Mathematical Simulation of the Wettability of Al₂O₃ Substrate through Different Aluminum Alloys

Round 1

Reviewer 1 Report

The paper is devoted to the investigation of the wetting of aluminum oxide by liquid aluminum. The authors succeed to get good correspondence of experimental data and calculations. However, the following remarks and comments are kindly advised to be reviewed.

1. Page 1. The title does not fully cover the content of the manuscript and should be revised. There is only Al2O3 substrate.
2. Page 1, raw 23. It is advised to double the number of keywords.
3. Page 4, raw 132. Please use µm or micrometers instead of micron and make related changes throughout the paper.
4. Page 4, raw 138. It is necessary to provide a reference for Al-Y/Al-La phase diagrams. Please check the lowest melting point for the Al-La phase diagram as well as its eutectic composition.
5. Page 4, raw 126, Table 1. Please specify atomic or weight percentage to describe purity or alloy composition. It is necessary to point out the condition of powders (Al, Y, La), the size, and if they were premixed before injection to the substrate.
6. Page 4-5. Please provide references for equations 7-13 in the text. It is required to indicate the temperature Gibbs energy was calculated and the formula used.
7. Page 6, raw 206. In Materials and Methods please indicate the model of SEM and EDS, as well as the parameters of investigation.
8. Page 7, raw 209. Please use lowercase for Al2O3 in brackets.
9. Page 7, raw 224. Please prove the high concentration of La and Y alloying elements by providing tables or spectrums from EDS analysis.
10. Page 7, raw 231, Figure 5. Please indicate each zone of the cross section, as well as diffusion direction. Put the bar as it was done for Figure 4.
11. Page 7, raw 234. Please paraphrase and put the sentence “The microstructure of the alumina is observed.” in the main text or remove it completely.
12. Page 9, raw 290. The reference list is too short; it is advised to increase the number up to at least 20 sources.

Author Response

Manuscript ID: jcs-1219712

Type of manuscript: Article

Title: Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys

Authors: Enrique Rocha-Rangel *, José A. Rodríguez-García, José A. Castillo-Robles, Eddie N. Armendáriz Mireles, Carlos A. Calles-Arriaga

Attached you can find the corrected version of the manuscript: " Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys", that has been submitted for its publication to the Scientific-Technical Journal of Composites Science, after minor modification to the text in agreement with comments of reviewers.

We hope that the manuscript now complies with the requirements for its publication in the Microsystem Technologies.

ATTENTION TO THE COMMENTS OF REVIEWERS

Reviewer: 1

COMMENTS FOR THE AUTHORS

The paper is devoted to the investigation of the wetting of aluminum oxide by liquid aluminum. The authors succeed to get good correspondence of experimental data and calculations. However, the following remarks and comments are kindly advised to be reviewed.

1. Page 1. The title does not fully cover the content of the manuscript and should be revised. There is only Al₂O₃ substrate.

Answer: the referee is right; we change the title of the manuscript.

1. Page 1, raw 23. It is advised to double the number of keywords.

Answer: we added three more keywords.

1. Page 4, raw 132. Please use µm or micrometers instead of micron and make related changes throughout the paper.

Answer: we use the term µm throughout the manuscript.

1. Page 4, raw 138. It is necessary to provide a reference for Al-Y/Al-La phase diagrams. Please check the lowest melting point for the Al-La phase diagram as well as its eutectic composition.

Answer: References were made to the phase diagrams used, as well as the eutectic compositions used in the study and the melting temperatures of the resulting alloys.

1. Page 4, raw 126, Table 1. Please specify atomic or weight percentage to describe purity or alloy composition. It is necessary to point out the condition of powders (Al, Y, La), the size, and if they were premixed before injection to the substrate.

Answer: this requested information was placed in the document.

1. Page 4-5. Please provide references for equations 7-13 in the text. It is required to indicate the temperature Gibbs energy was calculated and the formula used.

Answer: 3 chemical reactions that were repeated were eliminated and they were included the references from which the free energies of the remaining reactions were taken.

1. Page 6, raw 206. In Materials and Methods please indicate the model of SEM and EDS, as well as the parameters of investigation.

Answer: this requested information was placed in the document.

1. Page 7, raw 209. Please use lowercase for Al2O3 in brackets.

Answer: this requested information was placed in the document.

