Synthesis and Application of P(EDOT-co-Py)@MWCNT Hybrid as Cathode Electrode for Aqueous Aluminum-Ion Batteries

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

This study utilized EDOT and Py as monomers to synthesize multi-carbon nanotube materials. Characterization was performed via FT-IR, XRD, DSC and other methods. The design was well-conceived and experimental data were thoroughly documented. The developed P(EDOT-co-Py)@MWCNT hybrid material demonstrated outstanding electrochemical performance. Therefore, it has the potential to be published in this journal, provided that the following minor issues can be addressed to enhance the manuscript. The recommendations are listed below.

1. Section 3.2 provides detailed numerical comparisons of the material's performance against other materials in the literature. However, these comparisons are currently presented solely in textual form and as a table (Table S7). It is recommended that a performance comparison graph be added to highlight the material's advantages in terms of performance.
2. The paper indicates a capacity retention rate of 72% after 60 cycles and mentions that the coulombic efficiency approaches 100% following initial activation. This indicates favorable reversibility during cycling; however, the cause of capacity decay remains unexplored. It is recommended to perform SEM/TEM characterization of the cycled electrode material to observe any morphological or structural changes, supplemented by an in-depth analysis of the decay mechanism.
3. Figure 7 employs Nyquist plots and Bode plots to analyze impedance changes; please supplement with the corresponding equivalent circuit model.
4. “Figure 7. P(EDOT-co-Py)@MWCNT hybrid (A,B) Nyquist and (B) Bode plot. (C) Cycling stability and coulombic efficiency at 0.1 A g^-1.” Please verify this figure caption, as Figure 7D is missing.
5. It is recommended that the authors illustrate the storage and release mechanisms of each functional group in P(EDOT-co-Py)@MWCNT within aluminum-ion batteries, thereby enabling readers to gain a clearer understanding of the microscopic charge-discharge processes.

Author Response

 First, we would like to thank the reviewer for the valuable comments on the submitted manuscript. We have addressed all the points raised by the reviewer and hope that the revised version of the manuscript is now suitable for publication in Nanoenergy Advances. We took the liberty of correcting a translation error related to the hybrids: we initially used the acronym ATC, referring to trichloroacetic acid; however, the correct acronym in English is TCA. This change was applied throughout the entire manuscript, as well as in the supplementary material, figures, and their respective captions. We also made several minor corrections to improve our English writing.

The responses to the comments raised by Reviewer 1 are in the PDF file.

Author Response File: Author Response.pdf

Reviewer 2 Report

Comments and Suggestions for Authors

The authors proposed a synthesis of a material composed of a copolymer of 3,4-ethylenedioxythiophene and pyrrole anchored onto multi-walled carbon nanotubes via a multistep functionalization strategy, intended for use as an electrode material for aqueous aluminum-ion battery. According to the authors, spectroscopic, thermal, and microscopic analyses confirmed the successful functionalization, monomer anchoring, copolymer formation, and the presence of a homogeneous polymer coating without compromising the structural integrity of the nanotubes.

Furthermore, from the evaluation of electrochemical performances the authors observed that the material exhibits dual charge-storage mechanisms dependent on the applied current density.

The manuscript is generally well-written and presented in a clear and concise academic style. The structure is generally coherent, and the discussion is balanced and appropriately contextualized within the existing literature. The figures are clear and informative, although minor improvements could further enhance their readability. Minor revisions are required to improve clarity and presentation. I recommend acceptance of the manuscript after the following minor revisions:

1. Please verify the placement of some literature citations within the text.

2. In Scheme 1, a legend or nomenclature should be added for the molecules represented in 3D, clearly specifying, for instance, whether the species shown corresponds to HNO₃, for example, or other reagents.

3. Please, correct the errors in the captions of Figures 7A–7D and their corresponding citations in the text, particularly with regard to Figures 7B and 7C. Specifically, Figure 7C corresponds to the Bode plot, whereas Figure 7D illustrates specific capacity retention and coulombic efficiency.

4. Please include in the main text an explanatory note to equations (1)–(4), explicitly indicating the assumptions considered. For example, coulombic efficiency is defined in the manuscript as the ratio of discharge time to charge time, expressed as a percentage, rather than as the ratio of discharged charge to charged input during the charging process, explain the reason. Additionally, in hybrid systems, energy and specific capacity may include both faradaic and non-faradaic contributions. The authors should clarify whether and how these contributions are distinguished or combined in the calculations.

Author Response

First, we would like to thank the reviewer for the valuable comments on the submitted manuscript. We have addressed all the points raised by the reviewer and hope that the revised version of the manuscript is now suitable for publication in Nanoenergy Advances. We took the liberty of correcting a translation error related to the hybrids: we initially used the acronym ATC, referring to trichloroacetic acid; however, the correct acronym in English is TCA. This change was applied throughout the entire manuscript, as well as in the supplementary material, figures, and their respective captions. We also made several minor corrections to improve our English writing.

The responses to the comments raised by Reviewer 2 are in the PDF file.

Author Response File: Author Response.pdf

Round 2

Reviewer 1 Report

Comments and Suggestions for Authors

The authors have carefully and thoroughly revised the manuscript, addressing all previous concerns. I am pleased to recommend acceptance for publication.

Reviewer 2 Report

Comments and Suggestions for Authors

The authors have addressed all the comments and concerns effectively and the quality of the paper has improved. Therefore, the reviewer recommends the manuscript for acceptance in its current form.