Oxygen Measurement in Cuprate Superconductors Using the Dissolved Oxygen/Chlorine Method

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

In this article the Authors present a study on the development of a method for measuring copper valence and oxygen content in Bi-based superconductors. The authors claim an analysis time equal to approximately one-third of that of the iodometric titration method.

In my opinion this article needs to be improved in writing, some sentences are not clear and in general there is confusion between what has been done in the past and what is new in this article

Some suggestions:

1.        English needs improvement

2.        Abstract: the abstract is confusing and needs revision. To write a good abstract you need to keep in mind a simple sequence: 1) Background: Place the question addressed in a broad context and highlight the purpose of the study; 2) Methods: Describe briefly the main methods or treatments applied. Include any relevant preregistration numbers, and species and strains of any animals used; 3) Results: Summarize the article's main findings; and 4) Conclusion: Indicate the main conclusions or interpretations. Please rewrite the abstract following the scheme, attributing a maximum of four lines for each point.

3.        Table I: Where were the data reported in the table taken? In literature? Bibliographical references must be added for each line.

4.        The numbers must be accompanied by a unit of measurement. In the abstract and introduction numbers such as 0.013, 0.02, 0.016, 0.008 are reported, what are they? Percentages? Absolute values? Perhaps absolute or relative errors, or standard deviations.

5.        The analysis methods should be compared in terms of costs.

6.        The difference between the DO method and DO/Cl method must be explicit, to highlight the novelty, at the end of introduction and in conclusion. This is to understand the quality of the research.

7.        Self-citations are too many compared to the total number of citations

Comments on the Quality of English Language

English needs improvement

Author Response

Dear Reviewer,

Thank you for your thorough and constructive feedback on our manuscript. We appreciate your time and effort in providing detailed suggestions to improve our work. Below are our responses to each of your comments:

 1.English needs improvement:

• After all content modifications are completed, I will use MDPI's English Language Editing Services to polish the article.

2.Abstract: the abstract is confusing and needs revision:

• Thank you for teaching me how to write a good abstract. I have revised the abstract according to your suggestions: Lines 8 to 12 provide the background, lines 12 to 16 describe the method, lines 16 to 20 present the results, and lines 20 to 23 offer the conclusion.

3.Table I: Where were the data reported in the table taken? In literature? Bibliographical references must be added for each line:

• The sources and references for the data in Table I have been added accordingly.

4.The numbers must be accompanied by a unit of measurement. In the abstract and introduction numbers such as 0.013, 0.02, 0.016, 0.008 are reported, what are they? Percentages? Absolute values? Perhaps absolute or relative errors, or standard deviations:

• I agree that numbers must have units. However, the values 0.013, 0.02, 0.016, and 0.008 mentioned in the abstract and introduction represent the differences in copper content and oxygen atomic numbers between the two methods and do not have specific units.

5.The analysis methods should be compared in terms of costs:

• I have added a comparison of the costs associated with the different analytical methods in the manuscript. The comparison is mainly focused on the cost of physical analysis, as chemical analysis typically involves inexpensive reagents and does not provide significant value for cost comparison.

6.The difference between the DO method and DO/Cl method must be explicit, to highlight the novelty, at the end of introduction and in conclusion. This is to understand the quality of the research:

• I have made distinctions between the DO method and the DO/Cl method at the end of the introduction (lines 62–67) and in the conclusion to help highlight the novelty and quality of the research.

7.Self-citations are too many compared to the total number of citations:

• I have removed unnecessary or redundant self-citations to improve the citation balance.

Reviewer 2 Report

Comments and Suggestions for Authors

This paper reports a method to measure Cu valence and oxygen content in superconducting cuprates based on oxygen measurement during the chemical decomposition in the solution.
These materials have a lot of applications, therefore, cheap and fast composition determination are highly demanded.
The suggested method is indeed fast and cheap compared to iodometry, which requires titration. 
The key idea of the method is that the amplitude of the exponential decay of the oxygen content in a solution after the acid treatment is directly related to the oxygen content in the material.
Chlorine admixtures cause several side chemical reactions that could also be taken into account, as explained here.

The paper seems to be of technological importance; however, some issues require clarification:

 

1. The title is strange. The word "method" is used twice in the title, and the word "development" is not necessary.
2. Linear fit is used as shown in Fig. 4b; however, the choice of particular t2 and t3 values that define the fitting range is not explained. It seems that the linear region is chosen arbitrarily. Do these values vary from one experiment to another?
3. I wonder why the authors do not develop a more complex model to describe the whole curve in Figs. 4, 8, and 9.
4. Fig. 8 lacks a caption.
5. The Supplementary Materials section (lines 340–350) just repeats the figure captions. This is misleading.
6. Line 146. It is not clear where the citations [10] [12] should be.

Comments on the Quality of English Language

Language style could be a bit improved.

Author Response

Dear Reviewer,

Thank you for your valuable feedback on our manuscript. We appreciate your comments and have addressed each point accordingly:

1.The title is strange. The word "method" is used twice in the title, and the word "development" is not necessary:

• Thank you for your suggestion. I have revised the title accordingly.

2.Linear fit is used as shown in Fig. 4b; however, the choice of particular t2 and t3 values that define the fitting range is not explained. It seems that the linear region is chosen arbitrarily. Do these values vary from one experiment to another?:

• The choice of particular t2 and t3 values that define the fitting range is explained in lines 199-202. The method for determining t2 and t3 is based on using the least squares method. Specifically, we determined t2 and t3 such that they lie on a straight line where the correlation function of the least squares method reaches its minimum value and remains constant. This approach ensures that t2 and t3 are chosen within the range where the correlation function is minimized and constant, thus making the selection method consistent and not arbitrary. However, these values might vary from one experiment to another depending on the specific conditions and characteristics of the sample being tested.

3.I wonder why the authors do not develop a more complex model to describe the whole curve in Figs. 4, 8, and 9:

• The reason for not developing a more complex model to describe the whole curve in Figs. 4, 8, and 9 is detailed in lines 210-214.

4.Fig. 8 lacks a caption:

• I apologize for the oversight. The caption for Fig. 8 appears on the next page due to formatting issues. I will ensure more careful formatting in the future.

5.The Supplementary Materials section (lines 340–350) just repeats the figure captions. This is misleading:

• I apologize for the confusion caused by the repetition of figure captions in the Supplementary Materials section. I have deleted this section to avoid further misunderstanding.

6.Line 146. It is not clear where the citations [10] [12] should be:

• I have revised line 146 to clearly indicate where the citations [10] and [12] should be placed.

Round 2

Reviewer 2 Report

Comments and Suggestions for Authors

The authors replied my comments.

The paper could be published.

Comments on the Quality of English Language

English is acceptable.

Author Response

Thank you all for the exact review.