Investigation of the Quartz Distribution in Electro-Porcelain Materials

Round 1

Reviewer 1 Report

I acknowledge the time and effort invested in the preparation of your article entitled [Investigation of quartz distribution in electroporcelain materials]. However, after thorough analysis and consideration, I must inform you that your article needs to be revised and expanded to be considered suitable for publication.

I wish to stress that my decision is based on an objective assessment of your work and does not reflect a lack of appreciation for your research. There are several aspects that I believe need to be addressed to improve the quality and impact of the article. I list some of them below.

First, I note that the analytical procedures used in your study do not present significant novelties in the field. In addition, the inclusion of only two samples considerably limits the statistical quality of your results and makes it difficult to generalise your conclusions. I would recommend that you extend your study by analysing more samples and consider more rigorous statistical methods to support your findings.

In addition, the diffraction analyses you have carried out could be improved. I would suggest that you further develop the methods and techniques used in the characterisation of ceramic materials, looking for more advanced and precise approaches that add value to your research. In addition to indicating the origin of the materials and crystallinity used as internal standard for the quantification of crystalline phases (this is essential to endorse the validity of the results), if there are discrepancies in the results, there are also other analytical procedures to validate the results. The results obtained with the low quartz sample are very doubtful. 

 

The SEM analysis can also be improved. No error estimate is given for the results obtained. Please also check the number of significant figures in your results. 

There are inconsistent data in Table 4.

Another aspect to take into account is the novelty of the results within the ceramic sector. According to my assessment, the results presented in your paper do not stand out significantly in comparison to previous studies in the field, or the industrial knowledge of the subject matter. It would be beneficial to your work if you could identify and discuss innovative aspects or findings that differentiate your research from existing research.

 

Finally, I also consider that there is little novel scientific content in your article. I encourage you to deepen your analysis and include a greater level of detail, as well as to explore new perspectives or approaches that would enrich the scientific community's understanding of the topic in question.

I urge you to consider these suggestions and make the necessary modifications to improve your work, especially by increasing the number of study samples. The submitted text can be classified as a report of findings and expertise rather than a comprehensive research paper. 

Author Response

Dear editor, dear reviewer,

Thank you for your critical reviewing the paper. It allows the improvement of the paper and give us hints for the further work in this area.

We have read the remarks of the reviewer carefully. We have implemented the comments that did not require additional experimental work. Additional strength measurements and investigation of additional materials will be planned for future work. The aim of the paper was to evaluate the usability of the analytical methods on two extreme materials and, in particular, to quantify the formation of microcracks around quartz particles. The latter has not yet been described in the literature. However, it is an important parameter that can influence strength and ageing. The results were therefore also discussed in this context. We are aware that further work is needed to understand the relationship between quartz grain size and content and crack system size. However, we think that this paper provides new approaches for further work. Therefore, we have submitted the paper and still think that it is worth to be published.

To address this, we have added in the conclusion:

“We are aware that further work is needed to better understand the relationship between quartz grain size and content and crack system size and mechanical properties and ageing. However, the methods presented here can be a basis for such further investigations.”

 

Here are the detailed comments on the remarks:

Answer:

We understand the remarks, however we think that we have some new interesting results in the paper. This is on the one side the semiautomatic determination of the quartz distribution on large areas and the investigation of the crack system around the quartz grains. This was also outlined in the overall comment above.

We are aware that the work is only a beginning and that the direct correlation of mechanical properties and microstructure is necessary to better understand the ageing behavior. But this requires additional detailed investigations that could not be realized in the time available.

We have added into the paper the data to characterize the standards. The reviewer is right, that some amorphous content in the reference materials could have an influence on the results. However, we have found no hint concerning the amorphous content. The difference is most probably connected with some micro adsorption.

The validity of the data we tested with additional mixtures of Al₂O₃ and glass (supplement and also by comparing the xrd – data with the image analysis of the quartz particles. This validation gives a good basis for assessing the reliability of the method.

 

We added:

“Silicon (semiconductor grade, with a particle size < 20 µm, which was annealed to minimize stresses) or zinc oxide (SIGALD, product no. 205532; grain size < 4µm) was added as a standard to determine the amorphous content (glassy phase).”

