; Krieger, Ulrich K.
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 18
  • DOI: 10.1039/C6CP00634E

Reactive uptake of ozone by proxies for organic aerosols: Surface versus bulk processes
journal, June 2000

  • Moise, Tamar; Rudich, Yinon
  • Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D11
  • DOI: 10.1029/2000JD900071

Nanoscale interfacial gradients formed by the reactive uptake of OH radicals onto viscous aerosol surfaces
journal, January 2015

  • Davies, James F.; Wilson, Kevin R.
  • Chemical Science, Vol. 6, Issue 12
  • DOI: 10.1039/C5SC02326B

Reactive uptake studies of NO3 and N2O5 on alkenoic acid, alkanoate, and polyalcohol substrates to probe nighttime aerosol chemistry
journal, January 2009

  • Gross, Simone; Iannone, Richard; Xiao, Song
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 36
  • DOI: 10.1039/b904741g

Aging of Organic Aerosol: Bridging the Gap Between Laboratory and Field Studies
journal, May 2007

The reaction probabilities of ClONO 2 and N 2 O 5 on polar stratospheric cloud materials
journal, January 1991

  • Hanson, David R.; Ravishankara, A. R.
  • Journal of Geophysical Research, Vol. 96, Issue D3
  • DOI: 10.1029/90JD02613

Aerosol Mixing State: Measurements, Modeling, and Impacts
journal, May 2019

  • Riemer, N.; Ault, A. P.; West, M.
  • Reviews of Geophysics, Vol. 57, Issue 2
  • DOI: 10.1029/2018RG000615

Smoking Rain Clouds over the Amazon
journal, February 2004

Review of receptor modeling methods for source apportionment
journal, December 2015

Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies
journal, January 2011

  • Cubison, M. J.; Ortega, A. M.; Hayes, P. L.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 23
  • DOI: 10.5194/acp-11-12049-2011

Detailed heterogeneous chemistry in an urban plume box model: reversible co-adsorption of O 3 , NO 2 , and H 2 O on soot coated with benzo[a]pyrene
journal, January 2009

  • Springmann, M.; Knopf, D. A.; Riemer, N.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 19
  • DOI: 10.5194/acp-9-7461-2009

Structural fluctuations and orientational glass of levoglucosan—High stability against ordering and absence of structural glass
journal, March 2015

  • Tombari, Elpidio; Johari, G. P.
  • The Journal of Chemical Physics, Vol. 142, Issue 10
  • DOI: 10.1063/1.4913759

The Reaction Probability of OH on Organic Surfaces of Tropospheric Interest
journal, October 2001

  • Bertram, Allan K.; Ivanov, Andrey V.; Hunter, Martin
  • The Journal of Physical Chemistry A, Vol. 105, Issue 41
  • DOI: 10.1021/jp0114034

Integrating phase and composition of secondary organic aerosol from the ozonolysis of  -pinene
journal, May 2014

  • Kidd, C.; Perraud, V.; Wingen, L. M.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 21
  • DOI: 10.1073/pnas.1322558111

Formation of Glasses from Liquids and Biopolymers
journal, March 1995

The OH-initiated atmospheric reaction mechanism and kinetics for levoglucosan emitted in biomass burning
journal, November 2013

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