Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels

<p>Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties in reproducing the variability in OA concentrations in polluted areas, hindering understandin...

Descripción completa

Guardado en:
Detalles Bibliográficos
Autores principales: R. Miao, Q. Chen, M. Shrivastava, Y. Chen, L. Zhang, J. Hu, Y. Zheng, K. Liao
Formato: article
Lenguaje:EN
Publicado: Copernicus Publications 2021
Materias:
Acceso en línea:https://doaj.org/article/4009ba894fa843e9b03b99578cd6bd35
Etiquetas: Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
id oai:doaj.org-article:4009ba894fa843e9b03b99578cd6bd35
record_format dspace
spelling oai:doaj.org-article:4009ba894fa843e9b03b99578cd6bd352021-11-04T06:33:35ZProcess-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels10.5194/acp-21-16183-20211680-73161680-7324https://doaj.org/article/4009ba894fa843e9b03b99578cd6bd352021-11-01T00:00:00Zhttps://acp.copernicus.org/articles/21/16183/2021/acp-21-16183-2021.pdfhttps://doaj.org/toc/1680-7316https://doaj.org/toc/1680-7324<p>Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties in reproducing the variability in OA concentrations in polluted areas, hindering understanding of the OA budget and sources. Herein, we apply both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model–observation comparisons. The base models generally underestimate the SOA concentrations in China. In the revised schemes, updates were made on the emissions, volatility distributions, and SOA yields of semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) and additional nitrous acid sources. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic SVOCs and IVOCs are the dominant source of SOA, with a contribution of over 50 % in most of China, which should be considered for pollution mitigation in the future. The residential sector may be the predominant source of SVOCs and IVOCs in winter, despite large uncertainty remaining in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More SVOC and IVOC measurements are needed to constrain their emissions. Besides, the results highlight the sensitivity of SOA to hydroxyl radical (OH) levels in winter in polluted environments. The addition of nitrous acid sources can lead to over 30 % greater SOA mass concentrations in winter in northern China. It is important to have good OH simulations in air quality models.</p>R. MiaoQ. ChenM. ShrivastavaY. ChenL. ZhangJ. HuY. ZhengK. LiaoCopernicus PublicationsarticlePhysicsQC1-999ChemistryQD1-999ENAtmospheric Chemistry and Physics, Vol 21, Pp 16183-16201 (2021)
institution DOAJ
collection DOAJ
language EN
topic Physics
QC1-999
Chemistry
QD1-999
spellingShingle Physics
QC1-999
Chemistry
QD1-999
R. Miao
Q. Chen
M. Shrivastava
Y. Chen
L. Zhang
J. Hu
Y. Zheng
K. Liao
Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
description <p>Organic aerosol (OA) is a major component of tropospheric submicron aerosol that contributes to air pollution and causes adverse effects on human health. Chemical transport models have difficulties in reproducing the variability in OA concentrations in polluted areas, hindering understanding of the OA budget and sources. Herein, we apply both process-based and observation-constrained schemes to simulate OA in GEOS-Chem. Comprehensive data sets of surface OA, OA components, secondary organic aerosol (SOA) precursors, and oxidants were used for model–observation comparisons. The base models generally underestimate the SOA concentrations in China. In the revised schemes, updates were made on the emissions, volatility distributions, and SOA yields of semivolatile and intermediate-volatility organic compounds (SVOCs and IVOCs) and additional nitrous acid sources. With all the model improvements, both the process-based and observation-constrained SOA schemes can reproduce the observed mass concentrations of SOA and show spatial and seasonal consistency with each other. Our best model simulations suggest that anthropogenic SVOCs and IVOCs are the dominant source of SOA, with a contribution of over 50 % in most of China, which should be considered for pollution mitigation in the future. The residential sector may be the predominant source of SVOCs and IVOCs in winter, despite large uncertainty remaining in the emissions of IVOCs from the residential sector in northern China. The industry sector is also an important source of IVOCs, especially in summer. More SVOC and IVOC measurements are needed to constrain their emissions. Besides, the results highlight the sensitivity of SOA to hydroxyl radical (OH) levels in winter in polluted environments. The addition of nitrous acid sources can lead to over 30 % greater SOA mass concentrations in winter in northern China. It is important to have good OH simulations in air quality models.</p>
format article
author R. Miao
Q. Chen
M. Shrivastava
Y. Chen
L. Zhang
J. Hu
Y. Zheng
K. Liao
author_facet R. Miao
Q. Chen
M. Shrivastava
Y. Chen
L. Zhang
J. Hu
Y. Zheng
K. Liao
author_sort R. Miao
title Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
title_short Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
title_full Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
title_fullStr Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
title_full_unstemmed Process-based and observation-constrained SOA simulations in China: the role of semivolatile and intermediate-volatility organic compounds and OH levels
title_sort process-based and observation-constrained soa simulations in china: the role of semivolatile and intermediate-volatility organic compounds and oh levels
publisher Copernicus Publications
publishDate 2021
url https://doaj.org/article/4009ba894fa843e9b03b99578cd6bd35
work_keys_str_mv AT rmiao processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT qchen processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT mshrivastava processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT ychen processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT lzhang processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT jhu processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT yzheng processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
AT kliao processbasedandobservationconstrainedsoasimulationsinchinatheroleofsemivolatileandintermediatevolatilityorganiccompoundsandohlevels
_version_ 1718445081003819008