Phase Separation in Nonaqueous Systems Induced by a Solid Component
Round 1
Reviewer 1 Report
Comments and Suggestions for AuthorsThis paper presents a brief review of nonaqueous systems in which liquid-liquid phase splitting is induced by the addition of a third component, typically a salt or a carbohydrate. The authors provide a historical overview of studies in this area and then focus on recent results, both experimental and computational. In fact, a substantial portion of the recent results has originated from the authors’ laboratory. The review is well written and can be expected to be very useful for researchers working in this area. I enjoyed reading it. Thus, I recommend publishing this paper with the following minor revisions:
The abstract is much too terse. It is totally inadequate to an otherwise good paper. Statements like “possible applications and further topics of investigations are suggested” do not convey much information. Instead, a much more concrete summary should be given.
Section 4.2.2. It is unclear from this paragraph what kind of prediction can be obtained from the current ML techniques. What was actually calculated in the studies reviewed in this section? Can actual binodal curves be represented?
Also, some grammatical corrections should be made:
Line 307. I believe the authors mean “sensitive”, not “sensible” here.
Line 346. I do not understand the expression “pointed possible applications.”
Author Response
Reviewer 1
Comment 1: The abstract is much too terse. It is totally inadequate to an otherwise good paper. Statements like “possible applications and further topics of investigations are suggested” do not convey much information. Instead, a much more concrete summary should be given.
Response 1: The abstract was re-edited in accordance with the reviewer's suggestion. The revised version is as follows:
The research on nonaqueous two-phase systems, i.e., ternary nonaqueous systems with a liquid-liquid phase split induced by a solid component, is discussed. Previous scattered reports are reviewed and summarized. The first systematic studies are described in detail. They included qualitative testing of numerous ternary systems (a solid component and two liquid solvents, significantly different in polarity) to determine whether a liquid-liquid phase split occurred. Some correlations between this occurrence and the Hofmeister series were suggested. The liquid-liquid equilibrium was determined experimentally in a few systems, and the problems encountered during this determination are discussed. Possible applications and further topics of investigation are suggested.
Comment 2: Section 4.2.2. It is unclear from this paragraph what kind of prediction can be obtained from the current ML techniques. What was actually calculated in the studies reviewed in this section? Can actual binodal curves be represented?
Response 2: The purpose of the ML model application is to predict, with high probability, that a particular solid in a particular binary solvent will induce a liquid-liquid phase split. The following explanation has been added to the text (lines 374-379).
The large number of confirmed and potentially existing NATPS systems suggests the need for a tool to help identify them. This task would be strictly qualitative, focusing on the properties of all three components that guarantee a high probability of liquid-liquid phase separation. Since a vast amount of experimental data already exists [38], it is possible to find correlations between the desired state and certain molecular descriptions of the components. We have taken this approach using machine learning.
Comment 3: Also, some grammatical corrections should be made.
Response 3: English has been corrected extensively in the whole revised manuscript.
Reviewer 2 Report
Comments and Suggestions for AuthorsThis paper presents an overview of an emerging research area with potential applications in extraction, catalysis, and energy storage. Whilst the manuscript is presented as a “review”, in reality it is a mixture of review and original research carried out by the authors, although the latter is presented in a narrative form as opposed to the conventional presentation style used in the scientific literature. The topic is timely and the work presented is extensive, however the authors should consider several major points before publication.
General comments:
The title is too general and may be misleading. It is suggested to change it as “Phase separation in nonaqueous systems by solid particles” or something similar.
The unusual hybrid review and research format merges a literature review with original research results, without a clear section demarcation. This can confuse the reader about what is novel and what is a review.
A large part of the manuscript, especially the part about original research, is written using the first person, which is not the best choice in technical literature because it is perceived as less objective compared to the third person.
Research is presented in a merely qualitative fashion, with limited experimental evidence or theoretical support, and most of the discussion is vague and of speculative nature.
The conclusion does not summarize key findings or articulate a clear agenda for future research.
Figures are of a qualitative nature and not very informative.
