Microplastic–Pharmaceuticals Interaction in Water Systems

Round 1

Reviewer 1 Report (Previous Reviewer 3)

the manuscript has been significantly improved and can be considered to be published in JMSE,
still some typo mistakes can be noticed like in introduction or conclusions, but this could be easily temoved during final editing

 

Author Response

the manuscript has been significantly improved and can be considered to be published in JMSE,
still some typo mistakes can be noticed like in introduction or conclusions, but this could be easily removed during final editing.

Reply: regarding the abstract the following amendments highlighted in cyan have been made:

lines 19-22: ‘The review unites reports on experimental laboratory, mathematical, and field data on the MPs carrier role and accumulation role of PHs and their release and ecotoxicological effects for water bodies. The Knowledge gaps and key research priorities of MPs-PHs are identified to better understand and mitigate the environmental risks’ which was amended as:

 

Reply: regarding the conclusions the following amendments highlighted in cyan have been made:

lines 664-667: In particular, the electrostatic interaction is a physical mechanism driven by the pH of the aquatic system normally 5–9, when the surface charge of MPs varies among positive, negative, or neutral and polymers tend to aggregate. However, in the case of estuaries and coastal waters, the common pH is ~ 8.1, and there would be a tendency for many PHs to desorb from MPs due to the repulsion. Due to polymer features and Among all the environmental parameters, that might affect the interaction with drugs, pH represents the most important factor regulating sorption, since it affects MPs surface charges and drug speciation. Many studies report on the Trojan horse’s effect of MPsS on drugs and hence consider MPsS as a hidden source of toxicants that can be unintentionally taken up by biota. However, the effects on the bioavailability and toxicity forof aquatic organisms remain unpredictable as well as their ecological consequences. Thus, drug interaction with polymers remains yet a very complex subject in a marine water environment…

Reviewer 2 Report (New Reviewer)

Please find the following comments and recommendations: 1. The novelty of the study should be improved since the relation between the mentioned factors and MPs-PHs has already been investigated and reported in previous studies (e.g., 10.1016/j.envint.2020.106367). Please note that I am not requesting a direct citation of this specific paper, and I am not one of the authors of that work. 2. It appears that there is a missing paragraph in line 38. It is important to provide the necessary information to ensure the continuity of the content. 3. While discussing the frequent interaction of microplastics with other pollutants in wastewater treatment plants, you cited Figure 1. However, upon reviewing the legend of Figure 1, it is apparent that the environment is described as the sea. There is a discrepancy, and it is necessary to revise or remove Figure 1 accordingly. 4. In the section titled "3. MPs in aquatic systems," it is crucial to clearly establish the relevance of understanding MPs in aquatic systems and connect it to the purpose of writing this manuscript. 5. It is recommended to improve or revise the section headings, specifically "Association of PHs MPs," to ensure clarity and coherence with the content of the manuscript. 6. Please consider improving the resolution of Figure 2 for better visual clarity and interpretation by the readers. 7. I would like to emphasize the importance of including more tables and figures in review studies to enhance the presentation, clarity, and impact of the research. It would be valuable to incorporate additional tables and figures that discuss the latest studies on the interactions of PHs and MPs. Addressing these recommendations will significantly improve the quality and coherence of the manuscript.

Author Response

Please find the following comments and recommendations:

1. The novelty of the study should be improved since the relation between the mentioned factors and MPs-PHs has already been investigated and reported in previous studies (e.g., 10.1016/j.envint.2020.106367). Please note that I am not requesting a direct citation of this specific paper, and I am not one of the authors of that work.

Reply: the following paragraph was added (lines 90-94): The review aims to be an agile tool for consulting scientific news referring to a very limited time horizon limited to a few years. This is because the nature of the interaction, and the effects on biota are very complex and variable that perhaps only a systematic mechanic approach of data collection with a statistical approach big data and deep learning will contribute in the future to clarify.

 

2.It appears that there is a missing paragraph in line 38. It is important to provide the necessary information to ensure the continuity of the content.

Reply: the introduction was split in several paragraph and each has its heading to better drive the reader through the structure of the paper.

2. While discussing the frequent interaction of microplastics with other pollutants in wastewater treatment plants, you cited Figure 1. However, upon reviewing the legend of Figure 1, it is apparent that the environment is described as the sea. There is a discrepancy, and it is necessary to revise or remove Figure 1 accordingly.

Reply: Figure 1 was removed and indicated a graphical abstract

3. In the section titled "3. MPs in aquatic systems," it is crucial to clearly establish the relevance of understanding MPs in aquatic systems and connect it to the purpose of writing this manuscript.

Reply: this section was deeply enlarged and the importance to write the manuscript was stated.

4. It is recommended to improve or revise the section headings, specifically "Association of PHs MPs," to ensure clarity and coherence with the content of the manuscript.

Reply: section headings was improved and revised.

5. Please consider improving the resolution of Figure 2 for better visual clarity and interpretation by the readers.

Reply: This Figure was downloaded directly from the high resolution source of the Elsevier web site.

6. I would like to emphasize the importance of including more tables and figures in review studies to enhance the presentation, clarity, and impact of the research. It would be valuable to incorporate additional tables and figures that discuss the latest studies on the interactions of PHs and MPs. Addressing these recommendations will significantly improve the quality and coherence of the manuscript.

Reply: A new table was added indicating the effects of the association on aquatic organisms.

Reviewer 3 Report (New Reviewer)

Manuscript Number: jmse-2470200-peer-review-v1

Title: MICROPLASTIC-PHARMACEUTICALS INTERACTION IN WATER SYSTEMS

 

The purpose of this paper is to elucidate the interaction and association of MPs with pharmaceuticals, and the ecotoxicological implications on food webs. The content analysis of the manuscript is good, but the degree of innovation is not enough, the amount of data is small, and there is no great reference significance. It is recommended to reject the manuscript.

 

1. There are serious formatting issues throughout the text, including whether headings are top-notch, etc. Please revise carefully.

 

2. Fig. 1 is cited from other literature, but the manuscript does not contain an adequate analysis of it. Is it possible to remove it then?

 

3. Please note that abbreviations, such as OECD, DOC, etc. do not give their full names the first time they appear. Please check carefully.

