The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China
<p>The heterogeneous reaction of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> on Cl-containing aerosols (heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> &l...
| Main Authors: | , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2022-03-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/22/3743/2022/acp-22-3743-2022.pdf |
| _version_ | 1811273385052733440 |
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| author | X. Yang X. Yang Q. Wang Q. Wang N. Ma N. Ma W. Hu Y. Gao Z. Huang Z. Huang J. Zheng J. Zheng B. Yuan B. Yuan N. Yang N. Yang J. Tao J. Tao J. Hong J. Hong Y. Cheng H. Su |
| author_facet | X. Yang X. Yang Q. Wang Q. Wang N. Ma N. Ma W. Hu Y. Gao Z. Huang Z. Huang J. Zheng J. Zheng B. Yuan B. Yuan N. Yang N. Yang J. Tao J. Tao J. Hong J. Hong Y. Cheng H. Su |
| author_sort | X. Yang |
| collection | DOAJ |
| description | <p>The heterogeneous reaction of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> on Cl-containing aerosols (heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry) plays a key
role in chlorine activation, <span class="inline-formula">NO<sub><i>x</i></sub></span> recycling, and consequently <span class="inline-formula">O<sub>3</sub></span> and <span class="inline-formula">PM<sub>2.5</sub></span> formation. In this study, we use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry (i.e., the uptake coefficient of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M14" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">γ</mi><mrow class="chem"><msub><mi mathvariant="normal">N</mi><mn mathvariant="normal">2</mn></msub><msub><mi mathvariant="normal">O</mi><mn mathvariant="normal">5</mn></msub></mrow></msub></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="27pt" height="12pt" class="svg-formula" dspmath="mathimg" md5hash="3e69fa10f182be73e59bb5210ffccfe1"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00001.svg" width="27pt" height="12pt" src="acp-22-3743-2022-ie00001.png"/></svg:svg></span></span>) and the <span class="inline-formula">ClNO<sub>2</sub></span> yield (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M16" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">φ</mi><mrow class="chem"><msub><mi mathvariant="normal">ClNO</mi><mn mathvariant="normal">2</mn></msub></mrow></msub><mo>)</mo></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="38pt" height="15pt" class="svg-formula" dspmath="mathimg" md5hash="b573a3eb5ede5dc2cbb2d4ef9b26d387"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00002.svg" width="38pt" height="15pt" src="acp-22-3743-2022-ie00002.png"/></svg:svg></span></span>) to investigate the impacts of chlorine chemistry on air quality in China, the role of the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry, and the sensitivity of air pollution formation to chlorine emissions and parameterizations for <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M20" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">γ</mi><mrow class="chem"><msub><mi mathvariant="normal">N</mi><mn mathvariant="normal">2</mn></msub><msub><mi mathvariant="normal">O</mi><mn mathvariant="normal">5</mn></msub></mrow></msub></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="27pt" height="12pt" class="svg-formula" dspmath="mathimg" md5hash="7e2119a0a3269eeae62343c97b7f8c6a"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00003.svg" width="27pt" height="12pt" src="acp-22-3743-2022-ie00003.png"/></svg:svg></span></span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M21" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">φ</mi><mrow class="chem"><msub><mi mathvariant="normal">ClNO</mi><mn mathvariant="normal">2</mn></msub></mrow></msub></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="34pt" height="12pt" class="svg-formula" dspmath="mathimg" md5hash="3ca77ac30eaf51dee14f652eb6f1039a"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00004.svg" width="34pt" height="12pt" src="acp-22-3743-2022-ie00004.png"/></svg:svg></span></span>. The model simulations are evaluated against multiple observational datasets across China and show significant improvement in reproducing observations of particulate chloride, <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span>, and <span class="inline-formula">ClNO<sub>2</sub></span> when including anthropogenic chlorine emissions and updates to the parameterization of the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry relative to the default model. The simulations show that total tropospheric chlorine chemistry could increase annual mean maximum daily 8 <span class="inline-formula">h</span> average (MDA8) <span class="inline-formula">O<sub>3</sub></span> by up to 4.5 <span class="inline-formula">ppbv</span> but decrease <span class="inline-formula">PM<sub>2.5</sub></span> by up to 7.9 <span class="inline-formula">µg m<sup>−3</sup></span> in China, 83 % and 90 % of which could be attributed to the effect of the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry. The heterogeneous uptake of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> on chloride-containing aerosol surfaces is an important loss pathway of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> as well as an important source of <span class="inline-formula">O<sub>3</sub></span> and hence is particularly useful in elucidating the commonly seen ozone underestimations relative to observations. The importance of chlorine chemistry largely depends on both chlorine emissions and the parameterizations for the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry. With the additional chlorine emissions, the simulations show that annual MDA8 <span class="inline-formula">O<sub>3</sub></span> in China could be increased by up to 3.5 <span class="inline-formula">ppbv</span>. The corresponding effect on <span class="inline-formula">PM<sub>2.5</sub></span> concentrations varies largely with regions, with an increase of up to 4.5 <span class="inline-formula">µg m<sup>−3</sup></span> in the North China Plain but a decrease of up to 3.7 <span class="inline-formula">µg m<sup>−3</sup></span> in the Sichuan Basin. On the other hand, even with the same chlorine emissions, the effects on MDA8 <span class="inline-formula">O<sub>3</sub></span> and <span class="inline-formula">PM<sub>2.5</sub></span> in China could differ by 48 % and 27 %, respectively, between different parameterizations.</p> |
| first_indexed | 2024-04-12T22:58:10Z |
| format | Article |
| id | doaj.art-bc55ccb21cb14679880312bf3ba743b2 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-04-12T22:58:10Z |
| publishDate | 2022-03-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-bc55ccb21cb14679880312bf3ba743b22022-12-22T03:13:07ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242022-03-01223743376210.5194/acp-22-3743-2022The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in ChinaX. Yang0X. Yang1Q. Wang2Q. Wang3N. Ma4N. Ma5W. Hu6Y. Gao7Z. Huang8Z. Huang9J. Zheng10J. Zheng11B. Yuan12B. Yuan13N. Yang14N. Yang15J. Tao16J. Tao17J. Hong18J. Hong19Y. Cheng20H. Su21Institute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaGuangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, ChinaKey Laboratory of Marine Environment and Ecology, Ministry of Education, Ocean University of China, Qingdao 266100, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaInstitute for Environmental and Climate Research, Jinan University, Guangzhou 511443, ChinaGuangdong–Hongkong–Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 511443, ChinaMax Planck Institute for Chemistry, Mainz 55128, GermanyMax Planck Institute for Chemistry, Mainz 55128, Germany<p>The heterogeneous reaction of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> on Cl-containing aerosols (heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry) plays a key role in chlorine activation, <span class="inline-formula">NO<sub><i>x</i></sub></span> recycling, and consequently <span class="inline-formula">O<sub>3</sub></span> and <span class="inline-formula">PM<sub>2.5</sub></span> formation. In this study, we use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry (i.e., the uptake coefficient of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M14" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">γ</mi><mrow class="chem"><msub><mi mathvariant="normal">N</mi><mn mathvariant="normal">2</mn></msub><msub><mi mathvariant="normal">O</mi><mn mathvariant="normal">5</mn></msub></mrow></msub></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="27pt" height="12pt" class="svg-formula" dspmath="mathimg" md5hash="3e69fa10f182be73e59bb5210ffccfe1"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00001.svg" width="27pt" height="12pt" src="acp-22-3743-2022-ie00001.png"/></svg:svg></span></span>) and the <span class="inline-formula">ClNO<sub>2</sub></span> yield (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M16" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">φ</mi><mrow class="chem"><msub><mi mathvariant="normal">ClNO</mi><mn mathvariant="normal">2</mn></msub></mrow></msub><mo>)</mo></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="38pt" height="15pt" class="svg-formula" dspmath="mathimg" md5hash="b573a3eb5ede5dc2cbb2d4ef9b26d387"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00002.svg" width="38pt" height="15pt" src="acp-22-3743-2022-ie00002.png"/></svg:svg></span></span>) to investigate the impacts of chlorine chemistry on air quality in China, the role of the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry, and the sensitivity of air pollution formation to chlorine