Effects of NO  and SO2 on the secondary organic aerosol formation from the photooxidation of 1,3,5-trimethylbenzene: A new source of organosulfates

Yang, Zhaomin; Tsona, Narcisse T.; Li, Jianlong; Wang, Shuyan; Xu, Li; You, Bo; Du, Lin

doi:10.1016/j.envpol.2020.114742

Cited by 39 publications

(33 citation statements)

References 82 publications

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“…3, where it can be observed that the particle formation increased with increasing initial SO 2 levels, regardless of low-or high-NO x conditions. The present result is consistent with a previous research study, which found that limonene SOA formation is significantly Z. Yang et al: SO 2 and NH 3 enhance organosulfur compounds and particle formation promoted with SO 2 addition (Ye et al, 2018). SO 2 was found to perturb particle formation by inducing chemical reactions in the gas and particle phase (Wang et al, 2019a;Friedman et al, 2016).…”

Section: Soa Yield In So 2 -Added Photooxidationsupporting

confidence: 93%

SO2 and NH3 emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

Yang

Tsona

et al. 2021

Atmos. Chem. Phys.

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Abstract. Aromatic hydrocarbons can dominate the volatile organic compound budget in the urban atmosphere. Among them, 1,2,4-trimethylbenzene (TMB), mainly emitted from solvent use, is one of the most important secondary organic aerosol (SOA) precursors. Although atmospheric SO2 and NH3 levels can affect secondary aerosol formation, the influenced extent of their impact and their detailed driving mechanisms are not well understood. The focus of the present study is to examine the chemical compositions and formation mechanisms of SOA from TMB photooxidation influenced by SO2 and/or NH3. Here, we show that SO2 emission could considerably enhance aerosol particle formation due to SO2-induced sulfate generation and acid-catalyzed heterogeneous reactions. Orbitrap mass spectrometry measurements revealed the generation of not only typical TMB products but also hitherto unidentified organosulfates (OSs) in SO2-added experiments. The OSs designated as being of unknown origin in earlier field measurements were also detected in TMB SOA, indicating that atmospheric OSs might also be originated from TMB photooxidation. For NH3-involved experiments, results demonstrated a positive correlation between NH3 levels and particle volume as well as number concentrations. The effects of NH3 on SOA composition were slight under SO2-free conditions but stronger in the presence of SO2. A series of multifunctional products with carbonyl, alcohols, and nitrate functional groups were tentatively characterized in NH3-involved experiments based on infrared spectra and mass spectrometry analysis. Plausible formation pathways were proposed for detected products in the particle phase. The volatility distributions of products, estimated using parameterization methods, suggested that the detected products gradually condense onto the nucleation particles to contribute to aerosol formation and growth. Our results suggest that strict control of SO2 and NH3 emissions might remarkably reduce organosulfates and secondary aerosol burden in the atmosphere. Updating the aromatic oxidation mechanism in models could result in more accurate treatment of particle formation for urban regions with considerable SO2, NH3, and aromatics emissions.

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Section: Soa Yield In So 2 -Added Photooxidationsupporting

confidence: 93%

SO2 and NH3 emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

Yang

Tsona

et al. 2021

Atmos. Chem. Phys.

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“…Nitrogen oxides (NO x = NO + NO 2 ), which are mainly emitted from the combustion of fossil fuels, have received significant attention due to their effects on the photooxidation process of volatile organic compounds (VOCs) and SOA formation (Surratt et al, 2006;Ng et al, 2007b;Draper et al, 2015;Berkemeier et al, 2016;Sarrafzadeh et al, 2016;Zhao et al, 2018). A clear increase at first and then a decrease in the SOA yield was found with increasing NO x con-centration from the laboratory experiments with both anthropogenic (trimethylbenzene) and biogenic (β-pinene) VOCs (Sarrafzadeh et al, 2016;Yang et al, 2020). The competitive chemistry of organic peroxyl radicals (RO 2 ) with hydroperoxyl radicals (HO 2 ) and NO was responsible for the variability in SOA formation (Ng et al, 2007a;Xu et al, 2014;Jiang et al, 2020).…”

