Fine particle chemistry under a special dust transport event: impacts from unusually enhanced ozone and air mass backflows over the ocean

Lu, Da; Li, Hao; Wang, Guochen; Qin, Xiaofei; Zhao, Na; Huo, Juntao; Yang, Fan; Lin, Yanfen; Chen, Jia; Fu, Qingyan; Duan, Yusen; Dong, Xinyi; Deng, Congrui; Abdullaev, Sabur; Huang, Kan

doi:https://doi.org/10.5194/egusphere-2023-127

Preprints

https://doi.org/10.5194/egusphere-2023-127

Preprints

10 Mar 2023

| 10 Mar 2023

Fine particle chemistry under a special dust transport event: impacts from unusually enhanced ozone and air mass backflows over the ocean

Da Lu, Hao Li, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur Abdullaev, and Kan Huang

Abstract. A five-days long-lasting dust event was observed with a synergy of field measurements techniques in Shanghai in the autumn of 2019. Different from most dust events, this dust was an unusual one characterized of low wind speed, high relative humidity, high concentrations of gaseous precursors, and contrasting wind vectors between low and high altitudes. Three dust stages were identified and the first stage was a normal dust invasion with high particulate concentrations and short duration. In contrast, unusual enhancement of ozone was observed in the second stage, due to compound causes of weak synoptic system, transport from the ocean, and subsidence of high-altitude O₃ down drafted by dust. As a result, sulfate and nitrate moderately correlated with O₃ while had almost no correlation with aerosol liquid water content, indicating the dominant role of gas phase oxidations. During the third stage of dust, a special phenomenon of dust backflow was observed that the dust plume drifted from the Shandong Peninsula and travelled slowly over the Yellow Sea and the East China Sea, finally returning to Shanghai. The dust backflow was evidenced by the enrichment of marine vessel emissions (V and Ni) and increased solubility of calcium. Under the humid oceanic breezes, the formation of nitrate was dominated by aqueous processing, while the strong correlation between SO₄^2- and Na⁺ suggested that a considerable part of sulfate was aged and directly transported. Based on the thermodynamic modeling, sea salts probably involved more in the secondary aerosol formation than the dust heterogeneous reactions. By developing an upstream-receptor relationship method, the amounts of transported and secondarily formed aerosol species were separated. This study highlights that the transport pathway of dust and environmental conditions could significantly modify the aerosol properties, especially at the complex land-sea interface.

Received: 30 Jan 2023 – Discussion started: 10 Mar 2023

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Journal article(s) based on this preprint

07 Nov 2023

Secondary aerosol formation during a special dust transport event: impacts from unusually enhanced ozone and dust backflows over the ocean

Da Lu, Hao Li, Mengke Tian, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur F. Abdullaev, and Kan Huang

Atmos. Chem. Phys., 23, 13853–13868, https://doi.org/10.5194/acp-23-13853-2023,https://doi.org/10.5194/acp-23-13853-2023, 2023

Short summary

Da Lu, Hao Li, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur Abdullaev, and Kan Huang

Interactive discussion

Status: closed

RC1: 'Comment on egusphere-2023-127', Zhang xuelei, 19 Apr 2023

In this manuscript, the authors focused on the atmospheric physiochemical characterizations of a transported dust event that passed through the city of Shanghai and then circled back again. However, it was written in poor English and lacking for scientific questions/gaps, which made it just like a data analysis note of various instruments of a super monitoring site based on three stages of dust event. In general, this manuscript has no innovations and valuable contributions for the science community, and it should be reorganized and discussed with other authors. As it presented in low quality, and I cannot accept it for the publication in present status, and it should be rejected.

Major questions:

1. The title of this manuscript is obscure and unmatched to the research contents.

2. The Introduction part had lengthy writing and lacking for logics among paragraphs. Each paragraph also lacks the topic sentence. The mainstream references are lacking in this part. As mentioned above, the key defect is lacking of research gaps and scientific questions.

3. The math formulas should be provided in the methodology part, such as Lines 292-293 and Lines 535-550.

4. The authors claimed that they develop “a simple method of relating the upstream and receptor simultaneous measurements”, however, this method lacks for the basic scientific verifications, such as comparisons with other source apportionment methods (PMF, CMB, etc.).

