PONE-D-25-12190Selective Sonochemical post-synthesis Modification of LTA Zeolite with zinc speciesPLOS ONE

Dear Dr. De Leon Ramirez,

Thank you for submitting your manuscript to PLOS ONE. After careful consideration, we feel that it has merit but does not fully meet PLOS ONE’s publication criteria as it currently stands. Therefore, we invite you to submit a revised version of the manuscript that addresses the points raised during the review process.

Please submit your revised manuscript by May 25 2025 11:59PM. If you will need more time than this to complete your revisions, please reply to this message or contact the journal office at plosone@plos.org . When you're ready to submit your revision, log on to https://www.editorialmanager.com/pone/ and select the 'Submissions Needing Revision' folder to locate your manuscript file.

Please include the following items when submitting your revised manuscript:

• A rebuttal letter that responds to each point raised by the academic editor and reviewer(s). You should upload this letter as a separate file labeled 'Response to Reviewers'.
• A marked-up copy of your manuscript that highlights changes made to the original version. You should upload this as a separate file labeled 'Revised Manuscript with Track Changes'.
• An unmarked version of your revised paper without tracked changes. You should upload this as a separate file labeled 'Manuscript'.

If you would like to make changes to your financial disclosure, please include your updated statement in your cover letter. Guidelines for resubmitting your figure files are available below the reviewer comments at the end of this letter.

If applicable, we recommend that you deposit your laboratory protocols in protocols.io to enhance the reproducibility of your results. Protocols.io assigns your protocol its own identifier (DOI) so that it can be cited independently in the future. For instructions see: https://journals.plos.org/plosone/s/submission-guidelines#loc-laboratory-protocols . Additionally, PLOS ONE offers an option for publishing peer-reviewed Lab Protocol articles, which describe protocols hosted on protocols.io. Read more information on sharing protocols at https://plos.org/protocols?utm_medium=editorial-email&utm_source=authorletters&utm_campaign=protocols .

We look forward to receiving your revised manuscript.

Kind regards,

Mashallah Rezakazemi

Academic Editor

PLOS ONE

Journal Requirements:

When submitting your revision, we need you to address these additional requirements.

1. Please ensure that your manuscript meets PLOS ONE's style requirements, including those for file naming. The PLOS ONE style templates can be found at

https://journals.plos.org/plosone/s/file?id=wjVg/PLOSOne_formatting_sample_main_body.pdf and

https://journals.plos.org/plosone/s/file?id=ba62/PLOSOne_formatting_sample_title_authors_affiliations.pdf

2. Thank you for stating the following financial disclosure:

“This work was supported by the DGAPA-PAPIIT-UNAM IG101623 Project”

Please state what role the funders took in the study. If the funders had no role, please state: "The funders had no role in study design, data collection and analysis, decision to publish, or preparation of the manuscript."

If this statement is not correct you must amend it as needed.

Please include this amended Role of Funder statement in your cover letter; we will change the online submission form on your behalf.

3. Please expand the acronym “UNAM” (as indicated in your financial disclosure) so that it states the name of your funders in full.

This information should be included in your cover letter; we will change the online submission form on your behalf.

4. Thank you for stating the following in the Acknowledgments Section of your manuscript:

“This work was supported by the DGAPA-PAPIIT-UNAM IG101623 Project. J”

We note that you have provided funding information that is not currently declared in your Funding Statement. However, funding information should not appear in the Acknowledgments section or other areas of your manuscript. We will only publish funding information present in the Funding Statement section of the online submission form.

Please remove any funding-related text from the manuscript and let us know how you would like to update your Funding Statement. Currently, your Funding Statement reads as follows:

“This work was supported by the DGAPA-PAPIIT-UNAM IG101623 Project”

Please include your amended statements within your cover letter; we will change the online submission form on your behalf.

5. We notice that your supplementary figures are included in the manuscript file. Please remove them and upload them with the file type 'Supporting Information'. Please ensure that each Supporting Information file has a legend listed in the manuscript after the references list.

