New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling
Abstract Particulate 2-methyltetrols (2-MT) and 2-methylglyceric acid (2-MG) are typically used to indicate the abundance of isoprene-derived secondary organic aerosols (SOA). However, their formation and fate are not fully understood. In this study, we showed that particulate 2-MT and 2-MG collecte...
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Format: | Article |
Language: | English |
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Nature Portfolio
2023-06-01
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Series: | npj Climate and Atmospheric Science |
Online Access: | https://doi.org/10.1038/s41612-023-00394-3 |
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author | Jie Zhang Junyi Liu Xiang Ding Xiao He Tianle Zhang Mei Zheng Minsu Choi Gabriel Isaacman-VanWertz Lindsay Yee Haofei Zhang Pawel Misztal Allen H. Goldstein Alex B. Guenther Sri Hapsari Budisulistiorini Jason D. Surratt Elizabeth A. Stone Manish Shrivastava Dui Wu Jian Zhen Yu Qi Ying |
author_facet | Jie Zhang Junyi Liu Xiang Ding Xiao He Tianle Zhang Mei Zheng Minsu Choi Gabriel Isaacman-VanWertz Lindsay Yee Haofei Zhang Pawel Misztal Allen H. Goldstein Alex B. Guenther Sri Hapsari Budisulistiorini Jason D. Surratt Elizabeth A. Stone Manish Shrivastava Dui Wu Jian Zhen Yu Qi Ying |
author_sort | Jie Zhang |
collection | DOAJ |
description | Abstract Particulate 2-methyltetrols (2-MT) and 2-methylglyceric acid (2-MG) are typically used to indicate the abundance of isoprene-derived secondary organic aerosols (SOA). However, their formation and fate are not fully understood. In this study, we showed that particulate 2-MT and 2-MG collected at multiple monitoring sites under a wide range of atmospheric and emission conditions, with concentrations spanning six orders of magnitudes, are well reproduced with an expanded isoprene-SOA scheme implemented into the Community Multiscale Air Quality (CMAQ) model. The scheme considers their three-phase (gas-aqueous-organic phase) partitioning, formation from acid-driven multiphase reactions, and degradation by OH radicals in the gas and aqueous phases. The model results reveal that a non-aqueous formation pathway or direct biogenic emission is needed to supplement the commonly assumed acid-driven multiphase reaction process to explain the observed 2-MT concentrations. This missing pathway contributes to 20–40% of 2-MT in areas with aerosol pH<2 and more than 70% under less acidic conditions (pH~2–5), such as those encountered in the western US and China. The typical summertime gas-phase photochemical lifetimes of 2-MT and 2-MG are estimated to be 4–6 and 20–30 h, respectively, and their aqueous lifetimes are approximately 20–40 h. Our simulations show that predicted 2-MT is mainly influenced by its aqueous phase loss to OH, but 2-MG is more sensitive to gas phase OH loss due to the preferential partitioning of the two tracers in the aqueous and gas phases, respectively. |
first_indexed | 2024-03-13T04:51:51Z |
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id | doaj.art-c3a064137a6f4495ba3b51a928358805 |
institution | Directory Open Access Journal |
issn | 2397-3722 |
language | English |
last_indexed | 2024-03-13T04:51:51Z |
publishDate | 2023-06-01 |
publisher | Nature Portfolio |
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series | npj Climate and Atmospheric Science |
spelling | doaj.art-c3a064137a6f4495ba3b51a9283588052023-06-18T11:10:42ZengNature Portfolionpj Climate and Atmospheric Science2397-37222023-06-01611810.1038/s41612-023-00394-3New formation and fate of Isoprene SOA markers revealed by field data-constrained modelingJie Zhang0Junyi Liu1Xiang Ding2Xiao He3Tianle Zhang4Mei Zheng5Minsu Choi6Gabriel Isaacman-VanWertz7Lindsay Yee8Haofei Zhang9Pawel Misztal10Allen H. Goldstein11Alex B. Guenther12Sri Hapsari Budisulistiorini13Jason D. Surratt14Elizabeth A. Stone15Manish Shrivastava16Dui Wu17Jian Zhen Yu18Qi Ying19Zachary Department of Civil and Environmental Engineering, Texas A&M UniversityState Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking