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Article
Peer-Review Record

Fabrication of Silver-Doped UiO-66-NH2 and Characterization of Antibacterial Materials

Coatings 2022, 12(12), 1939; https://doi.org/10.3390/coatings12121939
by Feng Tian 1, Rengui Weng 1,*, Xin Huang 1, Guohong Chen 1 and Zhitao Huang 2
Reviewer 1:
Reviewer 2: Anonymous
Reviewer 4:
Coatings 2022, 12(12), 1939; https://doi.org/10.3390/coatings12121939
Submission received: 21 October 2022 / Revised: 22 November 2022 / Accepted: 8 December 2022 / Published: 9 December 2022

Round 1

Reviewer 1 Report (New Reviewer)

Authors reported Plant Fabrication of Ag/UiO-66-NH2 and Characterization of Anti- 2 bacterial Materials. Although the journals receive a large number of papers about Nanoparticles with various synthesis methods and applications. The authors must need to elaborate more to address the importance of this manuscript since the topic has been fairly active in  research area.

1.       What is the motivation behand this work, please give brief and clear explanation.

2.       Please clearly indicate advantages and disadvantages of plant extract based NP synthesis methods for comparison?

3.       Please explain formation mechanism of Ag NPs on UiO-66-NH2

4.       Please provide how experimental parameters (silver precursor,   reaction temperature and time and etc) affect the size and shape and formation of Ag/UiO-66-NH2

5.       Please povide the stability of the Ag Ag/UiO-66-NH2 in water, PBS and cultur medium

6.       Please revise the writing of manuscript to remove the typos

7.       The articles about syntehesis of metal-organic skeleton or hybrid NPs. Some of Followings should be considered for cite to improve the manuscript.

·         Materials Letters Volume 327, 15 November 2022, 133024

·         Adv. Mater. 25, 16, 2319-2325, 2013.

·         Angew. Chem. Int. Ed. 2009, 48, 219

·         J. Am. Chem. Soc. 134, 32, 13164-13167, 2012.

·         Nature Nanotech 2009; 4: 121 – 125.

·         Chem. Eur. J. 2013; 19: 7473 – 7479.

·         ACS Nano, 7, 10, 8972-8980, 2013.

·         Scientific Reports 2013;3: 2825.

·         ACS Nano, 8, 3, 2555-2561, 2014.

·         Scientific Reports2016; 6: 28900.

·         Plant Disease, 100, 1460-1465, 2016.

Author Response

Thanks for the advice. Based on your suggestion, I made the following modification.Please see the attachment.

Author Response File: Author Response.docx

Reviewer 2 Report (New Reviewer)

Tian et al., synthesized silver-doped metal-organic framework which was used as antimicrobial agents against E. coli and S. aureus. The work is good but there is need for improvement in the discussion of the characterization of the materials. The Figure for the synthesis of the material is different from the procedure described for the synthesis. The EDS, and elemental mapping characterization result should be included in the manuscript so as to establish that silver has truly doped the materials. In order to understand the internal morphologies and to know the distribution of the elements in the materials it is important to conduct TEM analysis.  The paper can be accepted after the major revision. The following points should be carefully addressed:

-          The title should be changed into silver-doped UiO-66-NH2 and the ‘2’ should be subscripted and this should be changed in the entire manuscript.

-          Explain in detail how you arrived at octahedron shape for the material by using SEM image only in line 182. Also, in line 184, you mentioned again that the shape was cubic shape. Is that not a contradiction?

-          Can you include the TEM, Elemental mapping and EDX images?  The particle size distribution should be obtained from the TEM image.

-          In line 11, the hyphen should be removed in’ in-troduced’.

-          The statement ‘material with….’ In line 12 should be revised to make better meaning.

-          In line 53, ‘ in various’ should be deleted.

-          In line 67, AG-MOF-1 should be changed into Ag-MOF-1.

-          In line 73, G should be changed into g in Graphene.

-          The list of the microbes in line 75-77 should be checked for correctness.

-          In line 87, IM should be defined in the first mention.