 

4. Line 116: what is “MPshave”?

 

5. Line 130: “Scanning Electron Microscope (SEM) and X-ray diffractometer (XRD) analysis revealed that microplastics have different surface characteristics and degree of crystallinity.” What is the role of microplastics with different surface characteristics and crystallinity, which is obvious, highlighted here? What follows does not mention that the surface characteristics and crystallinity of microplastics influence their adsorption of PHs.

 

6. Line 130-140: What is the basis for this part of the discussion? Please give references.

 

7. Fig.2 is too blurry and needs to provide a higher resolution image. What does "adopted from 18" mean?

 

8. Table 1: There are many duplicate MPs in the "Polymer" column, so it is recommended to merge them. And there are too many contents in "Interaction mechanism" in each row. From this table, I can't understand what the interactions between each MPs and PHs are.

 

9. Line172 is the title of the table, while Line173 is the subheading of the article, what's going on?

 

10. Conclusion did not summary the full text of the work well, please revise it.

 

11. The abstract is not a good summary of the paper, please revise it.

 

12. "Factors driving the interaction" should also be summarized in a clear and concise table. In general, the data analysis in this thesis is poorly presented, with few original figures and only a poorly presented table. It needs to be carefully organized.

 

 

 

Extensive editing of English language required

Author Response

Manuscript Number: jmse-2470200-peer-review-v1

Title: MICROPLASTIC-PHARMACEUTICALS INTERACTION IN WATER SYSTEMS

 The purpose of this paper is to elucidate the interaction and association of MPs with pharmaceuticals, and the ecotoxicological implications on food webs. The content analysis of the manuscript is good, but the degree of innovation is not enough, the amount of data is small, and there is no great reference significance. It is recommended to reject the manuscript.

1. There are serious formatting issues throughout the text, including whether headings are top-notch, etc. Please revise carefully.

Reply: the formatting issues have been checked and a new sequence of sections and subsections has been added in a chronological orde.

2. Fig. 1 is cited from other literature, but the manuscript does not contain an adequate analysis of it. Is it possible to remove it then?

 Reply: Figure 1 was removed and indicated as a graphical abstract.

3. Please note that abbreviations, such as OECD, DOC, etc. do not give their full names the first time they appear. Please check carefully.

 Reply: the meaning of the extended abbreviations was reported.

4. Line 116: what is “MPshave”?

Reply: a space was added between the two words. (See line 136).

Round 2

Reviewer 2 Report (New Reviewer)

the manuscript has been revised according to the suggestions and comments of the reviewers. With the revisions implemented, the manuscript is now ready to be published in Journal of Marine Science and Engineering. 

Reviewer 3 Report (New Reviewer)

Accept

Minor editing of English language required

This manuscript is a resubmission of an earlier submission. The following is a list of the peer review reports and author responses from that submission.

Round 1

Reviewer 1 Report

Some statements in the manuscript are not very clear, it is recommended to carefully revise and organize.

1) L10 It could be mentioned in the main text instead of here.

2) L30 Why is it necessary to use 'especially' here? The amount of plastic entering the oceans through these ways do not exceed that of other pathways.

3) L39 The persistence and low degradability seem to have the same meaning here.

4) L41 In ocean or before MPs enter the ocean, especially,

5) L73 Compared to hydrophobic pollutants？

6) L80 Several studies investigated PHs desorption from polymers

7) L84 Usually, pharmaceuticals are not as persistent in aquatic environments, so I suggest removing the word 'long range'.

8) L101 MPs in aquatic systems?

9) L104 I suggest the authors rearrange the logical order. For example, they can first describe the abundance of MPs in different aquatic environments, and then elaborate on the characteristics of microplastics within them. The status of MPs in sewage can be introduced at the end because it is the most unique and smallest environment.

10) L107 Some researchers estimated that the MPs in the water surface were not more than 30%. In fact, only pristine plastics are prone to float.

11) L113 Pls note that the natural organic matter and salt content in water are higher than those of drugs, making them more suitable to play this role.

12) L119 higher than that without MPs？ high sorption tendency?

13) L125 Do various MPs have similar trends, or is this just an “average” result?

14) L132 predict the sorption ability

15) L152 Do the authors mean that the electrostatic interactions, hydrogen bonds and van der Waals  are weaker, so they are dominant?

16) L182 dipole-dipole interactions or polarization effect

17) L206 This factor cannot be classified as one of the three categories mentioned above.

18) L207  Why do the authors suggest PE have the highest surface area? At similar size?

19) L228 Which PH do the adsorption capacity on/in PE commented here?

20) L232 I suggest not using the word 'adsorption' as there may be partition effect.

21) L251 Not all PHs with log Kow<1. For example, the log KOW of sertraline = 5.29.

22) L258 Environmental factors

23) L296 Other similar results

24) L331 What is the meaning of 'seawater was doubled'?

25) L338 This example seems more suitable in the previous paragraph.

26) L354 π–π conjugation?

27) L412 What is the difference between biofouling effect and biofilms?

28) L424 My suggestion is to discuss the isotherm model and kinetic model separately. Because the impacting factors for these two are different.

29) L460 I don't quite understand the reason that the authors suggested that the impact of MPs on the bioaccumulation is currently low.

There are not many syntax error in this manuscript, but quite a lot of writing style, such as punctuations, that are different from the papers written by native English writers. Authors are kindly requested to pay attention.

1) L8 Pls place abbreviations in parentheses after the full name. Furthermore, abbreviating pharmaceuticals as PHs is not appropriate, as it can easily be confused with the commonly used pH in chemistry. PPCPs is an abbreviation for pharmaceuticals and personal care products.

2) L89 PHS?

3) L94 including antibiotics, non-steroidal anti-inflammatory 

4) L132 polymers–pollutants or polymer-pollutant? Pls delete the second specific.

5) L144 PHs which present hydrophilic 

6) L222 , such as PE, while

7) L229 The crystallinity of polymers can be categorised

8) L243 with only C and H atoms

9) L283 is present as cation at a low pH

10) L320 pH sorption?

 

Author Response

Some statements in the manuscript are not very clear, it is recommended to carefully revise and organize.

• L10 It could be mentioned in the main text instead of here.

