Nanocomposite Materials Based on Electrochemically Synthesized Graphene Polymers: Molecular Architecture Strategies for Sensor Applications

Round 1

Reviewer 1 Report

The authors André Olean-Oliveira et al in here present a review article of Nanocomposite materials based on electrochemically synthesized graphene polymers: molecular architecture strategies for sensor and biosensor applications. In view of the use of graphene and its derivatives in the development of electrochemical sensors has been growing in recent decades, this topic may attract many readers. And the paper presents the main aspects for the construction of nanomaterials based on graphene oxide and conducting polymers, as well as the recent efforts made to apply this methodology in the development of sensors and biosensors which fill in the knowledge gap of this field. I recommend to publish it after very careful revision.

1. Compared to preciously published papers such as Liang, Yaru, et al. "Nanocomposite materials for the sodium–ion battery: a review." Small14.5 (2018): 1702514.; Nandihalli, Nagaraj, Chia-Jyi Liu, and Takao Mori. "Polymer based thermoelectric nanocomposite materials and devices: Fabrication and characteristics." Nano Energy(2020): 105186.; Fathi, Mohammed Shaalan Abed. "Mechanical Properties of Nanocomposite Materials: A Review." Journal of Southwest Jiaotong University 55.1 (2020).; Lalmalsawmi, Jongte, Diwakar Tiwari, and Dong Jin Kim. "Role of nanocomposite materials in the development of electrochemical sensors for arsenic: Past, present and future." Journal of Electroanalytical Chemistry (2020): 114630., the principle and innovation of this paper should be explained more in details.

2.In figure 1, the structure of Epoxide is recommended to re-paint by Chemdraw ？

3. In the conclusion part, more discussion in details is recommended to add.
4. There are many abbreviations in use. Please show the full names before use them
   5. There are some grammar errors which should be revised carefully.

Author Response

Point 1) Compared to preciously published papers such as Liang, Yaru, et al. "Nanocomposite materials for the sodium–ion battery: a review." Small14.5 (2018): 1702514.; Nandihalli, Nagaraj, Chia-Jyi Liu, and Takao Mori. "Polymer based thermoelectric nanocomposite materials and devices: Fabrication and characteristics." Nano Energy(2020): 105186.; Fathi, Mohammed Shaalan Abed. "Mechanical Properties of Nanocomposite Materials: A Review." Journal of Southwest Jiaotong University 55.1 (2020).; Lalmalsawmi, Jongte, Diwakar Tiwari, and Dong Jin Kim. "Role of nanocomposite materials in the development of electrochemical sensors for arsenic: Past, present and future." Journal of Electroanalytical Chemistry (2020): 114630., the principle and innovation of this paper should be explained more in details.

Response: Dear reviewer, we appreciate your comments. In relation to these articles, none of them specifically mentions the electrochemical synthesis route by reach in polymer-graphene nanocomposite films. Although their titles indicate an approach close to the subject of our review, the suggested articles do not use electrochemistry as a synthesis of the device.

In detail, the first one talks about nanocomposite, but not directed to graphene derivatives, neither synthesis by electrochemical routes. In fact, the authors dealt with nanocomposite only to refer to the set of two or more elements that make up the material used as energy storage devices. The second has the main aim using polymers for thermoelectric applications, diverging from our goal, which would be specifically derived from electrosynthesized graphene-polymer with an emphasis on sensory applications. The third has depth about carbon-based materials, but towards composition, again diverging from our goal. Finally, the fourth work focuses on sensory application, however, it does not have a specific focus on a specific category of nanomaterial, nor on electrochemical synthesis. Thus, the authors would like to reinforce, as described in the body of the text, that the innovation of the present revision work is seen for the electrochemical synthesis of materials based on graphene-polymer, since the literature offers a minimum volume of works addressed for this purpose.

Point 2) In figure 1, the structure of Epoxide is recommended to re-paint by Chemdraw.

Response: Ok, it was done.

Point 3) In the conclusion part, more discussion in details is recommended to add.

Response: OK, it was done.

Ponit 4) There are many abbreviations in use. Please show the full names before use them.

 Response: Ok, it was done.

Point 5) There are some grammar errors which should be revised carefully.

Response: The paper was appropriately revised before submission, please check the certificated attached with cover letter.

 

Reviewer 2 Report

Comments attached.

Comments for author File: Comments.pdf

Author Response

Pont 1) The addition of a separate section for advantages of electrochemical fabrication of nanocomposites compared to the chemical route can be more convenient for the readers.

