Preparation of Oxygen Reduction Catalyst Electrodes by Electrochemical Acidification and Synergistic Electrodeposition

Round 1

Reviewer 1 Report

In this work, the authors employed a novel acidification electrodeposition method to prepare a variety of Pt/CP catalysts. The catalysts are well characterized and show good electrocatalytic performance for ORR. However, there are some issues in the manuscript that need further improvement.

1. XRD results are only presented for CP before deposition of Pt. Was XRD performed after the addition of Pt?

2. In Figure 3. it is customary to present XPS spectra with higher B.E. on the left side of the scale (as in Figures S1, S2, and S3). Also, I highly suggest inserting inside Figure 3. the B.E. values and species assigned to every component in the spectra. Additionally, it would be useful for comprehension to move Table 1. below Figure 3.

3. Line 175 and 176. I find it hard to believe that only sp² carbon is present in the spectra. Usually, a mix of sp² and sp³ carbon is observed. Your XRD analysis also indicates a C-C/C=C mix.

4. Text for Figures 3c and 3d (and Figures themselves), should include B.E. values for all three components with references and discuss Pt^δ+, which I assume is the third component in the spectra.

5. Figure 4.  Inserts inside the figures that give the particle size distribution are difficult to read. Either improve their visibility or provide the size distribution as a separate figure.

6. Electrochemical results are variously presented vs SCE and vs. RHE (in the experimental section) reference electrodes. It is customary to present the results vs RHE. All potential values in text, figures, and tables need to be given vs RHE. Also, in the name of the electrodes Pt/CxVyCP, Vy should be given vs RHE.

7. Text should include how Pt_loading was calculated and how ECSA was determined vs Pt weight. It would be useful to give not only the total amount of Pt in mg/cm² but also the Pt Wt% in the electrode as determined by either XPS or EDX.

Author Response

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Reviewer 2 Report

In this work, the authors prepared Pt/C0.5V2.0CP self-supporting electrode by electrochemical acidification and synergistic electrodeposition for efficient and stable ORR. Various characterizations were conducted to demonstrate the performance origins. Some important issues should be solved before acceptance.

1.     The letters of the inner figures in Figure 4 are too small. Further TEM analysis should be conducted for Figure 5d.

2.     In Figure 5a, the Pt peaks obviously shift, which can be ascribed to the structural strain. Please refer to 10.1063/5.0083059 for demonstrating the structural strain of Pt.

3.     The underlying synergetic effects between Pt and C0.5V2.0CP should be further analyzed and demonstrated.

4.     A necessary schematic diagram for the synthesis processes should be presented.

5.     To highlight the important role of PEMFC in hydrogen use and improve the readability of the manuscript, the authors should combine some data in the introduction part. Please refer to 10.1039/D3EE02695G for this point.

Minor editing of English language required

Author Response

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Author Response File: Author Response.docx

Round 2

Reviewer 1 Report

The authors have answered all the issues and have sufficiently improved the manuscript. I recommend to accept it for publication.