Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments
Round 1
Reviewer 1 Report
Review of the Manuscript ID: coatings-2473659:“Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments” submitted for publication in the journal Coatings.
I have read with interest the manuscript :“Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments” and found it interesting and valuable for the engineers working in the field of asphalt. The paper is well written, structured and presented. I recommend publication of this article in Coatings journal after minor revision considering the specific comments made below.
1. Page 1, lines 31-32 the sentence: “During the decades service time, the asphalt would suffer from repeat vehicle load, temperature changing and water erosion, and explores under sun in a long time.” In my opinion needs a revision like this: “During the decades service time, the asphalt would suffer from repeat vehicle load, temperature changing and water erosion, and exposure under sun in a long time.”
2. Table 4. Typically SARA analysis is presented as wt% of saturates, aromatics, resins, and asphaltenes. The authors presented the asphalt SARA composition in Table 4 as wt% of saturates, asphaltenes, resins, and aromatics. I would recommend to change the order to fit the typical SARA composition representation.
3. Page 5, lines 137-139 the statement: “According to the recent findings and the FTIR test results of SK-70 matrix asphalt,the representative molecules (see Fig.3) were selected to represent asphalt components including asphaltene, resin, aromatic and saturat e[34-41].” can be supported by the references:
a. Martha L. Chacón-Patiño, Murray R. Gray, Christopher Rüger, Donald F. Smith, Taylor J. Glattke, Sydney F. Niles, Anika Neumann, Chad R. Weisbrod, Andrew Yen, Amy M. McKenna, Pierre Giusti, Brice Bouyssiere, Caroline BarreÌ€re-Mangote, Harvey Yarranton, Christopher L. Hendrickson, Alan G. Marshall, and Ryan P. Rodgers. Lessons Learned from a Decade-Long Assessment of Asphaltenes by Ultrahigh-Resolution Mass Spectrometry and Implications for Complex Mixture Analysis. Energy Fuels 2021, 35, 20, 16335–16376. https://doi.org/10.1021/acs.energyfuels.1c02107
b. Chacón-Patiño, M. L.; Rowland, S. M.; Rodgers, R. P. The Compositional and Structural Continuum of Petroleum from Light Distillates to Asphaltenes: The Boduszynski Continuum Theory as Revealed by FT-ICR Mass Spectrometry. In The Boduszynski Continuum: Contributions to the Understanding of the Molecular Composition of Petroleum; Ovalles, C., Moir, M. E., Eds.; ACS Symposium Series, Vol. 1282: Washington, DC, 2018; pp 113−171.
c. Chacón-Patiño, M. L.; Rowland, S. M.; Rodgers, R. P. Advances in Asphaltene Petroleomics. Part 1: Asphaltenes Are Composed of Abundant Island and Archipelago Structural Motifs. Energy Fuels 2017, 31 (12), 13509−13518.
d. Rodgers, R. P.; Mapolelo, M. M.; Robbins, W. K.; Chacon-Patino, M. L.; Putman, J. C.; Niles, S. F.; Rowland, S. M.; Marshall, A. G. Combating Selective Ionization in the High Resolution Mass Spectral Characterization of Complex Mixtures. Faraday Discuss. 2019, 218, 29−51.
e. Chacón-Patiño, M. L.; Rowland, S. M.; Rodgers, R. P. Advances in Asphaltene Petroleomics. Part 3. Dominance of Island or Archipelago Structural Motif Is Sample Dependent. Energy Fuels 2018, 32 (9), 9106−9120.
f. Giraldo-Dávila, D.; Chacón-Patiño, M. L.; McKenna, A. M.; Blanco-Tirado, C.; Combariza, M. Y. Correlations Between Molecular Composition and the Adsorption, Aggregation and Emulsifying Behavior of Petrophase 2017 Asphaltenes and Their TLC Fractions. Energy Fuels 2018, 32, 2769.
4. Page 6, line 157, the sentence: “ZnO is belong to crystal and its space group is P63mc(186).” Is better to express like this: “ZnO belongs to crystal and its space group is P63mc(186).”
5. Page 8, line 185, 4. Methodology, the sentence: “The objective of this study was try to investigate the interaction between ZnO particles and asphalt, and to reveal the effect of ZnO on the structure and physical properties on asphalt.” Needs revision like this: The objective of this study was to try to investigate the interaction between ZnO particles and asphalt, and to reveal the effect of ZnO on the structure and physical properties on asphalt.”
