Expression of Concern tarnishes copper oxide paper

jmcacoverArticles, like lawn furniture, aren’t supposed to rust after just two months. But the Journal of Materials Chemistry A has issued an Expression of Concern for a February 2014 paper by a group of chemists from India over possible problems with several figures in the article.

The paper, “Hierarchically macro/mesostructured porous copper oxide: Facile synthesis, Characterization, Catalytic performance and Electrochemical study of mesoporous copper oxide monoliths,” was written by Gowhar Ahmad Naikoo, of the department of chemistry at Dr. Hari Singh Gour Central University, in Sagar, and two colleagues. It purported to find that:

Hierarchically macro/meso structured porous copper-oxide monoliths with and without additives (dextran, 1, 3, 5-trimethylbenzene and silica nanoparticles) were successfully synthesized via facile Sol-Gel route and characterized by Scanning electron microscopy (SEM), Powder X-ray diffraction (PXRD), Thermagravimetric analysis (TGA), Brunauer-Emmet-Teller (BET) adsorption technique and FT-IR study. The results obtained reveal that the affect of additives have enhanced specific surface area from 0.558 m2/g to 229.5 m2/g and varied pore size from 8 µm to 39 nm are discussed. Furthermore, the hierarchically porous copper-oxide materials have shown excellent catalytic activity towards the wet oxidation of phenol and electrocatalytic performance of mesoporous copper oxide (mpCuO) against p-nitrophenol, demonstrating the significance of the porous nature of copper-oxide monoliths.

However, according to the statement:

This article has been published in Journal of Materials Chemistry A as a Just Accepted Manuscript and reports the synthesis of hierarchically macro/meso structured porous copper-oxide monoliths, which show catalytic activity towards the wet oxidation of phenol and electrocatalytic performance of mesoporous copper oxide (mpCuO) against p-nitrophenol.

Journal of Materials Chemistry A is publishing this Expression of Concern in order to alert our readers to the fact that we have received significant concerns from members of the community regarding the data presented in this article shown in Figure 1, Figure 2, Figure 5 and Figure 6. Significant concerns have been raised over the possible fabrication of the data presented in these figures.

In response to our inquiries, the institution of the corresponding author has been requested to carry out an investigation. This Expression of Concern will continue to be associated with the article until the investigation into this matter has been concluded.

The letter was signed by Liz Dunn, executive editor of the journal.

Here are tThe images in question are only available behind a paywall. We’re not sure where the “significant concerns” were raised.

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21 thoughts on “Expression of Concern tarnishes copper oxide paper”

  1. I am an author of this paper.
    In this manuscript there is neither any fabricated data nor any theft of data but a reader has raised comments, we believe, on the basis of personal conflict between the authors & reader.Otherwise this paper was evaluated by senior most scientists of the same field.
    In this case authors are sure about the name of reader & his group.
    In figures 1,2,5,6..authors have submitted original spectra & proper explanation where ever necessary but authors feel very hurt why not journal of Materials Chemistry A editorial board demanding for text data of the partcular figures from the authors instead of trying to defame authors much more.
    If this thing continues then the faith of esteemed journals will be rusted.

    1. Author must state what reason the journal has given regarding figures 1,2, 5 and 6.
      I would like to know what error journal has pointed out regarding the XRD, SEM, IR and mechanism?
      I read the comments and journal has not mentioned any details regarding the figures. If authors states clearly what reason were given by the journal, then it will be easy for others to comment regarding any data. This is a scientific forum and the authors must not write anything against any person or journal. Discuss in scientific terms here.

    2. For the figure 1 XRD, which are of samples prepared with differing additives,( i.e. they are different samples), the baseline noise levels of the XRD diffractograms shown are all exactly the same. This is simply not possible, as any person with experience in powder XRD measurements would confirm.

  2. In figures 1, 2, 5 & 6…. I did not feel any type of fabrication as authors have synthesized CuO monoliths. So, there xrd spectrum must be same as nicely reported by the authors. In SEM figure their is clear difference between A, B, C & D. But in figure 2 (D) there are some white spots also seen… as may be the presence of silica. In figure 5, I feel no doubt, clearly showing shift in wave numbers. In figure 6… about the mechanism of the catalytic reaction, the authors have nicely represented the mechanism.

  3. Dear scientists,
    In figure 1, xrd..reader has raised question why background of all spectra’s i.e Fig.1 A, B, C, D are same.
    Authors have synthedized CuO monoliths..So after calcination of samples there is present CuO in tenorite form…it is clear fact then their xrd spectras must be same…but slight difference in background.As authors have send the original spectra to the editorial board also to clear the confusion of reader.Authors are ready for sending the text data of four samples also.
    In figure 2…reader has raised question that Fig.2(C) & (D) are same…
    But, it is clearly visible that figure 2(D) is different from (C)..as in D …encapsulation of silica nanoparticles is clearly distinct & confirmed by EDX.(SIF).
    In Fig.5..reader raised question that Fig.5 (A) & (B) has same background..
    Authors have given clear explanation for that also & ready for providing text data of the figure.
    In figure 6 …reader raised question that it is copy paste mechanism but authors have given their own plausible mechanism but in our mechanism, 1..2 steps are matching with the mechanism reported in ref.34 (article)…but authors have already given the citation of that ref.34 in possible mechanism of our artcle.

