The Role of Functionalization in the Applications of Carbon Materials: An Overview
Round 1
Reviewer 1 Report
The paper is dedicated to the modification of the surface chemistry reviewing the different approaches also considering the different macro and nano allotropic forms of carbon. The title must be included overview or review.
The observations for the manuscript are:
In the manuscript there is no information about the mechanisms of functional groups formed by different modifications and functionalization on carbon, in addition the chemistry involved in the different process for modification. There are different techniques, why the author did not include plasma in the review. A description of material properties with the modifications must be described and discussed in the paper , also some applications must me included. A lack of references, specially because there are a lot of works with the emphasis in the Overview on the Surface Functionalization of carbon materials such as nanotubes.
some importants recent references :
1. Nayak L., Rahaman M., Giri R. (2019) Surface Modification/Functionalization of Carbon Materials by Different Techniques: An Overview. In: Rahaman M., Khastgir D., Aldalbahi A. (eds) Carbon-Containing Polymer Composites. Springer (2018) Overview on the Surface Functionalization Mechanism and Determination of Surface Functional Groups of Plasma Treated Carbon Nanotubes, Critical Reviews in Analytical Chemistry, 48:1, 1-14, DOI: 10.1080/10408347.2017.1356699 3. Vijay Kumar Thakur, Manju Kumari Thaku, Chemical Functionalization of Carbon Nanomaterials: Chemistry and Applications, CRC press
1st Edition
4.Kamran, U.; Heo, Y.-J.; Lee, J.W.; Park, S.-J. Functionalized Carbon Materials for Electronic Devices: A Review. Micromachines 2019, 10, 234.
Author Response
Reply to Reviewers’ comments
We thank the reviewers for their careful and thorough reading of the manuscript. Their comments have been very useful for improving the content of the manuscript. All corrections are highlighted in red in the manuscript. The responses to reviewers’ comments are outlined below.
Reviewer 1
The paper is dedicated to the modification of the surface chemistry reviewing the different approaches also considering the different macro and nano allotropic forms of carbon. The title must be included overview or review.
The author thanks the reviewer for the important comment.
To better fit the manuscript content, the original title: “Functionalization of carbon materials” was modified in “Role of the functionalization in the applications of carbon materials: an overview”
In the manuscript there is no information about the mechanisms of functional groups formed by different modifications and functionalization on carbon, in addition the chemistry involved in the different process for modification. There are different techniques, why the author did not include plasma in the review.
There are several works describing the techniques and the processes utilized to functionalize carbon nanomaterials. This work aims at a looking this topic from a different perspective: the work focuses on the most important application areas and shows why functionalization of the carbon material surface is needed. The use of plasma was mentioned in the original version of the manuscript to treat CNT, diamond for treatment and production, to treat carbon fibers, to functionalize graphene. However, as the reviewer suggests, it deserves more detailed description and parts regarding the plasma treatment were expanded along the manuscript (plasma is now described mode in details for functionalizing diamond section 2.1.4, graphite and graphene section 2.2.1, porous carbon, carbon fibers 2.2.2, CNT 2.2.3 and included in section 2.3.1)
A description of material properties with the modifications must be described and discussed in the paper , also some applications must be included. A lack of references, specially because there are a lot of works with the emphasis in the Overview on the Surface Functionalization of carbon materials such as nanotubes.
Some importants recent references :
Nayak L., Rahaman M., Giri R. (2019) Surface Modification/Functionalization of Carbon Materials by Different Techniques: An Overview. In: Rahaman M., Khastgir D., Aldalbahi A. (eds) Carbon-Containing Polymer Composites. Springer Cafer Saka(2018) Overview on the Surface Functionalization Mechanism and Determination of Surface Functional Groups of Plasma Treated Carbon Nanotubes, Critical Reviews in Analytical Chemistry, 48:1, 1-14, DOI: 10.1080/10408347.2017.1356699 Vijay Kumar Thakur, Manju Kumari Thaku, Chemical Functionalization of Carbon Nanomaterials: Chemistry and Applications, CRC press, 1st Edition Kamran, U.; Heo, Y.-J.; Lee, J.W.; Park, S.-J. Functionalized Carbon Materials for Electronic Devices: A Review. Micromachines 2019, 10, 234.
The author thanks the reviewer for the important references which are added in the manuscript and some of them are now cited more times along the manuscript.
Author Response File: 
Author Response.docx
Reviewer 2 Report
The author reports a review dedicated to the modification of carbon based materials (graphene, carbon nanotubes, carbon fibers, and nanodiamond) that could be applied for specific applications. In my opinion, in its current form, this review cannot be accepted for publication in the Journal of Carbon Research. The manuscript is riddled with errors; it is full of grammar and spelling errors. The report is difficult to read, badly written, poorly organized and some images lack clarity. The author starts with the Introduction section, and then continues with 2.1 Subsection, but the title of 2.Section is absent in the manuscript. This section (Section 2) should be divided by Subsubsections to facilitate the reading of the review. Each Subsubsection may include one type of material rather than all materials being included in a very large Subsection.
