Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain

<p>The variability of the mixing state of refractory black carbon aerosol (<span class="inline-formula"><i>r</i></span>BC) and the corresponding complicated light absorption capacity imposes great uncertainty for its climate forcing assessment. In this study,...

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Autores principales: Y. Zhang, H. Liu, S. Lei, W. Xu, Y. Tian, W. Yao, X. Liu, Q. Liao, J. Li, C. Chen, Y. Sun, P. Fu, J. Xin, J. Cao, X. Pan, Z. Wang
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Publicado: Copernicus Publications 2021
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Acceso en línea:https://doaj.org/article/339b1de701884e65878789d4754b413c
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id oai:doaj.org-article:339b1de701884e65878789d4754b413c
record_format dspace
institution DOAJ
collection DOAJ
language EN
topic Physics
QC1-999
Chemistry
QD1-999
spellingShingle Physics
QC1-999
Chemistry
QD1-999
Y. Zhang
Y. Zhang
H. Liu
H. Liu
S. Lei
S. Lei
W. Xu
Y. Tian
Y. Tian
W. Yao
W. Yao
X. Liu
X. Liu
X. Liu
Q. Liao
Q. Liao
J. Li
C. Chen
C. Chen
Y. Sun
Y. Sun
Y. Sun
P. Fu
J. Xin
J. Xin
J. Xin
J. Cao
X. Pan
Z. Wang
Z. Wang
Z. Wang
Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain
description <p>The variability of the mixing state of refractory black carbon aerosol (<span class="inline-formula"><i>r</i></span>BC) and the corresponding complicated light absorption capacity imposes great uncertainty for its climate forcing assessment. In this study, field observations using a single-particle soot photometer (SP2) were conducted to investigate the mixing state of <span class="inline-formula"><i>r</i></span>BC under different meteorological conditions at a rural site on the North China Plain. The results showed that the hourly mass concentration of <span class="inline-formula"><i>r</i></span>BC during the observation periods was <span class="inline-formula">2.6±1.5</span> <span class="inline-formula">µg m<sup>−3</sup></span> on average, with a moderate increase (<span class="inline-formula">3.1±0.9</span>) during fog episodes. The mass-equivalent size distribution of <span class="inline-formula"><i>r</i></span>BC exhibited an approximately lognormal distribution with a mass median diameter (MMD) of 213 <span class="inline-formula">nm</span>. We found that the count median diameter (CMD) of <span class="inline-formula"><i>r</i></span>BC particles during snowfall episodes was larger than that before snowfall, and the number of <span class="inline-formula"><i>r</i></span>BC particles with <span class="inline-formula"><i>D</i><sub>c</sub>&lt;121</span> <span class="inline-formula">nm</span> were reduced by 28.4 <span class="inline-formula">%</span> after snow. This may indicate that <span class="inline-formula"><i>r</i></span>BC-containing particles with small core sizes (<span class="inline-formula"><i>D</i><sub>c</sub></span>) were much more effectively removed by snow with light snow intensity (0.23 <span class="inline-formula">mm h<sup>−1</sup></span>). Based on the Mie scattering theory simulation, the relative and absolute coating thicknesses of <span class="inline-formula"><i>r</i></span>BC-containing particles were estimated to be <span class="inline-formula">∼1.6</span> and <span class="inline-formula">∼52</span> <span class="inline-formula">nm</span> for the <span class="inline-formula"><i>r</i></span>BC core with a mass-equivalent diameter (<span class="inline-formula"><i>D</i><sub>c</sub></span>) of 170 to 190 <span class="inline-formula">nm</span>, respectively, which indicates that most of the <span class="inline-formula"><i>r</i></span>BC-containing particles were thinly coated. Furthermore, a moderate light absorption enhancement (<span class="inline-formula"><i>E</i><sub>abs</sub>=1.3</span>) and relatively low absorption cross section (MAC <span class="inline-formula">=</span> 5.5 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span>) at 880 <span class="inline-formula">nm</span> were observed at the Gucheng (GC) site in winter compared with other typical rural sites.</p> <p><span id="page17632"/>The relationship between the microphysical properties of <span class="inline-formula"><i>r</i></span>BC and meteorological conditions was also studied. Relatively warm and high-RH environments (<span class="inline-formula">RH&gt;50 <i>%</i></span>, <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M31" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">4</mn><mspace width="0.125em" linebreak="nobreak"/><mrow class="unit"><msup><mi/><mo>∘</mo></msup><mi mathvariant="normal">C</mi></mrow><mo>&lt;</mo><mi>T</mi><mo>&lt;</mo><mn mathvariant="normal">4</mn><mspace linebreak="nobreak" width="0.125em"/><mrow class="unit"><msup><mi/><mo>∘</mo></msup><mi