Studying the decontamination process of an irradiated beryllium reflector in a chlorine environment

Yuliya Baklanova

doi:10.1371/journal.pone.0322723

Peer Review History

Original SubmissionJanuary 5, 2025
5 Jan 2025 Author Response https://doi.org/10.1371/journal.pone.0322723.r001
28 Jan 2025 Decision Letter - Mohammad Alrwashdeh, Editor PONE-D-25-00607Studying the decontamination process of an irradiated beryllium reflector in a chlorine environmentPLOS ONE Dear Dr. Baklanova, 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 Mar 14 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. 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If you need to cite a retracted article, indicate the article’s retracted status in the References list and also include a citation and full reference for the retraction notice. [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 ******** 2. Has the statistical analysis been performed appropriately and rigorously? Reviewer #1: Yes Reviewer #2: Yes ****** 3. Have the authors made all data underlying the findings in their manuscript fully available? 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Any typographical or grammatical errors should be corrected at revision, so please note any specific errors here. Reviewer #1: Yes Reviewer #2: 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: I have reviewed the article titled "Studying the decontamination process of an irradiated beryllium reflector in a chlorine environment". The article present an interesting study to decontaminate the beryllium used in nuclear reactor. My comments are as follows 1. There are few typos in the article. For examples in abstract it is written "H3 including tritium" when it should be "including H3 tritium". For the gamma radiation spectrum graphs, the ordinate and abscissa titles are not in English. Page 2, 118mAg is wrong. Similarly page 4, 60CoCl2 is not written correctly in 3rd paragraph. 2. In figure 1, 614 and 723 keV peaks are labelled as Ag-110 but in all the other figures the peaks are labelled as Ag-108. 3. In results and discussion, it has been mentioned that tritium chloride capture efficiency is only 3%. additional studies are needed to verify the "assumption" that this efficiency can be increased with contact time of gaseous tritium chloride with water and using multi-stage tritium chloride traps. 4. Page 5, iron chloride transportation in the system, which kind of candidate materials you have in mind to avoid this problem. 5. First line of introduction, "the beryllium loses it unique properties as a neutron moderator and reflector". I think this needs to be modified or relevant reference needs to be provided which shows that there is decreases in beryllium's moderation and reflection capabilities after irradiation. Reviewer #2: The manuscript focuses on an important topic in nuclear waste management - the decontamination of irradiated beryllium reflectors using chlorination processes. The underlying methodology is systematic and based on established chemical principles, validated through experimental measurements. The authors provide detailed documentation of the developed chlorination process and the results obtained from their pilot installation. The implementation of this decontamination approach addresses a significant challenge in nuclear waste management, particularly given the increasing global inventory of irradiated beryllium. Taking this into consideration, I recommend that the manuscript be considered for publication in PLOS ONE, subject to the following revisions: 1. A major limitation of this study concerns the experimental validation which is based on only one type of sample from the JMTR reflector. It would be important to justify why this sample is considered representative and how the results could be extrapolated to other types of irradiated beryllium reflectors. A discussion of potential variations expected with different types of samples would significantly strengthen the scope of the study. 2. The chosen operational parameters, particularly the temperature of 730°C and the 30 chlorination cycles, require more thorough justification. The authors should explain how these parameters were optimized and present the relative efficiency of each cycle. This information is crucial for understanding the robustness of the process and its potential for optimization. 3. The formation of iron chloride due to corrosion represents a significant technical challenge that is not sufficiently addressed. The authors should discuss in more detail possible alternatives in terms of construction materials, evaluate the impact of this corrosion on the installation's lifespan, and propose solutions to minimize this problem, particularly in the perspective of larger-scale application. 4. Regarding formal aspects, the manuscript requires several improvements: sections should be clearly numbered, figures lack detailed captions and some are of insufficient quality, particularly the gamma spectra. Error bars should be added to all graphs and results tables. The bibliography should be enriched with more recent references on beryllium decontamination methods. These clarifications and additions would make the manuscript more complete and relevant to the scientific and industrial community. ****** 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. 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Revision 1
21 Mar 2025 Author Response Response to Reviewer 1 General Comment: "I have reviewed the article titled 'Studying the decontamination process of an irradiated beryllium reflector in a chlorine environment'. The article presents an interesting study to decontaminate the beryllium used in nuclear reactors. My comments are as follows." Author Response: I sincerely appreciate your thoughtful review and constructive feedback. Your insights have helped improve the quality of the manuscript. I am grateful for your comments and have carefully addressed each of your concerns in detail below. Remark No. 1: "There are a few typos in the article. For example, in the abstract, it is written 'H3 including tritium' when it should be 'including H3 tritium'. For the gamma radiation spectrum graphs, the ordinate and abscissa titles are not in English. Page 2, 118mAg is wrong. Similarly, on page 4, 60CoCl2 is not written correctly in the third paragraph." Author Response to Remark No. 1: I apologize for the inaccuracies. I have corrected all