Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China

Qiu, Xionghui; Ying, Qi; Wang, Shuxiao; Duan, Lei; Zhao, Jian; Xing, Jia; Ding, Dian; Sun, Yele; Liu, Baoxian; Shi, Aijun; Yan, Xiao; Xu, Qingcheng; Hao, Jiming

doi:https://doi.org/10.5194/acp-19-6737-2019

Articles | Volume 19, issue 10

https://doi.org/10.5194/acp-19-6737-2019

© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

https://doi.org/10.5194/acp-19-6737-2019

© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Articles | Volume 19, issue 10

Research article

|

21 May 2019

Research article |

| 21 May 2019

Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China

Xionghui Qiu, Qi Ying, Shuxiao Wang, Lei Duan, Jian Zhao, Jia Xing, Dian Ding, Yele Sun, Baoxian Liu, Aijun Shi, Xiao Yan, Qingcheng Xu, and Jiming Hao

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Preprint (discussion started on 20 Dec 2018)
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Interactive discussion

Status: closed

AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment

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RC1: 'Comment on “Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China” by Xionghui Qiu et al.', Anonymous Referee #1, 08 Feb 2019
- AC1: 'Response to reviewer', Xionghui Qiu, 14 Apr 2019
- AC2: 'Response to reviewer#2', Xionghui Qiu, 14 Apr 2019
RC2: 'review', Anonymous Referee #2, 02 Mar 2019
- AC2: 'Response to reviewer#2', Xionghui Qiu, 14 Apr 2019

Peer-review completion

AR: Author's response | RR: Referee report | ED: Editor decision

AR by Xionghui Qiu on behalf of the Authors (14 Apr 2019)

ED: Referee Nomination & Report Request started (25 Apr 2019) by Andreas Hofzumahaus

RR by Anonymous Referee #3 (29 Apr 2019)

Suggestions for revision or reasons for rejection

Qiu et al., developed a revised regional CMAQ model, by updating several chloride contained reactions, to study the impact of chloride-related heterogeneous chemistry on summer particulate nitrate formation. This work is meaningful and improved the understanding of regional nitrate pollution as well as chloride chemistry. Several comments should be addressed before publishing in ACP.

Major comments:
1. Section 3.2, the uptake coefficient of O3 on chloride-contain aerosol were increased by a factor of 10 and showed the importance of O3 heterogeneous reaction and the Cl2 budget. The increasing of O3 uptake coefficient may also strongly affect the O3 lifetime, an intercomparison of modeled and observed O3 need to be conducted to verify the rationality and prove the significance.

2. Figure 3(e, f) do not show the higher OH plot in Het case, so the statement in line 366 can’t get the conclusion that high ANO3 is attribute to the elevated OH, although other studies presented the same conclusion. By the way, the photolysis of ClNO2 also release NO2 and enhance the reaction of OH + NO2. It would be good if the increasing of daytime NO2 and OH by ClNO2 photolysis can be quantified and used to assess the contribution from NO2 and OH.

Minor comments.
1. L89, high Cl- do not represent high ClNO2 yield, which may be subject to the aerosol liquid water content, organics and so on, please change to “When ClNO2 yield is high…”.
2. Line 229, Eqs. 8, change to γOH.
3. Line 321, Bracket is not complete.
4. Line 328, Tham et al., 2019 change to 2018.
5. Line 718-719, the font size is bigger than other words.
6. Line 332-336, the long sentence is difficult to read. Please divide into two sentences, “… and the larger constant N2O5 leads to…” change to “. The application of large and fixed N2O5 uptake coefficient … ”
7. Line 377, subscript of “PM2.5”.
8. Figure 4 should add the base case percentage like HET in the left edge.

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RR by Anonymous Referee #1 (03 May 2019)

ED: Publish subject to minor revisions (review by editor) (07 May 2019) by Andreas Hofzumahaus

AR by Xionghui Qiu on behalf of the Authors (09 May 2019) Author's response Manuscript

ED: Publish subject to technical corrections (10 May 2019) by Andreas Hofzumahaus

AR by Xionghui Qiu on behalf of the Authors (10 May 2019) Manuscript

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Short summary

Current chemical transport models cannot capture the diurnal and nocturnal variation in atmospheric nitrate, which may be relative to the missing atmospheric chlorine chemistry. In this work, the Community Multiscale Air Quality (CMAQ) model with improved chlorine heterogeneous chemistry is applied to simulate the impact of chlorine chemistry on summer nitrate concentrations in Beijing. The results of this work can improve our understanding of nitrate formation.