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Article
Peer-Review Record

Multifunctional Synergistic Response Induced by Phase Transition in Molecular Compounds

Magnetochemistry 2025, 11(5), 41; https://doi.org/10.3390/magnetochemistry11050041
by Xiao-Feng Chen 1, Tao Wang 1, Dan Liao 1, Nan Wu 1, Yan Peng 1,*, Shi-Yong Zhang 2,* and Zhao-Bo Hu 1,*
Reviewer 1:
Reviewer 2: Anonymous
Reviewer 3:
Magnetochemistry 2025, 11(5), 41; https://doi.org/10.3390/magnetochemistry11050041
Submission received: 31 March 2025 / Revised: 4 May 2025 / Accepted: 6 May 2025 / Published: 9 May 2025

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

The manuscript titled “Multifunctional Synergistic Response Induced by Phase Transition in Molecular Compounds” presents two organic-inorganic hybrid materials and reports a magnetic-dielectric coupling effect. The study is interesting and has potential significance; however, several issues should be addressed before the manuscript can be recommended for publication.

  1. Currently, only DSC data are provided for Compounds 1 and 2. To better characterize their thermal behavior, thermogravimetric (TG) analysis should be included. This would help determine key temperature points (e.g., onset decomposition temperature) and provide a more reliable reference for the DSC testing range.
  2. The vertical axis label in Figure 2 is given as “cm³ mol⁻¹ K”, which should be corrected to the standard format “cm³ K mol⁻¹” for consistency with SI conventions.
  3. Some figures in the main text appear inconsistent with the described content, and a few seem to be missing. Please carefully review and ensure all figures are properly included and correctly referenced.

  4. The temperature-dependent χMT plots (heating/cooling) are separated from their corresponding legends, making interpretation difficult. These should be placed on the same page for clarity.

  5. The dielectric properties section focuses solely on Complex 1, while Complex 2 is not discussed. For a comprehensive comparison, the dielectric behavior of Complex 2 should also be analyzed and included in the discussion.

Author Response

Comment 1: Currently, only DSC data are provided for Compounds 1 and 2. To better characterize their thermal behavior, thermogravimetric (TG) analysis should be included. This would help determine key temperature points (e.g., onset decomposition temperature) and provide a more reliable reference for the DSC testing range.

Response: We have added the TG curves in Supporting Information (Figure S4) for both compounds. And added the description in revised manuscript as follows:

The thermogravimetric analysis (TGA) curves of compounds 1 and 2 are shown in Figure S4. It can be seen from the figures that both compounds are decomposed at about 525 K, showing excellent thermal stability.

Comment 2: The vertical axis label in Figure 2 is given as “cm³ mol⁻¹ K”, which should be corrected to the standard format “cm³ K mol⁻¹” for consistency with SI conventions.

Response: As suggested, cm³ mol⁻¹ K have been changed to cm³ K mol⁻¹.

Comment 3: Some figures in the main text appear inconsistent with the described content, and a few seem to be missing. Please carefully review and ensure all figures are properly included and correctly referenced.

Response: The errors in the article have been corrected accordingly.

Comment 4: The temperature-dependent χMT plots (heating/cooling) are separated from their corresponding legends, making interpretation difficult. These should be placed on the same page for clarity.

Response: Plots and corresponding legends have been placed on the same page.

Comment 5: The dielectric properties section focuses solely on Complex 1, while Complex 2 is not discussed. For a comprehensive comparison, the dielectric behavior of Complex 2 should also be analyzed and included in the discussion.

Response: The analysis of the dielectric properties of compound 2 was supplemented as suggested.

Author Response File: Author Response.pdf

 

 

Reviewer 2 Report

Comments and Suggestions for Authors

The manuscript "Multifunctional synergistic response induced by 2 phase transition in molecular compounds" describes study of two complexes, which undergo phase transition at high temperature.

The manuscript should be thoroughly revised, I think some points should be improved before recommending its publication in "Magnetochemistry" journal:

In the part " 2. Materials and Methods ":

1) – the description of all physical methods should be given. What instrument was used for the magnetic measurements? Detailed information is needed. Mass of the sample, temperature sweep rate, etc. Have you tried repeating the heating-cooling cycles several times?

2) – An elemental analysis data should be given for the complexes.

In the part " 3. Results and Discussion ":

3) Temperature-dependent PXRD patterns for the complex 1 indicate the phase transition in the 309-320 K temperature range, whereas magnetic measurements revealed the transition at 329 K. An explanations or some comments should be given in the text.

4) The results of DSC study are missing in the text, although they are mentioned in the introduction.

5) What kind of sample (tiny powder, polycrystalline sample or single crystal) was used for the dielectric measurements? The text does not agree with the figure 3.

6) Is there hysteresis in the dielectric curves, like to magnetic data?

 

Author Response

Comment 1: the description of all physical methods should be given. What instrument was used for the magnetic measurements? Detailed information is needed. Mass of the sample, temperature sweep rate, etc. Have you tried repeating the heating-cooling cycles several times?

Response: The authors add the instrumentation for magnetic measurements in 2.1 Materials. We tried repeating the heating-cooling cycles several times.

Comment 2: An elemental analysis data should be given for the complexes.

Response: The elemental analysis data have been collected and the resulted were added in revised manuscript.

Comment 3: Temperature-dependent PXRD patterns for the complex 1 indicate the phase transition in the 309-320 K temperature range, whereas magnetic measurements revealed the transition at 329 K. An explanations or some comments should be given in the text.

