Articles | Volume 25, issue 19
https://doi.org/10.5194/acp-25-12721-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.Hydroxymethanesulfonate (HMS) formation in urban and marine atmospheres: role of aerosol ionic strength
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- Final revised paper (published on 10 Oct 2025)
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RC1: 'Comment on egusphere-2025-683', Anonymous Referee #1, 23 Apr 2025
- AC3: 'Reply on RC1', Rongshuang Xu, 17 Jun 2025
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RC2: 'Comment on egusphere-2025-683', Anonymous Referee #2, 25 Apr 2025
- AC1: 'Reply on RC2', Rongshuang Xu, 17 Jun 2025
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RC3: 'Comment on egusphere-2025-683', Anonymous Referee #3, 05 May 2025
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AR by Rongshuang Xu on behalf of the Authors (17 Jun 2025)
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ED: Referee Nomination & Report Request started (04 Jul 2025) by Markus Ammann
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RR by Anonymous Referee #3 (18 Jul 2025)

ED: Publish subject to minor revisions (review by editor) (18 Jul 2025) by Markus Ammann

AR by Rongshuang Xu on behalf of the Authors (23 Jul 2025)
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ED: Publish as is (24 Jul 2025) by Markus Ammann
AR by Rongshuang Xu on behalf of the Authors (30 Jul 2025)
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This paper investigates HMS formation as a function of particle pH and ionic strength (IS) based on two data sets: an urban site and a marine site. Modeling shows interesting interaction between IS and pH on HMS production rates. The concentrations of HMS are very low and a very small fraction of PM2.5 mass in both locations so it is unclear why the authors are attempting this analysis with this data – the contribution of HMS seems of little importance in these data. I guess the belief is the findings here have broad applicability. This could be made clearer. The analysis assume the HMS was formed under the conditions in which the measurements were made, otherwise the analysis falls apart. Other than low wind speeds, there is little proof offered to support this. Furthermore, how do the authors know that the formation didn’t occur in clouds not the aerosol, which are much more conducive to HMS formation. More evidence of formation in ALWC would be helpful. Aerosol pH is a critical parameter, but no evidence is provided to suggest it is reasonably predicted and assumptions are made due to lack of ammonia data. Extensive modeling analysis is performed, and the results are interesting, but little evidence is given that the data strongly support the model predictions; the main point seems to be that the model and data agree at the level of general trends in pH and IS. A more in-depth comparison might be helpful. A more direct comparison between model and measurements would be useful. Finally, given all the caveats stated in this manuscript relating to uncertainties in rate constants, phase separations, and possible surface vs bulk particle reactions, how does one interpret the modeling results as being reliable? This is why more direct comparisons would be useful. Overall, the modeling results are very interesting but there could be improvements to the manuscript. More details are given below.
Some main overall points.
Specific Comments:
Pg 3 First line, what is meant by “crucial”. Add justification (if there is any) for this characterization? Eg, the term “up to” is not specific (ie, it is the max value). What is the mass fraction of HMS in PM2.5 when HMS is 18 g/m3? Compare this to the typical HMS mass fraction in PM2.5? Campbell should not be in the ref list, that is not data from the N. China Plane, check all references here are NCP.
Line 10 pg 3, I believe the models of Moch et al are for cloud processing in the formation of HMS. Is this true for all the references here. Please specify, the route, ie clouds/fogs vs aerosol particle water – it matters.
Line 20 pg 3. Regarding meteorological effects. A big influence of temperature is the effect on pH. See Campbell Sci Adv 2024, DOI: 10.1126/sciadv.ado4373 Tao and Murphy ACP 2019 https://doi.org/10.5194/acp-19-9309-2019
Line 36-37 pg 3 that states; In controversy,.... Campbell et al. 2022. I do not agree with this sentence. If you read that paper carefully you will see that pH was estimated since total (gas plus particle) ammonium was not measured. For more discussion on pH in Fairbanks and relation to HMS see Campbell Sci Adv 2024, DOI: 10.1126/sciadv.ado4373
I also do not understand the line following the one above, line 37-40 page 3. As noted above, why does one assume that the conditions in which the aerosol is being measured represents the conditions under which HMS was formed under. This depends on the estimated lifetime of HMS. This should be considered in the interpretation of these studies and especially the interpretation of the data in this paper.
Line 13 page 4. To have ALWC of 100’s of ug/m3 in polluted urban areas it must correspond to very poor air quality only found in some countries – ie this is not typical. Be specific what urban areas would have this level of ALWC, ie, in cities in the NCP?
First lines of page 6. It makes no sense using the epsilon of 0.5 for NH3/NH4+ partitioning in the pH analysis based on Fairbanks Alaska data which is an extremely different environment than that of this study. One might consider an iterative approach, see doi:10.2533/chimia.2024.1
R1 and R2 are shown as equilibrium reactions, but then the reaction rate constants are discussed. This is confusing.
Fig 1 caption, typo change penal to panel. T in (a) is in C, t in (e) is in Kelvin, why? Why is HMS not shown in Fig 1d?
Last line page 7, referring to similar results from Moch et al. But wasn’t Moch’s results based on HMS formation in clouds, which is not what is assumed here? Also, next line on top of page 8, comparing HMS concentrations to Fairbanks makes little sense given how different the situation is.
Line 40 page 8, too strong a statement, correlation is not causation. This applies throughout the manuscript.
Fig 2 b (and in other places) specify if ratio of HMS/Sulfate is mass or molar.
Page 10 top of page, what is the lifetime of HMS, this would support the idea that it is formed locally. Low wind speed does support the idea of local formation but does not prove the conditions measured were those under which HMS was formed.
Fig 3a. I assume this graph is predicted IS vs measured RH; this should be clarified. IS depends on ALWC and ALWC depends on RH and other factors (particle composition). Why not focus on ALWC and IS, that is what matters and what is more generalizable to other locations vs RH.
Fig 4b, the colors for data, urban clean vs polluted are too close to being the same. Typo in caption (radium?). From this plot, does the data fit with the model? Looking at the urban polluted vs clean, it does not seem to fit that well, there are many blue markers on similar isopleths as urban clean and urban polluted. The graph does not actually show data on measured HMS formation rates, or maybe all one can do is show HMS concentration. So how does this plot assess the comparison between these data from this study and the predictions. At the very least state associated HMS concentrations for the groups of data shown on the plot. The data on HMS concentrations and production rates of HMS, eg Fig 2, should be added. Furthermore, the plot is for ALWC = 100 ug/m3, but the data seem to cover a wide range of ALWC. How is that reasonable?
I do not understand the first part of the last paragraph, how does cycling of HMS through formation and loss in the liquid drop make sulfate? Explain more.
Page 17, what is Enteromorpha ?