Declined for Publication

Decision made by Editorial Board Member and Chief Editor on Manuscript M: Declined for Publication (despite two highly positive recommendations) Comments 1: I am sorry to inform you that the handling editor has had to reject your paper. There is too much overlap with recently published papers in the journal "Chemosphere" (Year 2016, Vol 153, pp 528530 – 3 pages/compared to > 10 here!) and in "Clean-Soil Air Water" (Year 2016 – accepted 2014, vol. 44, pp 325-450 – something is not correct here, this would be a book!) and earlier publications (co-authored by C. Noubactep we assumed) since around 2010. Responses 1: This argumentation is surprising. Scientific publishing should avoid the propagation of false beliefs. It is well-established (since 2007) that falsehoods where introduced into the information stream of Aqueous Iron Corrosion. Since then, there are two types of reserachers on the large topic of 'remediation using iron metal': (i) the 'pacificists' seeking success with more papers get published, and (ii) the veristics ready to face resistances. Our approach is the second and we are challenging for the veritistic ideal. For this reason the number of papers co-authored by Noubactep since 2010 (three years after the still prevailing popular view was challenged) should be compared to the other many 100s. Moreover, the veritistic ideal should be the reference for comparison as the indexed falsehoods have introduced bias in the system. On the other hand, the paper at Clean (even both) was accepted in 2014 (2 years old already) and the one at Chemosphere (2016) was a short communication. What is the scientific argument against a Research Note from someone who has recently published a short communication (or 2 short communications and one review article)? There is also a 'Review of reviews' at Water Research (2015) desmonstrating/recalling that the prevailing view is mistaken. Would the pending manuscript have been rejected if it has been presented by another authorship? The work presented in Manuscript M summarizes research questions that have been performed by collaborating research groups in three countries: Cameroon, Germany and Tanzania. The results are organized in two good manuscripts. The second is to be submitted very soon (in the meantime published at Sustainabiliy). Manuscript M has been excellently reviewed by experts selected by the Editorial Boatrd of Journal J. It is not clear to us why this manuscript should not be published. We have advocated for open access partly to improve the compactness of the peer-review process. Let present the results to the reader of Journal J (open access) who is able at assessing it usefulness. Comments 2: Figure 1 of the current submission to "Journal J" has without any change been used as graphical abstract in the above mentioned publication in Chemosphere. Responses 2: Permission for reproduction is available. Chemosphere has also reproduced with permissions from Atlas of Science. We can prepare a new graphical abstract. Sincerely, Chicgoua Noubactep

Reviewer's comments are appended. Reviewer 1: English language and style ( ) Extensive editing of English language and style required ( ) Moderate English changes required (x) English language and style are fine/minor spell check required ( ) I don't feel qualified to judge about the English Language and Style Yes for all these questions: (other answers: Can be improved, Must be improved, Not applicable) Does the introduction provide sufficient background and include all relevant references? Is the research design appropriate? Are the methods adequately described? Are the results clearly presented? Are the conclusions supported by the results? Comments and Suggestions for Authors You have improved the manuscript and explained what you mean by Valley of Confusion so I consider the manuscript ready for publication after another and final spell check Date of manuscript submission 02 May 2016 22:02:27 Date of this review 14 Jun 2016 15:45:00 Reviewer 2: English language and style (x) Extensive editing of English language and style required ( ) Moderate English changes required ( ) English language and style are fine/minor spell check required ( ) I don't feel qualified to judge about the English Language and Style Comments and Suggestions for Authors I have reviewed the paper again and in my opinión, it can be accepted in the present form Date of manuscript submission 02 May 2016 22:02:27 Date of this review 01 Jun 2016 12:34:59 This manuscript is accepted with a delay of more than one year, solely the references were significantly actualized. This is in line with the quote of Johann Wolfgang von Goethe: "In the sciences, people quickly come to regard as their own personal property that which they have learned and had passed on to them at the universities and academies. If someone else comes along with new ideas that contradict the Credo and in fact even threaten to overturn it, then all passions are raised against this threat and no method is left untried to suppress it. People resist it in every way possible: pretending not to have heard about it; speaking disparagingly of it, as if it were not even worth the effort of looking into the matter. And so a new truth can have a long" Johann Wolfgang von Goethe (28.08.1749 - 22.03.1832), German writer, pictorial artist, biologist, theoretical physicist, and polymath. Conversations with Johann Peter Eckermann, December 30th 1823.