[Note: HTML markup is below. Please do not edit.]

Reviewers' comments:

Reviewer's Responses to Questions

Comments to the Author

1. Is the manuscript technically sound, and do the data support the conclusions?

The manuscript must describe a technically sound piece of scientific research with data that supports the conclusions. Experiments must have been conducted rigorously, with appropriate controls, replication, and sample sizes. The conclusions must be drawn appropriately based on the data presented.

Reviewer #1: Yes

Reviewer #2: Yes

Reviewer #3: Yes

Reviewer #4: Partly

Reviewer #5: Yes

**********

2. Has the statistical analysis been performed appropriately and rigorously?

Reviewer #1: Yes

Reviewer #2: N/A

Reviewer #3: No

Reviewer #4: N/A

Reviewer #5: Yes

**********

3. Have the authors made all data underlying the findings in their manuscript fully available?

The PLOS Data policy requires authors to make all data underlying the findings described in their manuscript fully available without restriction, with rare exception (please refer to the Data Availability Statement in the manuscript PDF file). The data should be provided as part of the manuscript or its supporting information, or deposited to a public repository. For example, in addition to summary statistics, the data points behind means, medians and variance measures should be available. If there are restrictions on publicly sharing data—e.g. participant privacy or use of data from a third party—those must be specified.

Reviewer #1: Yes

Reviewer #2: Yes

Reviewer #3: Yes

Reviewer #4: No

Reviewer #5: Yes

**********

4. Is the manuscript presented in an intelligible fashion and written in standard English?

PLOS ONE does not copyedit accepted manuscripts, so the language in submitted articles must be clear, correct, and unambiguous. Any typographical or grammatical errors should be corrected at revision, so please note any specific errors here.

Reviewer #1: Yes

Reviewer #2: Yes

Reviewer #3: Yes

Reviewer #4: No

Reviewer #5: Yes

**********

5. Review Comments to the Author

Please use the space provided to explain your answers to the questions above. You may also include additional comments for the author, including concerns about dual publication, research ethics, or publication ethics. (Please upload your review as an attachment if it exceeds 20,000 characters)

Reviewer #1: 1. Highlighting the roles of the species introduced into the NaA zeolite would be beneficial as to tie up all the characterization techniques that has been employed in this study. Plus the role of sonochemical treatment need to be shown that will affect the modification of properties for NaA zeolite. This can be included in the conclusion part.

2. Since this study emphasize a lot in the role of Zn species in the NaA zeolite, suggestion is to add lattice parameter data for all the exchangeable zeolites to show the significance.

3. The above highlights could be use to further enhance the conclusions with regards to the final morphology of the sonochemically ion exchanges NaA zeolites.

Reviewer #2: A comprehensive and organized investigation of the post-synthesis alteration of NaA (LTA) zeolite with zinc species utilizing a sono-assisted deposition approach is presented in the publication. The study is current and creative, providing an environmentally responsible method of customizing zeolitic materials for cutting-edge uses..

One of the key strengths of this work is the clear and systematic presentation of results. The data is well-supported with relevant references, and the findings are consistently correlated, reinforcing the reliability of the study. The discussion effectively highlights the impact of zinc species incorporation on the physicochemical properties of the modified zeolite, particularly in terms of surface charge redistribution and pore architecture.

Overall, this is a well-executed and insightful piece of work that contributes to the advancement of zeolite modification strategies. The clarity of the methodology, strong correlation between results and discussion, and the practical implications of the study make this manuscript a commendable contribution to the field.

Reviewer #3: the research topic is very interesting and could bring benefit to the scientific community. the research framework focus on the incorporation of various zinc compounds in the zeolites matrices and improving their properties. the introduction points out all the factors necessary for proper understanding of the research. the experimental part give enough information for reader to repeat synthesis and analysis of the zeolites. the results obtained are properly analyzed and discussed. the conclusion summariye all the major findings

the number of figure and tables are satisfactory and give additional value to the article making it more understanable. what NaA means?(please describe it )what was error of determination in Tables 2? what were the major benefits of the Zn incorporation comparing to the LTA?