1. Page 7, raw 224. Please prove the high concentration of La and Y alloying elements by providing tables or spectrums from EDS analysis.

Answer: this request could not be fulfilled as we do not have the required information, however, we modified the text of the document indicating that the formation of these products is probable without assurances as originally written.

1. Page 7, raw 231, Figure 5. Please indicate each zone of the cross section, as well as diffusion direction. Put the bar as it was done for Figure 4.

Answer: this requested information was placed in the document.

1. Page 7, raw 234. Please paraphrase and put the sentence “The microstructure of the alumina is observed.” in the main text or remove it completely.

Answer: the following sentence was deleted from the text; “The microstructure of the alumina is observed”.

1. Page 9, raw 290. The reference list is too short; it is advised to increase the number up to at least 20 sources.

Answer: 21 references are presented in the manuscript

Author Response File: Author Response.pdf

Reviewer 2 Report

Well Done!!

Author Response

Manuscript ID: jcs-1219712

Type of manuscript: Article

Title: Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys

Authors: Enrique Rocha-Rangel *, José A. Rodríguez-García, José A. Castillo-Robles, Eddie N. Armendáriz Mireles, Carlos A. Calles-Arriaga

Attached you can find the corrected version of the manuscript: " Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys", that has been submitted for its publication to the Scientific-Technical Journal of Composites Science, after minor modification to the text in agreement with comments of reviewers.

We hope that the manuscript now complies with the requirements for its publication in the Microsystem Technologies.

ATTENTION TO THE COMMENTS OF REVIEWERS

Reviewer: 2

COMMENTS FOR THE AUTHORS

(x) English language and style are fine/minor spell check required

Answer: The whole manuscript has been spelling and grammatically revised.

Reviewer 3 Report

The authors explore the effect of surface carbon coating and addition of La, Y solutes in Al on the wetting process and wettability of Al alloy droplet on Al₂O₃ substrate. From the wetting experiment, a three-stage wetting process is summarized which is explained by a diffusion-based wetting model. In addition, it is also revealed that the presence of carbon on the surface of Al₂O₃ substrate and the addition of La and Y in Al can both increase the wettability of the Al alloy droplet.

The findings in this work are of great significance which are beneficial to the design of ceramic-liquid metal interaction to promote the wettability. I would like to suggest to accept this manuscript if the following questions are well addressed.

(1) In the title of the manuscript, the authors claim the theoretical method proposed in this work can model “wettability”. In fact, in the mathematical model introduced in section 2, a parameter  (contact angle in equilibrium) is used which quantifies the wettability of a liquid droplet on a substrate. However, in the following work (Figure 6 and Figure 7 in section 4.3),  is obtained directly from experiments instead of from theoretical derivations. Therefore, the model itself is unable to predict wettability, and instead, it predicts the wetting process.

(2) The physical meaning of  in Equation 6 should be explained.

(3) In Line 102, “Integrating equation (5) with respect to ?, then introducing”. What is the content after “with respect to”?

(4) In Line 254, Equation 5 should be changed to Equation 6.

(5) In Figure 6, some of the systems (Such as ACY ACL et al.) do not reach equilibrium.

(6) Why is there a sharp decrease around 1200 s in the Al system in Figure 6?

(7) It is better to compare the experimental findings and theoretical results for all the seven systems in Figure 7.

(8) From Figure 5, it is unable to observe the formation of La₂O₃ and Y₂O₃. How the conclusion in Line 226 that “This confirms that reactions 11 and 12 take place” is obtained?

Author Response

Manuscript ID: jcs-1219712

Type of manuscript: Article

Title: Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys

Authors: Enrique Rocha-Rangel *, José A. Rodríguez-García, José A. Castillo-Robles, Eddie N. Armendáriz Mireles, Carlos A. Calles-Arriaga

Attached you can find the corrected version of the manuscript: " Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys", that has been submitted for its publication to the Scientific-Technical Journal of Composites Science, after minor modification to the text in agreement with comments of reviewers.

We hope that the manuscript now complies with the requirements for its publication in the Microsystem Technologies.

ATTENTION TO THE COMMENTS OF REVIEWERS

Reviewer: 3

COMMENTS FOR THE AUTHORS

(x) English language and style are fine/minor spell check required

Answer: the whole document was spelling and grammatically checked.

