A Mini-Review of Synthetic Organic and Nanoparticle Antimicrobial Agents for Coatings in Textile Applications

Round 1

Reviewer 1 Report

The current review "A Review of Synthetic Organic Antimicrobial Agents for Coatings in textile applications". I think this review can only be published after addressing several major issues as following:

1-      The authors should clarify the title to be appropriate to the content, as other factors such as nanoparticles, which are not organic materials, have been presented.

2-      All abbreviations used should be mentioned in the place of their first mention followed by an abbreviation and then only the abbreviation is written.

3-      In the introduction there are some paragraphs without references.

4-      Lines 35-36 "Staphylococcus aureus (S. aureus), Escherichia coli (E. coli), and Enterococcus faecalis (E. faecalis)" replace to italic form "Staphylococcus aureus (S. aureus), Escherichia coli (E. coli), and Enterococcus faecalis (E. faecalis)".

5-      Lines 47-49 "Escherichia coli, Klebsiella pneumonaie, Pseudomonas aeruginosa, Staphylococcus aureus, and Acinetobacter baumannii." replace to italic form "E. coli, Klebsiella pneumonaie, Pseudomonas aeruginosa, S. aureus, and Acinetobacter baumannii."

6-      Lines 93-94 "Klebsiella pneumonaie, Pseudomonas aeruginosa and Escherichia coli" replace to italic form "Klebsiella pneumonaie, Pseudomonas aeruginosa and Escherichia coli"

7-      Line 94 "Klebsiella pneumonaie" replace to italic form.

8-      Lines 96 and 98 "Pseudomonas aeruginosa" replace to italic form "Pseudomonas aeruginosa"

9-      Lines 100 and 101 "Escherichia coli and E. coli" replace to italic with uniform style.

10-  Lines 109 -110 "Aspergillus niger, Aspergillus fumigatus Trichoderma viride, Curvularia lunota and PenIcillium" replace to italic form with space between them "Aspergillus niger, Aspergillus fumigatus, Trichoderma viride, Curvularia lunota and PenIcillium sp."

11-  Lines 114 and 115 "Algae" replace to "algae"

12-  Lines 116-117 "Oscillatoria borneti, Selenastrum gracile, Schenedesmus quadricauda, Volvox sp, Anabaena cylindrical, Pleurococcus sp., Gonium sp. and Chlorella Vulgaris" replace to italic form with the first letter of the species is small "Oscillatoria borneti, Selenastrum gracile, Schenedesmus quadricauda, Volvox sp., Anabaena cylindrical, Pleurococcus sp., Gonium sp. and Chlorella vulgaris"

13-  Lines 151 "N atom" and line 153 "a nitrogen (N) atom"?

14-  Line 181 and 182 Staphylococcus aureus and Escherichia coli?

15-  Scientific name for microorganisms should be one form. Revised all manuscript.

16-  Line 322 "Mg2+ and Ca2+", Line 420 Kanazawa et al. [78] [79]? Line 422 "Gram-negative E. coli", line 427 " P. aeruginasa, E. coli, C. albicans, and S. aureus"?

17-  Line 438 "Gram-negative B. subtilis" How is the B. subtilis gram-negative? The authors have to modify it to gram-positive. "Gram positive B. subtilis"

18-  Lines 450-451 "Staphylococcus aureus, Escherichia coli, Bacillus subtilis and Pseudomonas aeruginosa."

19-    Lines 441-477. There are many paragraphs without references. These are recent references on nanotechnology that help clarify them: https://doi.org/10.1021/acs.iecr.0c04880, https://doi.org/10.3390/biology10030233; https://doi.org/10.1007/s12011-020-02138-3, https://doi.org/10.1016/j.micpath.2018.09.030.

20-  Lines 490-494 "One of these paths appears to be the use of silver nanoparticles. Their effectiveness against pathogens is proven in multiple studies, as well as the inability of microorganisms to develop immunity to them, unlike with many antibiotics. Nevertheless, factors like cytotoxicity or the eco-friendliness of the methods used in implementing AgNPs onto fabrics must be taken into consideration." Add these recent references on the development of silver nanoparticles in the treatment of fabrics:

https://doi.org/10.3390/nano10102082; https://doi.org/10.3390/antibiotics9100641

21-  Lines 505 and 514 "Curcuma longa" replace to italic. Lines 508-509 "Staphylococcus aureus, Streptococcus pyogenes, Escherichia coli, Pseudomonas aeruginosa and Candida albicans" replace to italic.

22-  Line 549 "fungus P. aeruginosa"????? How do bacteria turn into fungi?

23-  Add these references to the synthesis of silver particles by plant extract and fungi

https://doi.org/10.1016/j.arabjc.2022.103927; https://doi.org/10.3390/bioengineering9090452

https://doi.org/10.1007/s12668-022-01026-5; https://doi.org/10.1007/s13399-022-03507-9

24-  Line 610 "12h" and "24 hours"?

25-  Line 638 "S. aureus, S. epidermidis, E. coli, P. Aeruginosa and T. rubrum"??

26-  The discussion is very short.

27-  Authors should standardize the reference style.

28-  Add appendix for abbreviation.

29-  The whole manuscript must be checked to avoid the presentation of same information several times.

30-  The text must be checked carefully in order to correct the editing errors.

Author Response

Response to Reviewer 1 Comments

Dear sir, we thank you for your time, and effort in reviewing our work.  Following your valuable comments, we corrected and improved the manuscript. Thanks to your suggested references and statements, we believe that the new material and flow of text brought this revised script to an adequate level to contribute to the science.

The current review "A Review of Synthetic Organic Antimicrobial Agents for Coatings in textile applications". I think this review can only be published after addressing several major issues as follows:

Thank you for the valuable comments and great contribution. We are much obliged. We have addressed all points and problems in the text which is marked in red colour and new or modified sections are in the colour according to the relative comments (green, purple, ruby red)
Please see the attached revised script in colours for your convenience

1. The authors should clarify the title to be appropriate to the content, as other factors such as nanoparticles, which are not organic materials, have been presented.

The title has been modified accordingly including Nanoparticles

2. All abbreviations used should be mentioned in the place of their first mention followed by an abbreviation and then only the abbreviation is written.

