Study on the Stability of Fe/Al2O3 Interface in Metal-Based Cermets Using Thermodynamic Modeling
Round 1
Reviewer 1 Report
Comments and Suggestions for Authors1. 16/19 (85%) references in the article are from more than 5 years ago.
2. Introduction. It is important to describe more details about DFT and its applications related to the development of new materials.
3. Authors describe sections as "chapters." It doesn't seem to sound good for the article format.
4. Please, use capital letters to inform Figures throughout the text.
5. In the excerpt: " There is usually a difference in the length and angle of the boundary vector in the 65s urface lattice parameters of heterogeneous materials, which leads to the lattice mismatch 66a t the interface. ", please add citation to the statement.
6. Add more than one citation to Equation 1.
7. Replace numbers (1), (2), etc.in the text, with (i) (ii). Use numbering only in sections.
8. . Sentences written in the future tense must be reevaluated and reorganized.
9. . Add citations for Eq. 2, Eq.3, and Eq. 4.
Author Response
Please see the attachment.
Author Response File: 
Author Response.pdf
Reviewer 2 Report
Comments and Suggestions for AuthorsWei et al. introduced a series of Fe/Al2O3 ceramic/metal models with first-principle calculations. According to the abstract, difference types of terminal interfaces of Al2O3 (Al or O interacting with Fe) caused the difference in stability. Although the concept is interesting, this manuscript still requires a MAJOR revision to improve the novelty and presentation. Here are my comments/queries:
-From reading the abstract, density of states, charge density, and differential charge density measurements were mentioned with no connection to the stability. Authors need to provide some brief ideas about the mechanisms of stability enhancement of the O-terminal interface over the Al-terminal interface. As this manuscript focuses only on one system (even with 3 possible interfaces), deep understanding of the mechanisms of stability enhancement should be one the novelties of this study.
-The introduction mostly contains literature reviews on previous computational studies of similar problems but contain no pain-points on the need of using first-principle calculations to investigate the Fe/Al2O3 system. I can easily guess (even without DFT calculations) that O-terminal with a higher electronegativity should be more stable than the Al-terminal as they interact with a conductor.
-The last paragraph of the intro should contain objectives of this study. Authors need to write an additional paragraph.
-From figure 7, authors need to clearly define the x-axis variable Delta u_0.
-Authors need to revise their English grammar and writing styles. Also, the typos on the subscripting or the superscripting need more care. (e.g. Wad is found as Wad many times)
-The conclusions part should actually be in the discussion part. A ‘Conclusions’ part should contain a short paragraph summarizing what/how the study is done and how will the information from the study be useful.
-As the authors mentioned in the abstract that the model results can guide the preparation of the composites. Please explain how or any technology to control the terminal interface of Al2O3 (to intentionally contain Al-terminal or O-terminal)
Author Response
Comments 1: [The introduction mostly contains literature reviews on previous computational studies of similar problems but contain no pain-points on the need of using first-principle calculations to investigate the Fe/Al2O3 system. I can easily guess (even without DFT calculations) that O-terminal with a higher electronegativity should be more stable than the Al-terminal as they interact with a conductor.]
Response 1：Thank you for your suggestion. We have added several more literature reviews， it seems that the firstprinciples calculations method is very effective to understand the
relationship between interfacial bonding strength and mechanism.
Comments 2:[The last paragraph of the intro should contain objectives of this study. Authors need to write an additional paragraph.]
Response 2：We have added this new paragraph. Thank you for your correction.
Comments 3: [From figure 7, authors need to clearly define the x-axis variable Delta u_0.]
Response 3：Thank you. I have changed the name of my diagram, and the new name can well explain this meaning. The specific changes are on lines 327 and 328.
Comments 4: [Authors need to revise their English grammar and writing styles. Also, the typos on the subscripting or the superscripting need more care. (e.g. Wad is found as Wad many times)]
Response 4：Thank you for your reminder, all the writing formats have been corrected.
Comments 5: [The conclusions part should actually be in the discussion part. A ‘Conclusions’ part should contain a short paragraph summarizing what/how the study is done and how will the information from the study be useful.]
Response 5：Thank you for your suggestion, we added a new conclusion section at the end, and changed the previous conclusion to discussion. It's on lines 481 to 488.
Comments 6: [As the authors mentioned in the abstract that the model results can guide the preparation of the composites. Please explain how or any technology to control the terminal interface of Al2O3 (to intentionally contain Al-terminal or O-terminal)]
Response 6：Thank you for your reminder, how to prepare the O-terminal binding Al2O3/Fe interface structure in the experiment is the main direction of experimental research in the future. I have added this sentence to the final conclusion. The details are on lines 487-488.
The revised article is attached. Thank you for your correction. I hope to hear from you as soon as possible.
Reviewer 3 Report
Comments and Suggestions for AuthorsIn this work the authors performed a computational analysis of the nature, stability and properties of Fe/Al2O3 surface by means of DFT.
The work is of interest, while some revisions are needed to make the work suitable for publication.
1) When modelling interfaces, lattice mismatch is a delicate aspect as it can lead to spurious effects. In general, strain-free (or close to) models should be adopted [10.1038/s41467-022-33414-6; 10.1002/adfm.202009472]. This part of the discussion should be extended, and the authors should explain clearly the strategy used to minimize the strain.
2) The discussion is missing of two crucial properties, band edges alignment and interface poliration. Can the authors add such analysis?
Author Response
Comments 1: [When modelling interfaces, lattice mismatch is a delicate aspect as it can lead to spurious effects. In general, strain-free (or close to) models should be adopted [10.1038/s41467-022-33414-6; 10.1002/adfm.202009472]. This part of the discussion should be extended, and the authors should explain clearly the strategy used to minimize the strain.]
Response 1:Thank you very much for your suggestion. I got the conclusion from the literature on the lattice mismatch. Thank you for your new method.
Comments 2: [The discussion is missing of two crucial properties, band edges alignment and interface poliration. Can the authors add such analysis?]
Response 2:Thank you for your suggestion. I have not done any research in this area before. Thank you for providing me with new ideas. I am willing to explore and further study your suggestion in the follow-up work.
Round 2
Reviewer 1 Report
Comments and Suggestions for Authors.
Reviewer 2 Report
Comments and Suggestions for Authors-