-          The statement ‘under the synergy….’ In line 89 should be rephrased.

-          In the synthetic procedure, DMF and ethanol were mentioned as the solvent while Fig. 1 only showed DMF. Also, the procedure stated that the final product was dried while the Fig 1 indicated the final product as wet in DMF. This should be corrected in the Figure. In addition to that, the yellow powder was drawn to have a specific shape in the Figure whereas this has not been established via characterization at this stage. Can you explain how you arrived at that shape before the characterization of the material? Figure 1 requires total overhauling.

-          There are a lot of short paragraphs in the manuscript. For instance, lines 133-139.

-          In line 149-150, the statement “samples were powdered by grinding” is not grammatically correct.

-          Wrong unit of temperature in line 172.

-          OD mentioned in line 174 was not defined on first mention.

-          Line 201 should be rephrased.

-          In Figure 5, there are four peaks between 500 and 1000 wave number but you accounted for only three. The authors should account for the last peak in their FTIR explanation.

-          In line 248, the word ‘reported that’ indicates that there should be a citation, but no citation was found.

-          In the entire TGA analysis, there was no single citation and the result was not compared with any previous report. Can you improve on this?

-          Is there any positive control in the antimicrobial studies? This should be indicated in the manuscript.

-          Table 2, shows an increase in diameter of the inhibition zone with increase in silver doping up to A3 for both microbes but the value dropped for both organism from A3 to A4, can you account for the decrease in value. On the contrary, the OD600 for the two organisms decreased and then decreased as shown in Figure 11, please account for this as well.

 

 

Author Response

Thanks for the advice. Based on your suggestion, I made the following modification.Please see the attachment

Author Response File: Author Response.docx

Reviewer 3 Report (New Reviewer)

1-     The introduction and discussion should be focused more on the observations and novelty of this study and supported with related references. The authors may use the following references to support the introduction , methodology , discussion parts  

a.  https://doi.org/10.1155/2022/1058119

b. https://doi.org/10.3390/nano12122013

c. doi: 10.3390/nano12162808.

d. DOI: 10.1038/s41598-022-22193-1

2. Statistical analysis paragraph must be added to the materials and methods section.

3. TEM ,  size particle distribution histogram, and statically analysis are required.  

4. Table 2 , are the experiment was performed one time or replicates. Please add the S.D.

5. Many typos mistakes were observed , Thus, English language editing is required.

 

6. Reagents with materials must be added with their origin (city, country).

7. More concluding remarks must be also added. 

Author Response

Thanks for the advice. Based on your suggestion, I made the following modification.Please see the attachment

Author Response File: Author Response.docx

Reviewer 4 Report (New Reviewer)

In this manuscript, a new silver metal-organic skeleton (Ag/UiO-66-NH2) was developed as antibacterial material. Silver ions were in-troduced into the Ag/UiO-66-NH2 by thermal solvent method and the materials with different silver doping amount were synthesized by controlling silver doping amount. The thermal stability of UIO-66-NH2, containing varying amounts of silver ions, was lower than the thermal stability of UiO-66-NH2. The higher the silver ion content, the lower the thermal stability. Under these conditions, the specific surface area and pore volume increased 

The manuscript appears to be experimentally correct and the utilized methods and the proposed models are interesting. I recommend the paper for publication, however, there are some concerns, comments and suggestion should be addressed before publication: 

  1. There are grammar and typographic errors. Please correct these errors and further improve the language. 
  2. Abstract should be modified. Main results should be added to the abstract and in total is should not be less than 150 words. 
  3. Introduction can be modified by adding more discussion from 2020-2022. 
  4. Last paragraph of introduction should be modified and need to add more detail about the manuscript. 
  5. The results and figures are appropriate however; author should add more physical explanation for the observed results. 
  6. How to verify the accuracy and correctness of the results?

Author Response

Thanks for the advice. Based on your suggestion, I made the following modification.Please see the attachment

Author Response File: Author Response.docx

Round 2

Reviewer 3 Report (New Reviewer)

Accept

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

As i wrote before, I read just microbiology part. 