The authors explore the effect of surface carbon coating and addition of La, Y solutes in Al on the wetting process and wettability of Al alloy droplet on Al2O3 substrate. From the wetting experiment, a three-stage wetting process is summarized which is explained by a diffusion-based wetting model. In addition, it is also revealed that the presence of carbon on the surface of Al2O3 substrate and the addition of La and Y in Al can both increase the wettability of the Al alloy droplet.

The findings in this work are of great significance which are beneficial to the design of ceramic-liquid metal interaction to promote the wettability. I would like to suggest to accept this manuscript if the following questions are well addressed.

(1) In the title of the manuscript, the authors claim the theoretical method proposed in this work can model “wettability”. In fact, in the mathematical model introduced in section 2, a parameter  (contact angle in equilibrium) is used which quantifies the wettability of a liquid droplet on a substrate. However, in the following work (Figure 6 and Figure 7 in section 4.3), is obtained directly from experiments instead of from theoretical derivations. Therefore, the model itself is unable to predict wettability, and instead, it predicts the wetting process. Simulation.

Answer: the referee is right; we change the title of the manuscript.

(2) The physical meaning of  in Equation 6 should be explained.

Answer: the physical meaning of equation 6 is explained in the paper.

(3) In Line 102, “Integrating equation (5) with respect to ?, then introducing”. What is the content after “with respect to”?

Answer: we have corrected this part.

(4) In Line 254, Equation 5 should be changed to Equation 6.

Answer: we have corrected this part.

(5) In Figure 6, some of the systems (Such as ACY ACL et al.) do not reach equilibrium.

Answer: this is correct, however, the information here is based on that obtained at the time of experimentation.

(6) Why is there a sharp decrease around 1200 s in the Al system in Figure 6?

Answer: an explanation of this behavior was written in the manuscript.

(7) It is better to compare the experimental findings and theoretical results for all the seven systems in Figure 7.

Answer: Because there are many study systems and putting all the experimental and simulation information on a single graph would cause a lot of confusion in distinguishing the different curves. For this reason, only the experimental and simulation values of the best performing system were used, as explained in the text.

(8) From Figure 5, it is unable to observe the formation of La₂O₃ and Y₂O₃. How the conclusion in Line 226 that “This confirms that reactions 11 and 12 take place” is obtained?

Answer: we modified the text of the document indicating that the formation of these products is probable without assurances as originally written.

Round 2

Reviewer 1 Report

The reviewer appreciates the authors for the careful attention to all the remarks and for the responses. The manuscript is almost ready for publishing. However, the reviewer recommends correcting some minor issues.

1. Page 1. It is recommended to replace "Alumina
   Substrate" with "Al₂O₃ Substrate" in the title to be more specific. 
2. Page 6,7. Without proving data of high concentration of La and Y it is recommended to remove the sentence "Energy Dispersive Analysis of the sample grooves at the interfaces reveals a high concentration of the alloying elements La and Y in their respective samples compared to other interface zones." 

Author Response

May 28, 2021

Manuscript ID: jcs-1219712

Type of manuscript: Article

Title: Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys

Authors: Enrique Rocha-Rangel *, José A. Rodríguez-García, José A. Castillo-Robles, Eddie N. Armendáriz Mireles, Carlos A. Calles-Arriaga

Attached you can find the corrected version of the manuscript: " Mathematical Modeling of the Wettability of Alumina-Based Substrates Through Different Aluminum Alloys", that has been submitted for its publication to the Scientific-Technical Journal of Composites Science, after minor modification to the text in agreement with comments of reviewers.

We hope that the manuscript now complies with the requirements for its publication in the Microsystem Technologies.

ATTENTION TO THE COMMENTS OF REVIEWERS

Reviewer: 1

COMMENTS FOR THE AUTHORS

The reviewer appreciates the authors for the careful attention to all the remarks and for the responses. The manuscript is almost ready for publishing. However, the reviewer recommends correcting some minor issues.

Page 1. It is recommended to replace "Alumina Substrate" with "Al₂O₃ Substrate" in the title to be more specific.

Answer: we change the word alumina by Al₂O₃ in the title and in the key words.

Page 6,7. Without proving data of high concentration of La and Y it is recommended to remove the sentence "Energy Dispersive Analysis of the sample grooves at the interfaces reveals a high concentration of the alloying elements La and Y in their respective samples compared to other interface zones."

Answer: we remove the entire sentence referring to the Energy Dispersive Analysis.