Magnetoelectric Composites: Engineering for Tunable Filters and Energy Harvesting Applications

Round 1

Reviewer 1 Report

Please find attached reviewer's comment. 

Comments for author File: Comments.pdf

Author Response

Reviewer1

The manuscript titled “Magnetoelectric composites: Engineering for tunable filters and energy harvesting applications et al. was reviewed. The investigation of the magnetoelectric properties of materials is a growing and very useful research area. Multiferroic materials are widely acceptable and applicable for multifunctional applications because of their relative availability biological compatibility, and environment adaptability. The magnetic and electrical properties of multiferroic materials are tuneable for diverse application. Multiferroic energy harvesters would inhibit the non-sustainability of lithium-ion batteries and might promote the harvesting of solar energy which is less than 10% tapped. This work is an interesting thematic area that would be of great benefit to the scientific world. I recommend publication of the manuscript. The following highlights are to be properly addressed by the Authors:

Response.

Thank you very much to the reviewer for valuable comments and guidance on my manuscript. Thanks to them, my manuscript has become more valuable. All guidelines and suggestions have been taken into account, and additions and errors have been corrected in the new version of the manuscript. The changes in the text are highlighted.

1. The abstract sections is bereft of the benefits of the research. Authors should emphasize in simple communications the importance of the research.

Response.

We have made all changes according the Reviewer suggestions.

 

2. Authors should check in-text citations; lines 27, 39 and 239 etc have not followed same format. Please, check and adopt similar reporting format

Response.

All citations have been corrected according to the journal format.

3. Authors signified that 6 multiferroic composites were studied. A more detailed discussion on the studied properties vis-à-vis application should be incorporated into the manuscript

Response.

The results of the experimental studies presented in this manuscript are a continuation of the experimental studies presented in the earlier work [37]. In the [37] studies of X-ray diffraction patterns, microstructural, ferroelectric, dielectric, magnetic properties, and DC electrical conductivity of the composite materials were investigated. The researches presented in the work [37] were conducted in terms of searching for a composition with the best properties for new types of memory and electromagnetic converters. The studies have shown that at room temperature, the composite samples exhibit good magnetic and electrical properties. A reference to an earlier publication was cited and X-ray tests were added to the revised version of the manuscript. In the current work, the research was focused towards to obtain P-F multiferroic composite with two impedance peaks for dual-band filters or shields with equilibrium ferroelectric and magnetic structures preserving both properties at room temperature.

A more detailed discussion was added in revised manuscript.

In the Figures 1,2,3 the arrangement of the pictures has been changed according to the growth of the ferroelectric phase. Also in Tables 1,2 , the data has also been arranged in the above pattern.

[37] Bochenek, D.; Niemiec, P.; Chrobak; A. Effect of chemical composition on magnetic and electrical properties of ferroelectromagnetic ceramic composites. Materials, 2021, 14, 2488.

4. Manuscript would be further enhance if Authors can compare prepared composites with available materials as a reference

Response.

Additional literature was introduced to compare the obtained composite materials.

5. On line 101, “XRD studies”. It is imperative that the XRD images of the nanocomposites of the studied composites be included in the manuscript. The manuscript should be self-contained.

Response. 

The missing figure has been added.

6. Refer to Fig. 2 “grain size distribution” How was the grain size determined? Can authors also discuss the importance of grain size vis-à-vis application?

Response.

The average grain size in the multiferroic composites was measured using the graphic editor Image J program using SEM images taken at the same magnification of the whole series of samples.

As it is known, the physical (dielectric) properties of multiferroic materials depend on their microstructure, including homogeneity, grain size and density. The microstructure, in turn, is influenced by a properly conducted technological process of obtaining multiferroic materials (including the mixing powders, the appropriate selection of the method and conditions of synthesis and sintering). In general, the homogeneity of the microstructure of ceramic materials has a positive effect on their final properties, and in the case of dielectric properties, on the degree of diffusion of the phase transition (ferroelectric/paraelectric). Ceramic materials with high uniformity of microstructure show a sharp phase transition. Grain size also affects the dielectric properties of ceramic materials. Materials with smaller grains show a stronger effect of mechanical stress and the external effect of grain boundaries, which results in increased blurring of the phase transition, lower Curie temperature and lower permittivity [41,42]. The dielectric constant of the materials is linearly proportional to the average value of grain size and inversely proportional to the grain boundary thickness (as grain size increases, permittivity increases) [43].

