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Review
Peer-Review Record

Main Routes of Production of High-Value-Added 2,5-Furandincarboxylic Acid Using Heterogeneous Catalytic Systems

Catalysts 2023, 13(5), 880; https://doi.org/10.3390/catal13050880
by Ane Bueno, Asier Barredo, Nerea Viar and Jesus Requies *
Reviewer 1: Anonymous
Reviewer 2:
Reviewer 3: Anonymous
Reviewer 4:
Catalysts 2023, 13(5), 880; https://doi.org/10.3390/catal13050880
Submission received: 5 April 2023 / Revised: 3 May 2023 / Accepted: 10 May 2023 / Published: 13 May 2023
(This article belongs to the Special Issue Catalytic Materials: State-of-the-Art and Perspectives in Spain)

Round 1

Reviewer 1 Report

The authors present a review regarding the production of FDCA using catalytic systems. I do like that the review is focused on recent literature (for the most part, since 2017), but substantial changes must be made prior to being accepted for publication.

-      ---  The English of the paper needs to be improved throughout. The flow and grammar, in particular, are not at the standard expected for a journal article.

-        ---The tables appear too far from where they are first mentioned.

-       --- Tables 1 and 2 would be much easy to read and to compare rows on if more columns were added. For example, having columns with “Catalyst,” “Solvent,” “Separation,” (plus temperature, pressure, and time) would improve the readability.

-      ---  Most of the review is focused on just the facts and yield/conversion outcomes of the previous work. Adding in more discussion as to the “why” things happen would greatly benefit the manuscript. There are many details that could be excluded (for example on page 3, lines 92-106), but then the actual reasons why things happened added. That is, what are the main takeaways?

-        ---That leads to the conclusions, which do not state much of anything with value. Pulling out the “whys?’ and what researchers focus on in the future is a must.

This could be a valuable addition to the FDCA literature, but I do not believe this paper is ready for publication as it needs significant revisions to improve readability and more discussions as to the overall findings need to be made. That is, the literature review is solid, but it is missing the main takeaway from considering all of the research.

Author Response

The authors present a review regarding the production of FDCA using catalytic systems. I do like that the review is focused on recent literature (for the most part, since 2017), but substantial changes must be made prior to being accepted for publication.

  1. The English of the paper needs to be improved throughout. The flow and grammar, in particular, are not at the standard expected for a journal article.

Authors’ response: Following the reviewers’ suggestion, English grammar has been revised by one expertise

 

  1. The tables appear too far from where they are first mentioned.

Authors’ response: Following the reviewers’ suggestion, a division of tables has been made so that they can be in their corresponding section.

 

  1. Tables 1 and 2 would be much easy to read and to compare rows on if more columns were added. For example, having columns with “Catalyst,” “Solvent,” “Separation,” (plus temperature, pressure, and time) would improve the readability.

Authors’ response: Following the reviewers’ suggestion, more columns have been added.

 

  1. Most of the review is focused on just the facts and yield/conversion outcomes of the previous work. Adding in more discussion as to the “why” things happen would greatly benefit the manuscript. There are many details that could be excluded (for example on page 3, lines 92-106), but then the actual reasons why things happened added. That is, what are the main takeaways?

Authors’ response: Following the reviewers’ suggestion, a deeper discussion of the results has been added. Moreover, the details of line 92-106 have been suppressed.  

 

  1. That leads to the conclusions, which do not state much of anything with value. Pulling out the “whys?’ and what researchers focus on in the future is a must.

Authors’ response: Following the reviewer´s remark, the conclusions have been modified, including a general overview of the most important facts influencing the production of FDCA and the most promising routes for future research have been outlined.

 

Comments on the Quality of English Language

This could be a valuable addition to the FDCA literature, but I do not believe this paper is ready for publication as it needs significant revisions to improve readability and more discussions as to the overall findings need to be made. That is, the literature review is solid, but it is missing the main takeaway from considering all of the research.

Reviewer 2 Report

This review provided a general overview of the recent researches of the catalytic systems for the direct production of FDCA from sugars. This review is very timely and informative to researchers in the field of electrocatalysis and beyond. There are only a few comments need to be addressed.

 

1. The abstract should be revised to fully summarize the review topic.

2. Only one figure is presented. This is not enough for the review article.

3. The importance of this review topic should be further highlighted in the Introduction.

4. More categories should be presented in Section 4.

5. Please give perspective and useful suggestions for this research field.

6. Ref. 18 and Ref. 19 is the same paper. Please check.

7. Please cite more recently published papers from 2022-2023.

8. The very important related papers that not limited to 2,5-furandincarboxylic acid production should be cited, such as Journal of the American Chemical Society, 2022, 144 (5), 2079-2084; Applied Catalysis B: Environmental, 2023, 325, 122388.

no

Author Response

REVIEWER 2

This review provided a general overview of the recent researches of the catalytic systems for the direct production of FDCA from sugars. This review is very timely and informative to researchers in the field of electrocatalysis and beyond. There are only a few comments need to be addressed.