Author Response
Reply to Reviewers’ comments
We thank the reviewers for their careful and thorough reading of the manuscript. Their comments have been very useful for improving the content of the manuscript. All corrections are highlighted in red in the manuscript. The responses to reviewers’ comments are outlined below.
Reviewer 2
The author reports a review dedicated to the modification of carbon based materials (graphene, carbon nanotubes, carbon fibers, and nanodiamond) that could be applied for specific applications. In my opinion, in its current form, this review cannot be accepted for publication in the Journal of Carbon Research. The manuscript is riddled with errors; it is full of grammar and spelling errors. The report is difficult to read, badly written, poorly organized and some images lack clarity. The author starts with the Introduction section, and then continues with 2.1 Subsection, but the title of 2.Section is absent in the manuscript. This section (Section 2) should be divided by Subsubsections to facilitate the reading of the review. Each Subsubsection may include one type of material rather than all materials being included in a very large Subsection.
The author thanks the reviewer for highlighting the weakness of the manuscript. Title of the section 2 is added. The manuscript was carefully controlled and errors corrected. The article was reorganized in subsections as suggested and more information added where they were lacking.
Reviewer 3 Report
This is a useful review of the functionalization carbon materials including nanotubes, graphene, carbon dots and nano-diamond. I am happy for the paper to be published in essentially its present form, if the following comments are taken into account. I do not need to see the paper again.
The subject of porous carbon is introduced very briefly on p.2. The author should distinguish between the different forms of porous carbon, e.g. activated carbons and glassy carbon. Glassy carbon rather than “porous carbon” is the kind of carbon chiefly used in electrochemistry. He should also say something about the structure of these carbons, and mention recent ideas that they may have a fullerene-like structure. See, for example:
Harris, P.J.F. Fullerene-like models for microporous carbon. J. Mater. Sci. 2013, 48, 565–577.
Other articles which might be cited:
On carbon surface chemistry:
Burg, P., Cagniant, D. Characterization of carbon surface chemistry. Chemistry and Physics of Carbon 2008, 30, 129-175.
On sensing:
Qureshi, A. et al. Review on carbon-derived, solid-state, micro and nano sensors for electrochemical sensing applications. Diamond and Related Materials 2009, 18, 1401-1420.
Lin, Z., Wu, G. et al. Carbon nanomaterial-based biosensors A review of design and applications. IEEE Nanotechnology Magazine 2019, 13, 4-14.
On nanodiamonds:
Lai, H., Stenzel, M. H., Xiao, P. Surface engineering and applications of nanodiamonds in cancer treatment and imaging. International Materials Reviews, published online 26 Jun 2019.
On carbon dots:
Chatzimitakos, T.; Stalikas, C. Recent advances in carbon dots. C-Journal Of Carbon Research 2019, 5, 41.
On line 44 he says “in the seventies were identified novel forms of carbon …” but then discusses developments from the 1950s to the 1980s. The reference to the seventies should be changed.
The caption for Figure 2 is incorrectly formatted. It runs into the main text.
There are numerous typos and examples of poor English:
Line 11: “carbon atoms can from” should be “carbon atoms can form”
Line 39: “perpendicular this plane” should be “perpendicular to this plane”
Line 40: “week” should be “weak”
Lines 109, 369 and 518: “scarce” should be “low”
Line 118: “hydrophibic” should be “hydrophobic”
Line 127: “mononalyers” should be “monolayers”
Line 207: “vase” should be “vast”
Lines 210 and 477: “exagons” should be “hexagons”
Line 269: “recongize” should be “recognize”
Line 293: “hybrized” should be “hybridized”
Line 312: “anhydries” should be “anhydrides” (I assume)
Line 322: “hydrobobic” should be “hydrophobic” (I assume)
Line 329: “denaturated” should be “denatured”
Line 538: “sensibility” should be “sensitivity”
Line 573: “impedence” should be “impedance”
Line 706: “dispersable” should be “dispersible”
Line 707: “utililzed” should be “utilized”
There are some instances of repetition, e.g.:
Line 189: “There are also wet chemical procedures to functionalize CNTs. In this case are commonly used acids which induce formation of oxygen based functional groups and defects [84], [85] thus making the CNT soluble.”
Line 533: “Oxidation is the more common covalent functionalization of CNT and graphene. Oxygen functional groups are obtained on the carbon nanostructures using strong acid treatments in nitric acid and the mixture of nitric acid and sulfuric acid”
On p.7, the paragraph beginning “Another popular reaction is…..“ is repeated.
This repetition should be removed.
Finally, the references are not in the correct format for C – see Instructions for Authors.
