Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals

Richards-Henderson, Nicole K.; Goldstein, Allen H.; Wilson, Kevin R.

doi:10.1021/acs.est.5b05369

Title: Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals

Abstract

There remains considerable uncertainty in how anthropogenic gas phase emissions alter the oxidative aging of organic aerosols in the troposphere. Here we observe a 10-20 fold acceleration in the effective heterogeneous OH oxidation rate of organic aerosol in the presence of SO₂. This acceleration originates from the radical chain reactions propagated by alkoxy radicals, which are formed efficiently inside the particle by the reaction of peroxy radicals with SO₂. As the OH approaches atmospheric concentrations, the radical chain length increases, transforming the aerosol at rates predicted to be up to 10 times the OH-aerosol collision frequency. Model predictions, constrained by experiments over orders of magnitude changes in [OH] and [SO₂], suggest that in polluted regions the heterogeneous processing of organic aerosols by OH ([SO₂] ≥ 40 ppb) occur on similar time scales as analogous gas-phase oxidation reactions. These results provide evidence for a previously unidentified mechanism by which organic aerosol oxidation is enhanced by anthropogenic gas phase emissions. (Chemical Equation Presented).

Authors:

Richards-Henderson, Nicole K. ^[1]; Goldstein, Allen H. ^[2]; Wilson, Kevin R. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)

Publication Date:: Tue Mar 08 00:00:00 EST 2016

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1454461

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 50; Journal Issue: 7; Related Information: © 2016 American Chemical Society.; Journal ID: ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Richards-Henderson, Nicole K., Goldstein, Allen H., and Wilson, Kevin R. Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals.  United States: N. p., 2016. 
Web.  doi:10.1021/acs.est.5b05369.

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                    Richards-Henderson, Nicole K., Goldstein, Allen H., & Wilson, Kevin R. Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals.  United States.  https://doi.org/10.1021/acs.est.5b05369

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                    Richards-Henderson, Nicole K., Goldstein, Allen H., and Wilson, Kevin R. Tue .  
"Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals".  United States.  https://doi.org/10.1021/acs.est.5b05369.  https://www.osti.gov/servlets/purl/1454461.

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@article{osti_1454461,

  title        = {Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals},

  author       = {Richards-Henderson, Nicole K. and Goldstein, Allen H. and Wilson, Kevin R.},

  abstractNote = {There remains considerable uncertainty in how anthropogenic gas phase emissions alter the oxidative aging of organic aerosols in the troposphere. Here we observe a 10-20 fold acceleration in the effective heterogeneous OH oxidation rate of organic aerosol in the presence of SO2. This acceleration originates from the radical chain reactions propagated by alkoxy radicals, which are formed efficiently inside the particle by the reaction of peroxy radicals with SO2. As the OH approaches atmospheric concentrations, the radical chain length increases, transforming the aerosol at rates predicted to be up to 10 times the OH-aerosol collision frequency. Model predictions, constrained by experiments over orders of magnitude changes in [OH] and [SO2], suggest that in polluted regions the heterogeneous processing of organic aerosols by OH ([SO2] ≥ 40 ppb) occur on similar time scales as analogous gas-phase oxidation reactions. These results provide evidence for a previously unidentified mechanism by which organic aerosol oxidation is enhanced by anthropogenic gas phase emissions. (Chemical Equation Presented).},

  doi          = {10.1021/acs.est.5b05369},

  journal      = {Environmental Science and Technology},

  number       = 7,

  volume       = 50,

  place        = {United States},

  year         = {Tue Mar 08 00:00:00 EST 2016},

  month        = {Tue Mar 08 00:00:00 EST 2016}

}

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Works referencing / citing this record:

Heterogeneous OH oxidation of secondary brown carbon aerosol
journal, January 2018

Schnitzler, Elijah G.; Abbatt, Jonathan P. D.
Atmospheric Chemistry and Physics, Vol. 18, Issue 19
DOI: 10.5194/acp-18-14539-2018