  1. The abstract should be revised to fully summarize the review topic.

Authors’ response: Following the reviewers’ suggestion, the abstract has been modified to explain more precisely the topic of the review.

 

  1. Only one figure is presented. This is not enough for the review article.

Authors’ response: Following the reviewers’ suggestion, molecular structure of glucose humins image has been included.

 

  1. The importance of this review topic should be further highlighted in the Introduction.

Authors’ response: Following the reviewers’ suggestion, the text of the introduction has been changed. In addition to this a new graphics has been incorporated in the introduction section.

 

  1. More categories should be presented in Section 4.

Authors’ response: Following the reviewers’ suggestion, three subsections have been added.

 

  1. Please give perspective and useful suggestions for this research field.

Authors’ response: Following the reviewers’ suggestion, the most promising routes for future research have been outline in “Conclusions” section.

 

  1. Ref. 18 and Ref. 19 is the same paper. Please check.

Authors’ response: Ref 19 has been deleted.

 

  1. Please cite more recently published papers from 2022-2023.

Authors’ response: Following the reviewers’ suggestion, more recently published paper has been included from 2022-2023.

 

  1. The very important related papers that not limited to 2,5-furandincarboxylic acid production should be cited, such as Journal of the American Chemical Society, 2022, 144 (5), 2079-2084; Applied Catalysis B: Environmental, 2023, 325, 122388.

Authors’ response: Following the reviewers’ suggestion, the Applied Catalysis B: Environmental, 2023, 325, 122388 manuscript has been included in the introduction.

 

Comments on the Quality of English Language

No

Reviewer 3 Report

The authors described the synthesis of 2,5-furandicarboxylic acid by using diverse catalytic systems. Overall, some explanations are very general, and experimental data are missing. To understand how these catalytic systems lead to 2,5-furandicarboxylic acid, some important mechanisms should be included and briefly explained. I consider that the manuscript meets all requirements to be published in “Catalysts” after major revision. Additional suggestions and/or comments are included:    

(1) See introduction, lines 66-68. The authors mention that “In this work, we present a general overview of the latest advances in the main catalytic processes applied for the conversion of hexoses compounds into FDCA using heterogeneous catalysis”. I recommend including a general scheme or figure should be included for better clarity.

(2) See lines 79-83. Reaction conditions such as catalyst loading, temperature, reaction time, and main yield should be included.  

(3) See lines 92-106. The catalyst loading should be included.

(4) See lines 111-117. The catalyst loading should be included.

(5) See lines 118-125. The catalyst loading should be included.

(6) See Table 1. The catalyst loading should be included.

(7) See lines 123-125. The authors mention that “concluding that both Lewis and Brønsted acid sites were active in fructose dehydration. However, Lewis acid sites could also favor the formation of humins”. It is very important to include the percentage of Lewis and Brønsted acid sites in parenthesis.

(8) See lines 152-154. The authors mention that “Lastly, as in the previous research, the presence of heavy metals in the raw biomass was investigated, concluding that could be acting as Lewis acid sites, enhancing the catalytic activity”. It is very important to include the percentage of Lewis acid sites in parenthesis.

(9) See lines 172-254. The catalyst loading of all catalysts should be included.

(10) See lines 270-278. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

(11) See lines 279-288. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

(12) See lines 289-301. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

(13) See lines 302-312. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

(14) See the conclusion section. It seems like the conclusions of a research article. It should be improved. Also, the last paragraph should contain a perspective.  

(15) Some relevant mechanisms described in manuscripts should be included to understand the role of the catalyst.

(16) The title of the manuscript can be improved.

Moderate editing of English language

Author Response

REVIEWER 3

The authors described the synthesis of 2,5-furandicarboxylic acid by using diverse catalytic systems. Overall, some explanations are very general, and experimental data are missing. To understand how these catalytic systems lead to 2,5-furandicarboxylic acid, some important mechanisms should be included and briefly explained. I consider that the manuscript meets all requirements to be published in “Catalysts” after major revision. Additional suggestions and/or comments are included:    

(1) See introduction, lines 66-68. The authors mention that “In this work, we present a general overview of the latest advances in the main catalytic processes applied for the conversion of hexoses compounds into FDCA using heterogeneous catalysis”. I recommend including a general scheme or figure should be included for better clarity.

Authors’ response: Following the reviewers’ suggestion, an scheme of the reaction (Figure 2) has been included.

(2) See lines 79-83. Reaction conditions such as catalyst loading, temperature, reaction time, and main yield should be included.  

Authors’ response: Following the reviewers’ suggestion, catalyst loading, temperature and reaction time have been included. The main yield was included in line 89.

 

(3) See lines 92-106. The catalyst loading should be included.

Authors’ response: Following the reviewers’ suggestion, catalyst loading has been included.

 

(4) See lines 111-117. The catalyst loading should be included.

Authors’ response: Following the reviewers’ suggestion, catalyst loading has been included.

 

(5) See lines 118-125. The catalyst loading should be included.

