the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Non biogenic source is an important but overlooked contributor to aerosol isoprene-derived organosulfates during winter in northern China
Abstract. Previous measurement-model comparisons of atmospheric isoprene levels showed a significant unidentified source of isoprene in some northern Chinese cities during winter. Here, spatial variability in winter aerosol organosulfate (OS) formation in typical southern (Guangzhou and Kunming) and northern (Xi’an and Taiyuan) cities, China, was investigated to reveal the influence of potential non biogenic contributor on aerosol OS pollution levels. Monoterpene-derived OSs were significantly higher in southern cities than in northern cities, which was attributed to temperature dependent emission of monoterpenes (i.e., higher temperatures in southern cities drove more monoterpene emissions). However, isoprene-derived OSs (OSi) showed the opposite trend, with significantly higher levels in northern cities. Principal component analysis combined with field simulation combustion experiments suggested that biomass burning rather than gasoline, diesel, and coal combustion contributed significantly to the abundance of OSi in northern cities. The comparison of anthropogenic OS molecular characteristics between particles released from various combustion sources and ambient aerosol particles suggested that stronger biomass and fossil fuel combustion activities in northern cities promoted the formation of more anthropogenic OSs. Overall, this study provides direct molecular evidence for the first time that non biogenic sources can significantly contribute to the formation of OSi in China during winter.
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RC1: 'Comment on egusphere-2024-3823', Anonymous Referee #1, 18 Dec 2024
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General Comments:
This study investigated the spatial variations of the concentration of different types of organosulfates in cities in southern and northern China. The manuscript further analyzed the factors leading to significant regional differences in organosulfate concentration and composition between the southern and northern cities. Based on principal component analysis, correlation analysis, organosulfate formation mechanism analysis, and field simulation combustion experiments, the authors concluded that the emissions from biomass burning, rather than those from gasoline, diesel, and coal combustion, can play a significant role in the formation of isoprene-derived organosulfates. This is a significant and valuable finding. It thus follows that when attempting to predict winter isoprene emissions in China, it is essential that the influence of biomass combustion emissions is duly taken into account, with due consideration given to the regional differences in question. Overall, the manuscript presents high quality research data based on field observations and simulation experiments. The content presented here will be of interest to the readership of Atmospheric Chemistry and Physics. After the authors address the following minor comments, this manuscript would be suitable for publication.
Specific comments:
- Lines 142-143: I suggest that the authors add specific information about the columns used here or in the supplemental file. It is important to consider this when comparing the analysis method from this study with those from previous or future research.
- Lines 157-158: Why did the authors choose 111 of the OSs for further quantification? I have checked your previously published paper showing quantification of 106 OS species. Is there any difference here? Please clarify.
- Lines 172-174: How is this insignificance determined or evaluated?
- Line 196: Please remove any possible extra spaces between 'sulfate' and 'atmospheric oxidation capacity'.
- Line 217: Please change 'an' to 'the'.
- Lines 224-225: Was the correlation analysis presented in Figure S3 using all the data from this study? In addition, I suggest adding 'further' before 'given'.
- Line 248: Please remove any possible extra spaces before 'considering'.
- Line 261: Please change ' precisely' to 'further'.
- Line 269: I suggest the author delete 'fully' or replace it with a more appropriate word.
- I know that those isoprene-derived organosulfates were detected in the samples from the simulated combustion experiments, however, I would like to know how you think about their formation. This could be a critical question for future research in this area, although it does not affect the results of this study.
- I suggest the authors add a space after Ali. in Figure S3. Furthermore, how was the relative intensity calculated in Figure S5? Please clarify it.
Citation: https://doi.org/10.5194/egusphere-2024-3823-RC1
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