Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing

<p>Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants...

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Main Authors: D. J. Bryant, W. J. Dixon, J. R. Hopkins, R. E. Dunmore, K. L. Pereira, M. Shaw, F. A. Squires, T. J. Bannan, A. Mehra, S. D. Worrall, A. Bacak, H. Coe, C. J. Percival, L. K. Whalley, D. E. Heard, E. J. Slater, B. Ouyang, T. Cui, J. D. Surratt, D. Liu, Z. Shi, R. Harrison, Y. Sun, W. Xu, A. C. Lewis, J. D. Lee, A. R. Rickard, J. F. Hamilton
Format: Article
Language:English
Published: Copernicus Publications 2020-06-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/20/7531/2020/acp-20-7531-2020.pdf
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Summary:<p>Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular <span class="inline-formula">NO<sub><i>x</i></sub></span> and particulate <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M2" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><msubsup><mi mathvariant="normal">SO</mi><mn mathvariant="normal">4</mn><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="29pt" height="17pt" class="svg-formula" dspmath="mathimg" md5hash="74b4be02f6bf1e477b176a208786a61b"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-20-7531-2020-ie00001.svg" width="29pt" height="17pt" src="acp-20-7531-2020-ie00001.png"/></svg:svg></span></span>, led to the formation of iSOA under both high- and low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxy-organosulfates (NOSs). Ultra-high-performance liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM<span class="inline-formula"><sub>2.5</sub></span> filter extracts. The co-elution of the inorganic ions in the<span id="page7532"/> extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5&thinsp;ng&thinsp;m<span class="inline-formula"><sup>−3</sup></span>, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the sulfate available for reactive uptake, as shown by a strong correlation with the product of ozone (<span class="inline-formula">O<sub>3</sub></span>) and particulate sulfate (<span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M6" display="inline" overflow="scroll" dspmath="mathml"><mrow class="chem"><msubsup><mi mathvariant="normal">SO</mi><mn mathvariant="normal">4</mn><mrow><mn mathvariant="normal">2</mn><mo>-</mo></mrow></msubsup></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="29pt" height="17pt" class="svg-formula" dspmath="mathimg" md5hash="a8455a3a3390243c17ea2f3ca419ac4e"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-20-7531-2020-ie00002.svg" width="29pt" height="17pt" src="acp-20-7531-2020-ie00002.png"/></svg:svg></span></span>). A greater proportion of high-NO OS products were observed in Beijing compared with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62&thinsp;% of the oxidized organic aerosol measured by aerosol mass spectrometry on average, but this increased to <span class="inline-formula">∼3 <i>%</i></span> on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to OS products from heterogenous reactions.</p>
ISSN:1680-7316
1680-7324