mathvariant="normal">C</mi></mrow></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="80pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="5813c5afe23174f6f9e14a25ade99371"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-21-17631-2021-ie00001.svg" width="80pt" height="11pt" src="acp-21-17631-2021-ie00001.png"/></svg:svg></span></span>) were more favorable to <span class="inline-formula"><i>r</i></span>BC aging than dry and cold environments (<span class="inline-formula">RH&lt;60 <i>%</i></span>, <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M34" display="inline" overflow="scroll" dspmath="mathml"><mrow><mi>T</mi><mo>&lt;</mo><mo>-</mo><mn mathvariant="normal">8</mn><mspace width="0.125em" linebreak="nobreak"/><mrow class="unit"><msup><mi/><mo>∘</mo></msup><mi mathvariant="normal">C</mi></mrow></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="48pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="2f27c72cdc42b2b7f3e9a547bbeb00c6"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-21-17631-2021-ie00002.svg" width="48pt" height="11pt" src="acp-21-17631-2021-ie00002.png"/></svg:svg></span></span>). And the increase in ambient RH at the same temperature favors <span class="inline-formula"><i>r</i></span>BC aging. An increasing mass fraction of secondary inorganic aerosols (SIAs; especially sulfate and nitrate) and a decreasing mass fraction of organic aerosols in the environment support the formation of thick coatings by <span class="inline-formula"><i>r</i></span>BC. The RH dependence of absorption enhancement (<span class="inline-formula"><i>E</i><sub>abs</sub></span>) was likely caused by the relative coating thickness (RCT) as supported by the gradual increase in the mass concentration and mass fraction of secondary components as a function of RH in the ambient air. The mass fractions of aqueous-phase formation of secondary components had a limited effect on <span class="inline-formula"><i>E</i><sub>abs</sub></span> under a high-RH environment. The measured <span class="inline-formula"><i>r</i></span>BC concentrations and the mixing state of <span class="inline-formula"><i>r</i></span>BC in different meteorological environments will be useful for evaluating the radiative forcing of <span class="inline-formula"><i>r</i></span>BC in regional climate models.</p>
format article
author Y. Zhang
Y. Zhang
H. Liu
H. Liu
S. Lei
S. Lei
W. Xu
Y. Tian
Y. Tian
W. Yao
W. Yao
X. Liu
X. Liu
X. Liu
Q. Liao
Q. Liao
J. Li
C. Chen
C. Chen
Y. Sun
Y. Sun
Y. Sun
P. Fu
J. Xin
J. Xin
J. Xin
J. Cao
X. Pan
Z. Wang
Z. Wang
Z. Wang
author_facet Y. Zhang
Y. Zhang
H. Liu
H. Liu
S. Lei
S. Lei
W. Xu
Y. Tian
Y. Tian
W. Yao
W. Yao
X. Liu
X. Liu
X. Liu
Q. Liao
Q. Liao
J. Li
C. Chen
C. Chen
Y. Sun
Y. Sun
Y. Sun
P. Fu
J. Xin
J. Xin
J. Xin
J. Cao
X. Pan
Z. Wang
Z. Wang
Z. Wang
author_sort Y. Zhang
title Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain
title_short Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain
title_full Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain
title_fullStr Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain
title_full_unstemmed Mixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain
title_sort mixing state of refractory black carbon in fog and haze at rural sites in winter on the north china plain
publisher Copernicus Publications
publishDate 2021
url https://doaj.org/article/339b1de701884e65878789d4754b413c
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spelling oai:doaj.org-article:339b1de701884e65878789d4754b413c2021-12-03T11:08:18ZMixing state of refractory black carbon in fog and haze at rural sites in winter on the North China Plain10.5194/acp-21-17631-20211680-73161680-7324https://doaj.org/article/339b1de701884e65878789d4754b413c2021-12-01T00:00:00Zhttps://acp.copernicus.org/articles/21/17631/2021/acp-21-17631-2021.pdfhttps://doaj.org/toc/1680-7316https://doaj.org/toc/1680-7324<p>The variability of the mixing state of refractory black carbon aerosol (<span class="inline-formula"><i>r</i></span>BC) and the corresponding complicated light absorption capacity imposes great uncertainty for its climate forcing assessment. In this study, field observations using a single-particle soot photometer (SP2) were conducted to investigate the mixing state of <span class="inline-formula"><i>r</i></span>BC under different meteorological conditions at a rural site on the North China Plain. The results showed that the hourly mass concentration of <span class="inline-formula"><i>r</i></span>BC during the observation periods was <span class="inline-formula">2.6±1.5</span> <span class="inline-formula">µg m<sup>−3</sup></span> on average, with a moderate increase (<span class="inline-formula">3.1±0.9</span>) during fog episodes. The mass-equivalent size distribution of <span class="inline-formula"><i>r</i></span>BC exhibited an approximately lognormal distribution with a mass median diameter (MMD) of 213 <span class="inline-formula">nm</span>. We found that the count median diameter (CMD) of <span class="inline-formula"><i>r</i></span>BC particles during snowfall episodes was larger than