6. What does the abbreviation “MS” in the term “MS software” mean? Is that Microsoft?
7. What does the abbreviation “MSD” mean?
8. I would recommend the authors to add a list of used abbreviations to their manuscript.
Quality of English language is acceptable. Some minor ammendments are needed.
Author Response
Dear Editors and Reviewers:
Many thanks for your time and comments concerning our manuscript entitled “Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments” (No.coatings-2473659). Those comments are valuable and very helpful to improving our paper and research. We have made corrections which we believe satisfy the requirements of the reviewers. A summary of the corrections made in the paper and the responses to the reviewers’ comments are as following:
Point 1: Page 1, lines 31-32 the sentence: “During the decades service time, the asphalt would suffer from repeat vehicle load, temperature changing and water erosion, and explores under sun in a long time.” In my opinion needs a revision like this: “During the decades service time, the asphalt would suffer from repeat vehicle load, temperature changing and water erosion, and exposure under sun in a long time.”
Response 1: As reviewers’ suggested that we have revised the this sentence like that “During the decades service time, the asphalt would suffer from repeat vehicle load, temperature changing and water erosion, and exposure under sun in a long time.” Please see line 35 and 36.
Point 2:Table 4. Typically SARA analysis is presented as wt% of saturates, aromatics, resins, and asphaltenes. The authors presented the asphalt SARA composition in Table 4 as wt% of saturates, asphaltenes, resins, and aromatics. I would recommend to change the order to fit the typical SARA composition representation.
Response 2: We are very appreciate this suggestion, we have changed the order of the asphalt components in Table 4.
Point 3:Page 5, lines 137-139 the statement: “According to the recent findings and the FTIR test results of SK-70 matrix asphalt,the representative molecules (see Fig.3) were selected to represent asphalt components including asphaltene, resin, aromatic and saturat e[34-41].” can be supported by the references:
- Martha L. Chacón-Patiño, Murray R. Gray, Christopher Rüger, Donald F. Smith, Taylor J. Glattke, Sydney F. Niles, Anika Neumann, Chad R. Weisbrod, Andrew Yen, Amy M. McKenna, Pierre Giusti, Brice Bouyssiere, Caroline BarreÌ€re-Mangote, Harvey Yarranton, Christopher L. Hendrickson, Alan G. Marshall, and Ryan P. Rodgers. Lessons Learned from a Decade-Long Assessment of Asphaltenes by Ultrahigh-Resolution Mass Spectrometry and Implications for Complex Mixture Analysis. Energy Fuels 2021, 35, 20, 16335–16376. https://doi.org/10.1021/acs.energyfuels.1c02107
- Chacón-Patiño, M. L.; Rowland, S. M.; Rodgers, R. P. The Compositional and Structural Continuum of Petroleum from Light Distillates to Asphaltenes: The Boduszynski Continuum Theory as Revealed by FT-ICR Mass Spectrometry. In The Boduszynski Continuum: Contributions to the Understanding of the Molecular Composition of Petroleum; Ovalles, C., Moir, M. E., Eds.; ACS Symposium Series, Vol. 1282: Washington, DC, 2018; pp 113−171.
- Chacón-Patiño, M. L.; Rowland, S. M.; Rodgers, R. P. Advances in Asphaltene Petroleomics. Part 1: Asphaltenes Are Composed of Abundant Island and Archipelago Structural Motifs. Energy Fuels 2017, 31 (12), 13509−13518.
- Rodgers, R. P.; Mapolelo, M. M.; Robbins, W. K.; Chacon-Patino, M. L.; Putman, J. C.; Niles, S. F.; Rowland, S. M.; Marshall, A. G. Combating Selective Ionization in the High Resolution Mass Spectral Characterization of Complex Mixtures. Faraday Discuss. 2019, 218, 29−51.
- Chacón-Patiño, M. L.; Rowland, S. M.; Rodgers, R. P. Advances in Asphaltene Petroleomics. Part 3. Dominance of Island or Archipelago Structural Motif Is Sample Dependent. Energy Fuels 2018, 32 (9), 9106−9120.