The definition of any abbreviation is firstly given and then onwards only the abbreviations is used in the subsequent text.

3. In the introduction, there are some paragraphs without references.

All paragraphs but the first now have references. The first paragraph mentions the scope and rationale of the review article requested by the MDPI template.

4. Lines 35-36 "Staphylococcus aureus (S. aureus), Escherichia coli (E. coli), and Enterococcus faecalis (E. faecalis)" replace to italics form "Staphylococcus aureus (S. aureus), Escherichia coli (E. coli), and Enterococcus faecalis (E. faecalis)".

Microorganisms are now in italics format. The problem appeared transferring the document text into the manuscript template where the text format was replaced by that of the template.

5. Lines 47-49 "Escherichia coli, Klebsiella pneumonaie, Pseudomonas aeruginosa, Staphylococcus aureus, and Acinetobacter baumannii." replace to italics form " coli, Klebsiella pneumonaie, Pseudomonas aeruginosa, S. aureus, and Acinetobacter baumannii."

Same as correction 4, now in italics.

6. Lines 93-94 "Klebsiella pneumonaie, Pseudomonas aeruginosa and Escherichia coli" replace to italics form "Klebsiella pneumonaie, Pseudomonas aeruginosa and Escherichia coli"

Same as correction 4, now in italics and abbreviated.

7. Line 94 "Klebsiella pneumonaie" replace to italics form.

Same as correction 4, now in italics.

8. Lines 96 and 98 "Pseudomonas aeruginosa" replace to italics form "Pseudomonas aeruginosa"

Same as correction 4, now in italics and abbreviated.

9. Lines 100 and 101 "Escherichia coli and E. coli" replace with italics with a uniform style.

Same as correction 4, now in italics and abbreviated.

10. Lines 109 -110 "Aspergillus niger, Aspergillus fumigatus Trichoderma viride, Curvularia lunota and PenIcillium" replace to italics form with space between them "Aspergillus niger, Aspergillus fumigatus, Trichoderma viride, Curvularia lunota andPenIcillium"

Same as correction 4, now in italics

11. Lines 114 and 115 "Algae" replace to "algae"

The word “Algae” is now in lower case, “algae”

12. Lines 116-117 "Oscillatoria borneti, Selenastrum gracile, Schenedesmus quadricauda, Volvox sp, Anabaena cylindrical, Pleurococcus sp., Gonium sp. and Chlorella Vulgaris" replace to italics form with the first letter of the species is small "Oscillatoria borneti, Selenastrum gracile, Schenedesmus quadricauda, Volvox , Anabaena cylindrical, Pleurococcus sp., Gonium sp. andChlorella vulgaris"

Same as correction 4, now in italics and correctly lettered

13. Lines 151 "N atom" and line 153 "a nitrogen (N) atom"?

Both lines have now the correct wording ”nitrogen (N) atom”

14. Line 181 and 182 Staphylococcus aureus and Escherichia coli?

Same as correction 4, now in italics and abbreviated.

15. Scientific name for microorganisms should be one form. Revised all manuscript.

Scientific names for microorganisms are now in italics and a list of abbreviations was given in appendix A as requested in 28

16. Line 322 "Mg2+ and Ca2+",

The ²⁺ is now in superscript form. The problem arose transferring the document text into the manuscript template where the text format was replaced by that of the template.

Line 420 Kanazawa et al. [78] [79]?

Both references have reported the work of Kanazawa. The reference to Kanazawa has been added to the text [80] and stated as follows “reported by Kanazawa [80] and referenced in [81] and [82].”

Line 422 "Gram-negative E. coli",

Same as correction 4, now in italics and abbreviated.

line 427 " P. aeruginasa, E. coli, C. albicans, and S. aureus"?

Same as correction 4, now in italics and reported and abbreviated.

17- Line 438 "Gram-negative B. subtilis" How is the B. subtilis gram-negative? The authors have to modify it to gram-positive. "Gram positive B. subtilis"

"Gram-negative B. subtilis" has been corrected to " Gram-positive Bacillus subtilis (B. subtilis) "

18 Lines 450-451 "Staphylococcus aureus, Escherichia coli, Bacillus subtilis and Pseudomonas aeruginosa."

Same as correction 4, now in italics and used in abbreviated form (S. aureus, E. coli, B. subtilis and P. aeruginosa).

18. Lines 441-477. There are many paragraphs without references. These are recent references on nanotechnology that help clarify them: https://doi.org/10.1021/acs.iecr.0c04880, https://doi.org/10.3390/biology10030233; https://doi.org/10.1007/s12011-020-02138-3, https://doi.org/10.1016/j.micpath.2018.09.030.

All new references were added to the text in the referred section and the last in the multifunctional textile section.

20-  Lines 490-494 "One of these paths appears to be the use of silver nanoparticles. Their effectiveness against pathogens is proven in multiple studies, as well as the inability of microorganisms to develop immunity to them, unlike with many antibiotics. Nevertheless, factors like cytotoxicity or the eco-friendliness of the methods used in implementing AgNPs onto fabrics must be taken into consideration." Add these recent references on the development of silver nanoparticles in the treatment of fabrics:

https://doi.org/10.3390/nano10102082; https://doi.org/10.3390/antibiotics9100641

Both references were reviewed and added. Thank you

21-  Lines 505 and 514 "Curcuma longa" replace to italics.

Same as correction 4, now in italics

Lines 508-509 "Staphylococcus aureus, Streptococcus pyogenes, Escherichia coli, Pseudomonas aeruginosa and Candida albicans" replace to italics.

Same as correction 4, now in italics

22-  Line 549 "fungus P. aeruginosa"????? How do bacteria turn into fungi?

The word fungus has been corrected to bacteria.

23-  Add these references to the synthesis of silver particles by plant extract and fungi

https://doi.org/10.1016/j.arabjc.2022.103927; https://doi.org/10.3390/bioengineering9090452

https://doi.org/10.1007/s12668-022-01026-5; https://doi.org/10.1007/s13399-022-03507-9

The above reference references were introduced and referenced in the article’s text

24-  Line 610 "12h" and "24 hours"?      

The ”12h” and "24 hours" have been changed to “12 hours” and “24 hours”

25-  Line 638 "S. aureus, S. epidermidis, E. coli, P. Aeruginosa and T. rubrum"??