Reply: the paragraph was cancelled since it is not meaningful in the abstract as well as in the introduction.

• L30 Why is it necessary to use 'especially' here? The amount of plastic entering the oceans through these ways do not exceed that of other pathways.

Reply: the paragraph was rewritten: Plastics enter the oceans from different sources as domestic-agricultural-industrial sewage, and marine-based activities [4-8].

• L39 The persistence and low degradability seem to have the same meaning here.

Reply: the word persistence was deleted.

• L41 In ocean or before MPs enter the ocean, especially,

Reply: in oceans but especially… was deleted

• L73 Compared to hydrophobic pollutants？

Reply: the text was amended as suggested.

• L80 Several studies investigated PHs desorption from polymers

Reply: the text was amended as suggested

• L84 Usually, pharmaceuticals are not as persistent in aquatic environments, so I suggest removing the word 'long range'.

Reply: the text was amended as suggested

• L101 MPs in aquatic systems?

Reply: I do prefer to use the word aquatic systems since the main route of MPs entering the oceans is from WWTPs and freshwater courses. 

• L104 I suggest the authors rearrange the logical order. For example, they can first describe the abundance of MPs in different aquatic environments, and then elaborate on the characteristics of microplastics within them. The status of MPs in sewage can be introduced at the end because it is the most unique and smallest environment.

Reply: I do prefer to keep the order I indicated in the paper. I think it is better to indicate the nature of the polymers together with their acronyms commonly found in any water system, WWTPs-freshwater-ocean, and then the main differences among systems.

• L107 Some researchers estimated that the MPs in the water surface were not more than 30%. In fact, only pristine plastics are prone to float.

Reply: the phrase was cancelled since it is not meaningful.

• L113 Pls note that the natural organic matter and salt content in water are higher than those of drugs, making them more suitable to play this role.

Reply: At this point the text deals with the possible interactions between MPs and PHs. The role of natural organic matter and salt will be discussed in the next sections.

• L119 higher than that without MPs？ high sorption tendency?

Reply: the text was amended as follows: The nature of MPs, especially their hydrophobicity, and large surface area provide these materials a high adsorption potential [18, 50].

• L125 Do various MPs have similar trends, or is this just an “average” result?

Reply: this is a specific results from the studies of Li et al [52].

• L132 predict the sorption ability.

Reply: the text was amended as indicated.

• L152 Do the authors mean that the electrostatic interactions, hydrogen bonds and van der Waals are weaker, so they are dominant?

Reply: the text was amended to avoid misleading interpreatations.

• L182 dipole-dipole interactions or polarization effect

Reply: the text was amended as follows: Polymers with polar group display dipole–dipole or dipole-induced interactions with the polar groups of drugs [68].

• L206 This factor cannot be classified as one of the three categories mentioned above.

Reply: the heading of the section was renamed and well as the net ones.

• L207  Why do the authors suggest PE have the highest surface area? At similar size?

Reply: the statement was deleted.

• L228 Which PH do the adsorption capacity on/in PE commented here?

Reply: pH 2.0

• L232 I suggest not using the word 'adsorption' as there may be partition effect.

Reply: the word was amended as absorption

• L251 Not all PHs with log Kow<1. For example, the log KOW of sertraline = 5.29.

Reply: the statement was amended as follows: is generally quite low, log Kow< 1, and are thus considered hydrophilic or polar compounds [75]. There are some exceptions as sertraline with a Kow of 5.29.

• L258 Environmental factors

Reply: the text was amended

• L296 Other similar results

Reply: text was amended

• L331 What is the meaning of ‘seawater was doubled’?

Reply: the text was amended

• L338 This example seems more suitable in the previous paragraph.

Reply: the statement was redundant and deleted.

• L354 π–π conjugation?

Reply: the word conjugation was replaced by interaction.

• L412 What is the difference between biofouling effect and biofilms?

Reply: the paragraph 6.8 on the effects of biofilm was deleted since was a repletion of the effect of biofilm.

• L424 My suggestion is to discuss the isotherm model and kinetic model separately. Because the impacting factors for these two are different.

Reply: I do think that discussion of the theoretical sorption models and kinetics of pollutants sorption can be shown together. This also avoids to increase the number of sections and subsections.

• L460 I don't quite understand the reason that the authors suggested that the impact of MPs on the bioaccumulation is currently low.

Reply: the statement was deleted.

There are not many syntax error in this manuscript, but quite a lot of writing style, such as punctuations, that are different from the papers written by native English writers. Authors are kindly requested to pay attention.

Reply: the manuscript was reviewed for style and punctuations.

• L8 Pls place abbreviations in parentheses after the full name. Furthermore, abbreviating pharmaceuticals as PHs is not appropriate, as it can easily be confused with the commonly used pH in chemistry. PPCPs is an abbreviation for pharmaceuticals and personal care products.

Reply:

• L89 PHS?

Reply: Amended into MPs

• L94 including antibiotics, non-steroidal anti-inflammatory 

Reply: the text was amended deleting the word drugs.

• L132 polymers–pollutants or polymer-pollutant? Pls delete the second specific.

Reply: the text was amended.

• L144 PHs which present hydrophilic 

Reply: I do not agree with the proposed amendemt. I prefere the current version.

• L222 , such as PE, while

Reply: text was amended as…. there are polymer considered as rubbery such as  PE, while….

• L229 The crystallinity of polymers can be categorised

Reply: the text was amended as: The crystallinity of polymers can be categorised as

• L243 with only C and H atoms

Reply: the text was amended.

• L283 is present as cation at a low pH

Reply: the text was amended as suggested

• L320 pH sorption?

Reply: the statement at line 325 is correct: The role of ionic strength on PHs sorption

Reviewer 2 Report

see review attached

Comments for author File: Comments.pdf

moderate revision (proof-reading due to some slips of the pen and a few grammatical errors) required

Author Response

The author has compiled an extensive review on the interaction between pharmaceutically active compounds (PH) and microplastics (MP) in marine waters. He is tackling the important aspects in different chapters giving many useful references. Although the underlying literature search was focussed on the period from 2020 to 2023, approximately half of the references had appeared earlier. The reference list also includes two other extensive reviews from 2021 ([18], [78]) about the same topic raising the (unanswered) question what the new contribution to the scientific discussion of this new manuscript was. Moreover, when checking the cited literature for some of the referenced statements, I had large difficulties in finding them. I suspect that some of the references are just misplaced in the manuscript, because they do not explicitly include the “cited” statements, e.g.