Reviewer #4: Peer Review PONE-D-25-12190

The manuscript entitled “Selective Sonochemical Post-Synthesis Modification of LTA Zeolite with Zinc Species” employs a sonochemical approach to modify LTA zeolite by depositing zinc-based nanoparticles.

In my opinion, this work is interesting, but I suggest major revisions before further consideration.

GENERAL OBSERVATIONS: The manuscript presents an interesting study; however, it contains numerous typos, grammatical errors, and lacks clarity regarding the experimental conditions. I strongly recommend a thorough review of the text.

Additionally, it remains unclear what type of interaction exists between the zeolite and zinc species (ion exchange, surface deposition, deposition within cavities, etc.). Furthermore, the practical applicability of this composite material is not well elucidated.

Abstract

• The sentence: “In this study, we employed an eco-friendly post-synthesis modification of a NaA zeolite with zinc species: ZnO, ZnO₂, and Zn(OH)₂ by a sono-assisted deposition method. This approach significantly reduced synthesis time.”

o The meaning of "synthesis time" is unclear; please clarify what is being referred to.

• Provide additional information on the interaction between LTA zeolite and Zn species.

Introduction

• Lines 81-87: Review these sentences for clarity and grammatical correctness.

Experimental

• Line 94: Specify the precursor used.

• Line 100: Correct “sonoassisted” to “sono-assisted” if necessary.

• Properly comment on Figure A1 before describing modification methods.

• Line 116: “Adjusting the final pH (according to each Zn species) and volume to 50 mL” — clarify this procedure.

• The passage: “To confirm the effect of the preparation conditions on the zeolite structure, blank samples (excluding the addition of Zn²⁺ precursor solution) were prepared at the deposition solutions (pH, ultrasound duration, and temperature) and studied by X-ray diffraction analysis. Given that no difference was observed, these samples were excluded from the study, presenting the data as an appendix (Figure A2).”

o This statement is unclear; please rephrase for better readability.

• The section on microscopy techniques: “Transmission electron microscopy (TEM) measurements (Hitachi H7500, Hitachi Ltd., Tokyo, Japan) at 80 kV. Sample morphology was obtained by scanning electron microscopy (SEM) using a JEOL JIB-4500 (MA, USA). The images were processed in Image J imaging software, and a second set of samples was analyzed on a LEICA Stereoscan 440 Scanning Electron Microscope. The samples were pretreated with a gold sputtering coating. The energy dispersive X-ray spectroscopy (EDX) coupled to the microscope used for SEM was also recorded.”

o This section requires revision; specify the EDX instrument used and clarify why two different SEM instruments were employed for two different sets of samples. Which samples were analyzed by each method? The same applies to ICP-OES.

• “A quantity between 25-50 mg was dissolved…” — clarify what was dissolved.

• “The samples were degassed at 50°C for 60 minutes, followed by a heating ramp with a rate of 5°C min⁻¹ until reaching 250°C, maintaining this temperature for 360 minutes before the analysis.”

o Explain why this thermal treatment was performed.

• “The study was conducted from 30°C to 800°C, with a heating ramp of 20°C min⁻¹ in an O₂ atmosphere.”

o Specify whether the atmosphere was pure O₂ or a mixture (e.g., N₂/O₂).

• Provide additional details regarding the experimental conditions for FTIR and Raman spectroscopy.

• Figure 3: The authors present N₂ sorption/desorption isotherms, but this method is not described in the experimental section. A proper description should be included.

Results and Discussion

• The term “thermal stability” is unclear. The samples appear to be thermally unstable, as they exhibit significant weight loss at low temperatures. Thermal stability (or oxidative stability in this case) should be defined based on onset temperature from DTG curves.

• Sample ZnO₂@NaA exhibits a weight gain at higher temperatures, which may be due to nitrogen adsorption from the furnace atmosphere, as also observed in isotherm measurements.