    1. Ok Author. Now I exactly understand the concerns. I cannot comment on the mechanism since I am not well versed with what the problem is (I do not understand mechanisms).

      About XRD. Yes the concern seems genuine. As you say CuO is present in tenorite form, finally all four XRD (as per my 30 years experience in XRD), can never be same. All the XRD look like a mirror image of each other. Why dont you send the software data directly to the journal, along with the software? Do not send any text or excel files. The data ‘as obtained’ from the instrument should be sent in my opinion. Let the journal authorities open the software on their own. I think you understood what I am meaning.

      About SEM, well, journal does not seem totally incorrect in this matter since (B), (C) and (D) all are looking same. I am not here to criticize you. I am writing what I am seeing according to the comments you have mentioned. Experience says that there has to be a drastic difference between a 5 micron and 200 nm SEM. It is same as looking at a book from a ‘meter’ away and the same book from a ‘cm’ away distance. Will you not see only one part of the book rather than a whole page? Same is the case with SEM. The shining part in your SEM is the electron beam reflection. It means nothing else. As you mentioned about SiF, I cannot see any SiF with my eyes in the SEM. Also, I checked the EDX of the SEM. Where is F in it? I can only see Si. Sorry, however, I cannot give you any suggestion in this comment.

      About IR, you can solve this matter similar to the XRD suggestion. Send the software data to the journal and request them to open the data in the software itself. I think this is the perfect way to solve this query too. Text data never helps in these situations. Some log from instrument needs to be shown.
      Or take a print screen shot of the image from the instrument computer and send it to journal. If you say that cannot send either original software or a print screen shot from the instrument computer, then it is very difficult to reply to this query.

      I initially thought that the error raised by the journal must be related to some values in the data. However, if you are not hiding any points other than what you have mentioned here, then please try to solve the problem as I have suggested. XRD and IR queries can be solved in this way. SEM sorry, I am not able to reply. I will still search about it and let you know if I get some good reply. Mechanism query, I am sorry. I do not understand.

      1. Dear Grnzer:
        Thanks for you cooperation: I think you did not understood SIF….it is supplementary information file. There is only silica in Fig 2 (D)…which you have seen in EDX also.
        l can send SEM tif images of all samples also to clear this confusion also.

        1. I agree I have seen Si in the EDX. However, is it mentioned in the comment that Si is not seen? What you mentioned in your previous comment is: the SEM comment is about 2(C) and 2(D). No mention is about EDX. So do not mention about EDX in your reply. It will create further complications. Solve what is asked for rather than giving some reasons which are not asked.

          Do not go round the bush in your replies whenever you reply to the journal. Sending a scientific reason why 2(C) and 2(D) are not the same is needed. Please read again my explanation regarding 5 micron and 200 nm should have different images. I think you are not understanding what I wrote. Sending tif files for SEM will not help since you must have already sent tif files in your article (SEM cannot be made in word/excel).

          Sending same SEM data again is not going to help. Some strong scientific explanation may be needed for this. Unfortunately, I am unable to find any. I have been thinking a lot about any solution for this. However, every time I see both (C) and (D), I fail to find any difference between them (in terms of magnification-5 micron and 200nm difference)

          For XRD and IR, send the software files along with software (which journal can instal on their computer and open the files) and your claims can be verified easily. Send all XRD and IR software files directly so that editorial board can believe the claims. Please be very specific in your replies (and only be scientific in your reply). If you have any queries feel free to post here. I will try to reply to the best extent I can. All the best.

        2. Author. As I mentioned in reply to Mr. Cole, do a skype call with journal about SEM. Let the editor see on his/her own the images which resemble with magnification mentioned-‘live’. For XRD and IR, send original data+instrument software. For mechanism, experts have given you their suggestion already.

  4. I am not expert of the characterization of materials but i have worked alot on catalysis. I have gone through this paper deeply and i found that mechanism (Fig.6) given by the authors is not copy paste but 1, 2 steps of the given mechanism are matching with the reported mechanism (ref.34).
    When i thoroughly read the mechanism of the paper, authors have given citation of that reference 34 also. So, i can say only that in Fig. 6 there should not be any concern against the authors.

