Electrochemical Deposition of Hydroxyapatite on Stainless Steel Coated with Tantalum/Tantalum Nitride Using Simulated Body Fluid as an Electrolytic Medium

Round 1

Reviewer 1 Report

The paper ”Electrochemical Deposition of Hydroxyapatite on Stainless Steel Coated with Tantalum /Tantalum Nitride Using Simulated Body Fluid as Electrolytic Medium” is suitable for publication after some minor revision.

The authors should update and rephrase the introduction section with more references regarding electrochemical determinations/values obtained by other authors in the Tantalum /Tantalum Nitride coating field. 

Please present the reference for  BIOLINE stainless steel SS316LVM.

For X-ray diffraction please insert the step size of the determination.

Please improve the quality of figure 5. The microstructure is not very clear.

Also, it will be interesting if you could present the degradation rate of the uncoated and the coated sample.

Author Response

The paper ”Electrochemical Deposition of Hydroxyapatite on Stainless Steel Coated with Tantalum /Tantalum Nitride Using Simulated Body Fluid as Electrolytic Medium” is suitable for publication after some minor revision.

The authors should update and rephrase the introduction section with more references regarding electrochemical determinations/values obtained by other authors in the Tantalum /Tantalum Nitride coating field. 

• The introduction was updated. We expand the introduction on electrochemical deposition carried out on Ti, Ti alloys, steel. However there are not reports on electrochemical deposition of Hap on Ta or TaN.

 

Please present the reference for  BIOLINE stainless steel SS316LVM.

• This reference was incorporated in the manuscrpt in the materials and methods section

For X-ray diffraction please insert the step size of the determination.

• This was added to the XRD description in the materials and methods section

Please improve the quality of figure 5. The microstructure is not very clear.

• The quality of figure 5 was improved

Also, it will be interesting if you could present the degradation rate of the uncoated and the coated sample.

Unfortunately, the complete degradation rate experiments could not be carried out due to restrictions to attend in person to the lab during this period due to the covid pandemia restrictions that are still going on at our university.

Reviewer 2 Report

Please see attached file

Comments for author File: Comments.pdf

Author Response

The manuscript was improved with the other reviewers comments. Thanks very much for your review

Reviewer 3 Report

The entitled manuscript “Electrochemical Deposition of Hydroxyapatite on Stainless Steel Coated with Tantalum/Tantalum Nitride Using Simulated Body Fluid as Electrolytic Medium” introduced a novel method using the electrochemical deposition of hydroxyapatite using simulated body fluid (SBF) as electrolytic medium was carried out on Ta and Ta/TaN coatings on BIOLINE stainless steel SS316LVM (SS). From the results, this method is a reliable, fast, and accurate measurement, which is useful to the textile area. It’s recommended to be considered after major revision. Comments as follows:

1) The abstract should be extended. Please included more results from the author’s research, for instance, please briefly introduce the new method you proposed. After reading the abstract, I have not got your point.
2) The introduction also should be extended. Here are several papers strongly related to your manuscript. Authors may consider quoting. a) Effects of Chitin Nanocrystals on Coverage of Coating Layers and Water Retention of Coating Color; b) Synthesis of lignin-poly(N-methylaniline)-reduced graphene oxide hydrogel for organic dye and lead ions removal; c) Synthesis and Application of Granular Activated Carbon from Biomass Waste Materials for Water Treatment: A Review.
3) The quality of the figures should be significantly improved.
4) It’s recommended to show the contact angle images, which are presented in Table 3.
5) Some of the reference style is not fit to the requirement of the journal.
6) Please do more comparison in the Results and Discussion section, and extend the conclusion part. Please extend, since I have not got the significance of the author’s new method.

Author Response

The entitled manuscript “Electrochemical Deposition of Hydroxyapatite on Stainless Steel Coated with Tantalum/Tantalum Nitride Using Simulated Body Fluid as Electrolytic Medium” introduced a novel method using the electrochemical deposition of hydroxyapatite using simulated body fluid (SBF) as electrolytic medium was carried out on Ta and Ta/TaN coatings on BIOLINE stainless steel SS316LVM (SS). From the results, this method is a reliable, fast, and accurate measurement, which is useful to the textile area. It’s recommended to be considered after major revision. Comments as follows:

• The abstract should be extended. Please included more results from the author’s research, for instance, please briefly introduce the new method you proposed. After reading the abstract, I have not got your point.
• The abstract was extended
• 
  2) The introduction also should be extended. Here are several papers strongly related to your manuscript. Authors may consider quoting. a) Effects of Chitin Nanocrystals on Coverage of Coating Layers and Water Retention of Coating Color; b) Synthesis of lignin-poly(N-methylaniline)-reduced graphene oxide hydrogel for organic dye and lead ions removal; c) Synthesis and Application of Granular Activated Carbon from Biomass Waste Materials for Water Treatment: A Review.
• The introduction was extended adding related papers on the electrochemical deposition of hydroxyapatite using simulated body fluid as electrolyte
• 
  3) The quality of the figures should be significantly improved.
• The quality of the figures was improved

4) It’s recommended to show the contact angle images, which are presented in Table 3.