The attached file shows you that it is better to revise your writting completely. 

Comments for author File: Comments.pdf

Author Response

Thank you for your advice. According to your suggestion, I have made the following modifications.

Point 1: First time must be written in complete words.

Response 1: I changed “E. coli” into “Escherichia Coli” (in yellow,line 42)

 

Point 2: Questions about capitalization, abbreviations and abbreviations.

Response 2: I revised all the above questions in the text. (in yellow,line 68/74/79/81/82/89)

 

Point 3:Too many not necessary things is written.

Response 3: I modified the content. (in yellow,line 165-176)

 

Point 4: Word error.

Response 4: I changed “solution” into “solutions” (in yellow,line 294)

Reviewer 2 Report

This manuscript describes that some silver metal-organic skeleton (Ag/UiO-66-NH2) were synthesized changing Ag concentrations, then the characterization and antibacterial activity of the powder samples were investigated. This manuscript would be acceptable for publication with some corrections.

1. If the authors conclude that Ag/UiO-66-NH2 with the silver ion content of 4 % (A3) showed the best antibacterial activity, then error bars in Fig. 9 and Fig. 10 are necessary.

2. How was the diameter of the inhibition zone in the photographs in Fig. 8 measured? Does four significant digits in Table 2 obtain by that measurement method? And, from the photographs in Fig. 8, the inhibition zone of A0 appears to be about 1 mm. Therefore, authors should check the values of A0 (0.017 and 0.025) in Table 2.

3. The silver ion content in A0-A4 is indicated by the ratio at the preparation of Ag/UiO-66-NH2. On the other hand, the concentration of silver ion leaking from Ag/UiO-66-NH2 depends on antibacterial activity. To clarify the reason why A3 showed the best antibacterial activity, it is necessary to measure the concentration of silver ions leaking from A0-A4. 

4. UiO-66-NH2 in Fig. 1 is drawn as a regular octahedron. The figure of UiO-66-NH2 in SEM image of Fig. 2 explains to be cubic. It is better to unify the image. 

5. Line 268-269 in FT-IR analysis, 1433 cm-1 and 1255 cm-1 should be revised to 1434 cm-1 and 1256 cm-1 to match the peak number in Fig. 5. 

6. In Table 1, it is better to confirm the significant digits.

 

7. Miscellaneous

7-1. Escherichia coli, E. coli, Staphylococcus aureus and S. aureus show in italics.

7-2. Line 166-167: ATCC No. of Escherichia coli and Staphylococcus aureus, i.e., receiving institution should be listed.

7-3. Line 213: What is “enzyme instrument”? Reviewer thinks that it is a plate reader. The model's name is necessary.

 

Author Response

Thank you for your advice. According to your suggestion, I have made the following modifications.

Point 1: If the authors conclude that Ag/UiO-66-NH2 with the silver ion content of 4 % (A3) showed the best antibacterial activity, then error bars in Fig. 9 and Fig. 10 are necessary.

Response 1: Error bars have been added in Fig. 9. As for Fig.10, adding error lines will affect the aesthetics, and it is a trend chart, so it is not modified.

 

Point 2: How was the diameter of the inhibition zone in the photographs in Fig. 8 measured? Does four significant digits in Table 2 obtain by that measurement method? And, from the photographs in Fig. 8, the inhibition zone of A0 appears to be about 1 mm. Therefore, authors should check the values of A0 (0.017 and 0.025) in Table 2.

Response 2: The diameter of the inhibition zone was measured with a vernier caliper using the crisscross method. I added a scale in Fig.8, I didn't expect any real problems about the values of A0 (0.017 and 0.025) in Table 2.

 

Point 3: The silver ion content in A0-A4 is indicated by the ratio at the preparation of Ag/UiO-66-NH2. On the other hand, the concentration of silver ion leaking from Ag/UiO-66-NH2 depends on antibacterial activity. To clarify the reason why A3 showed the best antibacterial activity, it is necessary to measure the concentration of silver ions leaking from A0-A4

Response 3: I will add an experiment later about the concentration of silver ions leaking from A0-A4

 

Point 4:  UiO-66-NH2 in Fig. 1 is drawn as a regular octahedron. The figure of UiO-66-NH2 in SEM image of Fig. 2 explains to be cubic. It is better to unify the image. 

