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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Format: | Article in Journal/Newspaper |
Language: | English |
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Royal Society of Chemistry
2022
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Online Access: | http://nora.nerc.ac.uk/id/eprint/532520/ https://nora.nerc.ac.uk/id/eprint/532520/1/d2ea00013j.pdf https://pubs.rsc.org/en/content/articlelanding/2022/EA/D2EA00013J |
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ftnerc:oai:nora.nerc.ac.uk:532520 2023-05-15T13:41:46+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. 2022-04-12 text http://nora.nerc.ac.uk/id/eprint/532520/ https://nora.nerc.ac.uk/id/eprint/532520/1/d2ea00013j.pdf https://pubs.rsc.org/en/content/articlelanding/2022/EA/D2EA00013J en eng Royal Society of Chemistry https://nora.nerc.ac.uk/id/eprint/532520/1/d2ea00013j.pdf Shepherd, Rosalie H.; King, Martin D.; Rennie, Adrian R.; Ward, Andrew D.; Frey, Markus M. orcid:0000-0003-0535-0416 Brough, Neil orcid:0000-0002-2316-5292 Eveson, Joshua; Del Vento, Sabino; Milsom, Adam; Pfrang, Christian; Skoda, Maximilian W. A.; Welbourn, Rebecca J. L. 2022 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. Environmental Science: Atmospheres, 2. 574-590. https://doi.org/10.1039/D2EA00013J <https://doi.org/10.1039/D2EA00013J> cc_by CC-BY Publication - Article PeerReviewed 2022 ftnerc https://doi.org/10.1039/D2EA00013J 2023-02-04T19:53:14Z 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 ∼6–18 Å 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 × 10−10 cm3 molecule−1 s−1. These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be ∼0.6–1 except woodsmoke (∼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 albedo for these thin films on core–shell ... Article in Journal/Newspaper Antarc* Antarctica Natural Environment Research Council: NERC Open Research Archive Environmental Science: Atmospheres 2 4 574 590 |
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Open Polar |
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Natural Environment Research Council: NERC Open Research Archive |
op_collection_id |
ftnerc |
language |
English |
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 ∼6–18 Å 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 × 10−10 cm3 molecule−1 s−1. These bimolecular rate constants equate to initial OH radical uptake coefficients estimated to be ∼0.6–1 except woodsmoke (∼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 albedo for these thin films on core–shell ... |
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. |
spellingShingle |
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 |
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 |
Royal Society of Chemistry |
publishDate |
2022 |
url |
http://nora.nerc.ac.uk/id/eprint/532520/ https://nora.nerc.ac.uk/id/eprint/532520/1/d2ea00013j.pdf https://pubs.rsc.org/en/content/articlelanding/2022/EA/D2EA00013J |
genre |
Antarc* Antarctica |
genre_facet |
Antarc* Antarctica |
op_relation |
https://nora.nerc.ac.uk/id/eprint/532520/1/d2ea00013j.pdf Shepherd, Rosalie H.; King, Martin D.; Rennie, Adrian R.; Ward, Andrew D.; Frey, Markus M. orcid:0000-0003-0535-0416 Brough, Neil orcid:0000-0002-2316-5292 Eveson, Joshua; Del Vento, Sabino; Milsom, Adam; Pfrang, Christian; Skoda, Maximilian W. A.; Welbourn, Rebecca J. L. 2022 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. Environmental Science: Atmospheres, 2. 574-590. https://doi.org/10.1039/D2EA00013J <https://doi.org/10.1039/D2EA00013J> |
op_rights |
cc_by |
op_rightsnorm |
CC-BY |
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_ |
1766157858228928512 |