Reply: The above correspondences between statements and references have been checked and corrected as well as in other part of the paper as required by the other reviewers

• [41] describes effects of ibuprofen to a bivalve mollusc, but no “net dominance of antibiotics” in waters due

to misuse or overuse,

Reply: the reference was replaced with the correct one.

• [46] lists applications of PA in automotive trade, but does not justify the statement that PA is one of the most

common polymers detected in WWTPs (which is actually not true),

Reply: the reference is cited not for the prevalent presence of PA in WWTPs but for PA presence in wind turbines.

• [66] is on antibiotic resistance genes (ARG) rather than triclosan or tetracycline,

Reply: the reference was replaced with the correct one.

• [83] is on SMX not about tetracycline,

Reply: the reference was replaced with the proper one.

• [86] theoretically treats the pH of seawater, but not its effect on the mentioned processes,

Reply: the statement is reported by the cited reference.

• [92] describes general properties of DOM, but not the effects on PH-sorption to MP,

Reply: the text was modified justifying the presence of the reference.

• [106] does not include justification of the inverse relationship between surface area and particle size.

Reply: the reference was replaced by the proper one.

I am also puzzled by the fact that the author sometimes cites examples of compounds other than pharmaceuticals (e.g., POPs in general [22, 57], bisphenol A [55], the flame retardant BTBPE [77], PFOS [84], triclosan [90], or PCBs [98]) without clearly discussing the relevance of the investigations for the MP-PH issue. In addition, a structured distinction between the different groups of pharmaceuticals and their different properties with respect to their sorption behaviour is missing.

Reply: references have been added since MPS interaction with hydrophobic pollutants is much more known. Regarding the observation about the discrimination of sorption processes among different groups of drugs, it will be the aim of a future paper.  

Another critical point is that the presentation of the information in the different chapters generally resembles an unsorted enumeration of literature findings not sufficiently connected to each other. It provides an extensive list of relevant publication but does not put the information into perspective with respect to the general objective. This culminates in the vague conclusion, that “drug interaction with polymers remains (…) a complex subject” that needs to be investigated in more detail. However, the author does neither identify well-understood aspects nor provide a priority list of research gaps.

Reply: Many sections and subsections have been eliminated and the conclusions completely rewritten. The paper is more focused on the topics after the revisions of the four reviewers.

Formally, the manuscript is well structured into different paragraphs and written in understandable English, but it still needs extensive language polishing and proofreading to eliminate slips of the pen and a few grammatical errors.

Reply: Language was polished after responding to a very extensive review of the other revisors.

In summary, I am of the opinion, that the current manuscript version does not fulfil the quality requirements for publication as a review paper in the Journal of Marine Science and Engineering. Therefore, I suggest rejection with the opportunity of resubmission after thorough and extensive review with respect to the above comments.

Reply: Since the paper went to deep revision through 4 revisors I do think that now the overall quality is much improved.

Reviewer 3 Report

The manuscript fits well to JMSE scope. Both plastics and pharmaceuticals presence in the marine environment is emerging issue nowadays and  there is still an important gap in assessment of the resulting risk for ecosystems, this is particularly true for interactions of microplastics and pharmaceutical residues, underlying processes etc. In this context the review is an useful manuscript allowing the readers to know more about the processes and gaps. However before being accepted the manuscript needs some improvements. For some more detailed suggestions please see below.

General remark: in the title and in abstract it is suggested that the review is focused on marine ecosystems, however often more general approach is used: aquatic ecosystems, I’m pretty sure that some individual parts/chapters should be more focused on marine environment or at least at their end one/two sentences providing marine –oriented summary should appear . Obligatory, this remark applies to the conclusion part.

The manuscript focuses on sorption mechanism, however some sentences about leaching processes could be added.

Lines 42-45 “chemicals as polycyclic aromatic hydrocarbons, PAHs, polychlorinated biphenyls, PCBs, polybrominated diphenyl ethers, PBDEs, endocrine disruptors, EDCs, personal care products, PCPs, and pharmaceuticals” it is a mix of classifications due to chemical structure (PAHs, PCBs PBDEs..), use (personal care products, pharmaceuticals)  and action/effect (endocrine disruptors) it should be clarified/put in order

Figure 1 it seems to be a bit naïf for the main text, it looks rather as graphical abstract, I see no justification for this figure to appear in the text, perhaps the author could try to do something more useful in the context of the content of the manuscript.

Line 68 “Sorption depends on features of polymers as size, colour, morphology, surface area, crystallinity, functional groups, hydrophobicity” I wonder how colour influences sorption,

Line 70 “hydrophobicity or lipophilicity” it results in the same: hydrophobic compounds  liphophilic

line 71, temperature can also influence portioning Line 73 “Respect to hydrophobic pollutants, PHs have unique features, since they are polar and ionizable and hence pronounced hydrophilicity, with a low octanol–water partition coefficients, Kow,” I suggest to add most of PHs, because there are also some hydrophobic PHs e.g. albendazole, clofibric acid

line 90  focusing instead of focussing

line 93 and following chapter 2: Pharmaceutical in aquatic systems

I suggest to add some sentences concerning marine environment the same for chapter 3

Line 112 it is minor importance but I suggest “association of PHs with MPs”

Line 120 “sorption attitude”?

Line 127 “The adsorption decreased in the order of 125 ciprofloxacin, amoxicillin, trimethoprim, sulfadiazine, and tetracycline” explain why

Line 135 bisphenol A is not PHso it is not necessary to be mentioned

Line 141 remove was

Line 144 Most of PHs

Table 1 typo mistake tetracycline

Line 201 5.1 MPs properties - It does not need to be a separate subchapteror next subchapters should be numbered as 5.1.1 Particle size etc...

Line 258 Environmental ambiance? Please change the title

Line 261 and following the content of this subchapter is not so relevant to environmental conditions (extreme temperatures are taken into account while the review should concentrate on typical marine water temperatures. Please reorganize and add relevant information if exists.