  5. Dear Naikoo,
    Mr Grnzer has given u a good suggestion. You should send your original data along with the software to the editorial board to solve the problem of XRD and FTIR. This is simple.
    However, I disagree with Grnzer comment on SEM of Fig.2D. In fig 2 (C) & (D) there is a clear difference. I am also working in this field & used silica nanoparticles as additive. Actually, role of silica is shrinkage of pore size during the synthesis of sponges or monoliths of metal & metal oxides. So, I cant say that this thing wil not happen.
    As per Grnzer, i agree with him but i have some contradiction with him on the point that in Fig 2D..the shining is due to electron reflection beam…it is totally absurd point because if it was possible then it should come in fig 2 B,C also.
    I think Grnzer has not used silica naoparticles as additives in his research till now. I am sure to write this statement that there is a clear influence of silica nanoparticles on image magnification which is due to the pore shrinkage.

    1. Mr. Cole,

      You are correct I have never worked on Silica NPs. However, can you please tell me can you see this clear SEM at 200 nm? Even though I have never worked on this subject, it is not possible for me to still buy the fact that 2(B), 2(C) and 2(D) are not same. I think since you are well versed with SEM, how is it possible that exact same images are visible for 2(B)-2(D)? An SEM image at 200 nm should looks as if we are watching some thing very close enough. If there was only one portion visible in the SEM (I mean a subset of Figure 2(C)), I would have told author that they can fight strongly for this. I am unable to see a subset of 2(C) in 2(D).

      For author, I talked to my friend who is more well versed with me in SEM. He told me that you have not taken the SEM parameters directly from instrument. You have drawn the scale in some software. I think you need to send the ‘real’ SEM which were taken directly from instrument to the journal. Or you can do a skype conference with the journal about the SEM. Show them the data ‘live’.

      Finally it is your paper. You HAVE to give 200% of your efforts to solve any problems.

      So final solutions I and my colleague thinks: IR and XRD-send original instrumental data with software which the Journal can open on their computer. Please send ALL four XRD and IR of Figure 1 and 5 to them. For SEM, the same sample will give the same results. So do a skype call with the editorial board. After seeing the same images live, I and my colleagues do not think that you should have any further problem. As per mechanism is concerned, experts have already given their opinion. All the best.

  6. Dear Gowhar,
    I have gone through all these comments and i agree with Daniel and Grnzer to send your orginal software based data about XRD and FTIR.
    For SEM images, i thank Daniel for clearing my confusion too.
    I am sorry for fig 1, 2 and 5 as i have little knowledge in this field. so, could not comment any more. But, i have good expertise in heterogeneous catalysis. so, i can share my views about fig 6. i have deeply gone through the authors paper and Ref 34. the authors have mentioned free radical mechanism with clear view of canonical structures in step 1 and 3, but the authors of Ref 34 have mentioned odd electron within the ring which is little bit confusing.
    In addition to that i found some steps of the given mechanism are similar to ref 34, but there is a clear citation of ref 34 in the possible given mechanism. so, for fig 1, 2 and 5, i am helpless, but i am sure that Fig 6 is a clear plausible mechanism for the catalytic reaction.

  7. Gowhar, I agree with Wan, Cole and Grnzer. They have given perfect suggestions to you. As suggested by them send journal the software data and surely you must do skype for images as suggested earlier. You need to convince the editorial board about this. Solving this must not take you more than a few days.

  8. I have gone through all the comments mentioned above deeply.

    I am working on porous materials by using different organic and metallic, semi metallic nanopartcles as structural directing agents for the variation of pore morphology….
    So, I also want to share my views about the Fig.2 as solution of XRD, IR and Mechanism is clearly explained by several scientists..
    Using silica nanoparticles as structural directing agent during the process of monoliths fabrication….the pore morphology of the monoliths dramatically changes to mesoporous nature because of shrinking of the pores (agree with the Cole….) compared to organic structural directing agents which show swelling in the monoliths..
    when i have gone through the authors paper especially in Fig. 2 C and D, clear difference is noticed.
    In C, pores are quite swollen clearly different from pore morphology in D where pores are in mesh form.and also Fig, 2 D is not so clear as C, i think it may be the effect of higher magnification. So, i can say only that C and D are clearly different from each other…….

    Apart from this, i want to share my experience on SEM instruments (JEOL 5600 and NOVA NANOSEM 450) which i have operated till now…The Incharge professor of the SEM has never allowed me to take video of the SEM instrument, So, i dont think that author will be allowed to solve his problem on Skype, deadly, impossible. But, he can solve this problem only by sending the real tif images………………….
    …….

    1. Finally whatever author does to solve the problem is immaterial. He should get it solved ASAP. Journal is not going to see comments posted on this page. I think author must realize this. He must focus very hard to convey the editor. There is no point even discussing this topic on this forum since all suggestions have been given. Of course author knows very well how to solve the problem. Just solve it and get this ‘expression of concern’ removed. No point keeping on discussing on this same matter. All the best. Give good news soon.

  9. From the above mentioned comments, I agree with Cole, Mann, Wan and Grnzer. They have given their nice suggestions to the author. Now i feel editorial board of journal of Materials Chemistry A should clear the dispute of the paper as early as possible.

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