A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing

Yiqun Lu, Chao Yan, Yueyun Fu, Yan Chen, Yiliang Liu, Gan Yang, Yuwei Wang, Federico Bianchi, Biwu Chu, Ying Zhou, Rujing Yin, Rima Baalbaki, Olga Garmash, Chenjuan Deng, Weigang Wang, Yongchun Liu, Tuukka Petäjä, Veli-Matti Kerminen, Jingkun Jiang, Markku Kulmala & 1 andra Lin Wang

Forskningsoutput: TidskriftsbidragArtikelVetenskapligPeer review

Sammanfattning

Gaseous sulfuric acid (H2SO4) is known as one of the key precursors for atmospheric new particle formation (NPF) processes, but its measurement remains challenging. Therefore, a proxy method that is able to derive gaseous sulfuric acid concentrations from parameters that can be measured relatively easily and accurately is highly desirable for the atmospheric chemistry community. Although such methods are available for clean atmospheric environments, a proxy that works well in a polluted atmosphere, such as that found in Chinese megacities, is yet to be developed. In this study, the gaseous sulfuric acid concentration was measured in February-March 2018, in urban Beijing using a nitrate based -long time-of-flight chemical ionization mass spectrometer (LToF-CIMS). A number of atmospheric parameters were recorded concurrently including the ultraviolet radiation B (UVB) intensity, the concentrations of O-3, NOx (sum of NO and NO2), SO2, and HONO, and aerosol particle number size distributions. A proxy for atmospheric daytime gaseous sulfuric acid concentration was derived via a statistical analysis method using the UVB intensity, [SO2], the condensation sink (CS), [O-3], and [HONO] (or [NOx]) as the predictor variables, where square brackets denote the concentrations of the corresponding species. In this proxy method, we considered the formation of gaseous sulfuric acid from reactions of SO2 and OH radicals during the daytime, and the loss of gaseous sulfuric acid due to its condensation onto the preexisting particles. In addition, we explored the formation of OH radicals from the conventional gas-phase photochemistry using O-3 as a proxy and from the photolysis of HONO using HONO (and subsequently NOx) as a proxy. Our results showed that the UVB intensity and [SO2] are dominant factors in the production of gaseous sulfuric acid, and that the simplest proxy could be constructed with the UVB intensity and [SO2] alone. When the OH radical production from both homogenously and heterogeneously formed precursors were considered, the relative errors were reduced by up to 20 %.
Originalspråkengelska
TidskriftAtmospheric Chemistry and Physics
Volym19
Utgåva3
Sidor (från-till)1971-1983
Antal sidor13
ISSN1680-7316
DOI
StatusPublicerad - 13 feb 2019
MoE-publikationstypA1 Tidskriftsartikel-refererad