Line 268 and followingThere is a lot of information in this subchapter, however I suggest to focus a bit more on situation in marine waters where pH is about 8.

Line 331 “when seawater was doubled”?

Subchapter 6.5 and 6.8 please combine these two subchapters

Line 379 add MPs: “Effect of MPs aging”

Line 460 “The impact of MPs on the bioaccumulation is currently low” really?, f so please add references, I think that there is a misunderstanding or a “typo” mistake, e.g. in lines 471-480 the author reports the influence of MPs on PHs bioaccumulation

 

 

Author Response

The manuscript fits well to JMSE scope. Both plastics and pharmaceuticals presence in the marine environment is emerging issue nowadays and  there is still an important gap in assessment of the resulting risk for ecosystems, this is particularly true for interactions of microplastics and pharmaceutical residues, underlying processes etc. In this context the review is an useful manuscript allowing the readers to know more about the processes and gaps. However before being accepted the manuscript needs some improvements. For some more detailed suggestions please see below.

General remark: in the title and in abstract it is suggested that the review is focused on marine ecosystems, however often more general approach is used: aquatic ecosystems, I’m pretty sure that some individual parts/chapters should be more focused on marine environment or at least at their end one/two sentences providing marine –oriented summary should appear. Obligatory, this remark applies to the conclusion part.

Reply: I modified the title in water systems, since I think it is more correct. Polymers and pharmaceuticals have often the same route before reaching the marine environment and the main place where the come into contact is in wastewater treatment plants. So, I think it is better to talk in more a general way, in fact the behaviour and the effect of some critical factors as pH are different in different water scenarios.

The manuscript focuses on sorption mechanism, however some sentences about leaching processes could be added.

Reply: in reality leaching and releasing of pharmaceuticals have been considered when talking about desorption and the factors influencing such a process

Lines 42-45 “chemicals as polycyclic aromatic hydrocarbons, PAHs, polychlorinated biphenyls, PCBs, polybrominated diphenyl ethers, PBDEs, endocrine disruptors, EDCs, personal care products, PCPs, and pharmaceuticals” it is a mix of classifications due to chemical structure (PAHs, PCBs PBDEs..), use (personal care products, pharmaceuticals)  and action/effect (endocrine disruptors) it should be clarified/put in order

Reply: the observation is correct, and the text was amended indicating the chemical names.

Figure 1 it seems to be a bit naïf for the main text, it looks rather as graphical abstract, I see no justification for this figure to appear in the text, perhaps the author could try to do something more useful in the context of the content of the manuscript.

Reply: in reality this was the scope, to present a kind of graphical abstract giving a very general view and introduction to the main issues discussed later on. 

Line 68 “Sorption depends on features of polymers as size, colour, morphology, surface area, crystallinity, functional groups, hydrophobicity” I wonder how colour influences sorption,

Reply: The color could be altered by the extent of weathering of plastic polymers. Black beached MPs adsorb more organic chemical contaminants compared to white MPs  (Ma et al., 2020). Greater adsorption on black MPs was ascribed to the enhanced-photo-oxidative weathering under solar light irradiation (relative to aged white MPs). As such, the surface area of weathered black MPs increased for organics or chemical additive adsorption. Therefore, the color of plastic particles can also impact the pollutants adsorption.

Ma H., Pu S., Liu S., et al. Microplastics in aquatic environments: Toxicity to trigger ecological consequences. Environ. Pollut. 2020;261

Line 70 “hydrophobicity or lipophilicity” it results in the same: hydrophobic compounds  liphophilic

Reply: the word lipophilicity was deleted.

line 71, temperature can also influence portioning Line 73 “Respect to hydrophobic pollutants, PHs have unique features, since they are polar and ionizable and hence pronounced hydrophilicity, with a low octanol–water partition coefficients, Kow,” I suggest to add most of PHs, because there are also some hydrophobic PHs e.g. albendazole, clofibric acid

Reply: the statement was amended as suggested.

line 90  focusing instead of focussing

Reply: the text was amended.

line 93 and following chapter 2: Pharmaceutical in aquatic systems. I suggest adding some sentences concerning marine environment the same for chapter 3

Reply: As I already indicated other reviewer suggest to talk in a more general way of aquatic systems including wastewater, freshwater, marine water

Line 112 it is minor importance, but I suggest “association of PHs with MPs”

Reply: text was amended.

Line 120 “sorption attitude”?

Reply: the text was amended as also suggested by other reviewers.

Line 127 “The adsorption decreased in the order of 125 ciprofloxacin, amoxicillin, trimethoprim, sulfadiazine, and tetracycline” explain why

Reply: the text was amended.

Line 135 bisphenol A is not PHso it is not necessary to be mentioned

Reply: the text was amended.

Line 141 remove was

Reply: text was amended.

Line 144 Most of PHs

Reply: the text was amended.

Table 1 typo mistake tetracycline

Reply: text was amended.

Line 201 5.1 MPs properties - It does not need to be a separate subchapteror next subchapters should be numbered as 5.1.1 Particle size etc...

Reply: the numeration of sections and subsection from this point was changed as also indicated by other reviewers.

Line 258 Environmental ambiance? Please change the title

Reply: the text was amended.

Line 261 and following the content of this subchapter is not so relevant to environmental conditions (extreme temperatures are taken into account while the review should concentrate on typical marine water temperatures. Please reorganize and add relevant information if exists.

Reply: as it has already been said the focus in more wide and include all water bodies.

Line 268 and following There is a lot of information in this subchapter, however I suggest to focus a bit more on situation in marine waters where pH is about 8.

Reply: as it has already been said, we changed the focus on water bodies. The section contains a reference to the the behaviour of MPs and PHs in a pH 8,1 aqueous environment (see lines 303-305 of the upgraded version of the MS).

Line 331 “when seawater was doubled”?

Reply: text was amended as also indicated by other reviewer.

Subchapters 6.5 and 6.8 please combine these two subchapters

Reply: done.

Line 379 add MPs: “Effect of MPs aging”

Reply: the text was amended.