typos, including the phrase in the abstract, and thoroughly reviewed the text of the manuscript. The axis titles of all gamma radiation spectrum graphs have been translated into English for consistency. The incorrect isotope notation on page 2 has been corrected to Ag-108m. The chemical formula for cobalt chloride on page 4 has also been corrected to 60CoCl2. Remark No. 2: "In Figure 1, the 614 and 723 keV peaks are labeled as Ag-110, but in all the other figures, the peaks are labeled as Ag-108." Author Response to Remark No. 2: As you correctly pointed out, the correct isotope should be Ag-108m. I have now made the necessary corrections in Figure 1 to ensure consistency across all figures. Remark No. 3: "In the results and discussion, it has been mentioned that tritium chloride capture efficiency is only 3%. Additional studies are needed to verify the 'assumption' that this efficiency can be increased with the contact time of gaseous tritium chloride with water and using multi-stage tritium chloride traps." Author Response to Remark No. 3: I appreciate the reviewer’s attention to this point. In the manuscript, I have stated that tritium chloride absorption efficiency does not exceed 3% and suggested that efficiency could be improved by increasing the contact time of gaseous tritium chloride with water, employing bubbling devices, or using multi-stage tritium chloride traps. The relevant calculations have been provided in the following reference: Yu. Baklanova, A. Vurim, V. Kotov, A. Sitnikov, L. Chernova. Features of Chloride Technology for Processing Irradiated Beryllium. Polzunovsky Bulletin No. 3, 2019. [https://doi.org/10.25712/ASTU.2072-8921.2019.03.016] (In Russian). The current tritium capture system was primarily designed for proof-of-concept demonstration, and future research will focus on optimizing the system parameters to enhance tritium retention. Additionally, my future research, titled "Study of Corrosion Behavior of Austenitic Steel 12X18N10T in a Chlorine Medium," which has been submitted to the Journal of Corrosion and Materials Degradation, further explores this topic. I hope that the findings from this ongoing research will provide a more comprehensive understanding of the corrosion mechanisms involved. Remark No. 4: "Page 5, iron chloride transportation in the system, which kind of candidate materials you have in mind to avoid this problem" Author Response to Remark No. 4 I appreciate the reviewer’s question regarding potential materials to mitigate iron chloride formation. As noted in the manuscript, the formation of iron chloride results from the interaction of chlorine with stainless steel components, leading to corrosion. To address this issue, quartz glass, borosilicate glass, and nickel-based alloys are promising candidates for improving resistance to chlorine-induced corrosion. However, I acknowledge that this assumption requires further experimental verification to determine the long-term stability of these materials under operational conditions. Remark No. 5: "First line of introduction, "the beryllium loses it unique properties as a neutron moderator and reflector". I think this needs to be modified or relevant reference needs to be provided which shows that there is decreases in beryllium's moderation and reflection capabilities after irradiation." Author Response to Remark No. 5: I have revised the introduction to provide a more precise explanation of the degradation of beryllium's neutron-moderating and reflecting properties under prolonged irradiation. Specifically, I have included references to studies that demonstrate how neutron-induced swelling, helium and tritium accumulation, and impurity activation affect beryllium’s structural and neutron transport properties, ultimately impacting its performance in reactors. Response to Reviewer 2 General Comment: "The manuscript focuses on an important topic in nuclear waste management—the decontamination of irradiated beryllium reflectors using chlorination processes. The underlying methodology is systematic and based on established chemical principles, validated through experimental measurements. The authors provide detailed documentation of the developed chlorination process and the results obtained from their pilot installation. The implementation of this decontamination approach addresses a significant challenge in nuclear waste management, particularly given the increasing global inventory of irradiated beryllium. Taking this into consideration, I recommend that the manuscript be considered for publication in PLOS ONE, subject to the following revisions." Author Response: Dear Reviewer, I sincerely appreciate your careful review of the manuscript and your insightful comments. I am grateful for these detailed recommendations, which have allowed me to improve the clarity and scientific depth of the work. I hope the revisions sufficiently address your concerns and appreciate your support in improving the manuscript. Below, I provide my responses to each of your points. Comment 1: "A major limitation of this study concerns the experimental validation, which is based on only one type of sample from the JMTR reflector. It would be important to justify why this sample is considered representative and how the results could be extrapolated to other types of irradiated beryllium reflectors. A discussion of potential variations expected with different types of samples would significantly strengthen the scope of the study." Author Response: I acknowledge the reviewer’s concern regarding the representativeness of the JMTR reflector sample used in this study. The choice of this sample was based on its well-documented, certified irradiation history, operational conditions, and composition, making it a suitable case study for evaluating the chlorination-based decontamination process, as outlined in Ref. 18. To address the extrapolation aspect, I have expanded the discussion in the revised manuscript to include potential variations expected when applying this process to other irradiated beryllium reflectors, considering factors such as neutron fluence, impurity accumulation, and microstructural changes that may influence the chlorination efficiency. Comment 2: "The chosen operational parameters, particularly the temperature of 730°C and the 30 chlorination cycles, require more thorough justification. The authors should explain how these parameters were optimized and present the relative