Same as correction 4, now in italics and abbreviation was firstly defined (S. aureus, Staphylococcus epidermidis (S. epidermidis), E. coli, P. Aeruginosa and Trichophyton rubrum (T. rubrum))

26-  The discussion is very short.

The discussion section was kept short as the recommended structure for review articles does not include separate discussions. To be in line with the template this section is now included in the “9. Conclusions” section where and further analysis was presented with solid statements and suggestions.

27-  Authors should standardize the reference style

Some overlooked references in section 7 have been corrected in style in a unified standard form through Zotero

28-  Add appendix for abbreviation.

Appendix A with abbreviations has been added to the script.

29-  The whole manuscript must be checked to avoid the presentation of the same information several times.

To avoid repetitions of the antimicrobial action of several species the following changes have taken place:

Lines 451 to 456 “The way that these works is that when copper is exposed to water and oxygen, it releases ions that create organic complexes with elements found in the bacteria. As a result, the structure of nucleic acids proteins and the cell wall collapses, leading to cell destruction” have been replaced by: “The antimicrobial action does not differ from the mechanism previously analysed”

Lines 168 “The surfactant–microbe complex form causes the interruption of all essential functions of the cell membrane and the interruption of protein activity” has been replaced with “as described in the antimicrobial action section”

Lines 172-173 “including damage to cell membranes, denaturation of proteins and disruption of cell structure” have been deleted

Lines 182-183 have been simplified to avoid the repetition of the explanation of the antimicrobial action (“including damage to cell membranes, denaturation of proteins and disruption of cell structure”)

Lines 273-274 “as explained in the respective section” has been added.

Line 493 Newly added text makes reference to the main antimicrobial mechanism and avoids repetitions

30-  The text must be checked carefully in order to correct the editing errors.

Lines 146-148 have been deleted as they belonged to the template.

Lines 326-327 “Monomeric or dimeric biguanides exert antimicrobial activity of the corresponding monomeric or dimeric biguanides” has been rewritten as “Both monomeric and dimeric biguanides exert antimicrobial activity, while the latter is more effective against all types of bacteria.”

The chemical formula in figure 4 has been transformed to match the style of the rest figures

References 12 and 18 (lines 704 and 711) were checked and introduced again.

Please see the attached revised script in colours for your convenience 

Author Response File: Author Response.pdf

Reviewer 2 Report

The manuscript by Michail Karypidis et al. entitled A Review of Synthetic Organic Antimicrobial Agents for Coatings in textile applications takes up on the subject of the production of textiles with antimicrobial features. The subject is important, as currently available antimicrobial fabrics are far from perfect and the research in this field is on the rise, especially since the Covid-19 pandemic. The article is written pretty well in terms of English and style, it fits the scope of the Coatings for Antimicrobial Textiles special issue in the journal Coatings.

However, after reading the manuscript I have to advise to decline the publication of it. Atop of other reasons, there are two that are crucial in the matter. First, I do not see the novelty of the review – there is a number of current reviews on this topic available, some of which cited by the authors, which quite exhaust the subject. Secondly, it seems to me that the article needs a strong edition, as currently it seems that the authors had no aim of the study and sometimes the information given (whole chapters even) feels random and not come together to form a review.

Major comments:

1.    Chapter 2. The description is brief (even very brief). Instead of expanding the whole chapter 2 into something bigger, I would change the description of the chapter, as well as the sentence regarding it in the abstract to reflect that only the microbes affecting the quality of the textiles are taken into account. On the other hand, only bacteria and fungi are described in subchapter 2.5 and in the later chapters about the action of coated textiles, so I see little need for the other organisms? Also, this chapter could use a graphical figure to make it more appealing to the readers uncommon to the subject.

2.    The whole article – contains no discussion (apart from four sentences in misnumbered chapter Discussion – line 642). If new studies are reviewed, it would be nice to see the results of the findings discussed, not only rewritten from other reviews on the subject. The chapter 5 especially lacks some insight.

3.    Chapter 5: Lacks any discussion of the results. I would like to see if the synthesized polymers were tested for their coating on fabrics, which fabrics, whether they were attached in a stable manner, what about their potential ecological fate, etc. Also, most of the references in this chapter is at least 10 years old. To keep an up-to-date literature would be to use articles from up to five years.

4.    Chapter 6: Should be deleted or written from scratch – currently it is based on one reference, which is a book chapter. It is unacceptable as such. Also, it has little to do with the subject of the review, as there are even no examples of such applications given.

Less significant remarks:

5.    All systematic names of organisms should be in italic, whether it is a plant or a bacteria, etc.

6.    Sentence in lines 70-73 is pretty hard to understand. Perhaps you could rewrite it or split it into two sentences?

7.    Sentence in lines 146-148 should be deleted – it is from the template.

8.    All the chemical structures differ in drawing style. Please unify.

9.    “Monomeric or dimeric biguanides exert antimicrobial activity of the corresponding monomeric or dimeric biguanides”(line 326-327) – this sentence makes no sense.

10.  Please separate the disadvantages by introducing subchapter 4.2.

11.  References [78] and [79] are not by Kanazawa et al.(line 420).

12.  There seems to be something wrong with references 12 and 18 (lines 704 and 711).

Author Response

Response to Reviewer 2 Comments

Dear sir, we thank you for your time, and effort in reviewing our work. We corrected and improved the manuscript according to your valuable comments. Thanks to your strong remarks and guidance, we believe that the new revised and flow of context brought this revised script to an adequate level.

Comments and Suggestions for Authors

The manuscript by Michail Karypidis et al. entitled A Review of Synthetic Organic Antimicrobial Agents for Coatings in textile applications takes up on the subject of the production of textiles with antimicrobial features. The subject is important, as currently available antimicrobial fabrics are far from perfect and the research in this field is on the rise, especially since the Covid-19 pandemic. The article is written pretty well in terms of English and style, it fits the scope of the Coatings for Antimicrobial Textiles special issue in the journal Coatings.

Thank you for your kind words. We also feel that there is a lot to be gained from the use of antimicrobial textiles as the latter is an inseparable part of human life.