Response: The comment is pertinent, we appreciate the concern of the contribution made by the referee, however the authors understand that the aim of this work is to contribute on the theme to expand the possibilities of alternative routes for the synthesis of nanomaterials, not necessarily to carry out a ranking or to overcome other already existing synthesis strategies.

Point 2) The mechanism of graphene-conducting polymers formation via electrochemical routes can discuss in a separate section.

Response: It was done during section 3. We had explained the general mechanism of graphene due it is the focus of the paper and the special section. But, due to the particular strategy of electrosynthesis of nanocomposites, we decided to group them in two different sections: multiple-step and one-step. 

Point 3) This review articles addressing both sensor and biosensors applications. However, the biosensor sections not discussed well. Hence, individual discussion of such topics would be more beneficial.

Response: The theme "biosensor" has been replaced by a general theme for electrochemical sensors.

Point 4) Conducting polymer composites with graphene for use in chemical sensors and biosensors (Microchim Acta (2014) 181:707 722); Nanomaterial-doped conducting polymers for electrochemical sensors and biosensors (J. Mater. Chem. B, 2018,6, 4173-4190) - How does this review article is advantages/benefits than the above-reported review articles?

Response: Indeed, the cited works meet the objective of the proposed work. In response, the first benefit would be to update the works verified in the proposed theme, since the works contained in them are before 2014 and 2018. Also, the addressing of our work to the electrochemical synthesis form, especially those using graphene oxide. Although the works have sections dedicated to the theme, they do not address the subject as the main objective. Finally, our review extends the discussion about the characteristics and electrodeposition properties of graphene, with the polymer attached to it as an adjuvant. Based on the number of citations of the articles cited, the authors reiterate the importance of the topic for the publication of this review.

Point 5) The conclusion can be addressing the advantages of this review article for future developments. 

Response: OK

Point 6) Future perspectives are essential in review articles that can give future ideas/innovation to the readers for further development in this research area.

Response: It was done.

 

 

Reviewer 3 Report

Summary

The authors report a collection of articles describing the use of graphene for the modification of working electrodes to improve the electrochemical performances, its electrochemical synthesis pathways, its coupling with conductive polymers and some applications in the detection of different kind of analytes. The work is interesting, the introduction is well written and the basis of the research is well discussed.

However, there are some aspects of the work that needs to be addressed before accepting the manuscript, especially from the point of view of the text layout.

General comments

The authors state that the nanocomposites containing graphene and conducting polymers were applied in the development of sensors and biosensors. However, in my opinion, what is really missing is a comprehensive discussion on the reported papers. Why did the authors choose to discuss only some of them? As far as I have seen from the bibliography, the authors report only one biosensing approch without even discussing it. Moreover, it seems that in references 104, 108 and 109, the polymer is mainly used as a biomimetic receptor. In this sense, I would suggest to extend the comments of the presented approaches and clarify the role of the polymer in the detection.

Specific comments

• As a suggestion, please note that adding line numbers in the manuscript usually speeds up the revision process
• Affiliations 1 and 3 are missing some authors' initials
• There are many formatting mistakes in the text font, please correct them
• A) and B) indications in Figure 6 are missing, A) in Figure 7, B) in Figure 8, A) and B) in Figure 9, 
• Please homogenize the units throughout the manuscript
• Pay attention to superscripts/subscripts
• L should be capitalized for liters

Authors may find additional comments in the attached pdf file

Comments for author File: Comments.pdf

Author Response

Point 1) General comments
The authors state that the nanocomposites containing graphene and conducting polymers were applied in the development of sensors and biosensors. However, in my opinion, what is really missing is a comprehensive discussion on the reported papers. Why did the authors choose to discuss only some of them? As far as I have seen from the bibliography, the authors report only one biosensing approach without even discussing it. Moreover, it seems that in references 104, 108 and 109, the polymer is mainly used as a biomimetic receptor. In this sense, I would suggest extending the comments of the presented approaches and clarify the role of the polymer in the detection.

Response: We made the requested modification.

Point 2) Specific comments

• As a suggestion, please note that adding line numbers in the manuscript usually speeds up the revision process
• Affiliations 1 and 3 are missing some authors' initials OK
• There are many formatting mistakes in the text font, please correct them OK
• A) and B) indications in Figure 6 are missing, A) in Figure 7, B) in Figure 8, A) and B) in Figure 9, OK
• Please homogenize the units throughout the manuscript OK
• Pay attention to superscripts/subscripts OK
• L should be capitalized for liters OK

Authors may find additional comments in the attached pdf file OK

Response: All those suggestions were done.