5. Too many figures in this manuscript, and the authors can only use the linear analysis in them, and this reflects that this manuscript is written by a student and lacking for the basic guidance.

The whole paper needs to be rewritten in scientific language and vocabularies, and it is necessary that a native English speaker need to help the authors to revised it word by word.

Citation: https://doi.org/10.5194/egusphere-2023-127-RC1
RC2: 'Comment on egusphere-2023-127', Anonymous Referee #2, 15 May 2023

The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-127/egusphere-2023-127-RC2-supplement.pdf

Citation: https://doi.org/10.5194/egusphere-2023-127-RC2
AC1: 'Response to Comments on egusphere-2023-127', Kan Huang, 25 Jul 2023

Please check the attached responses. Thanks!

Citation: https://doi.org/10.5194/egusphere-2023-127-AC1

Interactive discussion

Status: closed

RC1: 'Comment on egusphere-2023-127', Zhang xuelei, 19 Apr 2023

In this manuscript, the authors focused on the atmospheric physiochemical characterizations of a transported dust event that passed through the city of Shanghai and then circled back again. However, it was written in poor English and lacking for scientific questions/gaps, which made it just like a data analysis note of various instruments of a super monitoring site based on three stages of dust event. In general, this manuscript has no innovations and valuable contributions for the science community, and it should be reorganized and discussed with other authors. As it presented in low quality, and I cannot accept it for the publication in present status, and it should be rejected.

Major questions:

1. The title of this manuscript is obscure and unmatched to the research contents.

2. The Introduction part had lengthy writing and lacking for logics among paragraphs. Each paragraph also lacks the topic sentence. The mainstream references are lacking in this part. As mentioned above, the key defect is lacking of research gaps and scientific questions.

3. The math formulas should be provided in the methodology part, such as Lines 292-293 and Lines 535-550.

4. The authors claimed that they develop “a simple method of relating the upstream and receptor simultaneous measurements”, however, this method lacks for the basic scientific verifications, such as comparisons with other source apportionment methods (PMF, CMB, etc.).

5. Too many figures in this manuscript, and the authors can only use the linear analysis in them, and this reflects that this manuscript is written by a student and lacking for the basic guidance.

The whole paper needs to be rewritten in scientific language and vocabularies, and it is necessary that a native English speaker need to help the authors to revised it word by word.

Citation: https://doi.org/10.5194/egusphere-2023-127-RC1
RC2: 'Comment on egusphere-2023-127', Anonymous Referee #2, 15 May 2023

The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-127/egusphere-2023-127-RC2-supplement.pdf

Citation: https://doi.org/10.5194/egusphere-2023-127-RC2
AC1: 'Response to Comments on egusphere-2023-127', Kan Huang, 25 Jul 2023

Please check the attached responses. Thanks!

Citation: https://doi.org/10.5194/egusphere-2023-127-AC1

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload

AR by Kan Huang on behalf of the Authors (25 Jul 2023) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (26 Jul 2023) by Dara Salcedo

RR by Anonymous Referee #3 (12 Aug 2023)

Suggestions for revision or reasons for rejection

General comments

This study reports a dust event with high relative humidity and low wind speeds occurred in Shanghai during the period of October 29-November 2, 2019. The dust event was divided into three obvious stages, of which the first stage was a dust invasion stage, the second stage was a dust development period, and the third stage was a dust backflow period. Meanwhile, chemical characteristics of aerosols in the three stages were investigated, and a simplified method was deployed to identify and estimate the amounts of major aerosol species from transport and secondary formation. The study method is reasonable, data is reliable, and conclusion is credible. But there existed a lot of aspects to be revised and improved in the manuscript. Written language and logical relationship need to be improved. I suggest to consider the paper for publication after a major revision.

Specific comments

1. In abstract, L28, the phrase “by with high concentrations of particulate matters but relatively short duration” should be changed to “by high concentrations of particulate matters but relatively short duration”.

2. In introduction, L121, the sentence “In contrast, this study aims to depict an atypical dust event was observed in Shanghai, a coastal mega-city in Eastern China.” is error.

3. In section 2.2, all the online instruments used in this study should be normally calibrated so as to guarantee data quality, therefore, normal calibrations of these monitoring instruments should be added in the section.