Response: Differences in sample preparation (e.g., crystallinity, grain size, or strain) between PXRD and magnetic measurements could lead to variations in the observed transition temperatures.

Comment 4: The results of DSC study are missing in the text, although they are mentioned in the introduction.

Response: The authors did not perform the DSC test and it is in the referenced literature.

Comment 5: What kind of sample (tiny powder, polycrystalline smple or single crystal) was used for the dielectric measurements? The text does not agree with the figure 3.

Response: Powder sample was used for the dielectric measurements. The authors have rewritten the dielectric properties section.

Comment 6: Is there hysteresis in the dielectric curves, like to magnetic data?

Response: Yes. We added the curve in revised Supporting Information (Figure S5).

Author Response File: Author Response.pdf

 

 

Reviewer 3 Report

Comments and Suggestions for Authors

The scientific content of the ms is interesting and this work thus deserves –according to my opinion- acceptance and publication in “Magnetochemistry”. I am sure that the article will attract the intense interest of scientists working in the area of molecular bistable materials, especially the organic-inorganic ones. Also, I do believe that the paper will receive a respectable number of citation in the future. Salient features of this work –which support my proposal for acceptance- are: (a) The two ionic compounds exhibit a first-order structural phase transition at high temperatures. (b) At the phase transition temperatures, both the magnetic and dielectric properties of both compounds show bistable behavior, and (c) There are magnetic-dielectric coupling effects in the two materials. The manuscript is well-organized. The quality of figures is high and the references list covers the topic under study satisfactorily. Supplementary Info is diagnostic and valuable.

Based on the above mentioned, I am more than happy to recommend acceptance of this fine piece of research in “Magnetochemistry”. Minor revision points/suggestions/comments are listed below:

  1. The experimental section lacks microanalytical data (C, H, N), yields and IR wavenumbers for the two complexes.
  2. The English of the ms should be polished.
  3. There are typographic errors, e.g. a comma is missing in the caption of Figure 1.
  4. The “Conclusions” section is short. It should become larger and the authors should briefly mention the perspectives of their work.
  5. According to my opinion, Figures S1 and S2 should be transferred into the main body of the ms.
  6. The authors should briefly discuss the content of Ref. [52], which describes the structures of the two complexes and highlight the new science in this article.
  7. “Introduction” and elsewhere: The authors should write the formulae of the complexes. The TMAA-MCl4 representation is confusing. The correct formulae should be written as (TMAA)2[MCl4]. The hydroxide should be written as (TMAA)OH.
  8. “Introduction”: The TMAA cation should be defined (it is defined only in the “Abstract”).  

Comments on the Quality of English Language

The English of the ms should be polished.

 

Author Response

Comment 1: The experimental section lacks microanalytical data (C, H, N), yields and IR wavenumbers for the two complexes.

Response: As suggested, microanalytical data (C, H, N), yields and IR wavenumbers for both compounds were added into 2.2 and 2.3 (Figure S3).

Comment 2: The English of the ms should be polished.

Response: We have checked the English carefully for whole manuscript.

Comment 3: There are typographic errors, e.g. a comma is missing in the caption of Figure 1.

Response: This comma has been added to the sentence as suggested. The sentence is as follows:

The molecular structures of 1 (a) and 2 (b). The pink, dark red, bright green blue, and gray spheres represent Co, Mn, Cl, N, and C atoms, respectively.

Comment 4: The “Conclusions” section is short. It should become larger and the authors should briefly mention the perspectives of their work.

Response: As suggested, the authors have added a concluding section.

Comment 5: According to my opinion, Figures S1 and S2 should be transferred into the main body of the ms.

Response: As suggested, Figures S1 and S2 were transferred to the body of the paper as Figures 1(a) and 1(b).

Comment 6: The authors should briefly discuss the content of Ref. [52], which describes the structures of the two complexes.

Response: Following the suggestion, the authors have deleted part of the crystal structure description of reference [52] and highlighted the new science in this manuscript.

Comment 7: “Introduction” and elsewhere: The authors should write the formulae of the complexes. The TMAA-MCl4 representation is confusing. The correct formulae should be written as (TMAA)2[MCl4]. The hydroxide should be written as (TMAA)OH.

Response: As suggested, TMAA-MCl4 have been changed to (TMAA)2[MCl4]. The hydroxide be written as (TMAA)OH.

Comment 8: “Introduction”: The TMAA cation should be defined (it is defined only in the “Abstract”).

Response: The TMAA cation s defined in the “Introduction”.

Author Response File: Author Response.pdf

 

 

 

Round 2

Reviewer 2 Report

Comments and Suggestions for Authors

The manuscript has been improved after the revision. Nevertheless, the novelty is low, the main results were already presented in the previous work (Shao, T.; Ren, R. Y.; Huang, P. Z.; Ni, H. F.; Su, C. Y.; Fu, D. W.; Xie, L. Y.; Lu, H. F. Metal ion modulation triggers dielectric double switching and green fluorescence in A2MX4-type compounds. Dalton Trans. 2022, 51, 2005-2011.). 

Elemental analysis indiсates the presence of water molecules, which is inconsistent with the XRD data. Water molecules should give H-bonds and can be easily detected on XRD.

Author Response

We focus on the synergetic effect of magnetic and dielectric properties, it is normal to test the reported molecules. The PXRD was measured by ourself with fresh prepared sample. The EA was measured in the instrumental analysis center in our university, which means we should send the samples to the center and wait for the measurements. Since such compounds are easy to absorb moisture, it is possible to have water molecules for the EA results.

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