Expanded Illite Filler in UV-Curable Polymer Electrolytes for All-Solid-State Li-Ion Batteries

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

1. There are many research works for the fabrication of polymer electrolytes. So what is the novelty of this work? The difference or innovation of this work should be stated in the introduction.

2. For the PSA result in Figure 3, it is difficult to read it for audience, so it should be redraw it.

3.  For Figure 5, the peak from crystalline plane should be marked.

4. More cycle number needed.

5. More electrochemical data needed, such as how the content of EI to effect the electrochemical performance of batteries?

6. A comparison table from this work and other similar works should provide to show the merits of this work.

Comments on the Quality of English Language

Should be improved 

Author Response

Review #1

Thank you for reviewing our manuscript. We all agree with your opinions and revised the manuscript. Please check the revised manuscript.

 

1. There are many research works for the fabrication of polymer electrolytes. So what is the novelty of this work? The difference or innovation of this work should be stated in the introduction.

Yes, there are many research related to polymer-based solid-state electrolyte for Li-ion batteries. However, in this study, we firstly used the illite from South Korea as a clay type filler. We emphasized and described this point in the introduction part. Please check the revised manuscript.

 

2. For the PSA result in Figure 3, it is difficult to read it for audience, so it should be redraw it.

Thank you for your advice, we redraw PSA result in revised manuscript. We have redrawn the data to make it simpler and easier for audience. Please check the figure 3.

 

3. For Figure 5, the peak from crystalline plane should be marked.

 We marked the crystalline plane in the Figure 5. Please check the revised Figure 5 in the manuscript.

 

4. More cycle number needed.

We agree that a higher cycle number is needed for a comprehensive research paper. To enhance the cyclability of the all-solid-state battery assembled with the polymer-based solid-state electrolyte containing EI, it is necessary to optimize the electrochemical conditions, including appropriate electrolyte components, cathode and anode active materials, and so on. For this reason, we are preparing a new manuscript focused on the optimization of a Li-ion battery using the polymer-based solid-state electrolyte with EI. However, we believe that this study provides a valuable guideline for the use of illite filler in solid-state batteries. This is why we submitted these results, even with the low cycle numbers.

 

5. More electrochemical data needed, such as how the content of EI to effect the electrochemical performance of batteries?

We added the CV in the supporting information. Also, we prepared the electrochemical performances depending on the amounts of EI. Please check our revised manuscript and supporting information.

 

6. A comparison table from this work and other similar works should provide to show the merits of this work.

As mentioned above, to the best of our knowledge, this is the first report on an all-solid-state battery using illite sourced from Yeongdong-eup, Republic of Korea. Therefore, it is very difficult to compare our work with published papers, as there is no existing research on solid-state batteries incorporating expanded illite from Korea and an NCM cathode.

Author Response File: Author Response.pdf

Reviewer 2 Report

Comments and Suggestions for Authors

 

Certainly! Here’s the revised comment with an explanation of how the filler enhances the properties of the electrolyte:

Dear Author,

Thank you for sharing this insightful study on the use of expanded illite (EI) as a filler in UV curable polymer electrolytes for all-solid-state Li-ion batteries. Your research on the potential of EI as a sustainable and efficient filler material is indeed promising. I have a few suggestions and questions that might further strengthen your work:

1. Figure Captions: Please consider avoiding the use of abbreviations in all figure captions. Detailed captions would be more informative and beneficial for the readers to fully understand the content presented.

2. Literature Review and Introduction: The literature review and introduction sections could benefit from further elaboration. A more comprehensive review of the existing research in this area would provide a stronger foundation for your study and highlight the novelty of your work more clearly.

3. Conclusion: The conclusion section could be expanded to better summarize the key findings of your study and discuss the broader implications of your work. Strengthening this section would enhance the overall impact of your paper.

4. Mechanical Properties: Illite is known to be a promising candidate for improving the mechanical properties of polymer-based solid-state electrolytes. It would be valuable to include an analysis of the mechanical properties of the electrolytes with varying contents of EI. This could provide a more comprehensive understanding of the impact of EI on the overall performance of the polymer electrolytes.

5. Electronic Conductivity: Ensuring poor electronic conductivity is crucial for solid-state electrolytes. Have you conducted any experiments to evaluate the electronic conductivity of the electrolytes with different EI contents? Including this data could reinforce the suitability of EI as a filler material.

6. Electrolyte Composition: To give readers a clearer picture of the electrolyte composition, could you consider tabulating the volume, volume %, mass, and mass % of the various components in your polymer electrolytes? This would enhance the reproducibility and clarity of your work.

7. Role of Filler in Electrolyte Properties: The inclusion of a filler like expanded illite in polymer electrolytes can significantly enhance their properties. Fillers often improve the mechanical strength of the electrolyte, which is crucial for maintaining structural integrity under various stress conditions. Additionally, fillers can help to increase the ionic conductivity by creating pathways that facilitate the movement of lithium ions while reducing the crystallinity of the polymer matrix. However, it's essential to ensure that the electronic conductivity remains low, as high electronic conductivity could lead to short circuits and reduced battery performance. A thorough investigation of these aspects in your study would provide a more complete understanding of the role of EI in enhancing the performance of polymer-based all-solid-state Li-ion batteries.

