Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors

<p dir="ltr">The phase behaviour of aerosol particles plays a profound role in atmospheric physicochemical processes, influencing their physical and optical properties and further impacting climate and air quality. However, understanding of the aerosol phase state is still incomplete...

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Main Author: Yu Wang (12152) (author)
Other Authors: Aristeidis Voliotis (16563090) (author), Yunqi Shao (8368584) (author), Taomou Zong (9927587) (author), Xiangxinyue Meng (6584552) (author), Mao Du (16563091) (author), Dawei Hu (2186113) (author), Ying Chen (9697) (author), Zhijun Wu (23909) (author), M. Rami Alfarra (1343493) (author), Gordon McFiggans (1965904) (author)
Published: 2021
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_version_ 1864513516667404288
author Yu Wang (12152)
author2 Aristeidis Voliotis (16563090)
Yunqi Shao (8368584)
Taomou Zong (9927587)
Xiangxinyue Meng (6584552)
Mao Du (16563091)
Dawei Hu (2186113)
Ying Chen (9697)
Zhijun Wu (23909)
M. Rami Alfarra (1343493)
Gordon McFiggans (1965904)
author2_role author
author
author
author
author
author
author
author
author
author
author_facet Yu Wang (12152)
Aristeidis Voliotis (16563090)
Yunqi Shao (8368584)
Taomou Zong (9927587)
Xiangxinyue Meng (6584552)
Mao Du (16563091)
Dawei Hu (2186113)
Ying Chen (9697)
Zhijun Wu (23909)
M. Rami Alfarra (1343493)
Gordon McFiggans (1965904)
author_role author
dc.creator.none.fl_str_mv Yu Wang (12152)
Aristeidis Voliotis (16563090)
Yunqi Shao (8368584)
Taomou Zong (9927587)
Xiangxinyue Meng (6584552)
Mao Du (16563091)
Dawei Hu (2186113)
Ying Chen (9697)
Zhijun Wu (23909)
M. Rami Alfarra (1343493)
Gordon McFiggans (1965904)
dc.date.none.fl_str_mv 2021-07-28T03:00:00Z
dc.identifier.none.fl_str_mv 10.5194/acp-21-11303-2021
dc.relation.none.fl_str_mv https://figshare.com/articles/journal_contribution/Phase_state_of_secondary_organic_aerosol_in_chamber_photo-oxidation_of_mixed_precursors/25771524
dc.rights.none.fl_str_mv CC BY 4.0
info:eu-repo/semantics/openAccess
dc.subject.none.fl_str_mv Earth sciences
Atmospheric sciences
Environmental sciences
Climate change impacts and adaptation
Aerosol phase behavior
Atmospheric physicochemical processes
Aerosol rebounding tendency
Bounce fraction
Secondary organic aerosol (SOA)
Volatile organic compounds (VOCs)
Deliquescent ammonium sulfate seed
Relative humidity (RH)
dc.title.none.fl_str_mv Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
dc.type.none.fl_str_mv Text
Journal contribution
info:eu-repo/semantics/publishedVersion
text
contribution to journal
description <p dir="ltr">The phase behaviour of aerosol particles plays a profound role in atmospheric physicochemical processes, influencing their physical and optical properties and further impacting climate and air quality. However, understanding of the aerosol phase state is still incomplete, especially that of multicomponent particles which contain inorganic compounds and secondary organic aerosol (SOA) from mixed volatile organic compound (VOC) precursors. We report measurements conducted in the Manchester Aerosol Chamber (MAC) to investigate the aerosol rebounding tendency, measured as the bounce fraction, as a surrogate of the aerosol phase state during SOA formation from photo-oxidation of biogenic (α-pinene and isoprene) and anthropogenic (ocresol) VOCs and their binary mixtures on deliquescent ammonium sulfate seed.</p><p dir="ltr">Aerosol phase state is dependent on relative humidity (RH) and chemical composition (key factors determining aerosol water uptake). Liquid (bounce fraction; BF < 0.2) at RH > 80 % and nonliquid behaviour (BF > 0.8) at RH < 30 % were observed, with a liquid-to-nonliquid transition with decreasing RH between 30 % and 80 %. This RH-dependent phase behaviour (RH<sub>BF=0.2, 0.5, 0.8</sub>) increased towards a maximum, with an increasing organic–inorganic mass ratio (MR<sub>org</sub><sub>/inorg</sub>) during SOA formation evolution in all investigated VOC systems. With the use of comparable initial ammonium sulfate seed concentration, the SOA production rate of the VOC systems determines the MR<sub>org/inorg</sub> and, consequently, the change in the phase behaviour. Although less important than RH and MR<sub>org/inorg</sub>, the SOA composition plays a second-order role, with differences in the liquid-to-nonliquid transition at moderate MR<sub>org/inorg</sub> of ∼ 1 observed between biogenic-only (anthropogenic-free) and anthropogenic-containing VOC systems. Considering the combining role of the RH and chemical composition in aerosol phase state, the BF decreased monotonically with increasing hygroscopic growth factor (GF), and the BF was ∼ 0 when GF was larger than 1.15. The real atmospheric consequences of our results are that any processes changing ambient RH or MR<sub>org/inorg</sub> (aerosol liquid water) will influence their phase state. Where abundant anthropogenic VOCs contribute to SOA, compositional changes in SOA may influence phase behaviour at moderate organic mass fraction (∼ 50 %) compared with purely biogenic SOA. Further studies are needed on more complex and realistic atmospheric mixtures.</p><h2>Other Information</h2><p dir="ltr">Published in: Atmospheric Chemistry and Physics<br>License: <a href="https://creativecommons.org/licenses/by/4.0/" target="_blank">https://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.5194/acp-21-11303-2021" target="_blank">https://dx.doi.org/10.5194/acp-21-11303-2021</a></p>