The above addition has been incorporated into the manuscript.

[41] Mao, Ch.; Yan, S.; Cao, S.; Yao, Ch.; Cao, F.; Wang, G.; Dong, X.; Hu, X.; Yang, Ch. Effect of grain size on phase transition, dielectric and pyroelectric propertiesof BST ceramics. J. Eur. Ceram. Soc. 2014, 34, 2933–2939.

[42] Bobić, J.D.; Ivanov, M.; Ilić, N.I.; Dzunuzović, A.S.; Vijatović Petrović, M.M.; Banys, J.; Ribic, A.; Despotovic, Z.; Stojanovic, B.D. PZT-nickel ferrite and PZT-cobalt ferrite comparative study: Structural, dielectric, ferroelectric and magnetic properties of composite ceramics. Ceram. Int. 2018, 44, 6551–6557.

[43] Nayak, P.; Badapanda, T.; Kumar Singh, A.; Panigrahi, S. An approach for correlating the structural and electrical properties of Zr⁴⁺-modified SrBi₄Ti₄O₁₅/SBT ceramic. RSC Adv. 2017, 7, 16319–16331.

7. The references are quite old; about 22 references out of the utilized 46 are quite old. Authors should update the references

Response.

Additional, more recent literature has been introduced.

8. The whole length of the manuscript needs to be checked for grammar and structure e.g. lines 254 – 257; 266 -268 in the conclusion section looks ambiguous. The conclusion should reflect in clear language the importance of the project to the scientific community.

Response.

We have made all changes according the Reviewer suggestions.

Author Response File: Author Response.docx

Reviewer 2 Report

The article is devoted to the study of methods of protection and shielding from the negative effects of electromagnetic radiation generated by a large number of devices, in view of the rapid development of the electronics industry. In general, the presented article is quite interesting and promising in terms of studying the creation of new types of so-called protective shielding materials used to reduce the negative impact of radiation on living organisms. In this regard, the presented results are very promising and interesting, and the problem statement itself is very non-trivial, which distinguishes this work from the total number of scientific studies. However, before this work can be accepted for publication, the authors should answer a number of questions that the reviewer has when reading it.

1. First, in the abstract, in addition to setting the problem, the authors should also indicate the reasons for choosing the multiferroics they propose, as well as what kind of material they propose for its creation.

2. The presented results of morphological features are very interesting, in view of the fact that they clearly show the presence of several phases, about which the authors should give more explanations and details when interpreting the presented SEM images.

3. Also, in addition to the data of mapping and energy-dispersive analysis, the authors should provide data on the phase composition of the samples obtained using the X-ray diffraction method.

4. As is known, the dielectric properties have a pronounced dependence on the density of the material, the authors should write about this in more detail.

5. Also, the authors should consider the possibility of using their materials to protect not only from electromagnetic radiation, but also from the effects of ionizing radiation. Can the materials they offer be used as shielding protective materials.

Author Response

Reviewer2

The article is devoted to the study of methods of protection and shielding from the negative effects of electromagnetic radiation generated by a large number of devices, in view of the rapid development of the electronics industry. In general, the presented article is quite interesting and promising in terms of studying the creation of new types of so-called protective shielding materials used to reduce the negative impact of radiation on living organisms. In this regard, the presented results are very promising and interesting, and the problem statement itself is very non-trivial, which distinguishes this work from the total number of scientific studies. However, before this work can be accepted for publication, the authors should answer a number of questions that the reviewer has when reading it.

Response.