Line 460 “The impact of MPs on the bioaccumulation is currently low” really? if so, please add references, I think that there is a misunderstanding or a “typo” mistake, e.g. in lines 471-480 the author reports the influence of MPs on PHs bioaccumulation

 Reply: the phrase was deleted as also indicated by other reviewers

Reviewer 4 Report

Manuscript: JMSE-2385782

Title: Microplastic-pharmaceuticals interaction in oceans. A review.

Authors: Michele Arienzo

 

 

Arienzo has reviewed the scientific papers that deal with the interactions between microplastics and pharmaceuticals in aquatic environment. The manuscript contains 141 references. There are two cited figures (that are not very informative or even necessary) and an original table in the manuscript. The manuscript lacks the structuring and the critical evaluation of the original papers, which has resulted in the text hard to read due to the loose sentences following one after another. The reader may easily lose the common thread while reading the text. The conclusions drawn of 141 publications are that “much is left to be understood” or “low is the knowledge”. The manuscript requires a thorough major revision before it can be published in Journal of Marine Science and Engineering.

 

 

General comments:

 

1.    The text should be structured. The sharpening the focus and brightening the common thread of the manuscript will support the structuring.

2.    As a replacement of figures 1 and 2, the figures and tables should be added that summaries the results and findings of the original papers.

3.    The conclusions should be fully rewritten. It is undoubted that future studies are needed but some conclusions should be able to be drawn from the published papers.

4.    The language should be proofread (only some instances are given below).

 

Specific comments (Line numbers from the manuscript submitted):

 

1.    Line 2: The title with two dots should be revised. In addition, “oceans” is mentioned in the title, but the content does not especially focus on the oceans.

2.    Lines 7 to 12: The mention of earlier review takes too lines of the abstract. Replace these lines with the description the present manuscript.

3.    Line 26: Revise “… is becoming every day an urgent issue”.

4.    Lines 35 to 36: Revise “… forming microplastics, MPs [10], with polyethylene, PE, being the most representative polymer”.

5.    Lines 43 to 45: To make reading easier, it is better to give abbreviations appearing for the first time in the brackets “…polycyclic aromatic hydrocarbons, PAHs, polychlorinated biphenyls, PCBs, polybrominated diphenyl ethers, PBDEs, endocrine disruptors, EDCs, personal care products, PCPs, and pharmaceuticals, PHs”. The other abbreviations, but not PHs, should be removed since they appear only once (here) in the manuscript.

6.    Figure 1: This figure does not give much, so it is better to remove. See also general comment #2.

7.    Line 65: Revise “[18Atugoda et a., 2021]”.

5.    Lines 77 to 85 and 112 to 127: While highlighting the role of microplastics in the environmental fate of (hydrophobic) pollutants, it should be also brought out why and how the microplastics as adsorbents differ from the natural particles that are clearly more abundant (and offer much large surface area for adsorption) in the environments.

8.    Lines 93 to 109: The text is very general and as such, fits better in the schoolbook. Remove or sharpen Sections 2 and 3.

9.    Lines 98 to 99: The reference 43 is not original papers, so replace it with the original paper(s).

10.  Lines 123 to 126: This is one of many loose sentences that are hard to read and its message is not too clear.

11.  Figure 2: This figure does not give much, so it is better to remove. See also general comment #2.

12.  Line 143: Revise “K_low”.

13.  Line 185: Add “such as” in front of “carboxyl”.

14.  Lines 207 to 208: What does mean “Among plastics 207 PE has the highest surface area followed by PS, PVC, and PP”?

15.  Lines 261 to 265: Is it somehow related to oceans? If not, revise.

16.  Line 279: Water systems or oceans?

17.  Lines 329 to 330, 331 to 333 and 340 to 343. Check the language.

18.  Lines 346 to 366: The message of this paragraph is unclear. It contains the cited sentences without critical assessment or any concluding remarks. This is just an instances of loose sentences mentioned above.

19.  Sections 6.5 and 6.8: What is the difference between biofouling and biofilms? Combine the sections if there is no specific difference.

20.  Line 378: Where is the section 6.6?

21.  Lines 387 to 389: Check the language.

22.  Lines 393 to 394: “… favours the formation of phenolic hydroxyl group on MPs surfaces”. Any microplastics or certain type of plastics? Revise.

23.  Lines 379 to 410: Use either aging, weathering or chemical transformation.

24.  Lines 412 to 422: Platisphere or plastisphere? Check the spelling.

25.  Lines 424 to 440: This entire section remains loose and it should be connected to the other sections.

26.  Lines 442 to 529: The review focuses on microplastics but in this section the microplastics and nanoplastics are mixed. Remove the nanoplastics from the text or explain in the text why they are included.

27.  Line 454: The link to the reference could not be opened. Is it published in newspaper? Remove the reference and “Trojan horses”.

28.  Line 477: Remove “in”.

29.  Lines 515 to 528: This paragraph deals with toxicity but is located under bioaccumulation. Remove or move to another section.

30.  Lines 536 to 537: Check the language.

31.  Lines 540 to 541: Some studies but only one reference. Rephrase or add the references.

32.  Lines 531 to 580: The review focuses on oceans, but this section presents findings also from freshwater experiments. Remove the freshwater findings text or explain in the text why they are included.

33.  Line 568: Check the spelling “bio fouled”.

34.  Lines 582 to 603: Rewrite the entire section.

See the comments above.

Author Response

Reviewer 4

Arienzo has reviewed the scientific papers that deal with the interactions between microplastics and pharmaceuticals in aquatic environment. The manuscript contains 141 references. There are two cited figures (that are not very informative or even necessary) and an original table in the manuscript. The manuscript lacks the structuring and the critical evaluation of the original papers, which has resulted in the text hard to read due to the loose sentences following one after another. The reader may easily lose the common thread while reading the text. The conclusions drawn of 141 publications are that “much is left to be understood” or “low is the knowledge”. The manuscript requires a thorough major revision before it can be published in Journal of Marine Science and Engineering.

 General comments:

1. The text should be structured. The sharpening the focus and brightening the common thread of the manuscript will support the structuring.

Reply: the text was structured in a more logical order and some sections were deleted or merged together as suggested by other reviewers..

2. As a replacement of figures 1 and 2, the figures and tables should be added that summaries the results and findings of the original papers.