Vetenskapsgrenar

  • 1172 Miljövetenskap
  • 114 Fysik
  • 116 Kemi

Citera det här

Lu, Yiqun ; Yan, Chao ; Fu, Yueyun ; Chen, Yan ; Liu, Yiliang ; Yang, Gan ; Wang, Yuwei ; Bianchi, Federico ; Chu, Biwu ; Zhou, Ying ; Yin, Rujing ; Baalbaki, Rima ; Garmash, Olga ; Deng, Chenjuan ; Wang, Weigang ; Liu, Yongchun ; Petäjä, Tuukka ; Kerminen, Veli-Matti ; Jiang, Jingkun ; Kulmala, Markku ; Wang, Lin. / A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing. I: Atmospheric Chemistry and Physics. 2019 ; Vol. 19, Nr. 3. s. 1971-1983.
@article{9ee4da9df63747099c0090792d8a06bf,
title = "A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing",
abstract = "Gaseous sulfuric acid (H2SO4) is known as one of the key precursors for atmospheric new particle formation (NPF) processes, but its measurement remains challenging. Therefore, a proxy method that is able to derive gaseous sulfuric acid concentrations from parameters that can be measured relatively easily and accurately is highly desirable for the atmospheric chemistry community. Although such methods are available for clean atmospheric environments, a proxy that works well in a polluted atmosphere, such as that found in Chinese megacities, is yet to be developed. In this study, the gaseous sulfuric acid concentration was measured in February-March 2018, in urban Beijing using a nitrate based -long time-of-flight chemical ionization mass spectrometer (LToF-CIMS). A number of atmospheric parameters were recorded concurrently including the ultraviolet radiation B (UVB) intensity, the concentrations of O-3, NOx (sum of NO and NO2), SO2, and HONO, and aerosol particle number size distributions. A proxy for atmospheric daytime gaseous sulfuric acid concentration was derived via a statistical analysis method using the UVB intensity, [SO2], the condensation sink (CS), [O-3], and [HONO] (or [NOx]) as the predictor variables, where square brackets denote the concentrations of the corresponding species. In this proxy method, we considered the formation of gaseous sulfuric acid from reactions of SO2 and OH radicals during the daytime, and the loss of gaseous sulfuric acid due to its condensation onto the preexisting particles. In addition, we explored the formation of OH radicals from the conventional gas-phase photochemistry using O-3 as a proxy and from the photolysis of HONO using HONO (and subsequently NOx) as a proxy. Our results showed that the UVB intensity and [SO2] are dominant factors in the production of gaseous sulfuric acid, and that the simplest proxy could be constructed with the UVB intensity and [SO2] alone. When the OH radical production from both homogenously and heterogeneously formed precursors were considered, the relative errors were reduced by up to 20 {\%}.",
keywords = "IONIZATION MASS-SPECTROMETER, NITROUS-ACID, PARTICLE FORMATION, NUCLEATION, HONO, H2SO4, GAS, NM, CHEMISTRY, GROWTH, 1172 Environmental sciences, 114 Physical sciences, 116 Chemical sciences",
author = "Yiqun Lu and Chao Yan and Yueyun Fu and Yan Chen and Yiliang Liu and Gan Yang and Yuwei Wang and Federico Bianchi and Biwu Chu and Ying Zhou and Rujing Yin and Rima Baalbaki and Olga Garmash and Chenjuan Deng and Weigang Wang and Yongchun Liu and Tuukka Pet{\"a}j{\"a} and Veli-Matti Kerminen and Jingkun Jiang and Markku Kulmala and Lin Wang",
year = "2019",
month = "2",
day = "13",
doi = "10.5194/acp-19-1971-2019",
language = "English",
volume = "19",
pages = "1971--1983",
journal = "Atmospheric Chemistry and Physics",
issn = "1680-7316",
publisher = "COPERNICUS GESELLSCHAFT MBH",
number = "3",

}

A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing. / Lu, Yiqun; Yan, Chao; Fu, Yueyun; Chen, Yan; Liu, Yiliang; Yang, Gan; Wang, Yuwei; Bianchi, Federico; Chu, Biwu; Zhou, Ying; Yin, Rujing; Baalbaki, Rima; Garmash, Olga; Deng, Chenjuan; Wang, Weigang; Liu, Yongchun; Petäjä, Tuukka; Kerminen, Veli-Matti; Jiang, Jingkun; Kulmala, Markku; Wang, Lin.

I: Atmospheric Chemistry and Physics, Vol. 19, Nr. 3, 13.02.2019, s. 1971-1983.

