Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility

Yu Wang; Ying Chen; Zhijun Wu; Dongjie Shang; Yuxuan Bian; Zhuofei Du; Sebastian H. Schmitt; Rong Su; Georgios I. Gkatzelis; Patrick Schlag; Thorsten Hohaus; Aristeidis Voliotis; Keding Lu; Limin Zeng; Chunsheng Zhao; M. Rami Alfarra; Gordon McFiggans; Alfred Wiedensohler; Astrid Kiendler-Scharr; Yuanhang Zhang; Min Hu

doi:10.5194/acp-20-2161-2020

Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility

Yu Wang^*
, Ying Chen
, Zhijun Wu
, Dongjie Shang
, Yuxuan Bian
, Zhuofei Du
, Sebastian H. Schmitt
, Rong Su
, Georgios I. Gkatzelis
, Patrick Schlag
, Thorsten Hohaus
, Aristeidis Voliotis
, Keding Lu
, Limin Zeng
, Chunsheng Zhao
, M. Rami Alfarra
, Gordon McFiggans
, Alfred Wiedensohler
, Astrid Kiendler-Scharr
, Yuanhang Zhang

Min Hu

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

93 Citations (Scopus)

Abstract

As has been the case in North America and western Europe, the <span classCombining double low line"inline-formula">SO2</span> emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in <span classCombining double low line"inline-formula">SO2</span> and <span classCombining double low line"inline-formula">NOx</span> concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (<span classCombining double low line"inline-formula"><math xmlnsCombining double low line"http://www.w3.org/1998/Math/MathML" idCombining double low line"M4" displayCombining double low line"inline" overflowCombining double low line"scroll" dspmathCombining double low line"mathml"><mrow classCombining double low line"chem"><mi>p</mi><msubsup><mi mathvariantCombining double low line"normal">NO</mi><mn mathvariantCombining double low line"normal">3</mn><mo>-</mo></msubsup></mrow></math><span><svg:svg xmlns:svgCombining double low line"http://www.w3.org/2000/svg" widthCombining double low line"32pt" heightCombining double low line"16pt" classCombining double low line"svg-formula" dspmathCombining double low line"mathimg" md5hashCombining double low line"80301589dd125f3933fea08fd04566b2"><svg:image xmlns:xlinkCombining double low line"http://www.w3.org/1999/xlink" xlink:hrefCombining double low line"acp-20-2161-2020-ie00001.svg" widthCombining double low line"32pt" heightCombining double low line"16pt" srcCombining double low line"acp-20-2161-2020-ie00001.png"/></svg:svg></span></span>) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM<span classCombining double low line"inline-formula">1</span> (NR-PM<span classCombining double low line"inline-formula">1</span>) being up to 44 % during wintertime in Beijing. Based on this typical <span classCombining double low line"inline-formula"><math xmlnsCombining double low line"http://www.w3.org/1998/Math/MathML" idCombining double low line"M7" displayCombining double low line"inline" overflowCombining double low line"scroll" dspmathCombining double low line"mathml"><mrow classCombining double low line"chem"><mi>p</mi><msubsup><mi mathvariantCombining double low line"normal">NO</mi><mn mathvariantCombining double low line"normal">3</mn><mo>-</mo></msubsup></mrow></math><span><svg:svg xmlns:svgCombining double low line"http://www.w3.org/2000/svg" widthCombining double low line"32pt" heightCombining double low line"16pt" classCombining double low line"svg-formula" dspmathCombining double low line"mathimg" md5hashCombining double low line"97eee6abb7442c3dca576c5397fcf50b"><svg:image xmlns:xlinkCombining double low line"http://www.w3.org/1999/xlink" xlink:hrefCombining double low line"acp-20-2161-2020-ie00002.svg" widthCombining double low line"32pt" heightCombining double low line"16pt" srcCombining double low line"acp-20-2161-2020-ie00002.png"/></svg:svg></span></span>-dominated haze event, the linkage between aerosol water uptake and <span classCombining double low line"inline-formula"><math xmlnsCombining double low line"http://www.w3.org/1998/Math/MathML" idCombining double low line"M8" displayCombining double low line"inline" overflowCombining double low line"scroll" dspmathCombining double low line"mathml"><mrow classCombining double low line"chem"><mi>p</mi><msubsup><mi mathvariantCombining double low line"normal">NO</mi><mn mathvariantCombining double low line"normal">3</mn><mo>-</mo></msubsup></mrow></math><span><svg:svg xmlns:svgCombining double low line"http://www.w3.org/2000/svg" widthCombining double low line"32pt" heightCombining double low line"16pt" classCombining double low line"svg-formula" dspmathCombining double low line"mathimg" md5hashCombining double low line"bf993075addbdcb9c5e94dd00bb6267c"><svg:image xmlns:xlinkCombining double low line"http://www.w3.org/1999/xlink" xlink:hrefCombining double low line"acp-20-2161-2020-ie00003.svg" widthCombining double low line"32pt" heightCombining double low line"16pt" srcCombining double low line"acp-20-2161-2020-ie00003.png"/></svg:svg></span></span> enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from <span classCombining double low line"inline-formula">ĝ1/410</span> % to 70 %, the aerosol particle liquid water increased from <span classCombining double low line"inline-formula">ĝ1/41</span> <span classCombining double low line"inline-formula">μg m-3</span> at the beginning to <span classCombining double low line"inline-formula">ĝ1/475</span> <span classCombining double low line"inline-formula">μg m-3</span> in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of <span classCombining double low line"inline-formula">N2O5</span> over particles. From the beginning to the fully developed haze, the condensational loss of <span classCombining double low line"inline-formula">N2O5</span> increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of <span classCombining double low line"inline-formula">HNO3</span> in the particle phase under the supersaturated <span classCombining double low line"inline-formula">HNO3</span> and <span classCombining double low line"inline-formula">NH3</span> in the atmosphere. All the above results demonstrated that <span classCombining double low line"inline-formula"><math xmlnsCombining double low line"http://www.w3.org/1998/Math/MathML" idCombining double low line"M19" displayCombining double low line"inline" overflowCombining double low line"scroll" dspmathCombining double low line"mathml"><mrow classCombining double low line"chem"><mi>p</mi><msubsup><mi mathvariantCombining double low line"normal">NO</mi><mn mathvariantCombining double low line"normal">3</mn><mo>-</mo></msubsup></mrow></math><span><svg:svg xmlns:svgCombining double low line"http://www.w3.org/2000/svg" widthCombining double low line"32pt" heightCombining double low line"16pt" classCombining double low line"svg-formula" dspmathCombining double low line"mathimg" md5hashCombining double low line"90de1192fbdc093890377c47914f9681"><svg:image xmlns:xlinkCombining double low line"http://www.w3.org/1999/xlink" xlink:hrefCombining double low line"acp-20-2161-2020-ie00004.svg" widthCombining double low line"32pt" heightCombining double low line"16pt" srcCombining double low line"acp-20-2161-2020-ie00004.png"/></svg:svg></span></span> is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP.

Original language	English
Pages (from-to)	2161-2175
Number of pages	15
Journal	Atmospheric Chemistry and Physics
Volume	20
Issue number	4
DOIs	https://doi.org/10.5194/acp-20-2161-2020
Publication status	Published - 26 Feb 2020
Externally published	Yes

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Wang, Y., Chen, Y., Wu, Z., Shang, D., Bian, Y., Du, Z., H. Schmitt, S., Su, R., I. Gkatzelis, G., Schlag, P., Hohaus, T., Voliotis, A., Lu, K., Zeng, L., Zhao, C., Rami Alfarra, M., McFiggans, G., Wiedensohler, A., Kiendler-Scharr, A., ... Hu, M. (2020). Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility. Atmospheric Chemistry and Physics, 20(4), 2161-2175. https://doi.org/10.5194/acp-20-2161-2020

