JHM（Journal of Hazardous Materials）文章审稿意见
Ms. Ref. No.: HAZMAT-D-13-03197
Title: Immobilization of simulated sodium-bearing waste in alkali-activated slag-fly ash-metakaolin hydroceramic materials: Preparation and characterization
Journal of Hazardous Materials
Dear Mr. Wang,
After careful review, I regret to inform you that I am unable to accept your above noted manuscript for publication in "Journal of Hazardous Materials". I have appended the comments of the reviewers in order for you to understand the basis for the final decision.
However, I do think it could be considered by another journal, and I would like to suggest that you take advantage of the article transfer service that "Journal of Hazardous Materials" is part of. This gives you the option to have your manuscript files and details transferred automatically to another journal. This removes the need for you to resubmit and reformat your manuscript, saving you valuable time and effort during the submission process.
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http://ees.elsevier.com/hazmat/l.asp?i=368021&l=O6UOX878
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Yours sincerely,
Wonyong Choi, Ph.D.
Editor
Journal of Hazardous Materials
Reviewers' comments:
Reviewer #2: In this study, the alkali-activated slag-fly ash-metakaolin hydroceramic (ASFMH) waste was prepared by the hydrothermal process to be stabilized and solidified the simulated sodium-bearing waste (SBW) into a solid form for geological disposal. The investigation was interesting; however, the objectives of the investigation were not well-designed. In addition, several statements were not clearly expressed and interpreted in the present form. Therefore, the manuscript presented in the current form can not be accepted. The following comments should be responded prior to publication:
General comments:
1. Highlights: The novelty should be clearly presented in the current manuscript.
2. Content: The content of this paper should be re-organized and presented in the clear and concise way.
3. Introduction: Parts of content shown in Introduction Section seem to be redundant, which should be synthesized and reorganized. Meanwhile, the results provided in the present manuscript are too short and brief, which should be further extended and interpreted.
4. Results and discussion: The physico-chemical properties of ASFMH such as density and grain size before and after experiments need to be provided and illustrated.
5. Results and discussion: The experimental data should be further elaborated and interpreted to provide more significant and important findings and conclusions. In other words, the method and criteria for evaluating the feasibility of proposed stabling process should be illustrated in detail.
6. Literature: More "relevant" and "recent" studies reported in the literature need to be comprehensively reviewed and critically compared in this investigation.
7. Figures and Tables: The quality of Figure 4 should be improved and presented in a scientific way to meet the journal's criteria. In addition, it suggests that more significant findings should be reported in terms of Figures and Tables.
Specific comments:
1. Page 3, Ln 37-62: More relevant studies (e.g., methods and their performance evaluation for stabling the radioactive SBW, etc) in the literature should be reviewed and compared.
2. Page 4, Line 15: The criteria of physico-chemical properties of the solidified sodium-bearing waste (SBW) should be stated in the Introduction Section.
3. Page 4, Ln 35: The novelty and objectives of the investigation need to be clearly stated in the Introduction.
4. Page 6, Ln 12: It suggests that the schematic diagram of experimental set-up (e.g., hydrothermal process, etc) should be presented.
5. Page 8, Ln 12-60: As indicated by the author in Introduction, the aim of the research was to form the zeolitic structure and superior strength of ASFMH. However, the results presented and discussion provided does not clearly indicate the feasibility of the developed process. It suggests that the the method and criteria for evaluating the feasibility of proposed stabling process should be illustrated in detail.
6. Page 15, Ln 43: More significant and important findings should be introduced in the Conclusion Section to reveal the significance and importance of the present study.
Reviewer #3: This work lies well within the scope of the journal. It has an interesting aim. However it is still not ripe for publication as many scientific and technical issues are not covered in a satisfactory way.
Here are most of my findings:
The language still needs significant improvement. I am not a native speaker but language is in some cases is poor (i.e. p.1.line56: .the simulated radioactive Sr2+ and Cs+.; or p.4 line 9 .the compound hydroceramic materials., p.8 line 39 .an available hydrothermal circumstance and adequate active silicon are supplied,. and many more). I can not name all the points that need to be rewritten/rephrased.
The text appears in different size in various places throughout the manuscript.
The novelty statement has to refer to conceptual thoughts and the related to achievements in a clear way. No abbreviations should be used in the novelty statement. In my view it needs to be rewritten.
The authors fail to provide in a concise way the highlights of this work. They have to rewrite the novelty statement and the highlights too. For example the aim of this work in my opinion can hardly be a highlight. On contrary the achievement of the targets set, might be.