Section: Introductionmentioning

confidence: 98%

Synergetic effects of NH3 and NOx on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation

et al. 2021

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Abstract. NH3 is the most important alkaline gas in the atmosphere and one of the key species affecting the behaviors of atmospheric aerosols. However, the impact of NH3 on secondary organic aerosol (SOA) formation remains poorly understood, especially the dynamic evolution of chemical compositions in the SOA formation process. In this study, a series of chamber experiments were performed to probe the individual and common effects of NH3 and NOx on toluene SOA formation through OH photooxidation. The chemical compositions of toluene SOA were characterized using the Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS). The SOA yield increased from 28.1 % in the absence of NH3 to 34.7 % in the presence of NH3 but decreased to 19.5 % in the presence of NOx. However, the highest SOA yield of 42.7 % and the lowest carbon oxidation state (OSC) occurred in the presence of both NH3 and NOx, indicating that the higher-volatility products that formed in the presence of NOx could partition into the particle phase when NH3 was added. This resulted in a synergetic effect on SOA formation when NH3 and NOx co-existed. The heterogeneous reaction was the main pathway by which NH3 participated in SOA formation in the photooxidation process. The synergetic effect of NH3 and NOx was also observed in SOA optical absorption. A peak at 280 nm, which is characteristic of organonitrogen imidazole compounds, was observed in the presence of NH3, and its intensity increased when NOx was added into the chamber. This work improves our understanding of how the synergistic interactions between NH3 and NOx influence SOA formation and offers new insights into mitigating haze pollution.

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“…In the absence of NH3, the RO intermediate, which is easily fragmented to produce relatively high-volatility compounds, was the dominant product of the NOx + RO2 reaction (Zhao et al, 2018;Liu et al, 2019a;Xu et al, 2020). Highly volatile compounds cannot readily precipitate into the particle-phase, which subsequently results in a lower SOA yield in the presence of NOx (Yang et al, 2020). Thereby, both OSC and the SOA mass concentration were lower when 60 ppb NOx was added into the chamber.…”

Section: Soa Chemical Compositionmentioning

confidence: 99%

“…Nitrogen oxides (NOx = NO + NO2), which are mainly emitted from the combustion of fossil-fuels, have received significant attention due to their effects on the photooxidation process of volatile organic compounds (VOCs) and SOA formation (Draper et al, 2015;Berkemeier et al, 2016;Zhao et al, 2018;Surratt et al, 2006;Ng et al, 2007b;Sarrafzadeh et al, 2016). Laboratory experiments have found that SOA formation was initially enhanced, but then suppressed with increasing NOx concentrations (Sarrafzadeh et al, 2016;Yang et al, 2020). The competitive chemistry of organic peroxy radicals (RO2) with hydroperoxyl radicals (HO2) and NO was responsible for the variability in SOA formation (Xu et al, 2014;Ng et al, 2007a;Jiang et al, 2020).…”

Effects of NO and SO2 on the secondary organic aerosol formation from the photooxidation of 1,3,5-trimethylbenzene: A new source of organosulfates

Cited by 39 publications

References 82 publications

SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

Synergetic effects of NH<sub>3</sub> and NO<sub><i>x</i></sub> on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation

Reviewer comment on acp-2021-560

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Effects of NO and SO2 on the secondary organic aerosol formation from the photooxidation of 1,3,5-trimethylbenzene: A new source of organosulfates

Cited by 39 publications

References 82 publications

SO&lt;sub&gt;2&lt;/sub&gt; and NH&lt;sub&gt;3&lt;/sub&gt; emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

SO&lt;sub&gt;2&lt;/sub&gt; and NH&lt;sub&gt;3&lt;/sub&gt; emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

Synergetic effects of NH&lt;sub&gt;3&lt;/sub&gt; and NO&lt;sub&gt;&lt;i&gt;x&lt;/i&gt;&lt;/sub&gt; on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation

Reviewer comment on acp-2021-560

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SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

Synergetic effects of NH<sub>3</sub> and NO<sub><i>x</i></sub> on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation