Conversion Study on the Formation of Mechanochemically Synthesized BaTiO₃

Round 1

Reviewer 1 Report

This manuscript reports the preparation and characterization of BaTiO3 by mechanochemical synthesis. Several parameters were investigated, namely the material of the grinding vessels, the rotational speed of the grinding vessel, and the number and density of the grinding balls.

The idea of the paper is interesting, and the results are valuable to be published as an original research paper. However, to publish it, some improvements are needed:

Suggestion: Please repeat the experiments with calcium doped zirconia grinding jars and include these results in the paper.

The introduction should include other information about other synthetic methodologies such as wet-chemical methods, hydrothermal synthesis, and which precursors are used for the preparation of BaTiO3 and indicate why the interest/advantages in mechanochemical synthesis.

Regarding the introduction, some references are missing Mechanochemical synthesis of barium titanate (10.1016/j.jeurceramsoc.2005.03.003)

In Figure 2, please include the PXRD for tetragonal BaTiO3 (JCPDS 05-0626) and the PXRD of BaO and TiO2 used in the experimental work.

In the Raman spectroscopy, please add some references https://doi.org/10.1016/j.jpcs.2013.02.010 and  https://doi.org/10.1002/jrs.1764.

Author Response

Dear Reviewer!

I would like to thank you for your helpful comments, on the basis of which the article has been corrected. I marked the changes with a yellow highlight.

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This manuscript reports the preparation and characterization of BaTiO3 by mechanochemical synthesis. Several parameters were investigated, namely the material of the grinding vessels, the rotational speed of the grinding vessel, and the number and density of the grinding balls. The idea of the paper is interesting, and the results are valuable to be published as an original research paper. However, to publish it, some improvements are needed:

• Suggestion: Please repeat the experiments with calcium doped zirconia grinding jars and include these results in the paper.

Thank you very much for the critical comment. I agree with the reviewer that he asks for the experiments to be repeated in zirconia grinding vessel since the basis of the article is also the examination of BaTiO₃ perovskites that can be produced in grinding vessels of different materials. Unfortunately, however, our research team does not have a zirconia vessel, and we could not get it from any other group. Nevertheless, in the introduction, we indicated a reference to the case of BaTiO₃ perovskite produced in the zirconia grinding vessel.

• The introduction should include other information about other synthetic methodologies such as wet-chemical methods, hydrothermal synthesis, and which precursors are used for the preparation of BaTiO3 and indicate why the interest/advantages in mechanochemical synthesis.

Thank you for your critical comment. In the introduction, we replaced the references to other synthesis methods and highlighted the advantage of the mechanochemical procedure against them.

• Regarding the introduction, some references are missing Mechanochemical synthesis of barium titanate (10.1016/j.jeurceramsoc.2005.03.003)

Thank you for your comments. I have placed the reference you suggested in the introduction in the description of the aforementioned zirconia grinding vessel.

• In Figure 2, please include the PXRD for tetragonal BaTiO3 (JCPDS 05-0626) and the PXRD of BaO and TiO₂ used in the experimental work.

Thank you very much for the comment of the reviewer. In Figure 2, I made up for the improvement of the characteristic reflections of TiO₂ and BaO.

• In the Raman spectroscopy, please add some references https://doi.org/10.1016/j.jpcs.2013.02.010 and  https://doi.org/10.1002/jrs.1764.

Thank you for your comments. I have placed the references you suggested in the in the description of the Raman discussion.

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Overall, thank you very much for the comments of the reviewer’s help, all of which I agreed with, and I amended the article following his advice. I hope that this has successfully increased the quality of the article and that it considers it acceptable in its present form.

Best regards!

Author Response File: Author Response.pdf

Reviewer 2 Report

The manuscript “Conversion study on the formation of mechanochemically synthesized BaTiO₃” addresses an interesting topic and clearly describes the results.

Moreover, the paper also uses a good English. Therefore, it may be recommended for publication.

In the introduction part it is recommended to add some more discussion. The following publication is recommended to fulfill this section:

• CATAURO, Michelina, et al. Antibacterial properties of sol–gel biomaterials with different percentages of PEG or PCL. In: Macromolecular Symposia. 2020. p. 1900056.

Author Response

Dear Reviewer!

I would like to thank you for your helpful comment, on the basis of which the article has been corrected. I marked the changes with a yellow highlight.