• Figure 6: It is recommended to invert the order of A and B to align with the discussion in the text.

Overall, the manuscript requires substantial revision for clarity, grammar, and experimental detail. The authors should ensure that all methods are thoroughly described and justified, particularly regarding sample preparation and characterization techniques.

Reviewer #5: Dear Editor,

I have carefully read the manuscript PONE-D-25-12190, entitled "Selective Sonochemical Post-Synthesis Modification of LTA Zeolite with Zinc Species", by J. I. De León-Ramírez et al., submitted to PLOS ONE.

Overall, I found this manuscript interesting, and I believe it merits publication in PLOS ONE after revision.

- First, the entire document should be reviewed by a native English speaker. The structure of some paragraphs is clearly inadequate but can be easily corrected. This would improve the readability and coherence of the text.

- The authors should improve the flow of the text around line 67. There is a noticeable gap that disrupts the reading at this point.

- In line 76, the authors state: "More recently, sonochemical approaches, such as sono-assisted precipitation (P-US), have emerged as innovative techniques for modifying zeolites." I believe this topic could be further developed. As it stands, the introduction section is weak. The authors should expand the literature review for each topic covered and include more details about the current state of the art. Based on this, clearly define the research gap and explain the limitations of previous studies in relation to your contribution. What is your novelty, specifically? While it becomes apparent throughout the manuscript, it needs to be stated more directly in the introduction to convince the reader.

- The methodology is clear and provides sufficient detail for reproducing the research independently—an essential aspect of scientific work. However, I encourage the authors to justify each methodological choice with appropriate citations.

- Figure 1(a): the graph presented alongside the image is unclear. While the authors successfully conveyed their message in parts (b)–(d), the same cannot be said for part (a). Please revise and improve its clarity.

- As a general comment, I would appreciate a comparison of the efficiency of the material synthesized in this work with that of equivalent materials produced using other techniques. An analysis of energy demand versus efficiency in the context of the sonochemical treatment would greatly enhance the value of this work.

- The conclusion section should be more quantitative. Include specific data to strengthen this section.

An excellent discussion on the characterization of the synthesized material was provided, which adds significant value to this manuscript. In my opinion, the manuscript can be considered for publication in PLOS ONE once these points are carefully addressed.

**********

6. PLOS authors have the option to publish the peer review history of their article (what does this mean? ). If published, this will include your full peer review and any attached files.

If you choose “no”, your identity will remain anonymous but your review may still be made public.

Do you want your identity to be public for this peer review? For information about this choice, including consent withdrawal, please see our Privacy Policy .

Reviewer #1: No

Reviewer #2: No

Reviewer #3: Yes:  Tomislav Tosti

Reviewer #4: No

Reviewer #5: No

**********

[NOTE: If reviewer comments were submitted as an attachment file, they will be attached to this email and accessible via the submission site. Please log into your account, locate the manuscript record, and check for the action link "View Attachments". If this link does not appear, there are no attachment files.]

While revising your submission, please upload your figure files to the Preflight Analysis and Conversion Engine (PACE) digital diagnostic tool, https://pacev2.apexcovantage.com/ . PACE helps ensure that figures meet PLOS requirements. To use PACE, you must first register as a user. Registration is free. Then, login and navigate to the UPLOAD tab, where you will find detailed instructions on how to use the tool. If you encounter any issues or have any questions when using PACE, please email PLOS at figures@plos.org . Please note that Supporting Information files do not need this step.

Selective Sonochemical post-synthesis Modification of LTA Zeolite with zinc species

PONE-D-25-12190R1

Dear Dr. De Leon Ramirez,

We’re pleased to inform you that your manuscript has been judged scientifically suitable for publication and will be formally accepted for publication once it meets all outstanding technical requirements.

Within one week, you’ll receive an e-mail detailing the required amendments. When these have been addressed, you’ll receive a formal acceptance letter and your manuscript will be scheduled for publication.