Editor's decision Re manuscript Number N. Metallic iron for water treatment: Leaving the valley of confusion. Dear Dr. Noubactep, I very much regret to have to tell you that publication in our journal is not recommended. … I hope that the comments contained therein will be of use to you. Thank you for your interest in Journal 2. Kind regards, The Editorial Board ......................................................... COMMENTS FROM THE EDITOR AND/OR REVIEWERS Editor: Based on limited novelty as indicated by the expert reviewers we cannot proceed with the paper. Reviewer #2 The manuscript describes a review - metallic iron for water treatment: leaving the valley of confusion. Rejecting this manuscript is based on the reasons, (1) the manuscript do not present new information and full version of metallic iron used for water treatment, indicating that the significance and novelty of the manuscript are poor, (2) there are many reviews concerning metallic iron, including iron nanoparticles, and (3) this manuscript does not meet the standard of Journal 2 since it is a high reputed journal. Hence I do not recommend this manuscript. Reviewer #3 In this manuscript, the authors raised their critical comments on the recent advance of the ZVI systeme for water decontamination, and suggested that future study on the system should move to the mainstream science. Moreover, the authors provided 12 directions to be reconsidered in this field. Really, numerous study concerning ZVI system are availale with contradictory conclusions particularly in how ZVI interact with the target contaminant and how decontamination occurrs. Personally, I agree with most of the authors opinions, and it is the time to reconsider the work performed in this field and to be carried out in future. My main comments on the manuscript lies on the following items (1) the authors provided similar opinions in their recent paper (Water Research 2015, 45, 114-123). I hope the authors could provide more insightful evidence on the structure-activity relationship of the ZVI systme, i.e., what does the real ZVI particles look like in its fine structure, and how does it affect its reaction with water and target pollutants; (2) as for thermodynamic and kinetic behavior of ZVI reaction with contaminants, the basic processes involved should be defined and their basic physical chemical properties should be detailed. Otherwise, superficial discussion with solid evidence seems far from the mainstream science. (3) as for the real application of ZVI system, large-scale or field application study should

be encouraged and the chemical composition of the influent water should be particularly focused on. We are very thankful to Reviwer 2 explaining the extent of confusion! Only when the majority of researchers will be aware on the real nature of the Fe 0/H2O system, will real research start. For this reason we just moved to the next journal: AWS!

Detailed responses to the comments Editor: Based on limited novelty as indicated by the expert reviewers we cannot proceed with the paper. The expertise of the reviewers has been questioned for ten (10) years now! Reviewer #2 The manuscript describes a review - metallic iron for water treatment: leaving the valley of confusion. Rejecting this manuscript is based on the reasons, Was the manuscript evaluated to be rejected? (1) the manuscript do not present new information and full version of metallic iron used for water treatment, indicating that the significance and novelty of the manuscript are poor, Such a statement can be virtually applied to every manuscript. Our manuscript has not claimed to present any new information, rather it further demonstrates that recent 'new information' was not really new and shows ways out of this confusing situation. This is not novel but this journal (and others) has been publishing wrong novelties for more than two decades. That is the point! (2) there are many reviews concerning metallic iron, including iron nanoparticles, And this is a reason not to publish a new review? The new review is evaluating available ones, explicitely (or critically). and (3) this manuscript does not meet the standard of this journal since it is a high reputed journal. Hence I do not recommend this manuscript. We would like to agree with this but Reviewer#2 has not addressed our manuscript by any scientific approach. Again, all the three points addressed are virtually applicable to any manuscript. Such useless comments are only significant based on a certain level of trust from the editorial board. Unfortunately, the expertise that has been keeping the Fe 0 remediation on the wrong path has been severely challenged and no contradictory argument has been presented apart from such reviewer's evaluation. This is truly a private opinion compared to some 20 papers (co-authored by the corresponding author) presenting the authors view. The 'tired argument' of 'already said' (déjà vu) was put forward since 2008 and has been repeated by reviewers all the years. However, the real 'déjà vu' is the view that Fe 0 is a reducing agent. This view is presented and repeated in some more than 3000 scientific articles and is partly supported by excellent results by sophisticated modern devices. Unfortunately good experimental results were and are wrogly interpreted

A real scientific and collegial approach would have been to demonstrate the fallacy of the arguments put forward in this manuscript. Until this is done, we will keep on living in the valley of confusion!