Response 4: I have unified the image. (in green,line 180-181)

 

Point 5: Line 268-269 in FT-IR analysis, 1433 cm-1 and 1255 cm-1 should be revised to 1434 cm-1 and 1256 cm-1 to match the peak number in Fig. 5.

Response 5:I have revised the “1433 cm-1 and 1255 cm-1 ” to “1434 cm-1 and 1256 cm-1”. (in green,line 228-229)

 

Point 6:  In Table 1, it is better to confirm the significant digits.

Response 6: I changed the value to two significant numbers.( in green, Table 1)

 

Point 7: Miscellaneous

Response 7:I added the ATCC No. of Escherichia coli and Staphylococcus aureus (in green,line 166-167)

Reviewer 3 Report

Dear Authors,

You have performed a good research and done a lot of work, but the quality of your results is very poor. Unfortunately, in this form, I cannot recommend the manuscript for publication, it requires significant revision:

1. design the manuscript according to the rules of theMDPI journals: this applies to intratext references, bibliography, font, and so on, as long as the text resembles the creation of Frankenstein

2. The description of materials and methods, especially the section on antibacterial activity, looks very strange. there are enough articles with open access, where you can see how this section should be described. now it looks more like a student's lab journal

3. too few references for some statements in the introduction, usually just one

4. put in order the use of Latin names: at the first mention, the full name of the species is given (Bacillus subtilis), then the abbreviated name is used in the text (B. subtilis). Latin names are in italics.

Author Response

Thank you for your advice. According to your suggestion, I have made the following modifications.

Point 1: design the manuscript according to the rules of theMDPI journals: this applies to intratext references, bibliography, font, and so on, as long as the text resembles the creation of Frankenstein

Response 1: The format of this paper has been modified by the editor.

 

Point 2: The description of materials and methods, especially the section on antibacterial activity, looks very strange. there are enough articles with open access, where you can see how this section should be described. now it looks more like a student's lab journal

Response 2: I modified the content. (in yellow,line 165-176)

 

Point 3: too few references for some statements in the introduction, usually just one

Response 3: In the introduction, some of the statements I made were just a reference that was enough to make sense of them.

 

Point 4:  put in order the use of Latin names: at the first mention, the full name of the species is given (Bacillus subtilis), then the abbreviated name is used in the text (B. subtilis). Latin names are in italics.

Response 4: I revised all the above questions in the text. (in yellow,line 68/74/79/81/82/89)

Round 2

Reviewer 1 Report

line 172: where did you write about the tubes, that now you took samples from them/ also you took samples at different time intervals , not took different sample. 

Line 174: 600 nm is visible not UV. 

Line 176: This is the influence of different contact time not different samples.

Lines 279-290: is extra.

Line 294: We do not have bacterial solution or solutions, it is bacterial suspension.

 

 

Author Response

Thanks for the advice. Based on your suggestion, I made the following modification.

Point 1: line 172: where did you write about the tubes, that now you took samples from them/ also you took samples at different time intervals , not took different sample.

Response 1: Not a tube, but a petri dish.(in blue,line 174)

 

Point 2: Line 174: 600 nm is visible not UV.

Response 2: The Ultraviolet spectrophotometer is an instrument for measuring wavelength, 600nm is the set wavelength of the instrument. (in blue,line 174)

 

Point 3: Line 176: This is the influence of different contact time not different samples. Response 3: I modified the content. (in blue,line 174)

 

Point 4: Lines 279-290: is extra.

Response 4: I modified the content. (in blue,line 280-282)

 

Point 5: Line 294: We do not have bacterial solution or solutions, it is bacterial suspension.

Response 5: I modified the content. (in blue,line 285)

Once again, thank you very much for your comments and suggestions.

Reviewer 3 Report

Now I can agree that manuscript could be published.

Author Response

 Thank you very much for your comments and suggestions.

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