Authors’ response: Following the reviewers’ suggestion, catalyst loading has been included.

 

(6) See Table 1. The catalyst loading should be included.

Authors’ response: Following the reviewers’ suggestion, catalyst loading has been included.

 

(7) See lines 123-125. The authors mention that “concluding that both Lewis and Brønsted acid sites were active in fructose dehydration. However, Lewis acid sites could also favor the formation of humins”. It is very important to include the percentage of Lewis and Brønsted acid sites in parenthesis.

Authors’ response: The reference does not mention the percentage of Lewis acid sites. The employed acids (Amberlyst 15, Nafion-NR50 and CrCl3·6H2O) are known to be Brønsted or Lewis acid sites, thus, the discussion is not based in the quantification of Lewis and Brønsted acid sites but in the nature of the acids chosen.

 

(8) See lines 152-154. The authors mention that “Lastly, as in the previous research, the presence of heavy metals in the raw biomass was investigated, concluding that could be acting as Lewis acid sites, enhancing the catalytic activity”. It is very important to include the percentage of Lewis acid sites in parenthesis.

Authors’ response: The reference does not mention the percentage of Lewis acid sites. The article states that “the heavy metal elements in the biomass migrated into the liquid phase during the heat process to act as a Lewis acid catalyst (the existence of heavy metals was found by detecting the product solution).

 

(9) See lines 172-254. The catalyst loading of all catalysts should be included.

Authors’ response: Following the reviewers’ suggestion, catalyst loading has been included.

 

(10) See lines 270-278. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

Authors’ response: Following the reviewers’ suggestion, catalyst loading, temperature and reaction time have been included.

 

(11) See lines 279-288. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

Authors’ response: Following the reviewers’ suggestion, catalyst loading, temperature and reaction time have been included.

 

(12) See lines 289-301. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

Authors’ response: Following the reviewers’ suggestion, catalyst loading, temperature and reaction time have been included.

 

(13) See lines 302-312. Reaction conditions such as catalyst loading, temperature, and reaction time, among others, should be included.  

Authors’ response: Following the reviewers’ suggestion, catalyst loading, temperature and reaction time have been included.

 

(14) See the conclusion section. It seems like the conclusions of a research article. It should be improved. Also, the last paragraph should contain a perspective.  

Authors’ response: Following the reviewer´s remark, the conclusions have been modified, including a general overview of the most important facts influencing the production of FDCA and the most promising routes for future research have been outlined.

 

(15) Some relevant mechanisms described in manuscripts should be included to understand the role of the catalyst.

Authors’ response: Following the reviewers’ suggestion, different routes from HMF to FDCA have been explained.

 

(16) The title of the manuscript can be improved.

Authors’ response: Following the reviewers’ suggestion, the manuscript title has been rewritten

 

Comments on the Quality of English Language

Moderate editing of English language.

Reviewer 4 Report

The conversion of biomass or its derivatives into valuable chemicals or other platform compounds is a hot topic. This manuscript reviewed the recent progress on the production of FDCA. Several techniques for the production of FDCA have been discussed and reviewed. Some major issues should be considered before it can be accepted for publication.

1. In the Introduction, the number of publications as a function of year can be added.

2. The advantages and disadvantages of one-step and two-step should be discussed. The comparisons should also be added.

3. This article is a review paper. So, the current issues for the production of FDCA is necessary. And how to solve these issues should be provided.

4. The possible development trend of FDCA preparation in the future needs to be prospected.

The English is well and can be understood.

Author Response

REVIEWER 4

The conversion of biomass or its derivatives into valuable chemicals or other platform compounds is a hot topic. This manuscript reviewed the recent progress on the production of FDCA. Several techniques for the production of FDCA have been discussed and reviewed. Some major issues should be considered before it can be accepted for publication.

  1. In the Introduction, the number of publications as a function of year can be added.

Authors’ response: Following the reviewers’ suggestion, Figure 1 has been added.

 

  1. The advantages and disadvantages of one-step and two-step should be discussed. The comparisons should also be added.

Authors’ response: Following the reviewer´s remark, the advantages and disadvantages of one and two step configurations have been included in “Conclusions” section.

 

  1. This article is a review paper. So, the current issues for the production of FDCA is necessary. And how to solve these issues should be provided.

Authors’ response: Following the reviewer´s remark, the main issues of each configuration have been described in “Conclusions” section, enhancing the need of future investigation.

 

  1. The possible development trend of FDCA preparation in the future needs to be prospected.

Authors’ response: Following the reviewer´s remark, the future perspective has been underlined in “Conclusions” section.

 

Comments on the Quality of English Language

The English is well and can be understood.

Round 2

Reviewer 2 Report

It can be accepted now.

Reviewer 3 Report

The authors have detailed the primary pathways for producing 2,5-furandicarboxylic acid with heterogeneous catalytic systems, which adds significant value to the final product. The authors have addressed most of the reviewers' comments, and I believe that the manuscript now satisfies all the requirements for publication in "Catalysts." Therefore, I recommend that the manuscript be published in its current form.

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