Critical Aspects in Fabricating Multifunctional Super-Nonwettable Coatings Exhibiting Icephobic and Anti-Biofouling Properties

Round 1

Reviewer 1 Report

Below you will find my impressions concerning the manuscript Critical aspects in the development of multifunctional su-per-nonwettable materials targeting icephobic and anti-fouling features from Karekin Esmeryan.

From my point of view the article is interesting. From reviewer’s opinion the viewpoint article does need moderate revisions before publication. I am convinced that after streamlining the topic and adding additional references the manuscript can be published.

 

Revisions

1.    Materials sound confusing (to general) “coatings”

2.    Please check and correct the keywords (carbon soot coating)

3.    Specify “multifunctional”.

4.    Page 2 line 46 f “since the weak interfacial attraction forces lead to liquid droplet contact angle exceeding 150 °, contact angle hysteresis below 5 ° and rolling angle less than 10 °, converting the solid to quasifrictionless and forming a slippery interface [12].” Missing references: Drelich, Bormashenko, Kash Mittal, Schmitt&Heib, Neumann Amirfazli, Marmur, A.. Most of them should at least be mentioned to round up the theoretical aspects.

5.    Concering the nanomaterial I miss reference from Anpo Masakazu and Hoffmann&Bahnemann,

6.    Concering fouling and boiling I miss references like Tanaka “Pool boiling on a superhydrophilic surface” using superhydrophilic surface for self cleaning Or Cambers and Wood (maritime biofouling)

7.    Line 110 “consisting” should be exchanged by “fabricated” or something similar. Compare to “Analysis of silanes and of siloxanes formation by Raman spectroscopy”

8.    Considering the chemical reactivity of the hole and the electron of the ZnO nanoparticle I suggest to cite some open access publications “Synthesis and testing of ZnO nanoparticles …”, Anpo Masakazu, Hoffmann&Bahnemann or patents.

9.    Looking for omnio-phobic surface (instead of super-nonwettable) might help to cover the lack in the cited references especially for section 2. “Marmur, A. Hydro- hygro- oleo- omnio-phobic? Terminology of wettability classification. Soft Matter 2012, 8, 6867–6870.”. The last HPDSA CA publications also contains some summaries concerning wetting.

10. Is there any relation between graphene like materials and the soot based materials. I think about using the procedures for the graphene’s also for the soot vis versa.

I am convinced that it is neither the intention of the author to describe all of the possibilities nor that an article can cover all of the topics which can be place under this title. Therefor I suggest to specify the title even more or/and to highlight other possibilities within the introduction/conclusion (e.g. no below water applications?!). The draft seems to be more focussed on soot-based coatings?

Author Response

Dr. Esmeryan would like to sincerely thank the reviewers for their time to review his manuscript and for the provision of helpful and constructive comments, suggestions and recommendations. The author did his very best to address them in the revised version of the manuscript. Revisions in the text related to the reviewers’ comments are highlighted in yellow. The responses are given below, each comment is shown in italic and the response shown in standard font.

 

Referee 1:

• Below you will find my impressions concerning the manuscript Critical aspects in the development of multifunctional su-per-nonwettable materials targeting icephobic and anti-fouling features from Karekin Esmeryan.

From my point of view the article is interesting. From reviewer’s opinion the viewpoint article does need moderate revisions before publication. I am convinced that after streamlining the topic and adding additional references the manuscript can be published.

• Materials sound confusing (to general) “coatings”

Response:

Dr. Esmeryan thanks the reviewer for his/her thorough and competent review report. The author agrees that “materials” might sound confusing, so this word is replaced by “coatings”.

Change in Manuscript:

The manuscript’s title has now been changed to “Critical aspects in fabricating multifunctional super-nonwettable coatings exhibiting icephobic and anti-biofouling properties”. In addition, the word “materials” has been replaced by the word “coatings” throughout the main text.

2) Please check and correct the keywords (carbon soot coating)

Response:

The keywords have been checked and corrected.

3) Specify “multifunctional”.

Response:

Thank you very much for this suggestion. The term “multifunctional” is now specified.

Change in Manuscript:

Information regarding the meaning of “multifunctional” is now available on Page 2 Lines 47-49 in the revised manuscript.

4) Page 2 line 46 f “since the weak interfacial attraction forces lead to liquid droplet contact angle exceeding 150 °, contact angle hysteresis below 5 ° and rolling angle less than 10 °, converting the solid to quasifrictionless and forming a slippery interface [12].” Missing references: Drelich, Bormashenko, Kash Mittal, Schmitt&Heib, Neumann Amirfazli, Marmur, A.. Most of them should at least be mentioned to round up the theoretical aspects.

Response:

Dr. Esmeryan sincerely acknowledges this recommendation. The suggested literature is indeed valuable and will add further scientific quality to the manuscript.