Thank you once again for your valuable contribution to this field. I look forward to seeing your responses and further developments in this area.

 

Comments on the Quality of English Language

Dear Author,

Thank you for providing a detailed description of the materials and methods used in your study. I appreciate the thoroughness with which you have outlined the procedures. I have a few suggestions that might enhance the clarity and effectiveness of this section:

Consistency in Units and Abbreviations: Please ensure consistency in the use of units and abbreviations throughout this section. For example, consider specifying whether the temperatures listed are in Celsius (℃) consistently, as well as the exact concentrations and ratios used, to avoid any ambiguity.

General Suggestions: To improve readability, consider breaking down the text into smaller paragraphs or bullet points, especially in sections where multiple steps are described in succession. This would make it easier for readers to follow the procedures.

Thank you for considering these suggestions. I believe they will contribute to making the methods section even more comprehensive and accessible to the audience.

 

 

Author Response

Review #2

Thank you for sharing this insightful study on the use of expanded illite (EI) as a filler in UV curable polymer electrolytes for all-solid-state Li-ion batteries. Your research on the potential of EI as a sustainable and efficient filler material is indeed promising. I have a few suggestions and questions that might further strengthen your work:

Thank you for reviewing our manuscript. We all agree with your opinions and revised the manuscript. Please check the revised manuscript.

 

1. Figure Captions: Please consider avoiding the use of abbreviations in all figure captions. Detailed captions would be more informative and beneficial for the readers to fully understand the content presented.

We agree your advice. We revised all captions. Please check the revised manuscript.

2. Literature Review and Introduction: The literature review and introduction sections could benefit from further elaboration. A more comprehensive review of the existing research in this area would provide a stronger foundation for your study and highlight the novelty of your work more clearly.

We have added additional background information to emphasize the novelty of our study. However, as mentioned in the manuscript, this is the first report on using expanded illite sourced from Yeongdong-eup, Republic of Korea. Therefore, there is limited information available for a comprehensive review.

 

3. Conclusion: The conclusion section could be expanded to better summarize the key findings of your study and discuss the broader implications of your work. Strengthening this section would enhance the overall impact of your paper.

 

We added more details on the contributions of this study in the conclusion. We believe this makes the conclusion clearer. Please check our revised manuscript.

 

4. Mechanical Properties: Illite is known to be a promising candidate for improving the mechanical properties of polymer-based solid-state electrolytes. It would be valuable to include an analysis of the mechanical properties of the electrolytes with varying contents of EI. This could provide a more comprehensive understanding of the impact of EI on the overall performance of the polymer electrolytes.

This is a very good point. We also believe that EI can enhance the mechanical stability of polymer-based solid electrolytes. However, in this study, we used small amounts of EI (0–8 wt%) to increase the ionic conductivity. As a result, there was no significant change in the mechanical properties of the polymer-based solid electrolyte fabricated with EI. We confirmed that the around 20wt% of EI amount can improve the mechanical stability of polymer-based solid electrolytes, but it shows poor ionic conductivity.

5. Electronic Conductivity: Ensuring poor electronic conductivity is crucial for solid-state electrolytes. Have you conducted any experiments to evaluate the electronic conductivity of the electrolytes with different EI contents? Including this data could reinforce the suitability of EI as a filler material.

 

We appreciate your advice. However, in this study, we focused on comparing the ionic conductivity based on the amount of EI, as this is the first step in synthesizing a polymer-based electrolyte using EI from the Republic of Korea. We plan to optimize the electrochemical performance of the all-solid-state battery using EI in the future, which will include various analyses, including the electronic conductivity of the electrolyte.

6. Electrolyte Composition: To give readers a clearer picture of the electrolyte composition, could you consider tabulating the volume, volume %, mass, and mass % of the various components in your polymer electrolytes? This would enhance the reproducibility and clarity of your work.

We added more detail information for electrolyte composition in the experimental senction. Please check the revised manuscript.

7. Role of Filler in Electrolyte Properties: The inclusion of a filler like expanded illite in polymer electrolytes can significantly enhance their properties. Fillers often improve the mechanical strength of the electrolyte, which is crucial for maintaining structural integrity under various stress conditions. Additionally, fillers can help to increase the ionic conductivity by creating pathways that facilitate the movement of lithium ions while reducing the crystallinity of the polymer matrix. However, it's essential to ensure that the electronic conductivity remains low, as high electronic conductivity could lead to short circuits and reduced battery performance. A thorough investigation of these aspects in your study would provide a more complete understanding of the role of EI in enhancing the performance of polymer-based all-solid-state Li-ion batteries.

Thank you for your comments, we do our best to submit our revised manuscript as soon as possible. Thank you again.

Author Response File: Author Response.pdf

Round 2

Reviewer 1 Report

Comments and Suggestions for Authors

Authors answered all comments from reviewers. It should be accepted in this version. 

Comments on the Quality of English Language

Should be polished