- Giraldo-Dávila, D.; Chacón-Patiño, M. L.; McKenna, A. M.; Blanco-Tirado, C.; Combariza, M. Y. Correlations Between Molecular Composition and the Adsorption, Aggregation and Emulsifying Behavior of Petrophase 2017 Asphaltenes and Their TLC Fractions. Energy Fuels 2018, 32, 2769.
Response 3: Considering the reviewer's suggestion, we have replaced the references to support the asphalt molecular model, and these references were listed from line 504 to 525.
Point 4:Page 6, line 157, the sentence: “ZnO is belong to crystal and its space group is P63mc(186).” Is better to express like this: “ZnO belongs to crystal and its space group is P63mc(186).”
Response 4: We have revised this sentence as your suggestion.Please see line 223.
Point 5:Page 8, line 185, 4. Methodology, the sentence: “The objective of this study was try to investigate the interaction between ZnO particles and asphalt, and to reveal the effect of ZnO on the structure and physical properties on asphalt.” Needs revision like this: The objective of this study was to try to investigate the interaction between ZnO particles and asphalt, and to reveal the effect of ZnO on the structure and physical properties on asphalt.”
Response 5: This sentence has been revised as the suggestion. Please see line 123 and line 124.
Point 6:What does the abbreviation “MS” in the term “Materials Studio software” mean? Is that Microsoft?
Response 6: The “MS” in the term “Materials Studio software” means “materials studio”, and we have replaced "Materials Studio software" with the full name of " Materials Studio software".
Point 7:What does the abbreviation “MSD” mean?
Response 7: The “MSD” means mean square displacement, and we have explained abbreviations before use it
Point 8:I would recommend the authors to add a list of used abbreviations to their manuscript.
Response 8: We have checked the all abbreviations, and explained them before use it, please see line 9, 14, 22 and 38 . So, it is not necessary to list them.
Once again, thank you very much for your comments and suggestions.
Author Response File: 
Author Response.docx
Reviewer 2 Report
The manuscript "Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments'' concerns a current and important scientific problem concerning the modification of asphalt mixtures with zinc oxide in order to improve their physical properties.
I believe that the manuscript may be considered for publication, subject to the following comments:
1. The abstract of the manuscript must be supplemented with information on the results of the conducted research.
2. The review of the current state of knowledge and the list of references mostly refer to literature items older than 7 years. The literature review should be supplemented with more recent works in the field of newly developed asphalt mix composites.
3. It is worth supplementing the manuscript with a brief analysis of the financial and ecological costs of the proposed modifications of asphalt mixes, e.g. with LCC and LCA methods.
4. Need to improve the legibility of the descriptions Figure 10, 15, 17.
5. A list of abbreviations and symbols must be included in the manuscript
6. The conclusions contained in the manuscript should clearly prove the innovativeness of the conducted research and analyses, this should be supplemented.
Author Response
Dear Editors and Reviewers:
Many thanks for your time and comments concerning our manuscript entitled “Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments” (No.coatings-2473659). Those comments are valuable and very helpful to improving our paper and research. We have made corrections which we believe satisfy the requirements of the reviewers. A summary of the corrections made in the paper and the responses to the reviewers’ comments are as following:
Point 1: The abstract of the manuscript must be supplemented with information on the results of the conducted research.
Response 1: As reviewers’ suggested that we have supplemented the quantitative results of our research, please see line from 15 to 23.
Point 2: The review of the current state of knowledge and the list of references mostly refer to literature items older than 7 years. The literature review should be supplemented with more recent works in the field of newly developed asphalt mix composites.
Response 2: We are very appreciate this suggestion, we have replaced the most references which published in recent 5 years, please see Reference section.
Point 3: It is worth supplementing the manuscript with a brief analysis of the financial and ecological costs of the proposed modifications of asphalt mixes, e.g. with LCC and LCA methods.
Response 3: The comparison of financial and ecological cost between ZnO modified asphalt and base asphalt had been conducted in our research “High and low temperature properties of nano-particles/polymer modified asphalt (published on the journal of Construction and Building Materials)”, bedsides, the objective of this article is to reveal the effect of ZnO particle on the properties of base asphalt. So, it’s unnecessary to repeat the cost here.
Point 4: Need to improve the legibility of the descriptions Figure 10, 15, 17.
Response 4: The Figures 10,15 and 17 refers to the molecular interaction between asphalt model anf ZnO model, the effect of ZnO on the structure and morphology of asphalt, respectively. We have checked the descriptions of these three figures and supplemented the explanation to make it easier to understand.