Reviewer #3 In this manuscript, the authors raised their critical comments on the recent advance of the ZVI systeme for water decontamination, and suggested that future study on the system should move to the mainstream science. Moreover, the authors provided 12 directions to be reconsidered in this field. Really, numerous study concerning ZVI system are availale with contradictory conclusions particularly in how ZVI interact with the target contaminant and how decontamination occurrs. Personally, I agree with most of the authors opinions, and it is the time to reconsider the work performed in this field and to be carried out in future. Many thanks for this evaluation. My main comments on the manuscript lies on the following items: (1) the authors provided similar opinions in their recent paper (Water Research 2015, 45, 114-123). Reviewer #3 is right the present manuscript is regarded as an extension of 'review of reviews'. However it is not limited at showing what was mistaken but has shown ways out of the confusion. The argumentation is similar but not identical. I hope the authors could provide more insightful evidence on the structure-activity relationship of the ZVI systme, i.e., what does the real ZVI particles look like in its fine structure, and how does it affect its reaction with water and target pollutants; This is really a good point but we are not presenting experimental results and we think that only sound concepts would enable better data. The extent of confusion is such that no single research group would solve the problem alone. In publishing good results you will always be 'forced' or prompted to consider aspects that have already been proven false. And this will not always make your work stronger! Moreover, The Fe0/H2O system is a dynamic one, meaning that any experimental observation (e.g. at the end of the experiment) is just an instant observation of a part of the system at that date. In a Fe0/H2O system, adsorption, co-precipitation, reduction and oxidation of dissolved species occur all in parallel. Iron hydroxides precipitate and are crystallised. Some crystallised oxide are dissolved by abiotic and biotic process. All there are reactions that are certain to occur and influence contaminant removal. There is a trend to investigate only forward reaction while parallely acknowledging that Fe 0 walls should work for years or even decades! It is not useless to reveal that we (as research group) have been performing the longest batch experiments for the past 18 years and that our column experiments typically with small amount of Fe 0 (and other additives) last for months. This occur in a context were even pilot scale demonstrations have been ran for just some few weeks and the results used to model the behaviour of barriers for decades. Sammarized, a new approach is needed to generate better data! (2) as for thermodynamic and kinetic behavior of ZVI reaction with contaminants, the basic processes involved should be defined and their basic physical chemical properties should be

detailed. Otherwise, superficial discussion with solid evidence seems far from the mainstream science. This is excately what we have done and are progressively doing, and doing this while critically considering two decades of scientific research is not and cannot just be a „superficial discussion“. Our impression is that the significance of our manuscript is belittled by a simplistic view. Again 5 generations of PhD students (à 4 years) have been dragued into confusion. Taking them (and coming researchers) out of this valley is more important than the fact that the chemistry of the Fe 0/H2O system was established before the invention of ZVI PRBs. Noubactep has recently argued that no chemist would have introduced Fe 0 for contaminant reduction under environmental conditions. However, you cannot further develop the technology without the chemistry of the system. Another lecture is that little progress was made because research was not based on the chemistry of the system. (3) as for the real application of ZVI system, large-scale or field application study should be encouraged and the chemical composition of the influent water should be particularly focused on. We fully agree with this point. It is our intention to prepare sustainable field application. We have already explained why some failures occured and stated that some success stories are yet to be rationalized (e.g. why should a pure Fe 0 barrier (100 % Fe0) last for several years?). We have introduced a sort of applied tracer test for the Fe 0/H2O system (methylene blue method (general) and one research group has already belittled it in presenting his on-contaminantsystem (example) – That is the atmosphere in which we are publishing. It will not be surprising that a researcher comes tomorrow and contrast 'general' and 'example' in rationalizing his proposal. Just because the 'example' was contrasted to the 'general' in it presentation without beeing an exception!). And we have been constantly saying for the past 8 years that progress would only be achieved in a real open collaboration. We are thankful for both reviewers. Even though we do not accept their decision, we have respected them and will use the arguments by Reviewer 3 to better present our concept in future. The current manuscript is enriched with a prolog and submitted elsewhere. Sincerely, Dr. Noubactep