However, after reading the manuscript I have to advise to decline the publication of it. Atop of other reasons, there are two that are crucial in the matter. First, I do not see the novelty of the review – there is a number of current reviews on this topic available, some of which cited by the authors, which quite exhaust the subject. Secondly, it seems to me that the article needs a strong edition, as currently it seems that the authors had no aim of the study and sometimes the information given (whole chapters even) feels random and not come together to form a review.

Thank you for your comments. A strong effort was made to address the problems mentioned and novel sources up to 2022 were included to promote novelty and address the problems in the major comments. Whole chapters have been reworked to follow the sequence of introduction into microbes, antimicrobial actions, traditional antimicrobial agents, antimicrobial polymeric structures, nanoparticles (including copper), green synthesis of antimicrobial agents, and conclusions including discussion. A short appendix is given to help the uncommon readers of the subject to follow the abbreviations used in the text.

We believe following your valuable guidance, advises and comments the whole work has improved and come to the adequate level. We are much obliged.

Major comments:

The problems and comments were addressed in blue colour and new or modified sections are in the colours (ruby red) of the relative (purple) to the comments (green) below

1. Chapter 2. The description is brief (even very brief). Instead of expanding the whole chapter 2 into something bigger, I would change the description of the chapter, as well as the sentence regarding it in the abstract to reflect that only the microbes affecting the quality of the textiles are taken into account.

The purpose of chapter 2 is not the in-depth analysis of the microbes but a short stimulus to the reader in the characterisation of types of microbes. The “uncommon to the subject” readers (as very well stated in the major reviewer comments) will be in a position to understand the action of biostatic and biocidal action of the antimicrobial agents. Accepting the reviewer’s valuable comments, the chapter is renamed “Short introduction to the types of microbes”.

On the other hand, only bacteria and fungi are described in subchapter 2.5 and in the later chapters about the action of coated textiles, so I see little need for the other organisms?

As mentioned in the text textile can be the media of transfer microbes besides the undesirable effects that can happen to them. For this reason, all types of microbes are equally important they are all given a very short but complete introduction.

“When bacteria come in contact with the fibres, undesirable effects take place on the textile material, such as the generation of unwanted odour and discolouration of the fabric with an overall drop in the fabric's mechanical strength as a result of the fibre damage [5] and possible contamination [1], [2], [3]. Natural fibres such as cotton are the ideal fabrics for the growth of pathogens.”
“These can cause pathogenic effects on human beings because of user contamination and cross-infection [7], [8].”

Also, this chapter could use a graphical figure to make it more appealing to the readers uncommon to the subject.

Thank you for your suggestion. A graphical figure (Scheme 1) has been drawn and added to explain the main antimicrobial action.

2. The whole article – contains no discussion (apart from four sentences in misnumbered chapter Discussion – line 642). If new studies are reviewed, it would be nice to see the results of the findings discussed, not only rewritten from other reviews on the subject. The chapter 5 especially lacks some insight.

The ill-numbered Discussion section was kept short as the recommended structure for review articles of MDPI does not include separate discussion. To be in line with the template this section is now included in the “9. Conclusions” section where and a further analysis was presented with solid statements and suggestion.

3. Chapter 5: Lacks any discussion of the results. I would like to see if the synthesized polymers were tested for their coating on fabrics, which fabrics, whether they were attached in a stable manner, what about their potential ecological fate, etc. Also, most of the references in this chapter is at least 10 years old. To keep an up-to-date literature would be to use articles from up to five years.

Thank you for your comment. Up-to-date literature has been added in the chapter with further analysis.

The reference [86-96] added are within the suggested period.

4. Chapter 6: Should be deleted or written from scratch – currently it is based on one reference, which is a book chapter. It is unacceptable as such. Also, it has little to do with the subject of the review, as there are even no examples of such applications given.

Thank you for your comment. This chapter is meant to be short as it covered only a brief presentation of the use of cooper as a microbial agent highlighting the strong antimicrobial action of the copper ions as well as their low toxicity due to compatibility with the human natural system.
The chapter was currently updated and re-written to included all new advances CNP’s (cooper nanoparticles) with a series of fresh references as [90] and [97 -114].

Less significant remarks:

4. All systematic names of organisms should be in italic, whether it is a plant or a bacteria, etc.

This was caused during the transfer of the information into the MDPI template (copy and paste as text). We apologise for overlooking it. All systematic names of organisms are set in italic.

5. Sentence in lines 70-73 is pretty hard to understand. Perhaps you could rewrite it or split it into two sentences?

The two sentences are re-written into three sentences making the text easier to follow. Thank you for your kind remark.

7. Sentence in lines 146-148 should be deleted – it is from the template.

We are sorry the sentence was overlooked. Thank you for mentioning it. The sentence has been removed.

8. All the chemical structures differ in drawing style. Please unify.

The chemical formula in figure 4 has been transformed in the appropriate style of the rest figures. Thank you for mentioning it.

9. “Monomeric or dimeric biguanides exert antimicrobial activity of the corresponding monomeric or dimeric biguanides”(line 326-327) – this sentence makes no sense.

The sentence has been rewritten as: “Both monomeric and dimeric biguanides exert antimicrobial activity, while the latter is more effective against all types of bacteria.”

10. Please separate the disadvantages by introducing subchapter 4.2

Thank you for kind comment. Chapter 4 has been adjusted to include the details arguments of advantages and disadvantages giving a more meaningful comparison. The subchapter 4.1 was absorbed.

11. References [78] and [79] are not by Kanazawa et al.(line 420).

Thank you for mentioning it. Both references have been reported the work of Kanazawa. The text has been corrected and the reference of Kanazawa has been added to the text [80] and stated as follows “reported by Kanazawa [80] and referenced in [81] and [82].”

12. There seems to be something wrong with references 12 and 18 (lines 704 and 711).

These references have been checked and correctly introduced once again. Thank you for your kind comment.

Author Response File: Author Response.pdf

Reviewer 3 Report

Antimicrobial function imparted to textiles is one of the most important functions which can attract diverse consumers. Relevant antimicrobial and technologies have been in progress. Antimicrobial textiles have been a hot research topic. In this manuscript, authors review the development, properties, advantages and disadvantages of diverse antimicrobial agents. The research accords with the scope of Coatings - Special Issues - Coatings for Antimicrobial Textiles. Most of the content is clearly and rightly discussed. Overall, the paper is well organized. The paper can be accepted for publishing after minor revision.