Point 5: A list of abbreviations and symbols must be included in the manuscript
Response 5: We have checked the all abbreviations, and explained them before use it, please see line 9, 14, 22 and 38. So, it is not necessary to list them.
Point 6: The conclusions contained in the manuscript should clearly prove the innovativeness of the conducted research and analyses, this should be supplemented.
Response 6: We have checked conclusions and highlighted the innovativeness of our methodologies, and analyzed the results according to the molecular dynamics simulations.
Once again, thank you very much for your comments and suggestions.
Author Response File: Author Response.doc
Reviewer 3 Report
The paper "Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments" is interesting publication since the authors make corrections throughout the document:
(a) The abstract can be examined, the authors must highlight the innovation and motivation, in addition to presenting the main quantitative results of this research;
(b) Throughout the introduction, some aspects of the study of the art of the theme should be mentioned, some illustrations and comparative tables can be added by the authors, note some suggested literature: 10.3390/ma15072598; 10.1061/JMCEE7.MTENG-14543; 10.1155/2023/8888248
(c) The description of the properties and characterization of the materials must be presented in a characterization results section, and must be duly granted;
(d) In the legend of Figure 1 add the aid scale used, in addition a punctual chemical characterization by EDS can be considered;
(e) The methodology section is too extensive, a review may be required by the authors;
(f) There are numerous results presented, however the discussions are limited. Authors should compare their findings with the international literature and give greater perspective to research evaluation;
(g) The reference list must be reviewed within the MDPI training rules. Note that there are two number sequences.
None.
Author Response
Dear Editors and Reviewers:
Many thanks for your time and comments concerning our manuscript entitled “Study on the Properties and Morphology of Nano-ZnO Modified Asphalt Based on Molecular Dynamics and Experiments” (No.coatings-2473659). Those comments are valuable and very helpful to improving our paper and research. We have made corrections which we believe satisfy the requirements of the reviewers. A summary of the corrections made in the paper and the responses to the reviewers’ comments are as following:
Point 1: The abstract can be examined, the authors must highlight the innovation and motivation, in addition to presenting the main quantitative results of this research.
Response 1: As reviewers’ suggested that we have added the motivation and innovation of this research (please see line 8 to 11), and the main quantitative results were presented in the abstract, please see line from 15 to 23.
Point 2: Throughout the introduction, some aspects of the study of the art of the theme should be mentioned, some illustrations and comparative tables can be added by the authors, note some suggested literature: 10.3390/ma15072598; 10.1061/JMCEE7.MTENG-14543; 10.1155/2023/8888248.
Response 2: We are very appreciate this suggestion, the suggested literature (including10.1061/JMCEE7.MTENG-14543 and 10.1155/2023/8888248 )has been noted in the introduction, please see line 52 to 59. This literature (10.3390/ma15072598) is not closely relevant to our research, so we didn’t note this one in the introduction. By the way, our article is not a review article, we think it’s not necessary to list a comparative tables of our reviewed literature to illustrate the effect of nano-particles materials on properties of asphalt.
Point 3: The description of the properties and characterization of the materials must be presented in a characterization results section, and must be duly granted;
Response 3: Thank you for your suggestion, we have arranged the part of properties and characterization of asphalt and nano-ZnO, and put this part in the first section of results section,please see line 214 to 273.
Point 4: In the legend of Figure 1 add the aid scale used, in addition a punctual chemical characterization by EDS can be considered;
Response 4: In the legend of Figure 1, the aid scale we used in the process of capturing the ZnO image had been placed at the bottom of figure 1, and the white blank means 100nm。
Point 5: The methodology section is too extensive, a review may be required by the authors;
Response 5: The methodology section has been shortened and summarized.
Point 6: There are numerous results presented, however the discussions are limited. Authors should compare their findings with the international literature and give greater perspective to research evaluation;
Response 6: As reviewers’ suggested that we have enriched the discussions of our research results, and some comparisons have been given in the results section, please see results and discussion part.
Point 7: The reference list must be reviewed within the MDPI training rules. Note that there are two number sequences.
Response 7: We have checked all references, and modified them within MDPI training rules.
Once again, thank you very much for your comments and suggestions.
Author Response File: Author Response.doc
Round 2
Reviewer 3 Report
Ok
Ok