Reply: Figure 1 is a good graphical abstract synthetizing the main aim of the paper. Figure 2 is a good graphic representation of the main interaction mechanisms also outlined by Table 1. Personally, I do prefer to show mechanisms, overall behaviours, processes in a graphical way since it calls the attentions of the readers. I do not prefer to synthesizes what has already been written in the form of tables, it is an unuseful repetition.  

3. The conclusions should be fully rewritten. It is undoubted that future studies are needed but some conclusions should be able to be drawn from the published papers.

Reply: conclusions were rewritten.

4. The language should be proofread (only some instances are given below).

Reply: the language was checked throughout all the text.

 Line 2: The title with two dots should be revised. In addition, “oceans” is mentioned in the title, but the content does not especially focus on the oceans.

Reply: the title was modified indicating ‘water systems’ in place of oceans. Double dot were deleted.

1. Lines 7 to 12: The mention of earlier review takes too lines of the abstract. Replace these lines with the description the present manuscript.

Reply: the paragraph was shortened as also required by reviewer 1.

2. Line 26: Revise “… is becoming every day an urgent issue”.

Reply: the statement was deleted and replaced with: The world is producing twice as much plastic waste as two decades ago, with the bulk of it ending up in landfill, incinerated or leaking into the environment, and only 9% successfully recycled, according to a new OECD report [1].

Lines 35 to 36: Revise “… forming microplastics, MPs [10], with polyethylene, PE, being the most representative polymer”.

Reply: the phrase was modified as: and polyethylene, PE, represents the most frequent detected polymer.

3. Lines 43 to 45: To make reading easier, it is better to give abbreviations appearing for the first time in the brackets “…polycyclic aromatic hydrocarbons, PAHs, polychlorinated biphenyls, PCBs, polybrominated diphenyl ethers, PBDEs, endocrine disruptors, EDCs, personal care products, PCPs, and pharmaceuticals, PHs”. The other abbreviations, but not PHs, should be removed since they appear only once (here) in the manuscript.

Reply: Personally, I prefer engravings to parentheses to indicate the long form of acronyms and for consistency the other acronyms will be indicated.

4. Figure 1: This figure does not give much, so it is better to remove. See also general comment #2.

Reply: personally I prefer to keep Figure 1, is a sort of graphical abstract and its graphic helps the reader to have a general overview of the paper.

7. Line 65: Revise “[18Atugoda et a., 2021]”.

Reply: it has been deleted.

8. Lines 77 to 85 and 112 to 127: While highlighting the role of microplastics in the environmental fate of (hydrophobic) pollutants, it should be also brought out why and how the microplastics as adsorbents differ from the natural particles that are clearly more abundant (and offer much large surface area for adsorption) in the environments.

Reply: the scope of this paragraph was to introduce the reader to the main core of the paper, highlighting the novelty of the microplastic-pharmaceutical interaction, the issues that need to be investigated deeper and with a note on the novelty represented by the fact that pharmaceuticals are hydrophilic compounds with a different behaviour compared to hydrophobic compounds. Arguments related to the different role of microplastics compared to other potential adsorbents in the environment are not relevant at this point in the review.

9.  Lines 93 to 109: The text is very general and as such, fits better in the schoolbook. Remove or sharpen Sections 2 and 3.

Reply: I do retain that the text is necessary and well written. It gives the reader useful information on the extent of the problem by providing statistical data on frequency and presence of pharmaceuticals and polymers in aqueous systems. We cannot talk about the interaction between pharmaceutical polymers without giving a brief and essential framework on the subject.

10. Lines 98 to 99: The reference 43 is not original papers, so replace it with the original paper(s).

Reply: the phrase was deleted and replaced with the one reported by the cited reference 43.

11. Lines 123 to 126: This is one of many loose sentences that are hard to read and its message is not too clear.

Reply: the paragraph was completely rewritten and enriched with more details.

12. Figure 2: This figure does not give much, so it is better to remove. See also general comment #2.

Reply: I think that this is a nice figure, representing what can happens on the surface of polymer particles in terms of different mechanism of interaction with drugs. All recent reviews on the same topic report at leas a figure similar to this one.

13. Line 143: Revise “K_low”.

Reply: the text was amended.

14. Line 185: Add “such as” in front of “carboxyl”.

Reply: the text was amended.

15. Lines 207 to 208: What does mean “Among plastics 207 PE has the highest surface area followed by PS, PVC, and PP”?

Reply: the phrase was deleted as also suggested by reviewer 1.

16. Lines 261 to 265: Is it somehow related to oceans? If not, revise.

Reply: Authors of reference 76 refer to experiments carried out in seawater, pure water and air, so the text was not modified

17. Line 279: Water systems or oceans?

Reply: it is subtended in water systems including oceans

18. Lines 329 to 330, 331 to 333 and 340 to 343. Check the language.

Reply: text was amended ad made more clear.

19. Lines 346 to 366: The message of this paragraph is unclear. It contains the cited sentences without critical assessment or any concluding remarks. This is just an instances of loose sentences mentioned above.

Reply: the text was enriched with more details on the contrasting role of DOM on drug interaction with polymers.

20. Sections 6.5 and 6.8: What is the difference between biofouling and biofilms? Combine the sections if there is no specific difference.

Reply: sections were merged as also suggested by reviewer 1.

21. Line 378: Where is the section 6.6?

Reply: the sections and subsections were re-numbered and differently named.

22. Lines 387 to 389: Check the language.

Reply: two statements were deleted since they were not too much pertinent.

23. Lines 393 to 394: “… favours the formation of phenolic hydroxyl group on MPs surfaces”. Any microplastics or certain type of plastics? Revise.

Reply: the word aged was added

24. Lines 379 to 410: Use either aging, weathering or chemical transformation.

Reply: the text was amended.

25. Lines 412 to 422: Platisphere or plastisphere? Check the spelling.

Reply: the word was deleted since the section was deleted.

26. Lines 424 to 440: This entire section remains loose and it should be connected to the other sections.

Reply: the two sections were merged as also suggested by reviewer 1.

27. Lines 442 to 529: The review focuses on microplastics but in this section the microplastics and nanoplastics are mixed. Remove the nanoplastics from the text or explain in the text why they are included.