@article{64caa8d197ec43c9ab74ddc1610c6a0d,

title = "Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility",

abstract = "As has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO3-) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM1 (NR-PM1) being up to 44\ \% during wintertime in Beijing. Based on this typical pNO3--dominated haze event, the linkage between aerosol water uptake and pNO3- enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ĝ1/410\ \% to 70\ \%, the aerosol particle liquid water increased from ĝ1/41\ μg m-3 at the beginning to ĝ1/475\ μg m-3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO3- is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1\ d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP.",

author = "Yu Wang and Ying Chen and Zhijun Wu and Dongjie Shang and Yuxuan Bian and Zhuofei Du and \{H. Schmitt\}, Sebastian and Rong Su and \{I. Gkatzelis\}, Georgios and Patrick Schlag and Thorsten Hohaus and Aristeidis Voliotis and Keding Lu and Limin Zeng and Chunsheng Zhao and \{Rami Alfarra\}, M. and Gordon McFiggans and Alfred Wiedensohler and Astrid Kiendler-Scharr and Yuanhang Zhang and Min Hu",

note = "Publisher Copyright: {\textcopyright} 2020. This work is distributed under the Creative Commons Attribution 4.0 License.",

year = "2020",

month = feb,

day = "26",

doi = "10.5194/acp-20-2161-2020",

language = "English",

volume = "20",

pages = "2161--2175",

journal = "Atmospheric Chemistry and Physics",

issn = "1680-7316",

publisher = "Copernicus Publications",

number = "4",

}

Wang, Y, Chen, Y, Wu, Z, Shang, D, Bian, Y, Du, Z, H. Schmitt, S, Su, R, I. Gkatzelis, G, Schlag, P, Hohaus, T, Voliotis, A, Lu, K, Zeng, L, Zhao, C, Rami Alfarra, M, McFiggans, G, Wiedensohler, A, Kiendler-Scharr, A, Zhang, Y & Hu, M 2020, 'Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility', Atmospheric Chemistry and Physics, vol. 20, no. 4, pp. 2161-2175. https://doi.org/10.5194/acp-20-2161-2020

TY - JOUR

T1 - Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility

AU - Wang, Yu

AU - Chen, Ying

AU - Wu, Zhijun

AU - Shang, Dongjie

AU - Bian, Yuxuan

AU - Du, Zhuofei

AU - H. Schmitt, Sebastian

AU - Su, Rong

AU - I. Gkatzelis, Georgios

AU - Schlag, Patrick

AU - Hohaus, Thorsten

AU - Voliotis, Aristeidis

AU - Lu, Keding

AU - Zeng, Limin

AU - Zhao, Chunsheng

AU - Rami Alfarra, M.

AU - McFiggans, Gordon

AU - Wiedensohler, Alfred

AU - Kiendler-Scharr, Astrid

AU - Zhang, Yuanhang

AU - Hu, Min

PY - 2020/2/26

Y1 - 2020/2/26

N2 - As has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO3-) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM1 (NR-PM1) being up to 44 % during wintertime in Beijing. Based on this typical pNO3--dominated haze event, the linkage between aerosol water uptake and pNO3- enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ĝ1/410 % to 70 %, the aerosol particle liquid water increased from ĝ1/41 μg m-3 at the beginning to ĝ1/475 μg m-3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO3- is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP.

AB - As has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO3-) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM1 (NR-PM1) being up to 44 % during wintertime in Beijing. Based on this typical pNO3--dominated haze event, the linkage between aerosol water uptake and pNO3- enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ĝ1/410 % to 70 %, the aerosol particle liquid water increased from ĝ1/41 μg m-3 at the beginning to ĝ1/475 μg m-3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO3- is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP.

UR - https://www.scopus.com/pages/publications/85080946572

U2 - 10.5194/acp-20-2161-2020

DO - 10.5194/acp-20-2161-2020

M3 - Article

AN - SCOPUS:85080946572

SN - 1680-7316

VL - 20

SP - 2161

EP - 2175

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 4

ER -

Mutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility

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