Vitreous Carbon, Geometry and Topology: A Hollistic Approach

Round 1

Reviewer 1 Report

Glass-like carbon (GLC) is a complex material with exceptional properties and thermal stability, attracting many researchers to understand its structure which remains little known. In this manuscript, the author reviewed the synthesis, characterization methods, electrical and mechanical properties, and stability as well as different models of the GLC proposed by researchers before. Via the tools of topology and geometry, the complex network architecture of GLC was understood and then several modified TPMS (Triply minimal surfaces structures) models were proposed. The paper is timely and the reviewer recommends its publication after addressing following minor issues.

The word ‘holistic’ is misspelled in the title and ‘an’ should be ‘a’.

1. The term ‘glassy like carbon (GLC)’ in the abstract seems ungrammatical. It should be better to replace it with ‘glass-like carbon’ or ‘glassy carbon’ such as in the references [2] and [3].
2. Should it be more precise to use “amorphous carbon”? glassy carbon has specially meaning there and the reviewer is not certain whether those amorphous state of carbon may behave like a glass. Indeed, recent works see to prefer monolayer amorphous carbon, e.g. Toh, et al. Nature 2020, 577, (7789), 199; and Xie et al. https://doi.org/10.1021/acs.nanolett.1c01462.
3. Indeed, special attention should be paid to low dimentional amorphous carbon, in contrast with its crystalline counterpart. A subsection may be added to include this cutting-edge research for the insightfulness of a comprehensive review.
4. The captions of figures and tables are ambiguous. For example, there are no ‘(a)’ in the Figure 6 and Figure 7, but it’s mentioned in the captions. In Table 1, the units of some quantities are represented and some others are not. Besides, what are ‘no’ and ‘-’ mean respectively?
5. Can you give a more detailed derivation of equation (15) to (17)? What is the relationship between F_k and V_n?
6. The logic of the manuscript is confusing. For example, a lot of variables are used before their definitions.
7. As described in Figure 24, an elemental cell of a Schwarzite TPMS structure was used to mimic the crossing region of the Franklin’s GLC, which seems contradict with Figure 2, where the element brick of the Franklin’s GLC was presented to be graphene sheet.
8. What’s the differences or advantages of the modified TPMS models proposed in the manuscript compared with the models proposed by researchers previously, especially Barborini’s 2002 model?
9. The English grammar and vocabulary of the manuscript need to be checked throughout.

Author Response

Glass-like carbon (GLC) is a complex material with exceptional properties and thermal stability, attracting many researchers to understand its structure which remains little known. In this manuscript, the author reviewed the synthesis, characterization methods, electrical and mechanical properties, and stability as well as different models of the GLC proposed by researchers before. Via the tools of topology and geometry, the complex network architecture of GLC was understood and then several modified TPMS (Triply minimal surfaces structures) models were proposed. The paper is timely and the reviewer recommends its publication after addressing following minor issues.

I would like to thank the reviewer for his/her positive and insightful comments on the manuscript. Below is my response to the issues

Other comments :

- some figures have been revisited for the sake of clarity

-all the modifications in the text are in red

-the revised title is : Vitreous carbon, geometry and topology: a hollistic approach

The word ‘holistic’ is misspelled in the title and ‘an’ should be ‘a’.

Response : corrected

1. The term ‘glassy like carbon (GLC)’ in the abstract seems ungrammatical. It should be better to replace it with ‘glass-like carbon’ or ‘glassy carbon’ such as in the references [2] and [3].

Response :To avoid any confusion one introduces glass-like carbon throughout the text

1. Should it be more precise to use “amorphous carbon”? glassy carbon has specially meaning there and the reviewer is not certain whether those amorphous state of carbon may behave like a glass. Indeed, recent works see to prefer monolayer amorphous carbon, e.g. Toh, et al. Nature 2020, 577, (7789), 199; and Xie et al. https://doi.org/10.1021/acs.nanolett.1c01462.

Response :A comment is added in the text including the suggested reference

1. Indeed, special attention should be paid to low dimentional amorphous carbon, in contrast with its crystalline counterpart. A subsection may be added to include this cutting-edge research for the insightfulness of a comprehensive review.