Author Response
Reply to Reviewers’ comments
We thank the reviewers for their careful and thorough reading of the manuscript. Their comments have been very useful for improving the content of the manuscript. All corrections are highlighted in red in the manuscript. The responses to reviewers’ comments are outlined below.
Reviewer 3
This is a useful review of the functionalization carbon materials including nanotubes, graphene, carbon dots and nano-diamond. I am happy for the paper to be published in essentially its present form, if the following comments are taken into account. I do not need to see the paper again.
The subject of porous carbon is introduced very briefly on p.2. The author should distinguish between the different forms of porous carbon, e.g. activated carbons and glassy carbon. Glassy carbon rather than “porous carbon” is the kind of carbon chiefly used in electrochemistry. He should also say something about the structure of these carbons, and mention recent ideas that they may have a fullerene-like structure. See, for example:
Harris, P.J.F. Fullerene-like models for microporous carbon. J. Mater. Sci. 2013, 48, 565–577.
The author thanks the reviewer for the important suggestion. A description of glassy and porous carbons is inserted now at beginning of the section 2.2.2 Porous carbon…
Examples of applications of glassy carbons and new references are inserted in the manuscript.
Concerning the use of glassy and porous carbon, here chemical processes are referred to a vast class of different processes not only catalysis but also electrochemistry which includes biosensing, fuel cells, batteries and supercaps which are reviewed in this work. In these applications an improvement of the electrode performances is obtained by increasing the specific surface thus enhancing the efficiency of the charge transfer (although porous carbon has a lower conductivity than glassy carbon). This is why the author utilized the term “porous carbon” which is referred to the disordered class of carbon materials including the glassy carbon as its commonly done also in literature.
Other articles which might be cited:
On carbon surface chemistry:
Burg, P., Cagniant, D. Characterization of carbon surface chemistry. Chemistry and Physics of Carbon 2008, 30, 129-175.
On sensing:
Qureshi, A. et al. Review on carbon-derived, solid-state, micro and nano sensors for electrochemical sensing applications. Diamond and Related Materials 2009, 18, 1401-1420.
Lin, Z., Wu, G. et al. Carbon nanomaterial-based biosensors A review of design and applications. IEEE Nanotechnology Magazine 2019, 13, 4-14.
On nanodiamonds:
Lai, H., Stenzel, M. H., Xiao, P. Surface engineering and applications of nanodiamonds in cancer treatment and imaging. International Materials Reviews, published online 26 Jun 2019.
On carbon dots:
Chatzimitakos, T.; Stalikas, C. Recent advances in carbon dots. C-Journal Of Carbon Research 2019, 5, 41.
The author thanks again the reviewer for the useful indications. All the suggested references are added to the manuscript.
On line 44 he says “in the seventies were identified novel forms of carbon …” but then discusses developments from the 1950s to the 1980s. The reference to the seventies should be changed.
The caption for Figure 2 is incorrectly formatted. It runs into the main text.
There are numerous typos and examples of poor English:
Line 11: “carbon atoms can from” should be “carbon atoms can form”
Line 39: “perpendicular this plane” should be “perpendicular to this plane”
Line 40: “week” should be “weak”
Lines 109, 369 and 518: “scarce” should be “low”
Line 118: “hydrophibic” should be “hydrophobic”
Line 127: “mononalyers” should be “monolayers”
Line 207: “vase” should be “vast”
Lines 210 and 477: “exagons” should be “hexagons”
Line 269: “recongize” should be “recognize”
Line 293: “hybrized” should be “hybridized”
Line 312: “anhydries” should be “anhydrides” (I assume)
Line 322: “hydrobobic” should be “hydrophobic” (I assume)
Line 329: “denaturated” should be “denatured”
Line 538: “sensibility” should be “sensitivity”
Line 573: “impedence” should be “impedance”
Line 706: “dispersable” should be “dispersible”
Line 707: “utililzed” should be “utilized”
Corrections are inserted in the text
There are some instances of repetition, e.g.:
Line 189: “There are also wet chemical procedures to functionalize CNTs. In this case are commonly used acids which induce formation of oxygen based functional groups and defects [84], [85] thus making the CNT soluble.”
Line 533: “Oxidation is the more common covalent functionalization of CNT and graphene. Oxygen functional groups are obtained on the carbon nanostructures using strong acid treatments in nitric acid and the mixture of nitric acid and sulfuric acid”
On p.7, the paragraph beginning “Another popular reaction is…..“ is repeated.
This repetition should be removed.
The author thanks the reviewer, repetitions are removed.
Finally, the references are not in the correct format for C – see Instructions for Authors.
References are now in the C-style.
Author Response File: Author Response.docx
Round 2
Reviewer 1 Report
the authors attended all the observations and suggestions
Reviewer 2 Report
In the revised manuscript, the author has addressed all questions from my previous review in a satisfactory way.