UniversityState Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry Chinese Academy of SciencesDivision of Environment & Sustainability, Hong Kong University of Science & TechnologyState Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking UniversityState Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking UniversityZachary Department of Civil and Environmental Engineering, Texas A&M UniversityDepartment of Civil and Environmental Engineering, Virginia Polytechnic Institute and State UniversityDepartment of Environmental Science, Policy and Management, University of CaliforniaDepartment of Chemistry, University of CaliforniaDepartment of Civil, Architectural and Environmental Engineering, University of Texas at AustinDepartment of Environmental Science, Policy and Management, University of CaliforniaDepartment of Earth System Science, University of CaliforniaDepartment of Environmental Sciences and Engineering, University of North Carolina at Chapel HillDepartment of Environmental Sciences and Engineering, University of North Carolina at Chapel HillDepartment of Chemistry, University of IowaPacific Northwest National LaboratoryInstitute of Mass Spectrometry and Atmospheric Environment, Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air Pollution, Jinan UniversityDivision of Environment & Sustainability, Hong Kong University of Science & TechnologyZachary Department of Civil and Environmental Engineering, Texas A&M UniversityAbstract Particulate 2-methyltetrols (2-MT) and 2-methylglyceric acid (2-MG) are typically used to indicate the abundance of isoprene-derived secondary organic aerosols (SOA). However, their formation and fate are not fully understood. In this study, we showed that particulate 2-MT and 2-MG collected at multiple monitoring sites under a wide range of atmospheric and emission conditions, with concentrations spanning six orders of magnitudes, are well reproduced with an expanded isoprene-SOA scheme implemented into the Community Multiscale Air Quality (CMAQ) model. The scheme considers their three-phase (gas-aqueous-organic phase) partitioning, formation from acid-driven multiphase reactions, and degradation by OH radicals in the gas and aqueous phases. The model results reveal that a non-aqueous formation pathway or direct biogenic emission is needed to supplement the commonly assumed acid-driven multiphase reaction process to explain the observed 2-MT concentrations. This missing pathway contributes to 20–40% of 2-MT in areas with aerosol pH<2 and more than 70% under less acidic conditions (pH~2–5), such as those encountered in the western US and China. The typical summertime gas-phase photochemical lifetimes of 2-MT and 2-MG are estimated to be 4–6 and 20–30 h, respectively, and their aqueous lifetimes are approximately 20–40 h. Our simulations show that predicted 2-MT is mainly influenced by its aqueous phase loss to OH, but 2-MG is more sensitive to gas phase OH loss due to the preferential partitioning of the two tracers in the aqueous and gas phases, respectively.https://doi.org/10.1038/s41612-023-00394-3 |
spellingShingle | Jie Zhang Junyi Liu Xiang Ding Xiao He Tianle Zhang Mei Zheng Minsu Choi Gabriel Isaacman-VanWertz Lindsay Yee Haofei Zhang Pawel Misztal Allen H. Goldstein Alex B. Guenther Sri Hapsari Budisulistiorini Jason D. Surratt Elizabeth A. Stone Manish Shrivastava Dui Wu Jian Zhen Yu Qi Ying New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling npj Climate and Atmospheric Science |
title | New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling |
title_full | New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling |
title_fullStr | New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling |
title_full_unstemmed | New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling |
title_short | New formation and fate of Isoprene SOA markers revealed by field data-constrained modeling |
title_sort | new formation and fate of isoprene soa markers revealed by field data constrained modeling |
url | https://doi.org/10.1038/s41612-023-00394-3 |
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