that before snowfall, and the number of <span class="inline-formula"><i>r</i></span>BC particles with <span class="inline-formula"><i>D</i><sub>c</sub>&lt;121</span> <span class="inline-formula">nm</span> were reduced by 28.4 <span class="inline-formula">%</span> after snow. This may indicate that <span class="inline-formula"><i>r</i></span>BC-containing particles with small core sizes (<span class="inline-formula"><i>D</i><sub>c</sub></span>) were much more effectively removed by snow with light snow intensity (0.23 <span class="inline-formula">mm h<sup>−1</sup></span>). Based on the Mie scattering theory simulation, the relative and absolute coating thicknesses of <span class="inline-formula"><i>r</i></span>BC-containing particles were estimated to be <span class="inline-formula">∼1.6</span> and <span class="inline-formula">∼52</span> <span class="inline-formula">nm</span> for the <span class="inline-formula"><i>r</i></span>BC core with a mass-equivalent diameter (<span class="inline-formula"><i>D</i><sub>c</sub></span>) of 170 to 190 <span class="inline-formula">nm</span>, respectively, which indicates that most of the <span class="inline-formula"><i>r</i></span>BC-containing particles were thinly coated. Furthermore, a moderate light absorption enhancement (<span class="inline-formula"><i>E</i><sub>abs</sub>=1.3</span>) and relatively low absorption cross section (MAC <span class="inline-formula">=</span> 5.5 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span>) at 880 <span class="inline-formula">nm</span> were observed at the Gucheng (GC) site in winter compared with other typical rural sites.</p> <p><span id="page17632"/>The relationship between the microphysical properties of <span class="inline-formula"><i>r</i></span>BC and meteorological conditions was also studied. Relatively warm and high-RH environments (<span class="inline-formula">RH&gt;50 <i>%</i></span>, <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M31" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">4</mn><mspace width="0.125em" linebreak="nobreak"/><mrow class="unit"><msup><mi/><mo>∘</mo></msup><mi mathvariant="normal">C</mi></mrow><mo>&lt;</mo><mi>T</mi><mo>&lt;</mo><mn mathvariant="normal">4</mn><mspace linebreak="nobreak" width="0.125em"/><mrow class="unit"><msup><mi/><mo>∘</mo></msup><mi mathvariant="normal">C</mi></mrow></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="80pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="5813c5afe23174f6f9e14a25ade99371"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-21-17631-2021-ie00001.svg" width="80pt" height="11pt" src="acp-21-17631-2021-ie00001.png"/></svg:svg></span></span>) were more favorable to <span class="inline-formula"><i>r</i></span>BC aging than dry and cold environments (<span class="inline-formula">RH&lt;60 <i>%</i></span>, <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M34" display="inline" overflow="scroll" dspmath="mathml"><mrow><mi>T</mi><mo>&lt;</mo><mo>-</mo><mn mathvariant="normal">8</mn><mspace width="0.125em" linebreak="nobreak"/><mrow class="unit"><msup><mi/><mo>∘</mo></msup><mi mathvariant="normal">C</mi></mrow></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="48pt" height="11pt" class="svg-formula" dspmath="mathimg" md5hash="2f27c72cdc42b2b7f3e9a547bbeb00c6"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-21-17631-2021-ie00002.svg" width="48pt" height="11pt" src="acp-21-17631-2021-ie00002.png"/></svg:svg></span></span>). And the increase in ambient RH at the same temperature favors <span class="inline-formula"><i>r</i></span>BC aging. An increasing mass fraction of secondary inorganic aerosols (SIAs; especially sulfate and nitrate) and a decreasing mass fraction of organic aerosols in the environment support the formation of thick coatings by <span class="inline-formula"><i>r</i></span>BC. The RH dependence of absorption enhancement (<span class="inline-formula"><i>E</i><sub>abs</sub></span>) was likely caused by the relative coating thickness (RCT) as supported by the gradual increase in the mass concentration and mass fraction of secondary components as a function of RH in the ambient air. The mass fractions of aqueous-phase formation of secondary components had a limited effect on <span class="inline-formula"><i>E</i><sub>abs</sub></span> under a high-RH environment. The measured <span class="inline-formula"><i>r</i></span>BC concentrations and the mixing state of <span class="inline-formula"><i>r</i></span>BC in different meteorological environments will be useful for evaluating the radiative forcing of <span class="inline-formula"><i>r</i></span>BC in regional climate models.</p>Y. ZhangY. ZhangH. LiuH. LiuS. LeiS. LeiW. XuY. TianY. TianW. YaoW. YaoX. LiuX. LiuX. LiuQ. LiaoQ. LiaoJ. LiC. ChenC. ChenY. SunY. SunY. SunP. FuJ. XinJ. XinJ. XinJ. CaoX. PanZ. WangZ. WangZ. WangCopernicus PublicationsarticlePhysicsQC1-999ChemistryQD1-999ENAtmospheric Chemistry and Physics, Vol 21, Pp 17631-17648 (2021)