Novel pathway of SO ₂ oxidation in the atmosphere: reactions with monoterpene ozonolysis intermediates and secondary organic aerosol
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Ye, Jianhuai; Abbatt, Jonathan P. D.; Chan, Arthur W. H.
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Organic peroxy radical chemistry in oxidation flow reactors and environmental chambers and their atmospheric relevance
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Atmospheric Chemistry and Physics, Vol. 19, Issue 2
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Title: Sulfur Dioxide Accelerates the Heterogeneous Oxidation Rate of Organic Aerosol by Hydroxyl Radicals

Abstract

Citation Formats

Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes: UBIQUITY AND DOMINANCE OF OXYGENATED OA journal, July 2007

Single-particle mass spectrometry of tropospheric aerosol particles: TROPOSPHERIC AEROSOL PARTICLES journal, September 2006

Fine-Particulate Air Pollution and Life Expectancy in the United States journal, January 2009

Evolution of Organic Aerosols in the Atmosphere journal, December 2009

Large Enhancement in the Heterogeneous Oxidation Rate of Organic Aerosols by Hydroxyl Radicals in the Presence of Nitric Oxide journal, October 2015

The direct observation of secondary radical chain chemistry in the heterogeneous reaction of chlorine atoms with submicron squalane droplets journal, January 2011

Aerosol Pollution Impact on Precipitation: A Scientific Review book, January 2009

Reaction of Organic Peroxyl Radicals with • NO 2 and • NO in Aqueous Solution: Intermediacy of Organic Peroxynitrate and Peroxynitrite Species journal, March 2004

Release of Gas-Phase Halogens by Photolytic Generation of OH in Frozen Halide−Nitrate Solutions: An Active Halogen Formation Mechanism? journal, June 2010

Rate Coefficients for the Reactions of Some C 3 to C 5 Hydrocarbon Peroxy Radicals with NO journal, May 1997

Organic peroxy radicals: Kinetics, spectroscopy and tropospheric chemistry journal, July 1992

A kinetics study of the reaction of SO2 with CH3O2 journal, February 1981

Oxidation of sulfur dioxide by methylperoxy radicals journal, April 1981

Atmospheric processing of organic aerosols journal, May 1999

Quantifying the reactive uptake of OH by organic aerosols in a continuous flow stirred tank reactor journal, January 2009

A mixed-phase relative rates technique for measuring aerosol reaction kinetics journal, January 2006

The importance of phase in the radical-initiated oxidation of model organic aerosols: reactions of solid and liquid brassidic acid particles journal, January 2009

The Influence of Molecular Structure and Aerosol Phase on the Heterogeneous Oxidation of Normal and Branched Alkanes by OH journal, May 2013

Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I - gas phase reactions of O<sub>x</sub>, HO<sub>x</sub>, NO<sub>x</sub> and SO<sub>x</sub> species journal, January 2004

Heterogeneous Chemistry of Butanol and Decanol with Sulfuric Acid: Implications for Secondary Organic Aerosol Formation journal, December 2006

Oxidation of a model alkane aerosol by OH radical: the emergent nature of reactive uptake journal, January 2015

Stochastic methods for aerosol chemistry: a compact molecular description of functionalization and fragmentation in the heterogeneous oxidation of squalane aerosol by OH radicals journal, January 2015

Autoxidation of Organic Compounds in the Atmosphere journal, September 2013

Gas chromatographic determination of Henry's constants of 12 gases in 19 solvents journal, July 1971

Vapour pressure and calorimetric data for the solution of sulfur dioxide in aprotic solvents journal, June 1979

Lubricating Oil Dominates Primary Organic Aerosol Emissions from Motor Vehicles journal, March 2014

The gas-phase reaction of the methylperoxy radical with sulphur dioxide journal, January 1986

Heterogeneous OH oxidation of secondary brown carbon aerosol journal, January 2018

