Graphene: Chemistry and Applications for Lithium-Ion Batteries

Round 1

Reviewer 1 Report

In this manuscript, the authors aim to give a brief review of the domination of graphene and its applications in lithium-ion batteries. It has been shown how graphene enhances the rate capability, performance and how it reduces the shutter effects in lithium-ion batteries. Optimistically it is not far away when the effective application of graphene-based anode in rechargeable batteries will be treated as an innovation in battery performance. For practical applications of bare graphene further reduction of discharge and charge voltages are needed.

I consider the content of this manuscript will definitely meet the reading interests of the readers of the Electrochem journal. However, the discussion is still slightly monotonous. This paper could be a comprehensive work after revision.

Therefore, I suggest giving a minor revision and the authors need to clarify some issues or supply some more data to enrich the content. In particular, the authors should pay special attention to the grammar errors. I will point out some of them, but not all of them.

1. Abstract and Introduction

• Just starting from the Abstract, the grammar errors are obvious. For example, it should be ‘In the present era’, ‘It is considered as...’, ‘... it is predominantly applied in electronic devices’. And the final sentence of the abstract, ‘In this review, we target to give a brief review of the domination of graphene and its applications in lithium-ion batteries.’ I suggest the authors double-check the grammar issues throughout the whole manuscript.

 

• Line 42, ‘Carbon is a significant component used in electrochemical applications such as batteries, supercapacitors, photoelectrochemical water splitting, solar cells, fuel cells...’For redox flow cells designed for large-scale energy storage, carbon-based electrodes are also very important components [Electrochimica Acta 336 (2020): 135646; International Journal of Energy Research 44.5 (2020): 3839-3853]. This device is suggested to be mentioned as well.

 

• Line 44, ‘Initially, the battery research was focused on positive and negative electrodes. The research on the negative electrodes was based on Li metal and lithium alloys [1–3].’ 

This sentence should be stressed first, for lithium-ion batteries, ‘the battery research focused on electrodes, and negative electrode was mainly based on Li metal/alloys.’ As before the lithium battery, there is also other batteries, such as a lead-acid battery. Initially, the battery research is not for electrodes based on Li at all.

And for a review paper, the first reference that appears from here is not suitable. For the previously mentioned sentences, there should also be certain references about carbon materials and their applications.

 

• Line 69, ‘Currently, the carbon allotrope database offers several carbon allotropes, and graphite leads a fanciful role in both the industry and research fields [8].’ 

    What is the carbon allotrope database? A (represents carbon allotrope) database offers several A, seems meaningless, and this sentence should be revised somehow to clarify everything.

 

• Line 108, ‘For a better understanding of the development of graphene, the time scale of its evolution is summarized in the Figure. 3’.

 

2. Graphene; Properties and synthesis

 

• Line 194, ‘The very first method which used to isolate one mono-layer graphene... Hence this method is widely known as Scotch tape or the Peel-off method [23]. ’

 

• Line 202, ‘Chemical exfoliation: It is referred to as the finest method. In this method, in which graphene is produced from bulk graphite and graphite intercalation compounds.’

 

• Line 228, ‘however, there are significant expenses and moderately low yields. On the other hand, this methodology has an extraordinary potential that can be added for the additional improvement.’

 

3. Lithium-ion battery-A brief overview

 

• Line 248, ‘... the application levels are extended to more different fields including defense, aerospace and automobile industries and renewable energy integration. The performance of LIBs greatly depends on physicochemical properties of both anodes and cathodes.’

 

• This brief overview is too short, and it should be expanded a bit. In particular, technology has advantages and disadvantages. All the descriptions here seem this technique to have a bright future. However, it must be noted that it does not tolerate over-discharge, overcharging, having ageing issues and overheating should be avoided. There may be flammable and explosive risks. Such shortcomings should not be completely ignored.

There are also different types of lithium batteries that should be briefly introduced, such as "LiNiO₂" (nickel lithium battery), "LiNi_0.8Co_0.2O₂" (nickel cobalt lithium battery), "LiMn₂O₄" (manganese lithium battery), "LiNi_0.3Co_0.3Mn_0.3O₂" (ternary battery), and Lithium iron phosphate (LFP) battery.

