Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol
The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atm...
Published in: | Environmental Science: Atmospheres |
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Language: | English |
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Uppsala universitet, Institutionen för kemi - Ångström
2022
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Online Access: | http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-481772 https://doi.org/10.1039/d2ea00013j |
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ftuppsalauniv:oai:DiVA.org:uu-481772 2023-05-15T14:02:17+02:00 Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol Shepherd, Rosalie H. King, Martin D. Rennie, Adrian R. Ward, Andrew D. Frey, Markus M. Brough, Neil Eveson, Joshua Del Vento, Sabino Milsom, Adam Pfrang, Christian Skoda, Maximilian W. A. Welbourn, Rebecca J. L. 2022 application/pdf http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-481772 https://doi.org/10.1039/d2ea00013j eng eng Uppsala universitet, Institutionen för kemi - Ångström STFC Rutherford Appleton Lab, Res Complex Harwell, Cent Laser Facil, Oxford OX11 0FA, England.;Royal Holloway Univ London, Dept Earth Sci, Egham TW20 0EX, Surrey, England. Royal Holloway Univ London, Dept Earth Sci, Egham TW20 0EX, Surrey, England. STFC Rutherford Appleton Lab, Res Complex Harwell, Cent Laser Facil, Oxford OX11 0FA, England. British Antarctic Survey, Nat Environm Res Council, High Cross,Madingley Rd, Cambridge CB3 0ET, England. Univ Birmingham, Sch Geog Earth & Environm Sci, Birmingham B15 2TT, W Midlands, England. Rutherford Appleton Lab, ISIS Pulsed Neutron & Muon Source, Oxford OX11 0QX, England. Royal Society of Chemistry (RSC) Environmental Science : Atmospheres, 2022, 2:4, s. 574-590 orcid:0000-0001-8185-3272 http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-481772 doi:10.1039/d2ea00013j ISI:000826362600001 info:eu-repo/semantics/openAccess Meteorology and Atmospheric Sciences Meteorologi och atmosfärforskning Article in journal info:eu-repo/semantics/article text 2022 ftuppsalauniv https://doi.org/10.1039/d2ea00013j 2023-02-23T22:01:13Z The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atmospheric aerosol were found to have stable, compressible, films at the air-water interface that were typically similar to 6-18 angstrom thick. These films are reactive towards gas-phase OH radicals and decay exponentially, with bimolecular rate constants for reaction with gas-phase OH radicals of typically 0.08-1.5 x 10(-10) cm(3) molecule(-1) s(-1). These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be similar to 0.6-1 except woodsmoke (similar to 0.05). The film thickness and the neutron scattering length density of the extracted atmosphere aerosol material (from urban, remote and wood burning) were measured by neutron reflection as they were exposed to OH radicals. For the first time neutron reflection has been demonstrated as an excellent technique for studying the thin films formed at air-water interfaces from materials extracted from atmospheric aerosol samples. Additionally, the kinetics of gas-phase OH radicals with a proxy compound, the lipid 1,2-distearoyl-sn-glycero-3-phosphocholine (DSPC) was studied displaying significantly different behaviour, thus demonstrating it is not a good proxy for atmospheric materials that may form films at the air-water interface. The atmospheric lifetimes, with respect to OH radical oxidation, of the insoluble organic materials extracted from atmospheric aerosol at the air-water interface were a few hours. Relative to a possible physical atmospheric lifetime of 4 days, the oxidation of these films is important and needs inclusion in atmospheric models. The optical properties of these films were previously reported [Shepherd et al., Atmos. Chem. Phys., 2018, 18, 5235-5252] and there is a significant change in top of the atmosphere ... Article in Journal/Newspaper Antarc* Antarctica Uppsala University: Publications (DiVA) Environmental Science: Atmospheres 2 4 574 590 |
institution |
Open Polar |
collection |
Uppsala University: Publications (DiVA) |
op_collection_id |
ftuppsalauniv |
language |
English |
topic |
Meteorology and Atmospheric Sciences Meteorologi och atmosfärforskning |