Change in Manuscript:

The articles of Drelich, Bormashenko, Schmitt, Amirfazli, etc. are now cited in the revised manuscript under numbers [17-20].

5) Concering the nanomaterial I miss reference from Anpo Masakazu and Hoffmann&Bahnemann.

Response:

The work of prof. Anpo Masakazu is highly appreciated and the author decided to cite it.

Change in Manuscript:

Tha article of prof. Masakazu reporting the photocatalytic activity of reduced graphene oxide is cited under number [29] and commented upon Page 3 Lines 94-95 in the revised manuscript.

6) Concerning fouling and boiling I miss references like Tanaka “Pool boiling on a superhydrophilic surface” using superhydrophilic surface for self cleaning Or Cambers and Wood (maritime biofouling).

Response:

Well, the article of prof. Tanaka is indeed valuable, but it seems to be out-of-the scope of the present manuscript due to the fact that it reports a superhydrophilic surface i.e., a surface that is wettable very well by water. The idea of the viewpoint article is to consider multifunctional non-wettable coatings. Therefore, Dr. Esmeryan respects the reviewer’s comment, but thinks that citing the above-mentioned article would be inappropriate and odd.

7) Line 110 “consisting” should be exchanged by “fabricated” or something similar. Compare to “Analysis of silanes and of siloxanes formation by Raman spectroscopy”.

Response:

Thanks for this comment. The word “consisting” is replaced by “composed of”.

Change in Manuscript:

The suggested revision is available on Page 4 Line 119 in the revised manuscript.

8) Considering the chemical reactivity of the hole and the electron of the ZnO nanoparticle I suggest to cite some open access publications “Synthesis and testing of ZnO nanoparticles …”, Anpo Masakazu, Hoffmann&Bahnemann or patents.

Response:

Dr. Esmeryan believes that the work M. Schmitt (“Synthesis and testing of ZnO nanoparticles”) fits very well to the topic of the viewpoint article, so it has been cited.

Change in Manuscript:

The article of prof. Schmitt is now cited under number [31] and commented upon Page 5 Lines 136-137 in the revised manuscript.

9) Looking for omnio-phobic surface (instead of super-nonwettable) might help to cover the lack in the cited references especially for section 2. “Marmur, A. Hydro- hygro- oleo- omnio-phobic? Terminology of wettability classification. Soft Matter 2012, 8, 6867–6870.”. The last HPDSA CA publications also contains some summaries concerning wetting.

Response:

There is only one problem with the kind reviewer’s recommendation. Namely, the coatings reported in the viewpoint article are not superomniphobic, because this term implies non-wettability towards alcohols(https://www.nature.com/articles/am201434#:~:text=Abstract,are%20known%20as%20superomniphobic%20surfaces). Unfortunately, this is not the case and the alcohols wet the coatings considered herein. Therefore, the suggested literature cannot be cited.

10) Is there any relation between graphene like materials and the soot based materials. I think about using the procedures for the graphene’s also for the soot vis versa.

Response:

This is a very interesting question. In general, the soot belongs to the family of graphite-like materials and from that point-of-view, Dr. Esmeryan believes that there might be any relation between graphene and soot in terms of functional properties. Saying that, the author has taken into account the reviewer’s question and new information is now available in the revised manuscript.

Change in Manuscript:

A comment between the possible relation between the soot and graphene, in terms of functional properties, is now available on Page 8 Lines 239-242 in the revised manuscript. Another important literature source has been cited too under number [40].

11) I am convinced that it is neither the intention of the author to describe all of the possibilities nor that an article can cover all of the topics which can be place under this title. Therefor I suggest to specify the title even more or/and to highlight other possibilities within the introduction/conclusion (e.g. no below water applications?!). The draft seems to be more focussed on soot-based coatings?

Response:

The reason why the manuscript is more focused on soot-based coatings is due to the fact that the author is not aware of other individual coatings exhibiting both anti-icing and anti-biofouling characteristics. Prior to writing the article, Dr. Esmeryan performed a thorough literature research in all reputable scientific databases, but the outcome showed profound lack of articles reporting simultaneous possession of icephobic and anti-bioadhesive properties by a given functional coating. Likely, there might be some exceptions, but it is very difficult to find them (if exist).

Change in Manuscript:

The manuscript’s title is now changed and Dr. Esmeryan firmly believes that the new title much more adequately addresses the main topic of the viewpoint article.

Author Response File: Author Response.pdf

Reviewer 2 Report

Dear author, I found your work very interesting and original, however in my opinion, the manuscript needs some minor revisions.

Since it is a mini-review, I think that 29 references are not enough so, I recommend you to add some more references. 

In the introduction, you should better explain why it is important to design an anti-icing and anti-microbial surface: for instance, which are the main applications?