 

4. Graphene as components in lithium-ion batteries

 

• Line 442, ‘with a capacity retention of 102, 2.38 and 2.98%, respectively [43].’ Please double-check this result, especially capacity retention of 102% is true or not.

 

• Line 638,‘For instance, Lee et al. [46] Si nanoparticles incorporated graphene sheet (Si/GS) has been synthesized by sandwiching conductive 3D graphite network with well-dispersed Si nanoparticles inside the graphene layers. ’ Here, ‘Lee et al.’ and ‘Si nanoparticles... has been synthesized’ seems two independent sentences, and should be merged together or described independently but with complete sentences.

 

• Line 734,‘Even though sulfur, nitrogen and boron have been reported as dopants in graphene-based anodes, in the case of cathodes... Nitrogen-doped GNS was synthesized by the hydrothermal method by mixing the GO with urea...’

 

• Line 770, ‘The presence of an oxygenated functional group on the rGO surface adheres to the nano MoS3 particles on its surface ensuring the synergistic effect of both the components.'

   

 

Author Response

We thank to referee for the valuable suggestions. We have carefully checked the whole manuscript and comprehensively edited. Now the language and the quality of the manuscript is improved significantly in our level best. The abstract also has been affected necessary changes to avoid the suggested mistakes

Line 42, has been edited. A separate sentence was added regarding redox flow batteries and necessary the references has been incorporated.

Line 44, was edited carefully and necessary changes are affected as per the reviewer’s suggestion.

Line 69, was corrected as per the reviewer’s suggestion as ‘Current scenario, wide variety of carbon allotropes has been discovered and studied among which graphite leads a fantastic role in both the industry and research field [8].’

Line 108, was edited to ‘For a better understanding of the development of graphene, the time line of its evolution is summarized in the Figure. 3.’

We thank the referee for the suggestion.  We have carefully checked the whole manuscript and comprehensively edited. We have corrected all the mistakes noted in the manuscript and necessary changes are affected in the revised manuscript.

We thank the referee for the suggestion.  We have carefully checked the whole manuscript and comprehensively edited. We have corrected all the mistakes noted in the manuscript and necessary changes are affected in the revised manuscript.

Thank you for the valued comments. As per the reviewer suggestion the line 442 is modified and edited for more clarification.

‘The cycling was extended up to 200 cycles at a current density of 0.5 A g⁻¹, where N-GRs/MoS₂, N-GNs/MoS₂, and pristine MoS₂ anodes delivered a discharge capacity of 925, 389, and 311 mAh g⁻¹ respectively, wherein N-GRs/MoS₂ displayed a capacity retention of 102%, which is 2.38 and 2.98 % higher than that of N-GNs/MoS₂ and pristine MoS₂ respectively [43].’

 

Line 638 was recorrected “Lee et al. [46] reported Si nanoparticles

Author Response File: Author Response.pdf

Reviewer 2 Report

Pay Attention to Title Subscripts Spelling Mistakes in References, e.g., the reference 2, 11, 28, 40, 41, 42, 43, 45, 47, 48, 52, 53, 55, 56, 57, 58, 59, 60, 61, 68, 69, 70, 71, 72, 73, 74, 75, 76, 77, 78, 79, 90, 92, 102, 103, and 104.

Author Response

We thank the referee for the valuable suggestions. We have carefully checked the whole manuscript and references. The necessary corrections and modifications are affected in the revised manuscript.

Author Response File: Author Response.pdf

Reviewer 3 Report

The authors highlight the history and present the current literature on the application of graphene in batteries. The authors have presented a good overview of batteries' fabrication techniques and cell performance with graphene and its various derivatives in electrodes. 

The only comment I have for the authors is if they could comment on the usage of graphene (especially rGO) as a current collector. This is another area of research to reduce the size of the current collectors to decrease the mass of a cell.

There are some typos in the manuscript that the authors could easily address:

• Figure 3: The spelling of graphene is incorrect
• Line 217: typo: from 't'
• Line 335: revealed (typo)
• Line 553: at a current of 10 (the units are missing)

Author Response

We thank the referee for the valuable suggestions.

The suggested changes have been incorporated in the revised manuscript.

Line 553 corrected to ‘at a current density of 100 mA g^-1’

Author Response File: Author Response.pdf