Please note the following issues:

There are 11 keywords? Please note the instructions for authors and the requirements for keywords.

Lines 86-88: “In the test, the Gram-positive bacteria were coloured dark blue or with crystal violet dye due to a high concentration of peptidoglycan in the cell wall. The Gram-negative bacteria did not retain the violet dye and presented a red or pink hue”: “were”, “did”, and “presented” should be replaced by “are”, “do”, and “present”.

Lines 99-100: “E. coli are” should be replaced by “is”.

Lines 113-114: “In areas which are in constant contact with water form algae, thus making it a common problem”: Please check this sentence.

Line 138: “Scheme 1. General chemical structure of Quaternary ammonium compounds (QACs)”: “Quaternary” should be replaced by “quaternary”.

Lines 139-148: Authors mention polymer antimicrobial agents. However, some organic antimicrobial agents are not polymers. For example, some quaternary ammonium compounds (e.g., linear alkylammonium compounds), triclosan, and small molecular halamines are not polymers. So please note the relative technical terms.

Line 157: “N⁺R1R2R3R4X−”: “−” should be written in superscript.

Lines 177-184: Authors mention the antibacterial property of poly(D,L-lactide) (PDLLA) fibrous membranes modified with quaternary ammonium parts. When I read the contents before and after Lines 177-184, I think that this example is unnecessary. Conversely, the presence of this example lowers the quality of this section. Additionally, nanofiber membranes are not textiles, and furthermore they have not found good, practical applications in textiles although wide researches have been carried out. So I suggest authors to delete lines 177-184.

Line 192: “The QACs monomers were named surfactant monomers or “surfmers””: “were” should be replaced by “are”.

Lines 207-221: Authors discuss antimicrobial cationic dyes and antimicrobial cationic, reactive dyes.

In general, cationic dyes are used for the dyeing of anionic acrylic fiber bearing -SO₃H. In Ref. 39, a long-chain alkyl quaternary ammonium is introduced into a dye chromophore with the aim of imparting antibacterial function to acrylic fiber. In this research, the cationic groups of dyes are different from classical cationic dyes used for acrylic fiber. In Ref. 39, the durability of antibacterial property to washing is poor, while the color fastness (similarly durability) of dyed fabric to washing is good, as revealed by the changes of color depth (K/S) after different cycles of washing in Table 4.

Classic reactive dyes bearing –SO₃Na and reactive groups are anionic, and used for the dyeing of natural (e.g., cotton, linen, and ramie) and regenerated (e.g., viscose, lyocell and modal) cellulose fibers. In Ref. 40, a long-chain alkyl quaternary ammonium is introduced into a dye chromophore with the aim of imparting antibacterial function to cotton fiber. In this research, the charge character of dyes (cationic) is different from that of classical reactive dyes (anionic). In Ref. 40, the durability of antibacterial property to washing is poor, as indicated by the data in Table II. In my opinion, the cationic reactive dyes are not ones for dyeing cellulosic fibers in terms of dyeing behaviors.

In Lines 207-221: I suggest authors only to mention that two cationic dyes without and with reactive groups, the former being used for the dyeing of acrylic fiber and the latter being used for the dyeing of cotton fiber, can impart antibacterial function to fibers which has poor durability to washing. If possible, authors do not discuss the reason for the poor durability of antibacterial property to washing. Otherwise, the academic error occurs. The durability of colors in dyed fibers is different from that of antibacterial property, the latter of which is complex and depends on many factors including the distribution of functional dyes on the surface and interior of fibers and the measurement methods of antibacterial activity.

Line 230: Sub-title “3.1. The N-halamines” should be replaced by “3.2. The N-halamines”.

Line 260: “hydroxyl groups on cellulose fibres” might be replaced by “hydroxyl groups of (or in) cellulose fibres”.

Line 263: “react with the cellulose hydroxyl groups” might be replaced by “react with hydroxyl groups of (or in) cellulose”.

Line 296: “Triclosan” should be replaced by “triclosan”.

Regarding Figures 1-4:

Please check whether Figures 1-4 are mentioned in text or not.

Figure 1. General chemical structure of Quaternary ammonium compounds (QACs)

Figure 2. Molecular structure of N-halamines

Figure 3. Molecular Structure of Triclosan

Figure 4. Molecular Structure of poly(hexamethylenebiguanide) (PHMB).

Quaternary-quaternary, Structure-structure, Triclosan-triclosan

Line 316: “Guanidine salt” should be replaced by “guanidine salt”.

4. Advantages and Disadvantages of synthetic antimicrobial agents

Disadvantages-disadvantages

7. Green Methods of creating and applying AgNPs onto cotton fabrics

Methods-methods

Line 368: “Quaternary Ammonium Compounds (QACs)” should be replaced by “QACs” because its full name is mentioned before.

Line 419: “The antimicrobial activity in these two polymers”: “in” should be replaced by “of”.

Lines 419-422: Regarding English tenses: was, was, have, and was. Please take a check.

Line 433: “Novel” should be replaced by “novel”.

Lines 446-449: Regarding the name of bacterial strain: full name? abbreviation？

Regarding “6. Copper in polymeric matrices”:

The STANDARD 100 by OEKO-TEX® is a worldwide consistent, independent testing and certification system for raw, semi-finished, and finished textile products at all processing levels, as well as accessory materials used. In this standard, the following heavy metals are limited to very low values: Sb, As, Pb, Cd, Cr, Co, Cu, Ni, and Hg; the limited value of Cu content is 25 mg/kg for baby textiles, 50 mg/kg and other textiles.

https://www.oeko-tex.com/en/apply-here/standard-100-by-oeko-tex

https://www.oeko-tex.com/importedmedia/downloadfiles/STANDARD_100_by_OEKO-TEX_R__-_Standard_en.pdf

Copper and its salts are used as antibacterial agents many years ago. However, nowadays, for the use of them, special attention should be paid in terms of limited value of Cu content. So I suggest authors to simply mention the limited value of Cu content in a widely accepted STANDARD 100 by OEKO-TEX.