emissions and parameterizations for <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M20" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">γ</mi><mrow class="chem"><msub><mi mathvariant="normal">N</mi><mn mathvariant="normal">2</mn></msub><msub><mi mathvariant="normal">O</mi><mn mathvariant="normal">5</mn></msub></mrow></msub></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="27pt" height="12pt" class="svg-formula" dspmath="mathimg" md5hash="7e2119a0a3269eeae62343c97b7f8c6a"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00003.svg" width="27pt" height="12pt" src="acp-22-3743-2022-ie00003.png"/></svg:svg></span></span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M21" display="inline" overflow="scroll" dspmath="mathml"><mrow><msub><mi mathvariant="italic">φ</mi><mrow class="chem"><msub><mi mathvariant="normal">ClNO</mi><mn mathvariant="normal">2</mn></msub></mrow></msub></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="34pt" height="12pt" class="svg-formula" dspmath="mathimg" md5hash="3ca77ac30eaf51dee14f652eb6f1039a"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-22-3743-2022-ie00004.svg" width="34pt" height="12pt" src="acp-22-3743-2022-ie00004.png"/></svg:svg></span></span>. The model simulations are evaluated against multiple observational datasets across China and show significant improvement in reproducing observations of particulate chloride, <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span>, and <span class="inline-formula">ClNO<sub>2</sub></span> when including anthropogenic chlorine emissions and updates to the parameterization of the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry relative to the default model. The simulations show that total tropospheric chlorine chemistry could increase annual mean maximum daily 8 <span class="inline-formula">h</span> average (MDA8) <span class="inline-formula">O<sub>3</sub></span> by up to 4.5 <span class="inline-formula">ppbv</span> but decrease <span class="inline-formula">PM<sub>2.5</sub></span> by up to 7.9 <span class="inline-formula">µg m<sup>−3</sup></span> in China, 83 % and 90 % of which could be attributed to the effect of the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry. The heterogeneous uptake of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> on chloride-containing aerosol surfaces is an important loss pathway of <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> as well as an important source of <span class="inline-formula">O<sub>3</sub></span> and hence is particularly useful in elucidating the commonly seen ozone underestimations relative to observations. The importance of chlorine chemistry largely depends on both chlorine emissions and the parameterizations for the heterogeneous <span class="inline-formula">N<sub>2</sub>O<sub>5</sub></span> <span class="inline-formula">+</span> <span class="inline-formula">Cl</span> chemistry. With the additional chlorine emissions, the simulations show that annual MDA8 <span class="inline-formula">O<sub>3</sub></span> in China could be increased by up to 3.5 <span class="inline-formula">ppbv</span>. The corresponding effect on <span class="inline-formula">PM<sub>2.5</sub></span> concentrations varies largely with regions, with an increase of up to 4.5 <span class="inline-formula">µg m<sup>−3</sup></span> in the North China Plain but a decrease of up to 3.7 <span class="inline-formula">µg m<sup>−3</sup></span> in the Sichuan Basin. On the other hand, even with the same chlorine emissions, the effects on MDA8 <span class="inline-formula">O<sub>3</sub></span> and <span class="inline-formula">PM<sub>2.5</sub></span> in China could differ by 48 % and 27 %, respectively, between different parameterizations.</p>https://acp.copernicus.org/articles/22/3743/2022/acp-22-3743-2022.pdf |
| spellingShingle | X. Yang X. Yang Q. Wang Q. Wang N. Ma N. Ma W. Hu Y. Gao Z. Huang Z. Huang J. Zheng J. Zheng B. Yuan B. Yuan N. Yang N. Yang J. Tao J. Tao J. Hong J. Hong Y. Cheng H. Su The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China Atmospheric Chemistry and Physics |
| title | The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China |
| title_full | The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China |
| title_fullStr | The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China |
| title_full_unstemmed | The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China |
| title_short | The impact of chlorine chemistry combined with heterogeneous N<sub>2</sub>O<sub>5</sub> reactions on air quality in China |
| title_sort | impact of chlorine chemistry combined with heterogeneous n sub 2 sub o sub 5 sub reactions on air quality in china |
| url | https://acp.copernicus.org/articles/22/3743/2022/acp-22-3743-2022.pdf |
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