Response :A comment is added in the text (section SYNTHESIS OF GLC THIN FILMS)

1. The captions of figures and tables are ambiguous. For example, there are no ‘(a)’ in the Figure 6 and Figure 7, but it’s mentioned in the captions. In Table 1, the units of some quantities are represented and some others are not. Besides, what are ‘no’ and ‘-’ mean respectively?

Response :

• is suppressed in figures 6 and 7, in table 1 the density unit is precised, some symbols « – « and « n »  are replaced by « no relevant ». References are added

1. Can you give a more detailed derivation of equation (15) to (17)? What is the relationship between F_k and V_n?

Response :Equation 15 is equation 5. The text has been modified and corrected  for the sake of clarity 

1. The logic of the manuscript is confusing. For example, a lot of variables are used before their definitions.

Response :Variables are introduced

1. As described in Figure 24, an elemental cell of a Schwarzite TPMS structure was used to mimic the crossing region of the Franklin’s GLC, which seems contradict with Figure 2, where the element brick of the Franklin’s GLC was presented to be graphene sheet.

Response :This is right , the figure 2 caption has been modified to take into account both graphene sheets and Schwarzites for the crossing region

1. What’s the differences or advantages of the modified TPMS models proposed in the manuscript compared with the models proposed by researchers previously, especially Barborini’s 2002 model?

Response :This is the same model. In the Barborini’s model t=0 in Weierstrass equation. In our case t is a positive number  taking into account the large porosity (the thickness). In addition, the TPMS is a simple primitive network in the Barborini’s model , in our case a gyroid.

1. The English grammar and vocabulary of the manuscript need to be checked throughout.

Response :The English will be checked.

Reviewer 2 Report

The paper reviews research on glassy like carbons, including geometry, topology, properties, and applications. The author believes that the possibility to synthesize GLC with well-controlled conditions should allow for future a better possible confrontation of problems. Moreover, Melinon stated that it remains a fascinating study subject with many secrets yet to be discovered. The presentation of methods and scientific results are satisfactory for publication in the Materials journal. The minor and significant drawbacks to be addressed can be specified as follows:
1.    English language needs to be corrected.
2.    Page 1, Fig. 1. This figure is illegible. The main problem is too much text. I propose to introduce coloured inscriptions and sort their importance. The most crucial element of this scheme - GLC - is also lost. Analyzing this scheme, it seems that amorphous carbon is the essential material.
3.    Page 1, Figs. 1 and others, figure captions. Ric. (in Russian) ---> Fig. 1.
4.    I miss a reference to the paper (Suarez-Martinez, I.; Grombert, N.; Ewels, C.P. Nomenclature of sp2 carbon nanoforms. Carbon 2012, 50, 741–747) in the text.
5.    Page 3, Figs. 2 and others. (a) What about the permission? This information is missing in the figure captions. (b) our model --->  the current model.
6.    Page 3, Tab. 1. (a) The author included many numerical values. However, he only provides one reference. What about the rest? (b) Please make the names bold to make the table easier to read.
7.    Page 4, Fig. 3. Why introduce (a) and (b) if they are not used in the description (figure captions)?
8.    Page 7, Fig. 5. "The figures are adapted from the reference [39]" Is this for sure?
9.    There are many annoying errors and inaccuracies, i.e. line 153 - useless space after and lines 157 and 158 - no dot at the end of the sentence and problem with the appearance of the next paragraph., lines 258-260 - text formatting problem. Line 658 - 5.8.2. defect ---> 5.8.2. Defect (see also line 685).
10.    Page 11, line 302. BVK?
11.    Page 16, Fig. 11. Physics ---> physics.
12.    The author, unfortunately, omitted a lot of essential works on gyroid carbonaceous adsorbents (topology, properties, diffusion), i.e. http://dx.doi.org/10.1016/j.carbon.2015.10.042, doi:10.1021/jp511919d, doi: 10.5488/CMP.19.13003, https://doi.org/10.1039/B618747A, Gupta, Sanju, Saxena, Avadh (Eds.), The Role of Topology in Materials, 2018 and chapter 7.
13.    (a) The title needs to be changed. The word "film" is barely used at work,i.e. lines 120, 128, 133, 135, 139, 145, 146, 187, 737 and figure captions (Figs. 4 and 5). (b) What height are these "thin films" supposed to be?