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identifier_str_mv 10.5194/acp-21-11303-2021
network_acronym_str Manara2
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oai_identifier_str oai:figshare.com:article/25771524
publishDate 2021
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rights_invalid_str_mv CC BY 4.0
spelling Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursorsYu Wang (12152)Aristeidis Voliotis (16563090)Yunqi Shao (8368584)Taomou Zong (9927587)Xiangxinyue Meng (6584552)Mao Du (16563091)Dawei Hu (2186113)Ying Chen (9697)Zhijun Wu (23909)M. Rami Alfarra (1343493)Gordon McFiggans (1965904)Earth sciencesAtmospheric sciencesEnvironmental sciencesClimate change impacts and adaptationAerosol phase behaviorAtmospheric physicochemical processesAerosol rebounding tendencyBounce fractionSecondary organic aerosol (SOA)Volatile organic compounds (VOCs)Deliquescent ammonium sulfate seedRelative humidity (RH)<p dir="ltr">The phase behaviour of aerosol particles plays a profound role in atmospheric physicochemical processes, influencing their physical and optical properties and further impacting climate and air quality. However, understanding of the aerosol phase state is still incomplete, especially that of multicomponent particles which contain inorganic compounds and secondary organic aerosol (SOA) from mixed volatile organic compound (VOC) precursors. We report measurements conducted in the Manchester Aerosol Chamber (MAC) to investigate the aerosol rebounding tendency, measured as the bounce fraction, as a surrogate of the aerosol phase state during SOA formation from photo-oxidation of biogenic (α-pinene and isoprene) and anthropogenic (ocresol) VOCs and their binary mixtures on deliquescent ammonium sulfate seed.</p><p dir="ltr">Aerosol phase state is dependent on relative humidity (RH) and chemical composition (key factors determining aerosol water uptake). Liquid (bounce fraction; BF < 0.2) at RH > 80 % and nonliquid behaviour (BF > 0.8) at RH < 30 % were observed, with a liquid-to-nonliquid transition with decreasing RH between 30 % and 80 %. This RH-dependent phase behaviour (RH<sub>BF=0.2, 0.5, 0.8</sub>) increased towards a maximum, with an increasing organic–inorganic mass ratio (MR<sub>org</sub><sub>/inorg</sub>) during SOA formation evolution in all investigated VOC systems. With the use of comparable initial ammonium sulfate seed concentration, the SOA production rate of the VOC systems determines the MR<sub>org/inorg</sub> and, consequently, the change in the phase behaviour. Although less important than RH and MR<sub>org/inorg</sub>, the SOA composition plays a second-order role, with differences in the liquid-to-nonliquid transition at moderate MR<sub>org/inorg</sub> of ∼ 1 observed between biogenic-only (anthropogenic-free) and anthropogenic-containing VOC systems. Considering the combining role of the RH and chemical composition in aerosol phase state, the BF decreased monotonically with increasing hygroscopic growth factor (GF), and the BF was ∼ 0 when GF was larger than 1.15. The real atmospheric consequences of our results are that any processes changing ambient RH or MR<sub>org/inorg</sub> (aerosol liquid water) will influence their phase state. Where abundant anthropogenic VOCs contribute to SOA, compositional changes in SOA may influence phase behaviour at moderate organic mass fraction (∼ 50 %) compared with purely biogenic SOA. Further studies are needed on more complex and realistic atmospheric mixtures.</p><h2>Other Information</h2><p dir="ltr">Published in: Atmospheric Chemistry and Physics<br>License: <a href="https://creativecommons.org/licenses/by/4.0/" target="_blank">https://creativecommons.org/licenses/by/4.0/</a><br>See article on publisher's website: <a href="https://dx.doi.org/10.5194/acp-21-11303-2021" target="_blank">https://dx.doi.org/10.5194/acp-21-11303-2021</a></p>2021-07-28T03:00:00ZTextJournal contributioninfo:eu-repo/semantics/publishedVersiontextcontribution to journal10.5194/acp-21-11303-2021https://figshare.com/articles/journal_contribution/Phase_state_of_secondary_organic_aerosol_in_chamber_photo-oxidation_of_mixed_precursors/25771524CC BY 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/257715242021-07-28T03:00:00Z
spellingShingle Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
Yu Wang (12152)
Earth sciences
Atmospheric sciences
Environmental sciences
Climate change impacts and adaptation
Aerosol phase behavior
Atmospheric physicochemical processes
Aerosol rebounding tendency
Bounce fraction
Secondary organic aerosol (SOA)
Volatile organic compounds (VOCs)
Deliquescent ammonium sulfate seed
Relative humidity (RH)
status_str publishedVersion
title Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
title_full Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
title_fullStr Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
title_full_unstemmed Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
title_short Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
title_sort Phase state of secondary organic aerosol in chamber photo-oxidation of mixed precursors
topic Earth sciences
Atmospheric sciences
Environmental sciences
Climate change impacts and adaptation
Aerosol phase behavior
Atmospheric physicochemical processes
Aerosol rebounding tendency
Bounce fraction
Secondary organic aerosol (SOA)
Volatile organic compounds (VOCs)
Deliquescent ammonium sulfate seed
Relative humidity (RH)