Forskningsoutput: TidskriftsbidragArtikelVetenskapligPeer review

TY - JOUR

T1 - A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing

AU - Lu, Yiqun

AU - Yan, Chao

AU - Fu, Yueyun

AU - Chen, Yan

AU - Liu, Yiliang

AU - Yang, Gan

AU - Wang, Yuwei

AU - Bianchi, Federico

AU - Chu, Biwu

AU - Zhou, Ying

AU - Yin, Rujing

AU - Baalbaki, Rima

AU - Garmash, Olga

AU - Deng, Chenjuan

AU - Wang, Weigang

AU - Liu, Yongchun

AU - Petäjä, Tuukka

AU - Kerminen, Veli-Matti

AU - Jiang, Jingkun

AU - Kulmala, Markku

AU - Wang, Lin

PY - 2019/2/13

Y1 - 2019/2/13

N2 - Gaseous sulfuric acid (H2SO4) is known as one of the key precursors for atmospheric new particle formation (NPF) processes, but its measurement remains challenging. Therefore, a proxy method that is able to derive gaseous sulfuric acid concentrations from parameters that can be measured relatively easily and accurately is highly desirable for the atmospheric chemistry community. Although such methods are available for clean atmospheric environments, a proxy that works well in a polluted atmosphere, such as that found in Chinese megacities, is yet to be developed. In this study, the gaseous sulfuric acid concentration was measured in February-March 2018, in urban Beijing using a nitrate based -long time-of-flight chemical ionization mass spectrometer (LToF-CIMS). A number of atmospheric parameters were recorded concurrently including the ultraviolet radiation B (UVB) intensity, the concentrations of O-3, NOx (sum of NO and NO2), SO2, and HONO, and aerosol particle number size distributions. A proxy for atmospheric daytime gaseous sulfuric acid concentration was derived via a statistical analysis method using the UVB intensity, [SO2], the condensation sink (CS), [O-3], and [HONO] (or [NOx]) as the predictor variables, where square brackets denote the concentrations of the corresponding species. In this proxy method, we considered the formation of gaseous sulfuric acid from reactions of SO2 and OH radicals during the daytime, and the loss of gaseous sulfuric acid due to its condensation onto the preexisting particles. In addition, we explored the formation of OH radicals from the conventional gas-phase photochemistry using O-3 as a proxy and from the photolysis of HONO using HONO (and subsequently NOx) as a proxy. Our results showed that the UVB intensity and [SO2] are dominant factors in the production of gaseous sulfuric acid, and that the simplest proxy could be constructed with the UVB intensity and [SO2] alone. When the OH radical production from both homogenously and heterogeneously formed precursors were considered, the relative errors were reduced by up to 20 %.

AB - Gaseous sulfuric acid (H2SO4) is known as one of the key precursors for atmospheric new particle formation (NPF) processes, but its measurement remains challenging. Therefore, a proxy method that is able to derive gaseous sulfuric acid concentrations from parameters that can be measured relatively easily and accurately is highly desirable for the atmospheric chemistry community. Although such methods are available for clean atmospheric environments, a proxy that works well in a polluted atmosphere, such as that found in Chinese megacities, is yet to be developed. In this study, the gaseous sulfuric acid concentration was measured in February-March 2018, in urban Beijing using a nitrate based -long time-of-flight chemical ionization mass spectrometer (LToF-CIMS). A number of atmospheric parameters were recorded concurrently including the ultraviolet radiation B (UVB) intensity, the concentrations of O-3, NOx (sum of NO and NO2), SO2, and HONO, and aerosol particle number size distributions. A proxy for atmospheric daytime gaseous sulfuric acid concentration was derived via a statistical analysis method using the UVB intensity, [SO2], the condensation sink (CS), [O-3], and [HONO] (or [NOx]) as the predictor variables, where square brackets denote the concentrations of the corresponding species. In this proxy method, we considered the formation of gaseous sulfuric acid from reactions of SO2 and OH radicals during the daytime, and the loss of gaseous sulfuric acid due to its condensation onto the preexisting particles. In addition, we explored the formation of OH radicals from the conventional gas-phase photochemistry using O-3 as a proxy and from the photolysis of HONO using HONO (and subsequently NOx) as a proxy. Our results showed that the UVB intensity and [SO2] are dominant factors in the production of gaseous sulfuric acid, and that the simplest proxy could be constructed with the UVB intensity and [SO2] alone. When the OH radical production from both homogenously and heterogeneously formed precursors were considered, the relative errors were reduced by up to 20 %.

KW - IONIZATION MASS-SPECTROMETER

KW - NITROUS-ACID

KW - PARTICLE FORMATION

KW - NUCLEATION

KW - HONO

KW - H2SO4

KW - GAS

KW - NM

KW - CHEMISTRY

KW - GROWTH

KW - 1172 Environmental sciences

KW - 114 Physical sciences

KW - 116 Chemical sciences

U2 - 10.5194/acp-19-1971-2019

DO - 10.5194/acp-19-1971-2019

M3 - Article

VL - 19

SP - 1971

EP - 1983

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

SN - 1680-7316

IS - 3

ER -