Reply: I do not think that it is necessary to remove NPs from the text or explain why they have been included. They are a natural by product of MPs forming when microplastics are exposed to ultraviolet (UV) light.

28. Line 454: The link to the reference could not be opened. Is it published in newspaper? Remove the reference and “Trojan horses”.

Reply: the text was amended with the correct link.

29. Line 477: Remove “in”.

Reply: deleted.

30. Lines 515 to 528: This paragraph deals with toxicity but is located under bioaccumulation. Remove or move to another section.

Reply: the paragraph was moved to the next section.

31. Lines 536 to 537: Check the language.

Reply: the text was amended.

32. Lines 540 to 541: Some studies but only one reference. Rephrase or add the references.

Reply: the word was replaced by authors.

33. Lines 531 to 580: The review focuses on oceans, but this section presents findings also from freshwater experiments. Remove the freshwater findings text or explain in the text why they are included.

Reply: the title of the paper was modified in a more general statement ‘water systems’.

34. Line 568: Check the spelling “bio fouled”.

Reply: the spelling is correct ‘biofouling’

35. Lines 582 to 603: Rewrite the entire section.

Reply: conclusions were rewritten reporting the main

 

Round 2

Reviewer 1 Report

Updated comments, including some comments have not been replied.

i) 8 Pls place abbreviations in parentheses after the full name. Furthermore, abbreviating pharmaceuticals as PHs is not appropriate, as it can easily be confused with the commonly used pH in chemistry. PPCPs is an abbreviation for pharmaceuticals and personal care products.

ii) L99 Please forgive the misunderstanding I caused. For the sentence "About 160 drugs, antibiotics, non steroidal anti inflammatory drugs, NSAIDs, psychological and cardiovascular drugs", if "the antibiotics", "non steroidal anti inflammatory drugs", etc. listed by authors were all included in those 160 drugs, this sentence should be changed to 'About 160 drugs, including antibiotics, non-steroidal anti-inflammatory drugs (NSAIDs), psychological and cardiovascular drugs'.

iii) L115 I suggest changing the title of this section to "MPs in aqueous systems", as the authors only discuss microplastics rather than all polymers in this section.

iv) L126 Perhaps in pure aqueous system, the interactions between MPs and PHs are possible. But the authors should proactively state that the premise of the phenomenon is in the pure water system. Otherwise, it is unnecessary to describe phenomena that cannot occur in the wastewater environment, freshwater environment, and seawater environment the authors cared about in this review.

v) L262 the absorption capacity of PE to common PHs (or a specific one?) is greater than PS

vi) L370 the salinity of seawater

Improved.

Author Response

Updated comments, including some comments have not been replied.

1. 8 Pls place abbreviations in parentheses after the full name. Furthermore, abbreviating pharmaceuticals as PHs is not appropriate, as it can easily be confused with the commonly used pH in chemistry. PPCPs is an abbreviation for pharmaceuticals and personal care products.

Reply: Personally, I prefer to use engravings, the text is more fluid avoiding a lot of parenthesis. The abbreviations PHs is commonly used in literature.

1. L99 Please forgive the misunderstanding I caused. For the sentence "About 160 drugs, antibiotics, non steroidal anti inflammatory drugs, NSAIDs, psychological and cardiovascular drugs", if "the antibiotics", "non steroidal anti inflammatory drugs", etc. listed by authors were all included in those 160 drugs, this sentence should be changed to 'About 160 drugs, including antibiotics, non-steroidal anti-inflammatory drugs (NSAIDs), psychological and cardiovascular drugs'.

Reply: the text was amended as suggested.

• L115 I suggest changing the title of this section to "MPs in aqueous systems", as the authors only discuss microplastics rather than all polymers in this section.

Reply: the text was amended as suggested.

1. L126 Perhaps in pure aqueous system, the interactions between MPs and PHs are possible. But the authors should proactively state that the premise of the phenomenon is in the pure water system. Otherwise, it is unnecessary to describe phenomena that cannot occur in the wastewater environment, freshwater environment, and seawater environment the authors cared about in this review.

Reply: the following phrase, lines 125-127,  was added: ‘MPs provide a large solid surface especially within pure aqueous environments, and the amounts of organic contaminants accumulated on the plastic surface can be several orders of magnitude higher than that in the surrounding waters. In section 4 are reported many examples of more significant association in simulated aqueous system with MPs than without.

1. L262 the absorption capacity of PE to common PHs (or a specific one?) is greater than PS

Reply: the text was rewritten since it was confused.

1. L370 the salinity of seawater

Reply: the text was amended

Reviewer 2 Report

The author has thoroughly responded to the reviewer’s comments. He corrected the listed misplaced citations and significantly improved the structure of the manuscript with respect to the general objective. The revised conclusion section is more concise to the point. However, I am still not completely convinced, that the manuscript tackles enough significantly new aspects, especially in comparison to two other recent reviews from 2021 ([18], [77]) about the same topic. In this context, I am not happy with the response that a structured discussion of the sorption mechanisms among the different groups of pharmaceuticals and their different properties will eventually be treated in a future paper. This distinction was helpful in refuting my criticism of not enough new aspects.

Formally, the manuscript still needs proofreading to eliminate slips of the pen especially in the revised sections.

In summary, I am of the opinion, that the revised manuscript fulfils minimum quality requirements for publication in the Journal of Marine Science and Engineering. Therefore, I can suggest publication after minor revision with the limitation of the questionable novelty of the review. I leave the decision, in how far this aspect finally speaks against publication to the editor.

Proofreading of the revised section recommended.

Author Response

Reply: the manuscript was checked for pen slips.

Reviewer 3 Report

The manuscript could be accepted now. I'm satisfied with author's answers to my comments concerning original draft

Author Response

Nothing to respond

Reviewer 4 Report

The author has made only minor editorial revisions, which is not definitely sufficient for the manuscript. The clear common thread is still missing and the text is tiring to read due to the lack of structuring. The figures are not original. The manuscript should be rejected.

The reason of rejection is not the language, so there is no need to proofreading.

Author Response

the only thing I can say that I made an extensive work to reply queries of the reviewer.