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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Main Authors: 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
Format: Article
Language:English
Published: Nature Portfolio 2023-06-01
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.
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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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