In a scientific text it is not appropriate the use of units from other measuring systems such as gallons (p.2 line 34). The units should be consistent throughout the text, manuscript and tables.
The authors state "immobilization property". What is the meaning?
In table 1 authors show chemical compositions with a total content in some cases 99%+ much close to 100%. This is not the case for slag and Na silicate that 93.71% is given. What about the difference to 100%?
In p.5 line 20 the term modulus is used. The corresponding chemical meaning/ratio should be given in brackets (SiO2/Na2O molar ratio).
Interesting is why all the nitrates need to be dissolved in a 3M nitric acid. No solution volumes are given but later condensation is mentioned to be needed. How much? More experimental details should be provided.
In p.5 line 58 the term/method of "denitration" should be described in few words. Especially as according to XRD and FTIR there is a huge amount of nitrates still present.
Table 2 has some text missing. In my view Table 2 can be more informative if the elemental ratio was given along with the %wt of reagents mixture. However it is not clear why the component (meaning the element) is given and next to it the "nitrate" and next the "Chemical reagent". The concentration (values can not be read) on the 4th column refers to which one? This table can be improved.
In my opinion Table 3 would be more informative if given in %wt rather than showing SBW in %wt, raw materials in grams and Na silicate in %.
The Material Characterization Center-1 should be stated rather than just MCC-1 (p7 line17). How was the method modified? A short descrition is needed (How were the article suspended, Volume of leachant etc).
Typing errors exist i.e. p7line20 "simualted", p.15 line50 "mophorlogy" and more.
p.9 line 14. The authors suggest just after a short discussion over the XRD results and the anaclime phase formation that " . ASFMH materials are very suitable for immobilizing simulated SBW." At this point there is no sufficient evidence for such a claim.
Therefore in the same discussion part authors should comment on the importance of anaclime phase.
A big part of the discussion is supported by referring to the previous knowledge of the group. It would be good to seek for 1-2 more literature findings to support the interesting findings and discussion presented here.
In the SEM images there is no designation of the particles (single crystals according to authors). Thus there is no way to understand what is what.
How it is clear that tobermorite is observed. What is the supporting data? Why it is not observed in XRD? An explanation should be given.
What does C-S-H stands for? (S in particular)
In Figure 4 caption EDX is mentioned. No EDX is shown in Figure 4. EDX results are shown in Table 4.
In p.12line 17- The authors refer to SEM/EDX as a tool to investigate "the immobilization mechanism for the cations of simulated SBW". This is not supported by the following discussion. No mechanism is discussed or proposed after experimental findings. The text should be modified.
It is not clear how it can be concluded that the very small amount observed by the EDX (considering the uncertainty of such a measurement) can be enough to assume that SBW cations are "immobilized as exchangeable cations" in the structure or voids of analcime. On the other hand and according to my understanding the terms immobilization and exchangeable can be contradictory. Sample G2025-3 contains 25% wt SBW. SBW contains 0.47% Cs (maybe less - see my previous comment on Table 2) and similarly Sr. By EDX the detected Cs and Sr values are much lower. Please comment.
The formula of phases should be given in brackets as in p12 line 34. At least once when the phase name is found for the first time in the text.
Regarding the discussion in Part 3.3 is very general and fails to go deeper in order to propose a scenario for the mechanical deterioration of the article prepared by high SBW content. The importance of the highly soluble sodium nitrate gradual formation is not deeply considered. It is mentioned in two lines and the authors focus on general remarks about chemical bonds that I strongly question. A more interesting discussion would be on the alkaline activation and the related reactions and their products including the sodium nitrate formation. As the authors observed sodium nitrate becomes the predominant phase in the material when SBW>37.5%.
The MCC-1 method is a static leaching method and the leaching values reported are normalized rather than rates. The leaching rate is expected to be presented as a mass value over time. In p.15 line18-19 it is mentioned that the leaching rates are low after 14 days. This means that after 14 days in static conditions Sr and Cs still wash out. If so, what are the requirements and how does Sample G2025-3 meets them? How does the mitigation of Sr and Cs from G2025-3 is compared to the total Sr and Cs content? What are the final concentrations in the leachate? Would be this values meet other international waste management standards? A comparison would be useful.
The conclusions should be rewritten considering the above comments. The "universal testing machine" is not a testing method/technique. It is not clear the remark of a "good shaped" analcime (p.16, line14).
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