Author Response

The paper reviews research on glassy like carbons, including geometry, topology, properties, and applications. The author believes that the possibility to synthesize GLC with well-controlled conditions should allow for future a better possible confrontation of problems. Moreover, Melinon stated that it remains a fascinating study subject with many secrets yet to be discovered. The presentation of methods and scientific results are satisfactory for publication in the Materials journal. The minor and significant drawbacks to be addressed can be specified as follows:

I would like to thank the reviewer for his/her positive and insightful comments on the manuscript. Below is my response to the issues

Other comments :

- some figures have been revisited for the sake of clarity

-all the modifications in the text are in red

-the revised title is : Vitreous carbon, geometry and topology: a hollistic approach

1. 
      English language needs to be corrected.

Response :The English will be checked.

2. 
      Page 1, Fig. 1. This figure is illegible. The main problem is too much text. I propose to introduce coloured inscriptions and sort their importance. The most crucial element of this scheme - GLC - is also lost. Analyzing this scheme, it seems that amorphous carbon is the essential material.

Response : Figure1 has been revisited

3. 
      Page 1, Figs. 1 and others, figure captions. Ric. (in Russian) ---> Fig. 1.

Response : This is a latex problem with a reference in Russian (see Bukalov 2014). I suppressed  the Russian characters

4.    I miss a reference to the paper (Suarez-Martinez, I.; Grombert, N.; Ewels, C.P. Nomenclature of sp2 carbon nanoforms. Carbon 2012, 50, 741–747) in the text.

Response : The reference has been added

5. 
      Page 3, Figs. 2 and others. (a) What about the permission? This information is missing in the figure captions. (b) our model --->  the current model.

Response : Done, permissions are given. I found that the figure 2 presents striking similaritites with a recent figure published by Shiell (2021). This reference is indicated in the caption.

6. 
      Page 3, Tab. 1. (a) The author included many numerical values. However, he only provides one reference. What about the rest? (b) Please make the names bold to make the table easier to read.

Response : Table 1 has been revisited

7. 
      Page 4, Fig. 3. Why introduce (a) and (b) if they are not used in the description (figure captions)?

Response : a and b  are deleted

8. 
      Page 7, Fig. 5. "The figures are adapted from the reference [39]" Is this for sure?

Response : Some figures are taken from the reference (46) now. It is a piece of my work.

9. 
      There are many annoying errors and inaccuracies, i.e. line 153 - useless space after and lines 157 and 158 - no dot at the end of the sentence and problem with the appearance of the next paragraph., lines 258-260 - text formatting problem. Line 658 - 5.8.2. defect ---> 5.8.2. Defect (see also line 685).

Lines 157-158 “Emergent phenomena in topological physics are probably all around us even in a

Response :  piece of rock" is cited by Castelvecchi. The sentence is separated from the main text and the name of the author is given

Response : lines 258-260 spaces have been added

10. 
       Page 11, line 302. BVK?

Response : BVK see text (Born Von Karman)

11. 
       Page 16, Fig. 11. Physics ---> physics.

Response : Corrected

12. 
       The author, unfortunately, omitted a lot of essential works on gyroid carbonaceous adsorbents (topology, properties, diffusion), i.e. http://dx.doi.org/10.1016/j.carbon.2015.10.042, doi:10.1021/jp511919d, doi: 10.5488/CMP.19.13003, https://doi.org/10.1039/B618747A, Gupta, Sanju, Saxena, Avadh (Eds.), The Role of Topology in Materials, 2018 and chapter 7.
    13.    (a) The title needs to be changed. The word "film" is barely used at work,i.e. lines 120, 128, 133, 135, 139, 145, 146, 187, 737 and figure captions (Figs. 4 and 5). (b) What height are these "thin films" supposed to be?

Response : The references are included with some comments

Response : The terms film, 2D or 3D are explained in the text (see referee 1)

Reviewer 3 Report

The properties of GLC are listed and explained in this review. The characterization, synthesis and geometry of GLC are thoroughly described. In my opinion this work is very interesting and very complete. For these reasons I believe it can be accepted on Nanomaterials

Author Response

The properties of GLC are listed and explained in this review. The characterization, synthesis and geometry of GLC are thoroughly described. In my opinion this work is very interesting and very complete. For these reasons I believe it can be accepted on Nanomaterials

Response: I would like to thank the reviewer for this positive evaluation.

Round 2

Reviewer 2 Report

Congratulations on a great job. The author has made a substantial improvement for this article. The manuscript can be accepted for publishment in the present form.