Line 571: Sub-title “Green Methods of creating and applying AgNPs onto cotton fabrics”: I suggest authors to delete “cotton” because AgNPs can be applied for many fibers or fabrics. Of course, authors can take cotton fabrics as examples.

In addition, to the best of my knowledge, silane quaternary ammonium compounds are widely applied in textiles on a commercial scale. So, if possible, I suggest authors to add some relevant content.

I had read the partial content of the following paper. I think it is a good paper. Maybe, it is helpful to authors.

Lena Windler, Murray Height, Bernd Nowack. Comparative evaluation of antimicrobials for textile applications. Environment International 53 (2013) 62-73.

http://dx.doi.org/10.1016/j.envint.2012.12.010

Author Response

Response to Reviewer 3 Comments

Dear sir/madam,

we thank you for your time, and effort in reviewing our work. Following your valuable comments, we corrected and improved the quality of the manuscript. Thanks to your contribution, we believe that the revised script has come to an adequate level to contribute to the science.

Antimicrobial function imparted to textiles is one of the most important functions which can attract diverse consumers. Relevant antimicrobial and technologies have been in progress. Antimicrobial textiles have been a hot research topic. In this manuscript, authors review the development, properties, advantages and disadvantages of diverse antimicrobial agents. The research accords with the scope of Coatings - Special Issues - Coatings for Antimicrobial Textiles. Most of the content is clearly and rightly discussed. Overall, the paper is well organized. The paper can be accepted for publishing after minor revision.

Thank you for your kind comments and valuable remarks. We are much obliged. We have addressed all points and problems in the text which is marked in red colour and new or modified sections are in the colour 

Please see the attached revised script in colours for your convenience

1. There are 11 keywords? Please note the instructions for authors and the requirements for keywords
   Thank you for mentioning it. According to the template, 3-10 keywords are allowed. The “textiles;” and “coatings;” have been united “textile coatings;” as one keyword.

2. Lines 86-88: “In the test, the Gram-positive bacteria were coloured dark blue or with crystal violet dye due to a high concentration of peptidoglycan in the cell wall. The Gram- negative bacteria did not retain the violet dye and presented a red or pink hue”: “were”, “did”, and “presented” should be replaced by “are”, “do”, and “present”.
   The changes have been applied. Thank you for mentioning them.

3. Lines 99-100: “ coli are” should be replaced by “is”.
   The change has been applied. Thank you for mentioning it.

4. Lines 113-114: “In areas which are in constant contact with water form algae, thus making it a common problem”: Please check this
   Thank you for pointing it out. The sentence has been rewritten more comprehensively as follows:“A common problem that often arises is that surfaces in constant contact with water favour the growth of algae.”

5. Line 138: “Scheme General chemical structure of Quaternary ammonium compounds (QACs)”: “Quaternary” should be replaced by “quaternary”.
   The change has been applied. Thank you for mentioning it.

6. Lines 139-148: Authors mention polymer antimicrobial However, some organic antimicrobial agents are not polymers. For example, some quaternary ammonium compounds (e.g., linear alkylammonium compounds), triclosan, and small molecular halamines are not polymers. So please note the relative technical terms.
   Thank you for mentioning it. The technical term of polymer has been replaced by chemical species, compounds and by molecules for the aforementioned types of chemicals.

7. Line 157: “N+R1R2R3R4X−”: “−” should be written in
   Well spotted. Thank you for mentioning it. The change has been applied.

8. Lines 177-184: Authors mention the antibacterial property of poly(D,L-lactide) (PDLLA) fibrous membranes modified with quaternary ammonium parts. When I read the contents before and after Lines 177-184, I think that this example is unnecessary. Conversely, the presence of this example lowers the quality of this Additionally, nanofiber membranes are not textiles, and furthermore, they have not found good, practical applications in textiles although wide researches have been carried out. So I suggest authors to delete lines 177-184.
   We accept the well-set argument and we have removed 177-184 rectifying the reference numbering accordingly.

9. Line 192: “The QACs monomers were named surfactant monomers or “surfmers””: “were” should be replaced by “are”.
   The change has been applied. Thank you for mentioning it.

10. Lines 207-221: Authors discuss antimicrobial cationic dyes and antimicrobial cationic, reactive
    In general, cationic dyes are used for the dyeing of anionic acrylic fiber bearing -SO₃H. In Ref. 39, a long-chain alkyl quaternary ammonium is introduced into a dye chromophore with the aim of imparting antibacterial function to acrylic fiber.
    1. In this research, the cationic groups of dyes are different from classical cationic dyes used for acrylic fiber. In Ref. 39, the durability of antibacterial property to washing is poor, while the color fastness (similarly durability) of dyed fabric to washing is good, as revealed by the changes of color depth (K/S) after different cycles of washing in Table 4
       In acceptance of your comment, line 218 (on previous script line numbering) “The disadvantage, however, is the low wash fastness of the dyed acrylic fibres” has been removed as it can be contradictory and misleading. The authors' opinion in Ref 39 claims only superficial and core dye removal expressed by marginal colour change (K/S) of the dyed samples. Their claim extends to explain the affected antimicrobial activity which dropped after washings.
    2. Classic reactive dyes bearing –SO3Na and reactive groups are anionic, and used for the dyeing of natural (e.g., cotton, linen, and ramie) and regenerated (e.g., viscose, lyocell and modal) cellulose fibers. In Ref. 40, a long-chain alkyl quaternary ammonium is introduced into a dye chromophore with the aim of imparting antibacterial function to cotton fiber. In this research, the charge character of dyes (cationic) is different from that of classical reactive dyes (anionic). In Ref. 40, the durability of antibacterial property to washing is poor, as indicated by the data in Table In my opinion, the cationic reactive dyes are not ones for dyeing cellulosic fibers in terms of dyeing behaviors.
       In Lines 207-221: I suggest authors only to mention that two cationic dyes without and with reactive groups, the former being used for the dyeing of acrylic fiber and the latter being used for the dyeing of cotton fiber, can impart antibacterial function to fibers which has poor durability to washing. If possible, authors do not discuss the reason for the poor durability of antibacterial property to washing. Otherwise, the academic error occurs. The durability of colors in dyed fibers is different from that of antibacterial property, the latter of which is complex and depends on many factors including the distribution of functional dyes on the surface and interior of fibers and the measurement methods of antibacterial activity.
       Accepting your accurate suggestion, we have removed the suggested mechanism “due to the deactivation occurring between the negatively charged anionic detergent of the wash and the positively charged QACs dye part.” (lines 225-227 previous scrip numbering) and we have just mentioned only the “decrease the antimicrobial activity of both these dyes”.
       Additionally, lines 210-211 (previous scrip numbering) “Unlikewise, antimicrobial dyes on cotton exhibit with good better fast-ness to washing.” and line 222 (previous scrip numbering) “improve the wash fastness of the antimicrobial dye” have been removed based on the suggestions on the superficial dye wash off, mentioned earlier (Ref 40 claims the same mechanism as Ref 39).
       Thank you so much for the great reasoning and suggestion.
11. Line 230: Sub-title “3.1. The N-halamines” should be replaced by “3.2. The N-halamines”.
    The subchapter has been renumbered in the correct sequence. Thank you for pointing it out.
12. Line 260: “hydroxyl groups on cellulose fibres” might be replaced by “hydroxyl groups of (or in) cellulose fibres”.
    The change has been applied. Thank you.
13.  Line 263: “react with the cellulose hydroxyl groups” might be replaced by “react with hydroxyl groups of (or in) cellulose”.
    The change has been made. Thank you.
14. Line 296: “Triclosan” should be replaced by “triclosan”.Regarding Figures 1-4:
    The change has been applied. Thank you for mentioning it.