Other comments:
Line 26, this issue -> this emerging research area
Line 27, separate -> independent
Line 49, for acetone -> with an acetone
Line 54, yet -> as early as
Line 59, all among -> all of the
Line 106, discussed -> these
Line 118, “in the pure solvent…”
Line 172 & 176, ideality -> the ideal case
Line 197, superiority -> superior effectiveness
Line 201, there appear -> there are
Line 203, regularities -> patterns
Line 214, focusing -> with regards to
Lines 217-218, the two sentences should be connected.
Line 222, position -> ranking
Line 232, has been -> was
Line 239, “The remaining…”
Line 285, “the binary…”
Liner 346, pointed -> mentioned
Refs 39,56,59 are not published therefore should not be published
Author Response
Reviewer 2
Comment 1: The title is too general and may be misleading. It is suggested to change it as “Phase separation in nonaqueous systems by solid particles” or something similar.
Response 1: We agree that the term “nonaqueous two-phase systems” may be misunderstood and is still widely not accepted as a name for a well-defined system, such as “aqueous two-phase systems (ATPS)”. Therefore, at the reviewer’s suggestion, we are changing the title to “Phase separation in nonaqueous systems induced by a solid component”.
Comment 2: The unusual hybrid review and research format merges a literature review with original research results, without a clear section demarcation. This can confuse the reader about what is novel and what is a review.
Response 2: We recognize this problem and were unsure how to classify this manuscript. We propose classifying it as “perspective” rather than “review.” It is a summary of our research in a new field, along with initial suggestions on this theme that can be traced in the literature.
Comment 3: A large part of the manuscript, especially the part about original research, is written using the first person, which is not the best choice in technical literature because it is perceived as less objective compared to the third person.
Response 3: We have found it slightly artificial to describe our own research in the third person. Nevertheless, following the reviewer’s suggestion, we significantly reduced our use of this form of presentation.
Comment 4: Research is presented in a merely qualitative fashion, with limited experimental evidence or theoretical support, and most of the discussion is vague and of speculative nature.
Response 4: Please have a look at this manuscript, presented as a Perspective. These are the first examinations, and it is not possible to draw definitive conclusions. We would like to know exactly what factors determine the observed behavior. As this is merely the beginning of the study, we can identify some correlations and speculate. Regarding the objection that “most of the discussion is vague,” we need more details to respond to these allegations.
Comment 5: The conclusion does not summarize key findings or articulate a clear agenda for future research.
Response 5: The key findings, namely the prevalence of NATPS systems and the identification of the main factors that positively influence phase splitting, are now presented in the “Conclusions and future works” section. Suggestions for future research are also included in this section (lines 405-408, 419-427).
Comment 5: Figures are of a qualitative nature and not very informative.
Response 5: Our aim was to introduce a new research field and the problems associated with it rather than present new data. We agree that it may be insufficient, and we have added one figure illustrating experimental data (Fig. 4, lines 328-356).
Comment 6: Other comments [and here a list of linguistic corrections appears].
Response 6: These are linguistic suggestions. We decided to perform an extensive revision of the entire manuscript to improve the English. We hope that these and similar deficiencies have been finally removed.
Comment 7: Refs 39,56,59 are not published therefore should not be published.
Response 7: This is a question about how to cite finished but still unpublished research. It may be cited as is, or alternatively, these references (“to be submitted”) may be removed, leaving the main body of the text untouched. I think it is the Editor’s role to decide which form is more appropriate. From the reader’s perspective, this issue is immaterial.
Round 2
Reviewer 1 Report
Comments and Suggestions for AuthorsThe authors have revised the manuscript in accordance with my recommendations. I have only one minor comment after reading the revised version. In the Author Contribution section, the authors write "data curation, X.X" instead of including the correct initials. After this minor correction is made, the paper can be published in its current form. I consider this paper a very useful contribution to the literature.
Reviewer 2 Report
Comments and Suggestions for AuthorsThe authors have improved the manuscript compared to the first submission.