• The contact angle images were incorporated in table 3

5) Some of the reference style is not fit to the requirement of the journal.

• The references style was corrected

6) Please do more comparison in the Results and Discussion section, and extend the conclusion part. Please extend, since I have not got the significance of the author’s new method.

• The Results and Discussion comparing with other authors's results and the conclusion section was extended

Reviewer 4 Report

The authors present a fairly important study that could reach a wide range of readers. The results and conclusions are quite consistent with each other. The superficial characterization supports the proposed hypothesis in a good way.

It would be of great help if the authors provided a scheme for the formation of hydroxyapatite on the two surfaces tested. Additionally, it is recommended to discuss in greater depth regarding the intermolecular interactions and spatial arrangement of functional groups present between the surfaces and the hydroxyapatite. This would give greater support and clarity to the results presented.

Author Response

The authors present a fairly important study that could reach a wide range of readers. The results and conclusions are quite consistent with each other. The superficial characterization supports the proposed hypothesis in a good way.

It would be of great help if the authors provided a scheme for the formation of hydroxyapatite on the two surfaces tested. Additionally, it is recommended to discuss in greater depth regarding the intermolecular interactions and spatial arrangement of functional groups present between the surfaces and the hydroxyapatite. This would give greater support and clarity to the results presented.

• A scheme of the formation of hydroxyapatite on the surfaces tested was added (Figure 11) and a discussion of the mechanism of formation of HAp the intermolecular interactions were discussed . This was incorporated in the manuscript.

Reviewer 5 Report

 

This manuscript deals with the electrodeposition of HA on SS or modified SS

• The arrangement of results and the way they are presented are misleading which needs a very careful revision. The focus is on the deposition while the results section commences with corrosion and electrochemical investigations.
• The formation of HA needs to be confirmed by XRD. EDS is problematic with the detection of phosphorous and gives errors.
• The morphology of the HA coatings given by SEM shows a porous and very rough surface. Are these results consistent with the others’ works?
• What is the purpose of reporting corrosion behavior of bare substrates? If this is associated with the coating performance, the results will be useful.

 

Minor corrections:

Many typos and English errors exists:

  is concern -> concerned

others:

Since the focus of the study is SBF, it is recommended to:

• Expand the literature surface on using SBF as the electrodeposition electrolyte or related mechanisms of the formation of HA from SBF.
• Expand the section: 3. Preparation of Simulated Body Fluid (SBF)

 

Author Response

• The arrangement of results and the way they are presented are misleading which needs a very careful revision. The focus is on the deposition while the results section commences with corrosion and electrochemical investigations.
• The arrangements of the results were organized in this way since we first characterized the capacitive properties of the different bare substrates ( SS, Ta/SS and Ta/TaN/ SS) through  electrochemical impedance spectroscopy and polarization curves before that  the  electrochemical deposition of HAp  were carried out, in order to obtain the resistivity of the different substrates and obtain  the best conditions for futher HAp electrochemical coating deposition. Also, cyclic voltammetry test were carried out first to obtain the optimal potentials for the electrochemical deposition.  Then, we are not analysing the corrosion behavior of the materials at that stage, only studying the characteristics of the bare substrates.                                                         We add a brief introduction in the Results and Discussion section to clarify this part.
•  
• The formation of HA needs to be confirmed by XRD. EDS is problematic with the detection of phosphorous and gives errors.

• The XRD grazing angle experiments showing HAp formation on the double layer Ta/TaN/SS was incorporated in the manuscript.

• The morphology of the HA coatings given by SEM shows a porous and very rough surface. Are these results consistent with the others’ works?
• The morphology of hydroxyapatite obtained from electrochemical deposition depends on many different parameters, pH, temperature, current density, roughness of the substrate. However, the morphology obtained in our work is very similar to that reported in other works. This discussion was added in the manuscript.
•  
• What is the purpose of reporting corrosion behaviour of bare substrates? If this is associated with the coating performance, the results will be useful.
• Certainly the capacitive behaviour of the different substrates and the polarization curves, were performed before the Hap deposition to analyzed the coating performance before the HAp coating deposition and to be able to determine the best conditions to perform electrochemical depositions.

Minor corrections:

Many typos and English errors exists:

  is concern -> concerned

corrected

others:

Since the focus of the study is SBF, it is recommended to:

• Expand the literature surface on using SBF as the electrodeposition electrolyte or related mechanisms of the formation of HA from SBF.
• This was expanded, although there are few works reported in the literature. The mechanism of formation of hydroxyapatite was included in the manuscript
•  
• Expand the section: 3. Preparation of Simulated Body Fluid (SBF)
• The section on preparation od SBF was expanded in the materials and methods section

 

 

Round 2

Reviewer 5 Report

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