4. In sections 2.3 and 2.4, the models used in this study should be detailed.

5. In section 2.5, the sentence “Initially, the quasi-first-order reaction rate constant for heterogeneous conversion from NH3 to NH4+ (khet, s-1) is calculated according to (Liu et al., 2022).” is incomplete. In addition, the two formulas should be numbered. All the formulas in this study should be numbered in turn.

6. In section 2 methodology, sampling duration should be supplemented.

7. In section 3.1, L216-218, the sentence “From October 25 to 28, the mean wind speed remained relatively low of 0.9±0.72m/s with a peak value of 3.1m/s, and predominantly blowing from the northwest.” is suggested to be changed to “From October 25 to 28, the mean wind speed was 0.9±0.72m/s with a peak value of 3.1m/s, remaining relatively low, and predominantly blowing from the northwest.”

8. L218, the sentence “The mean concentration of PM2.5 and PM10 was 34.7 and 44.2 μg/m3, respectively.” should be revised to “The mean concentrations of PM2.5 and PM10 were 34.7 and 44.2 μg/m3, respectively.”

9. L214-228, in this paragraph dust and non-dust periods should be identified, but authors did not give related discussion.

10. In Figure 1, P1, P2 and P3 should be put in Figure 1d and separated with vertical lines.

11. What did aerosol depolarization ratio was used to explain? Please explain correlation between the depolarization ratio values and the dust event and impacts of relative humidity on the depolarization ratio.

12. L237-244, “In this study………non-dust period”, please supply specific start and end time.

13. Huang et al., 2010a and Huang et al., 2010b were the same reference. Please check the reference.

14. L337-342, in “Firstly, …... ∼1 ppbv/h (Wang et al., 2020).”, related explanation is lack of logic. Please think it over and revise the explanation. In the text, there are many similar logical problems need to be further checked and revised.

15. L345, Figure 5b here should be Figure 4b.

16. In correlation heatmaps, please explain the meaning of dot size.

17. L494, how to understand the sentence “both SO42- and NO3- showed moderate to significant correlations with Na+.”

18. The mean states of P2, P3 and NDS illustrated in Figure 7c were unclear, hope to better present these states.

19. In section 3.5, in the formula TPPD,i = AVLYG,i × (1-k), please explain the meaning of “1-k ”.

20. The conclusions need to be further condensed.

Referee Report: PDF

Hide

RR by Anonymous Referee #4 (23 Aug 2023)

ED: Reconsider after major revisions (24 Aug 2023) by Dara Salcedo

AR by Kan Huang on behalf of the Authors (28 Aug 2023) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (01 Sep 2023) by Dara Salcedo

RR by Anonymous Referee #3 (16 Sep 2023)

ED: Publish as is (19 Sep 2023) by Dara Salcedo

AR by Kan Huang on behalf of the Authors (20 Sep 2023)

Journal article(s) based on this preprint

07 Nov 2023

Secondary aerosol formation during a special dust transport event: impacts from unusually enhanced ozone and dust backflows over the ocean

Da Lu, Hao Li, Mengke Tian, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur F. Abdullaev, and Kan Huang

Atmos. Chem. Phys., 23, 13853–13868, https://doi.org/10.5194/acp-23-13853-2023,https://doi.org/10.5194/acp-23-13853-2023, 2023

Short summary

Da Lu, Hao Li, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur Abdullaev, and Kan Huang

Supplement

https://doi.org/10.5194/egusphere-2023-127-supplement

Da Lu, Hao Li, Guochen Wang, Xiaofei Qin, Na Zhao, Juntao Huo, Fan Yang, Yanfen Lin, Jia Chen, Qingyan Fu, Yusen Duan, Xinyi Dong, Congrui Deng, Sabur Abdullaev, and Kan Huang

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Short summary

Environmental conditions during dust are usually not favorable for the secondary aerosol formation. While in this study, an unusual dust event was captured in a Chinese mega-city and showed the “anomalous” meteorology and a special dust backflow transport pathway. The underlying formation mechanisms of secondary aerosols are probed in the context of this special dust event. This study shows significant implications on the varying dust aerosol chemistry in the future changing climate.


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