15. Regarding Figures 1-4:

    1. Please check whether Figures 1-4 are mentioned in text or not.
       All Figures (1-4) are now mentioned in the text.
       Additionally, Scheme 1 was added to the text.
    2. Figure 1. General chemical structure of Quaternary ammonium compounds (QACs)
       Figure 2. Molecular structure of N-halamines
       Figure 3. Molecular Structure of Triclosan
       Figure 4. Molecular Structure of poly(hexamethylenebiguanide) (PHMB).
       Quaternary-quaternary, Structure-structure, Triclosan-triclosan
       The above corrections have been applied to the text in all captions. Thank you.
16. Line 316: “Guanidine salt” should be replaced by “guanidine salt”.
    The correction has been applied. Thank you.
17. 4.Advantages and Disadvantages of synthetic antimicrobial agents
    Disadvantages-disadvantages
    The correction has been applied. Thank you.
18. 7.Green Methods of creating and applying AgNPs onto cotton fabrics
    Methods-methods
    The correction has been applied. Thank you.
19. Line 368: “Quaternary Ammonium Compounds (QACs)” should be replaced by “QACs” because its full name is mentioned before.
    The correction has been applied. Thank you.
20. Line 419: “The antimicrobial activity in these two polymers”: “in” should be replaced by “of”.
    The correction has been applied. Thank you for mentioning it.
21. Lines 419-422: Regarding English tenses: was, was, have, and Please take a check.
    The text was checked and all verbs are now in the past tense (i.e. the verb “to have” has been changed to “had”)
22. Line 433: “Novel” should be replaced by “novel”.
    The correction has been applied. Thank you for mentioning it.
23. Lines 446-449: Regarding the name of bacterial strain: full name? abbreviation？
    Both the full name and abbreviation of the fungi are now given. The abbreviations have been also added to appendix I.
24. Regarding “6. Copper in polymeric matrices”:
    The STANDARD 100 by OEKO-TEX® is a worldwide consistent, independent testing and certification system for raw, semi- finished, and finished textile products at all processing levels, as well as accessory materials used. In this standard, the following heavy metals are limited to very low values: Sb, As, Pb, Cd, Cr, Co, Cu, Ni, and Hg; the limited value of Cu content is 25 mg/kg for baby textiles, 50 mg/kg and other textiles.

    https://www.oeko-tex.com/en/apply-here/standard-100-by-oeko-tex
    https://www.oeko-tex.com/importedmedia/downloadfiles/STANDARD_100_by_OEKO-TEX_R-Standard_en.pdf
    Copper and its salts are used as antibacterial agents many years ago. However, nowadays, for the use of them, special attention should be paid in terms of limited value of Cu content. So I suggest authors to simply mention the limited value of Cu content in a widely accepted STANDARD 100 by OEKO-TEX.
    The values for all classes (class I and class II, III &IV) are mentioned and referenced. Furthermore, the threshold values by ECO PASSPORT by OEKO-TEX for the textile producers are now included. Thank you for your suggestions.

25. Line 571: Sub-title “Green Methods of creating and applying AgNPs onto cotton fabrics”: I suggest authors to delete “cotton” because AgNPs can be applied for many fibers or fabrics. Of course, authors can take cotton fabrics as
    Cotton fabrics are more prominent to bacteria attack due to their hydrophilic properties are researchers tend to concentrate their work on them more than other substrates. We accept the suggestion and we have removed the word “cotton” from the title. Thank you for raising the point.

26. In addition, to the best of my knowledge, silane quaternary ammonium compounds are widely applied in textiles on a commercial So, if possible, I suggest authors to add some relevant content.
    I had read the partial content of the following paper. I think it is a good paper. Maybe, it is helpful to authors.

    Lena Windler, Murray Height, Bernd Nowack. Comparative evaluation of antimicrobials for textile applications. Environment International 53 (2013) 62-73.
    http://dx.doi.org/10.1016/j.envint.2012.12.010

    This great work has already been referenced in the text regarding the benefits and risks associated with the use of any antimicrobial agents. However now, thanks to your suggestion, the Si-QAC’s have been added to the text of the manuscript as the type of QAC’s most traded worldwide. This new text replaced the unnecessary example Poly(D,L-lactide) (PDLLA) fibrous membranes modified with quaternary ammonium parts (i.e. suggested deletion of lines 177-184).

    The abbreviation has been added to appendix I. The mechanism of antimicrobial action and characteristics of this specie is covered by the general behaviour of this type of agent. In lines 201-206 (previous script numbering), the use tetraalkoxysilane (Si(OR)₄) with QACs is mentioned based on the reference of Ref 31 (previous script numbering, Tomsic, 2010).

    We are much obliged for your contribution to making this article more complete.

Round 2

Reviewer 1 Report

The manuscript is good for publication.