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The manuscript “Conversion study on the formation of mechanochemically synthesized BaTiO₃” addresses an interesting topic and clearly describes the results.

Moreover, the paper also uses a good English. Therefore, it may be recommended for publication.

In the introduction part it is recommended to add some more discussion. The following publication is recommended to fulfill this section:

• CATAURO, Michelina, et al. Antibacterial properties of sol–gel biomaterials with different percentages of PEG or PCL. In: Macromolecular Symposia. 2020. p. 1900056.
  • Thank you for your critical comment. I used your suggestion in the re-edited and extended introduction.

Reviewer 3 Report

In this study was investigated the followed the formation of perovskite structured barium titanate from BaO and TiO₂ precursors with X-ray diffractometric (XRD) and Raman spectroscopic measurements.

Major revisions:

1. The abstract is very general, and there is a lot of irrelevant information. The abstract should be explained and showed the important aspects of work. So, this abstract in the present form is unacceptable.
2. The previous work is very low, and isn't sufficient. It is recommended updated this section with new references, and compared them with your paper.
3. The results of experimental have not been directly compared and it is difficult to evaluate them.
4. No details on the specimens can be found in the paper (pictures ....)
5. The paper must be improved with charts, statistical studies and substantiated comments. More statistical analysis should been added, for example, the coefficient of variation (CV, standard deviation) of the experimental data should been added and discussed.
6. The conclusions should be broader and indicate the importance of the results and how to implement them.

Author Response

Dear Reviewer!

I would like to thank you for your helpful comments, on the basis of which the article has been corrected. I marked the changes with a yellow highlight.

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In this study was investigated the followed the formation of perovskite structured barium titanate from BaO and TiO₂ precursors with X-ray diffractometric (XRD) and Raman spectroscopic measurements.

Major revisions:

• The abstract is very general, and there is a lot of irrelevant information. The abstract should be explained and showed the important aspects of work. So, this abstract in the present form is unacceptable.

Thank you for your critical comment. Since I agreed with the critical position, I redesigned the abstract in its entirety according to the criteria given by the reviewer. In this version, I tried to put great emphasis on the surplus results of the thesis compared to the present state of science.

• The previous work is very low, and isn't sufficient. It is recommended updated this section with new references, and compared them with your paper.

Thank you very much for the comment of the reviewer, which I agreed with. Based on his comments, I made further additions to the introduction, where based on new references I present the surplus results of the thesis compared to other works.

• No details on the specimens can be found in the paper (pictures ....)

I agree with the reviewer and thank you for the comment. Based on electron microscopy measurement (TEM) of the samples the manuscript was supplemented with a brief analysis (TEM images, and size-distribution histograms, Fig.6).

• The results of experimental have not been directly compared and it is difficult to evaluate them.

Thank you for your critical comment. Based on this, I provided additional literary references and comments in the results section to compare the results obtained during the measurements.

• The paper must be improved with charts, statistical studies and substantiated comments. More statistical analysis should been added, for example, the coefficient of variation (CV, standard deviation) of the experimental data should been added and discussed.

Thank you for your critical advice. As far as possible, based on the reviewer's recommendation, we supplemented the results of the XRD measurements and represented them in the function of the applied ball-impact (E_b) energy (Fig.3). Thus, we were creating a so-called “milling map”, which better displays the relationship between the XRD results and the E_b. In addition, the microscopic study, proposed by the reviewer, was supplemented with histograms of the size distribution of the BaTiO₃ particles (Fig.6). Since we were only able to make 3 parallel series of measurements for energy-dispersive X-ray spectroscopy measurements, we supplemented the figure presenting the results of the EDS by indicating the measurement errors of the data (Fig.4).

• The conclusions should be broader and indicate the importance of the results and how to implement them.

Thank you for your critical comment, which I agree with. Based on the reviewer’s proposal, the conclusion part was supplemented and modified in accordance with the criteria given.

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Overall, thank you very much for the comments of the reviewer’s help, all of which I agreed with, and I amended the article following his advice. I hope that this has successfully increased the quality of the article and that it considers it acceptable in its present form.

Best regards!

Author Response File: Author Response.pdf

Round 2

Reviewer 3 Report

The paper in the revised form can be published, because it fulfills all the conditions of a valuable scientific paper.

Author Response

Dear Reviewer!

Let me to thank you again for your helpful comments and your positive opinion of the article about the final review.

Best regards! The authors, Gábor Kozma