Novel pathway of SO 2 oxidation in the atmosphere: reactions with monoterpene ozonolysis intermediates and secondary organic aerosol journal, January 2018

Organic peroxy radical chemistry in oxidation flow reactors and environmental chambers and their atmospheric relevance journal, January 2019

Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes: UBIQUITY AND DOMINANCE OF OXYGENATED OA
journal, July 2007

Single-particle mass spectrometry of tropospheric aerosol particles: TROPOSPHERIC AEROSOL PARTICLES
journal, September 2006

Fine-Particulate Air Pollution and Life Expectancy in the United States
journal, January 2009

Evolution of Organic Aerosols in the Atmosphere
journal, December 2009

Large Enhancement in the Heterogeneous Oxidation Rate of Organic Aerosols by Hydroxyl Radicals in the Presence of Nitric Oxide
journal, October 2015

The direct observation of secondary radical chain chemistry in the heterogeneous reaction of chlorine atoms with submicron squalane droplets
journal, January 2011

Aerosol Pollution Impact on Precipitation: A Scientific Review
book, January 2009

Reaction of Organic Peroxyl Radicals with ^• NO ₂ and ^• NO in Aqueous Solution: Intermediacy of Organic Peroxynitrate and Peroxynitrite Species
journal, March 2004

Release of Gas-Phase Halogens by Photolytic Generation of OH in Frozen Halide−Nitrate Solutions: An Active Halogen Formation Mechanism?
journal, June 2010

Rate Coefficients for the Reactions of Some C ₃ to C ₅ Hydrocarbon Peroxy Radicals with NO
journal, May 1997

Organic peroxy radicals: Kinetics, spectroscopy and tropospheric chemistry
journal, July 1992

A kinetics study of the reaction of SO2 with CH3O2
journal, February 1981

Oxidation of sulfur dioxide by methylperoxy radicals
journal, April 1981

Atmospheric processing of organic aerosols
journal, May 1999

Quantifying the reactive uptake of OH by organic aerosols in a continuous flow stirred tank reactor
journal, January 2009

A mixed-phase relative rates technique for measuring aerosol reaction kinetics
journal, January 2006

The importance of phase in the radical-initiated oxidation of model organic aerosols: reactions of solid and liquid brassidic acid particles
journal, January 2009

The Influence of Molecular Structure and Aerosol Phase on the Heterogeneous Oxidation of Normal and Branched Alkanes by OH
journal, May 2013

Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I - gas phase reactions of O<sub>x</sub>, HO<sub>x</sub>, NO<sub>x</sub> and SO<sub>x</sub> species
journal, January 2004

Heterogeneous Chemistry of Butanol and Decanol with Sulfuric Acid: Implications for Secondary Organic Aerosol Formation
journal, December 2006

Oxidation of a model alkane aerosol by OH radical: the emergent nature of reactive uptake
journal, January 2015

Stochastic methods for aerosol chemistry: a compact molecular description of functionalization and fragmentation in the heterogeneous oxidation of squalane aerosol by OH radicals
journal, January 2015

Autoxidation of Organic Compounds in the Atmosphere
journal, September 2013

Gas chromatographic determination of Henry's constants of 12 gases in 19 solvents
journal, July 1971

Vapour pressure and calorimetric data for the solution of sulfur dioxide in aprotic solvents
journal, June 1979

Lubricating Oil Dominates Primary Organic Aerosol Emissions from Motor Vehicles
journal, March 2014

The gas-phase reaction of the methylperoxy radical with sulphur dioxide
journal, January 1986

Heterogeneous OH oxidation of secondary brown carbon aerosol
journal, January 2018

Novel pathway of SO ₂ oxidation in the atmosphere: reactions with monoterpene ozonolysis intermediates and secondary organic aerosol
journal, January 2018

Organic peroxy radical chemistry in oxidation flow reactors and environmental chambers and their atmospheric relevance
journal, January 2019