spellingShingle |
Meteorology and Atmospheric Sciences Meteorologi och atmosfärforskning Shepherd, Rosalie H. King, Martin D. Rennie, Adrian R. Ward, Andrew D. Frey, Markus M. Brough, Neil Eveson, Joshua Del Vento, Sabino Milsom, Adam Pfrang, Christian Skoda, Maximilian W. A. Welbourn, Rebecca J. L. Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
topic_facet |
Meteorology and Atmospheric Sciences Meteorologi och atmosfärforskning |
description |
The presence of an organic film on a cloud droplet or aqueous aerosol particle has the potential to alter the chemical, optical and physical properties of the droplet or particle. In the study presented, water insoluble organic materials extracted from urban, remote (Antarctica) and wood burning atmospheric aerosol were found to have stable, compressible, films at the air-water interface that were typically similar to 6-18 angstrom thick. These films are reactive towards gas-phase OH radicals and decay exponentially, with bimolecular rate constants for reaction with gas-phase OH radicals of typically 0.08-1.5 x 10(-10) cm(3) molecule(-1) s(-1). These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be similar to 0.6-1 except woodsmoke (similar to 0.05). The film thickness and the neutron scattering length density of the extracted atmosphere aerosol material (from urban, remote and wood burning) were measured by neutron reflection as they were exposed to OH radicals. For the first time neutron reflection has been demonstrated as an excellent technique for studying the thin films formed at air-water interfaces from materials extracted from atmospheric aerosol samples. Additionally, the kinetics of gas-phase OH radicals with a proxy compound, the lipid 1,2-distearoyl-sn-glycero-3-phosphocholine (DSPC) was studied displaying significantly different behaviour, thus demonstrating it is not a good proxy for atmospheric materials that may form films at the air-water interface. The atmospheric lifetimes, with respect to OH radical oxidation, of the insoluble organic materials extracted from atmospheric aerosol at the air-water interface were a few hours. Relative to a possible physical atmospheric lifetime of 4 days, the oxidation of these films is important and needs inclusion in atmospheric models. The optical properties of these films were previously reported [Shepherd et al., Atmos. Chem. Phys., 2018, 18, 5235-5252] and there is a significant change in top of the atmosphere ... |
format |
Article in Journal/Newspaper |
author |
Shepherd, Rosalie H. King, Martin D. Rennie, Adrian R. Ward, Andrew D. Frey, Markus M. Brough, Neil Eveson, Joshua Del Vento, Sabino Milsom, Adam Pfrang, Christian Skoda, Maximilian W. A. Welbourn, Rebecca J. L. |
author_facet |
Shepherd, Rosalie H. King, Martin D. Rennie, Adrian R. Ward, Andrew D. Frey, Markus M. Brough, Neil Eveson, Joshua Del Vento, Sabino Milsom, Adam Pfrang, Christian Skoda, Maximilian W. A. Welbourn, Rebecca J. L. |
author_sort |
Shepherd, Rosalie H. |
title |
Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
title_short |
Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
title_full |
Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
title_fullStr |
Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
title_full_unstemmed |
Measurement of gas-phase OH radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
title_sort |
measurement of gas-phase oh radical oxidation and film thickness of organic films at the air-water interface using material extracted from urban, remote and wood smoke aerosol |
publisher |
Uppsala universitet, Institutionen för kemi - Ångström |
publishDate |
2022 |
url |
http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-481772 https://doi.org/10.1039/d2ea00013j |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_relation |
Environmental Science : Atmospheres, 2022, 2:4, s. 574-590 orcid:0000-0001-8185-3272 http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-481772 doi:10.1039/d2ea00013j ISI:000826362600001 |
op_rights |
info:eu-repo/semantics/openAccess |
op_doi |
https://doi.org/10.1039/d2ea00013j |
container_title |
Environmental Science: Atmospheres |
container_volume |
2 |
container_issue |
4 |
container_start_page |
574 |
op_container_end_page |
590 |
_version_ |
1766272440074240000 |