Thank you very much to the reviewer for valuable comments and guidance on my manuscript. Thanks to them, my manuscript has become more valuable. All guidelines and suggestions have been taken into account, and additions and errors have been corrected in the new version of the manuscript. The changes in the text are highlighted.

1. First, in the abstract, in addition to setting the problem, the authors should also indicate the reasons for choosing the multiferroics they propose, as well as what kind of material they propose for its creation.

Response.

The description was supplemented as suggested by the reviewer.

Composite materials composed of two components were selected for detailed studies: (i) ferroelectric (Bi, Nb, Mn-doped PZT material) and (ii) magnetic (nickel-zinc ferrite) with a change in their percentage. The selection of the ferroelectric material (i) was made based on its high dielectric and ferroelectric properties, while in the case of the magnetic component (ii) the relatively high resistance and appropriately, high magnetic properties of ferrite were decisive.

2. The presented results of morphological features are very interesting, in view of the fact that they clearly show the presence of several phases, about which the authors should give more explanations and details when interpreting the presented SEM images.

Response.

The interpretation of microstructural studies has been extended according to the reviewer's comment. In the Figures 1,2,3 the arrangement of the pictures has been changed according to the growth of the ferroelectric phase. Also in Tables 1,2 the data has also been arranged in the above pattern.

3. Also, in addition to the data of mapping and energy-dispersive analysis, the authors should provide data on the phase composition of the samples obtained using the X-ray diffraction method.

Response.  

The missing figure has been added.

4. As is known, the dielectric properties have a pronounced dependence on the density of the material, the authors should write about this in more detail.

Response.

As it is known, the physical (dielectric) properties of multiferroic materials depend on their microstructure, including homogeneity, grain size and density. The microstructure, in turn, is influenced by a properly conducted technological process of obtaining multiferroic materials (including the mixing powders, the appropriate selection of the method and conditions of synthesis and sintering). In general, the homogeneity of the microstructure of ceramic materials has a positive effect on their final properties, and in the case of dielectric properties, on the degree of diffusion of the phase transition (ferroelectric/paraelectric). Ceramic materials with high uniformity of microstructure show a sharp phase transition. Grain size also affects the dielectric properties of ceramic materials. Materials with smaller grains show a stronger effect of mechanical stress and the external effect of grain boundaries, which results in increased blurring of the phase transition, lower Curie temperature and lower permittivity [41,42]. The dielectric constant of the materials is linearly proportional to the average value of grain size and inversely proportional to the grain boundary thickness (as grain size increases, permittivity increases) [43].

The above addition has been incorporated into the manuscript.

[41] Mao, Ch.; Yan, S.; Cao, S.; Yao, Ch.; Cao, F.; Wang, G.; Dong, X.; Hu, X.; Yang, Ch. Effect of grain size on phase transition, dielectric and pyroelectric propertiesof BST ceramics. J. Eur. Ceram. Soc. 2014, 34, 2933–2939.

[42] Bobić, J.D.; Ivanov, M.; Ilić, N.I.; Dzunuzović, A.S.; Vijatović Petrović, M.M.; Banys, J.; Ribic, A.; Despotovic, Z.; Stojanovic, B.D. PZT-nickel ferrite and PZT-cobalt ferrite comparative study: Structural, dielectric, ferroelectric and magnetic properties of composite ceramics. Ceram. Int. 2018, 44, 6551–6557.

[43] Nayak, P.; Badapanda, T.; Kumar Singh, A.; Panigrahi, S. An approach for correlating the structural and electrical properties of Zr⁴⁺-modified SrBi₄Ti₄O₁₅/SBT ceramic. RSC Adv. 2017, 7, 16319–16331.

5. Also, the authors should consider the possibility of using their materials to protect not only from electromagnetic radiation, but also from the effects of ionizing radiation. Can the materials they offer be used as shielding protective materials.

Response.

Thank very much for this new idea! We have really just found very last publication for successful application of ferroelectric an magnetic composites against ionizing radiation and add it at the end of Introduction Section

Author Response File: Author Response.docx

Round 2

Reviewer 2 Report

The authors answered all the questions, the article can be accepted for publication.