 

Please also check the number of significant figures in your results. 

Answer:

We have added the errors of the glass composition in table 2. This data were estimated based on the result of table S3.

Additionally we have added in table 3 the confidence intervals.

There are inconsistent data in Table 4.

We have checked this: The difference to table 3 is the different parameter maximum feret in comparison to equivalent circle diameter. We have changed the description in the table. Additionally there was a mistake with the digits. We have changed this.

 

Reviewer 2 Report

The work talks about the "microstructure of electro porcelain and its influence on the mechanical, electrical and ageing behavior. The microstructure of two electro porcelain materials with low and high quartz content were analyzed in respect to the distribution of quartz. Using an adequate evaluation of EDS mapping data, a reproducible analysis of the size distribution and quantity of quartz was achieved. Independent on the overall amount of quartz in the materials a wide distribution of the grain size was observed. Around the large quartz particles microcrack systems with length of several 100 μm were observed. They are linearly correlated with the equivalent circle diameter of the quartz grains. The evaluation of the cracks allowed to determine the critical size below which no cracks around the quartz particles are formed."
Apart from the comments that you will find in the pdf, I would like to point out that your article shows a fair amount of originality. I also think that with further effort in the experimental part, better results can be achieved, giving strength to what you propose. In particular, I would ask you to increase the number of samples analysed for the low quartz (lq) sample in order to obtain better estimates and smaller measurement errors. With this in mind, you could also imagine using a polynomial with n greater than 1 which could better explain the behaviour in relation to the size of the quartz grains and which could possibly take into account what has been described in relation to breakage phenomena for neighbouring quartz grains.

I would also suggest doing an additional step on mechanical strengths to confirm what you have mathematically calculated in the discussion section.

Apart from a few sentences where it is possible to write more clearly, the article is fluent to read.

Author Response

Dear editor, dear reviewer,

Thank you for your critical reviewing the paper. It allows the improvement of the paper and give us hints for the further work in this area.

We have read the remarks of the reviewer carefully. We have implemented the comments that did not require additional experimental work. Additional strength measurements and investigation of additional materials will be planned for future work. The aim of the paper was to evaluate the usability of the analytical methods on two extreme materials and, in particular, to quantify the formation of microcracks around quartz particles. The latter has not yet been described in the literature. However, it is an important parameter that can influence strength and ageing. The results were therefore also discussed in this context. We are aware that further work is needed to understand the relationship between quartz grain size and content and crack system size. However, we think that this paper provides new approaches for further work. Therefore, we have submitted the paper and still think that it is worth to be published.

To address this, we have added in the conclusion:

“We are aware that further work is needed to better understand the relationship between quartz grain size and content and crack system size and mechanical properties and ageing. However, the methods presented here can be a basis for such further investigations.”

 

Here are the detailed comments on the remarks:

 

 

Reviewer 2:

I would like to point out that your article shows a fair amount of originality. I also think that with further effort in the experimental part, better results can be achieved, giving strength to what you propose.

I would ask you to increase the number of samples analysed for the low quartz (lq) sample in order to obtain better estimates and smaller measurement errors. With this in mind, you could also imagine using a polynomial with n greater than 1 which could better explain the behaviour in relation to the size of the quartz grains and which could possibly take into account what has been described in relation to breakage phenomena for neighboring quartz grains.

 

Answer:

It is clear, that for the material with the low quartz content the accuracy is limited. However, we have analysed even a large area of 12.5 mm². This is the problem of the low concentration.

Describing the relationship between grain size and crack length with a polynomial with n greater than 1 was an option we also discussed when preparing the paper. We decided to use the linear relation and correlate only the smaller grains due to the fact, that this looks the more reliable way for determining the critical grain size. Therefore, we would not like to change this.

Reviewer 3 Report

The manuscript is well written and within the scope of the journal. Congratulations.

Author Response

Dear editor, dear reviewer,

Thank you for your critical reviewing the paper. It allows the improvement of the paper and give us hints for the further work in this area.