Author Response

Dear reviewer 

We sincerely thank you for your time and effort in reviewing our work and your contribution. We hope to cross paths in future publications.

Reviewer 2 Report

Dear authors, thank you for the changes made.

Unfortunately, the prepared manuscript still bears the same weak spots as before – it lacks the novelty and is poorly written. Although some fragments have been corrected, still the whole article is written in a significantly chaotic way, contains passages that do not fit into the whole, and at times one gets the impression that the aim of the work has not been precisely defined.

Because of that, my recommendation is still to reject the manuscript from being published.

Author Response

Response to Reviewer 2 Comments

Dear authors, thank you for the changes made.

We are much obliged to have your valuable help in the right direction.

Unfortunately, the prepared manuscript still bears the same weak spots as before – it lacks the novelty and is poorly written.

As mentioned in our previous reply we have closely followed the official template and we have added much new information from references up to 2022. We made every effort to correct and improve our written English and, in some cases, whole sections were rewritten. We apologise that English is not our first language, but we did all possible to bring it to an adequate level and we kindly ask for your understanding. Please don’t hesitate to identify parts of the script that need further improvement either on novelty or language.

Although some fragments have been corrected, still the whole article is written in a significantly chaotic way, contains passages that do not fit into the whole, and at times one gets the impression that the aim of the work has not been precisely defined.

Sadly, we have noticed that the total punctuation of the revised script has significantly dropped beside the aforementioned corrected segments. Please note that much of the modified text obeyed the suggested corrections and remarks of other reviewers. In any case, we are sorry that our manuscript was perceived as unclear and chaotic by your reading. We would like to provide an introduction to the structure of the script which may help its comprehension.

The article intends to review the types of the most known synthetic antimicrobial agents for functional applications in the textile sector against the main types of microbes and reveals their environmental friendliness. Its rationale is to present advances in novel antimicrobial coatings, which have a lower environmental impact, many of which are based on natural sources. It signifies the pass-over from traditional antimicrobial agents to nanotechnology and the novel biological method of formulation.

To do so it is necessary to define what is the role of the microbes, where they are found and the impact that they have on textiles, and the influence of the textiles causing cross-contamination. It is necessary to give a brief introduction to the reader unfamiliar with the subject and a quick insight into the types of microbes, where they are found and how they are identified. Very important is to explain the mode of anti-microbial action. We have introduced a schematic representation based on your remark. We thank you for this suggestion.

With this information, the reader can be introduced to classic synthetic organic antimicrobial agents which are widely used. This includes the Quaternary ammonium compounds (QACs) explaining their structure and mode of action, fastness to fabric and improvements. Sol-gel technology and Si-QACs are mentioned. Novel cationic antimicrobial dyes containing QAC are discussed which exhibit together colouration and anti-microbial action. Discussion on their fastness was asked to be removed by other reviewers. Following that N-halamines were similarly presented, including their bonds with the substrate and their antimicrobial action. Similar structures and their synergistic effects (combining N-halamines with N-halamine siloxane and QACs siloxane) were mentioned.  In the same manner, triclosan could not be left out as it is one of the most widely used antimicrobial agents. Commercial fabric examples were presented. Along with antimicrobial action, the toxicity of the agents had to be presented. A very important category is the Polybiguanidines. The presentation of these agents was also given in the same manner and extent as the rest of the antimicrobial agents.

The following chapter is dedicated to the presentation of the advantages and disadvantages of the previously presented antimicrobial agents. The list could not be exhaustive as there are points in the literature which either contradict or are unclear. This chapter states only the solid facts as they are referenced in literature rising several points of discussion.

The following chapter presents the potential application of other synthetic polymers on textiles which are yet not in commercial use. Several important older and newer specimens found in the literature were presented and referenced. Antimicrobial agents in combination with common textile finishes, such as cross-linking, showed improved fastness and performance. This provides ground for fresh ideas for research. These innovations bring about the passing over to nano-technology. An introduction to the latter is given as the rest of the article will deal with the subject.

Copper is one of the oldest anti-microbial agents and could not be excluded from the list. An introduction to the potential of copper as an anti-microbial agent coupled with its low toxicity was given. Reviewers asked to mention quantity limits found on the quality standards systems such as Oeko-Tex. The limited introduction to the important copper nanoparticles CNPs ignited reviewer comments and the result was their great contribution as they specialised in the area. The chapter covered the impressive advances of copper nanoparticles, their properties and their complexes with other agents which will play an important role in the future because of their unique characteristics. At the end of this chapter, the advances in the novel green nanoparticle formation are presented through the CuO-NPs /proteins formulation.

The following chapter is dedicated to the previously built knowledge and the most widely used antimicrobial nanoparticle, namely silver (AgNPs). Its structure was defined and the antimicrobial action coupled to wound healing was introduced, highlighting its low toxicity. Antimicrobial application on the most vulnerable substrate, namely cotton, was announced. Other improved properties such as wash fastness and UV protection were discussed. Green synthesis of AgNPs is of the most recent developments and daily novel green formulations were presented. The most important examples were presented using fungi aloe vera, gum tragacanth and chitosan.

Finally, the review could not omit the multifunctional fabrics which possess antimicrobial action accompanied by other important functions such as UV-protection, mosquito repelling action, thermal isolation, flame retardant properties, and electric conductivity. To do so ZnO and the latest AgNPs were discussed.

Having presented a wide range of the most important and novel antimicrobial agents, the review summarises the important topics of discussion on the environmental impact and human toxicity. The importance of nanoparticles is highlighted based on their lower toxicity, enhanced fastness, lower concentrations of application and green synthesis. New antimicrobial agents should be made either from plant sources or microorganisms as sustainability is of utmost importance. Although they exhibit lower efficiency compared to synthetic antimicrobial agents, there is room for improvement.

The article closes by stating that the next generation of antimicrobial agents should bear not only antimicrobial performance but human and environmental friendliness as the top priority accompanied by ease of application, durability and cost. Although the optimum recipe has not yet been discovered, significant advances lit the way.

Because of that, my recommendation is still to reject the manuscript from being published.

Based on the new insight provided and having applied the minor changes and remarks of all other reviewers to the revised manuscript, we ask for your kind re-evaluation once again, and/or specify points of improvement of the revised script.

We remain at your discretion and look forward to having your kind reply.