An invoice will be generated when your article is formally accepted. Please note, if your institution has a publishing partnership with PLOS and your article meets the relevant criteria, all or part of your publication costs will be covered. Please make sure your user information is up-to-date by logging into Editorial Manager at Editorial Manager®  and clicking the ‘Update My Information' link at the top of the page. If you have any questions relating to publication charges, please contact our Author Billing department directly at authorbilling@plos.org.

If your institution or institutions have a press office, please notify them about your upcoming paper to help maximize its impact. If they’ll be preparing press materials, please inform our press team as soon as possible -- no later than 48 hours after receiving the formal acceptance. Your manuscript will remain under strict press embargo until 2 pm Eastern Time on the date of publication. For more information, please contact onepress@plos.org.

Kind regards,

Mashallah Rezakazemi

Academic Editor

PLOS ONE

Additional Editor Comments (optional):

Reviewers' comments:

Reviewer's Responses to Questions

Comments to the Author

1. If the authors have adequately addressed your comments raised in a previous round of review and you feel that this manuscript is now acceptable for publication, you may indicate that here to bypass the “Comments to the Author” section, enter your conflict of interest statement in the “Confidential to Editor” section, and submit your "Accept" recommendation.

Reviewer #2: All comments have been addressed

Reviewer #3: All comments have been addressed

Reviewer #5: All comments have been addressed

**********

2. Is the manuscript technically sound, and do the data support the conclusions?

The manuscript must describe a technically sound piece of scientific research with data that supports the conclusions. Experiments must have been conducted rigorously, with appropriate controls, replication, and sample sizes. The conclusions must be drawn appropriately based on the data presented.

Reviewer #2: (No Response)

Reviewer #3: Yes

Reviewer #5: Yes

**********

3. Has the statistical analysis been performed appropriately and rigorously?

Reviewer #2: (No Response)

Reviewer #3: Yes

Reviewer #5: Yes

**********

4. Have the authors made all data underlying the findings in their manuscript fully available?

The PLOS Data policy requires authors to make all data underlying the findings described in their manuscript fully available without restriction, with rare exception (please refer to the Data Availability Statement in the manuscript PDF file). The data should be provided as part of the manuscript or its supporting information, or deposited to a public repository. For example, in addition to summary statistics, the data points behind means, medians and variance measures should be available. If there are restrictions on publicly sharing data—e.g. participant privacy or use of data from a third party—those must be specified.

Reviewer #2: (No Response)

Reviewer #3: Yes

Reviewer #5: Yes

**********

5. Is the manuscript presented in an intelligible fashion and written in standard English?

PLOS ONE does not copyedit accepted manuscripts, so the language in submitted articles must be clear, correct, and unambiguous. Any typographical or grammatical errors should be corrected at revision, so please note any specific errors here.

Reviewer #2: (No Response)

Reviewer #3: Yes

Reviewer #5: Yes

**********

6. Review Comments to the Author

Please use the space provided to explain your answers to the questions above. You may also include additional comments for the author, including concerns about dual publication, research ethics, or publication ethics. (Please upload your review as an attachment if it exceeds 20,000 characters)

Reviewer #2: (No Response)

Reviewer #3: the authors made an effort to fulfill the reviewers' suggestions and improve article quality. the implemented changes brings improvements and article meets minimum requirements for publication. But I have one more remark regarding abbreviations in abstract in my opinion the abstract must contain full name especially for first time mentioning.

Reviewer #5: Tha authors reviewed the manuscript criteriously. My questions were properly answered. I also noticed they did a good job answering the questions from the other reviewers. The manuscript can now be accepted for publication.

**********

7. PLOS authors have the option to publish the peer review history of their article (what does this mean? ). If published, this will include your full peer review and any attached files.

If you choose “no”, your identity will remain anonymous but your review may still be made public.

Do you want your identity to be public for this peer review? For information about this choice, including consent withdrawal, please see our Privacy Policy .

Reviewer #2: No

Reviewer #3: Yes:  Tomislav Tosti

Reviewer #5: No

**********