We have read the remarks of the reviewer carefully. We have implemented the comments that did not require additional experimental work. Additional strength measurements and investigation of additional materials will be planned for future work. The aim of the paper was to evaluate the usability of the analytical methods on two extreme materials and, in particular, to quantify the formation of microcracks around quartz particles. The latter has not yet been described in the literature. However, it is an important parameter that can influence strength and ageing. The results were therefore also discussed in this context. We are aware that further work is needed to understand the relationship between quartz grain size and content and crack system size. However, we think that this paper provides new approaches for further work. Therefore, we have submitted the paper and still think that it is worth to be published.

Reviewer 4 Report

The microstructure of low and high quartz based electro porcelains was studied by EDS mapping. The size distribution and quantity of quartz were shown in this work. The observed microcrack length was correlated with the equivalent circle diameter of the quartz grains. The whole result is helpful for the community.

Some comments:

1) The XRD patterns with Rietveld fitting should be shown, not just the Table data;

2) Some discussion of the benefit and weaknesses of this method should be shown. 

3) In the INTRODUCTION section, other measurement techniques for size distribution should be introduced. 

4) Can this method be used by other materials, such as micro/nano-materials?

If these points could be addressed, the work could be reconsidered.

 

Author Response

Dear editor, dear reviewer,

Thank you for your critical reviewing the paper. It allows the improvement of the paper and give us hints for the further work in this area.

We have read the remarks of the reviewer carefully. We have implemented the comments that did not require additional experimental work. Additional strength measurements and investigation of additional materials will be planned for future work. The aim of the paper was to evaluate the usability of the analytical methods on two extreme materials and, in particular, to quantify the formation of microcracks around quartz particles. The latter has not yet been described in the literature. However, it is an important parameter that can influence strength and ageing. The results were therefore also discussed in this context. We are aware that further work is needed to understand the relationship between quartz grain size and content and crack system size. However, we think that this paper provides new approaches for further work. Therefore, we have submitted the paper and still think that it is worth to be published.

To address this, we have added in the conclusion:

“We are aware that further work is needed to better understand the relationship between quartz grain size and content and crack system size and mechanical properties and ageing. However, the methods presented here can be a basis for such further investigations.”

 

Here are the detailed comments on the remarks:

Reviewer 4:

• The XRD patterns with Rietveld fitting should be shown, not just the Table data;

Answer:

We have added the figure S1 in the supplement material showing the typical Rietveld results of the determination of the phases in the porcelain.

• Some discussion of the benefit and weaknesses of this method should be shown. 

Answer:

We have the comparison of the methods in the discussions, showing the limits of the methods. Therefore, we would not further elaborate the methods.  

3) In the INTRODUCTION section, other measurement techniques for size distribution should be introduced. 

Answer:

We have added in the introduction, that the grain size analysis can be determined by image analysis after etching with HF. This is the standard method however more and more laboratories want to avoid the HF etching. This was also one of our motivations for the analysis in the paper. To make this clearer we have added in the introduction : 

“Based on such etched cross sections quantitative image analysis is possible [1,2].”

4) Can this method be used by other materials, such as micro/nano-materials?

Answer:

We are sure that the method can be used for other materials too. We have added into the conclusions:

“Furthermore, such methods can also be applied for other particle-reinforced materials

Round 2

Reviewer 1 Report

The resubmitted article addresses certain minor issues, such as the refinement of result presentation and the inclusion of uncertainty values in specific tables. However, it fails to address the fundamental concern that led to its initial rejection, namely the limited number of samples analyzed in the study. All measurements were conducted on only two samples, thereby compromising the statistical significance of the findings, and limiting their applicability solely to the analyzed samples. As previously noted, the content of the article leans more towards an expert report rather than a research article, which is the expected standard for publication in this esteemed journal. Diluting the quality of our publications tarnishes the reputation of the journal. Nevertheless, I acknowledge that this viewpoint represents my personal opinion, and the final decision rests with the editorial board.

 

Reviewer 2 Report

The presented work is quite interesting and original. I regret that no further EDS analysis was carried out to broaden the sampling base and improve the fit of the experimental data with the interpolation line in Figure 6, which would have enhanced Pearson's coefficient and the estimation of the critical diameter relative to the low-quartz sample (currently the estimate has a relative error of 50%). Therefore, with a further effort by the authors, it would have been possible to increase the robustness of the estimates and improve the interpolation line. Despite this, the work can be published in the journal.