efficiency of each cycle. This information is crucial for understanding the robustness of the process and its potential for optimization." Author Response: I appreciate this suggestion and have revised the manuscript to better explain the selection of 730°C as the reaction temperature and the 30-cycle process. These parameters were determined based on prior computational and experimental data (see Ref. 17 and 24) and thermodynamic analysis, ensuring efficient chlorination while preventing excessive volatilization losses. Additionally, I have expanded the discussion on the efficiency of each cycle by summarizing the results of preliminary optimization studies, which demonstrated that 730°C provides a balance between decontamination effectiveness and minimization of unwanted side reactions. The following sentences inserted into the text of the manuscript. The installation's performance is calculated based on the fact that the operation of the proposed device consists of two phases: active and passive. After heating each unit of the installation to operating temperatures is supplied into the reaction chamber during the active phase of operation. The hot beryllium chloride flow reaches the filter, gradually increasing the temperature of its working elements. The active phase ends when the temperature of the filter's working elements reaches 700°C. During the passive phase, chlorine supply is stopped, and the direct-flow system is cooled with argon, The selection of operating temperatures is based on the phase transition temperatures of the obtained chlorides [22, 25]: the boiling point of beryllium chloride is 500°C, and the melting point of cobalt chloride is 724°C. The duration of the active phase was determined by the time required to heat nickel rods by 200°C in a flow of hot beryllium chloride, which was 6 minutes, while the duration of the passive phase is 5 minutes. Comment 3: "The formation of iron chloride due to corrosion represents a significant technical challenge that is not sufficiently addressed. The authors should discuss in more detail possible alternatives in terms of construction materials, evaluate the impact of this corrosion on the installation's lifespan, and propose solutions to minimize this problem, particularly in the perspective of larger-scale application." Author Response: The iron chloride formation due to corrosion poses a significant challenge in maintaining the integrity of the installation. In response to the reviewer’s request for more details: Alternative Materials: Quartz glass, borosilicate glass, and nickel-based alloys are considered promising candidates for improved corrosion resistance. However, further experimental validation is required to assess their long-term stability in chlorination environments. Impact on Installation Lifespan: The formation of iron chloride can lead to material degradation, reducing the operational lifespan of reactor components. Solutions for Large-Scale Application: Design modifications such as improved gas flow control, protective coatings, and alternative construction materials may help mitigate this issue. These points have been inserted into the revised manuscript to provide a more comprehensive discussion of long-term system stability. Comment 4: "Regarding formal aspects, the manuscript requires several improvements: sections should be clearly numbered, figures lack detailed captions and some are of insufficient quality, particularly the gamma spectra. Error bars should be added to all graphs and results tables. The bibliography should be enriched with more recent references on beryllium decontamination methods. These clarifications and additions would make the manuscript more complete and relevant to the scientific and industrial community." Author Response: I appreciate these recommendations and have implemented the following revisions: Sections have been numbered for better organization. Figure captions have been expanded to provide clearer descriptions of the data presented. Gamma spectra figures have been improved, and higher-quality versions have been included. Error bars have been added to tables to better represent measurement uncertainties. The references section has been updated with additional recent sources on beryllium decontamination methods to enhance the manuscript’s relevance to current research. Attachments Attachment Submitted filename: Response to reviewers.docx https://doi.org/10.1371/journal.pone.0322723.r003
26 Mar 2025 Decision Letter - Mohammad Alrwashdeh, Editor Studying the decontamination process of an irradiated beryllium reflector in a chlorine environment PONE-D-25-00607R1 Dear Dr. Baklanova, 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, Mohammad Alrwashdeh Academic Editor PLOS ONE Additional Editor Comments (optional): Reviewers' comments: https://doi.org/10.1371/journal.pone.0322723.r004
Formally Accepted
Acceptance Letter - Mohammad Alrwashdeh, Editor PONE-D-25-00607R1 PLOS ONE Dear Dr. Baklanova, I'm pleased to inform you that your manuscript has been deemed suitable for publication in PLOS ONE. Congratulations! Your manuscript is now being handed over to our production team. At this stage, our production department will prepare your paper for publication. This includes ensuring the following: * All references, tables, and figures are properly cited * All relevant supporting information is included in the manuscript submission, * There are no issues that prevent the paper from being properly typeset You will receive further instructions from the production team, including instructions on how to review your proof when it is ready. Please keep in mind that we are working through a large volume of accepted articles, so please give us a few days to review your paper and let you know the next and final steps. Lastly, if your institution or institutions have a press office, please let them know about your upcoming paper now to help maximize its impact. If they'll be preparing press materials, please inform our press team within the next 48 hours. 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. If we can help with anything else, please email us at customercare@plos.org. Thank you for submitting your work to PLOS ONE and supporting open access. Kind regards, PLOS ONE Editorial Office Staff on behalf of Dr. Mohammad Alrwashdeh Academic Editor PLOS ONE https://doi.org/10.1371/journal.pone.0322723.r005

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