Fig. 4: The green spheres in 4(a) seem to be particles but in (c) are described as "silica sol". So, are they precipitated particles or colloidal? Moreover, I recommend you to add the acronymous (ERMs) to the tag in fig. 4(b), since in the legend of Fig 4(c) the acronymous ERM is the only one reported. 

Line 169-171: you should add the bibliographic info.

Fig. 5 left part: why you coloured the spheres that represent the oxygen functional groups with two different blue?  I think they should be coloured with the same colour since they should represent the same molecules.

The legend of Fig. 5 should be improved: you should describe what happened on the left side and on the right side of the figure, as the same as you did in figure 6.

From line 213 to line 215: you write that to achieve the target, a pattern of pillars in a specific range of dimensions should be prepared. How did you calculate the proposed dimensions? Is there any bibliographic reference for it or this is a result of one of your study? Please, add some more explanations.

Author Response

Dr. Esmeryan would like to sincerely thank the reviewers for their time to review his manuscript and for the provision of helpful and constructive comments, suggestions and recommendations. The author did his very best to address them in the revised version of the manuscript. Revisions in the text related to the reviewers’ comments are highlighted in yellow. The responses are given below, each comment is shown in italic and the response shown in standard font. 

Referee 2:

Dear author, I found your work very interesting and original, however in my opinion, the manuscript needs some minor revisions.

1) Since it is a mini-review, I think that 29 references are not enough so, I recommend you to add some more references.

Response:

Dr. Esmeryan sincerely thanks the reviewer for his/her positive and useful review report. The author agrees that 29 references are not enough, although it is a viewpoint and not a mini-review article, and currently, the manuscript contains 40 references i.e., 11 new literature sources have been added.

 

Change in Manuscript:

Eleven new literature sources have been added in the revised manuscript under numbers [6-9, 17-20, 29, 31 and 40].

2) In the introduction, you should better explain why it is important to design an anti-icing and anti-microbial surface: for instance, which are the main applications?

Response:

This is a very good point, so thank you very much. Your comment is fully taken into account.

 

Change in Manuscript:

A short paragraph revealing the importance of fabricating anti-icing and anti-microbial surfaces is now available on Page 1 Lines 37-41 and Page 2 Lines 42-43 in the revised manuscript.

3) Fig. 4: The green spheres in 4(a) seem to be particles but in (c) are described as "silica sol". So, are they precipitated particles or colloidal? Moreover, I recommend you to add the acronymous (ERMs) to the tag in fig. 4(b), since in the legend of Fig 4(c) the acronymous ERM is the only one reported.

Response:

Figure 4 is not an original work of the author. It is taken from ref. [27] and used with permission from Elsevier (the copyright forms have been submitted to the editorial office during the first submission). Therefore, Dr. Esmeryan thinks that it would be highly inappropriate to make any changes in the figure, since it is not a result of his personal contribution. Regarding the green spheres, and based on the information provided in ref. [27], the author considers these particles as colloidal.

Change in Manuscript:

A clarification is now available on Page 4 Line 119 in the revised manuscript.

4) Line 169-171: you should add the bibliographic info.

Response:

Well, after several checks of Lines 169-171 in the first draft, Dr. Esmeryan cannot see where a bibliographic info (he assumes the reviewer means citation brackets) should be added. Here is what lines 169-171 were representing in the first draft: “Instead, the biomass attachments are suppressed by increasing the substrate-to-foulant separation distance and the kinetic threshold for bioadhesion [26] or rupturing the cells through the tensile stress exerted by the nanopillars [25].” As seen, the relevant literature is cited.

5) Fig. 5 left part: why you coloured the spheres that represent the oxygen functional groups with two different blue?  I think they should be coloured with the same colour since they should represent the same molecules.

Response:

Nice question, thanks a lot. The opaque blue spheres indicated already frozen condensates, whereas the sky-blue spheres denote the unfrozen (liquid) condensates.

Change in Manuscript:

Information regarding the color of the spheres is available as a caption below Figure 5.

6) The legend of Fig. 5 should be improved: you should describe what happened on the left side and on the right side of the figure, as the same as you did in figure 6.

Response:

Dr. Esmeryan completely agrees with the reviewer’s opinion. The legend of Figure 5 has been improved accordingly.

Change in Manuscript:

A more detailed legend of Figure 5 is now available as a caption below it.

7) From line 213 to line 215: you write that to achieve the target, a pattern of pillars in a specific range of dimensions should be prepared. How did you calculate the proposed dimensions? Is there any bibliographic reference for it or this is a result of one of your study? Please, add some more explanations.

 

Response:

Good point. The proposed dimensions are based on the size of Pseudomonas species, recently reported in ref. [35].

Change in Manuscript:

A novel information regarding the proposed topographical arrangement is now available on Page 8 Lines 230-231 in the revised manuscript. In addition, some phrases in the manuscript have been changed in order to improve its readability.

Author Response File: Author Response.pdf