The Structural and Dielectric Properties of Bi3−xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75, 1.0)
Round 1
Reviewer 1 Report
The authors report Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75, 1.0) compounds. I have minor comments.
There are many missing spaces:
"X-ray structural studies have shown that all compounds are single-phase and have the structure of Aurivillius phases (APs) with close parameters of orthorhombic unit cells corresponding tospace group A21am."
-> “tospace” should be “to space”
"The piezoelectric constantd33was measured for all compounds of the synthesized series."
-> “constantd33was” should be “constant d33 was”
"The structure of Bi2Am-1BmO3m+3 compounds above the Curie point TC is tetragonal andbelongs to the space group I4 / mmm."
-> “andbelongs to” should be “and belongs to”
"This workconsiders the conditions for the existence of these compounds [11]"
-> “workconsiders” should be “work considers”
"as well as on the cell parameters, was carried out in [12].Some anomalies in the"
-> “[12].Some” should be “[12]. Some”
“skite layers m.Despite the fact that” -> “skite layers m. Depsite the fact that”
“(piezoelectric, ferroelectric, etc.).They demonstrate low” -> “(piezoelectric, ferroelectric, etc.). They demonstrate low”
“sin addition to high Curie temperatures(TC ≤ 965°C)[14, 15].” -> “s in addition to high Curie temperatures(TC ≤ 965°C)[14, 15].”
“has been placed on the design and studies ofnew APs" -> “has been placed on the design and studies of new APs"
“SrBi4Ti4O15 (SBTi),SrBi2Ta2O9 (SBTa),” -> “SrBi4Ti4O15 (SBTi), SrBi2Ta2O9 (SBTa),”
“(Bi2O2) 2+ layers between whichthere are (BiTiNbO7) 2– layers [26]” -> “(Bi2O2) 2+ layers between which there are (BiTiNbO7) 2– layers [26]”
“(A-position) isreplaced by neodymium ions of the basic composition Bi3Ti1.5W0.5O9.” -> “(A-position) is replaced by neodymium ions of the basic composition Bi3Ti1.5W0.5O9.”
“a laboratory muffle furnace in air.Then, the samples were repeatedly” -> “a laboratory muffle furnace in air. Then, the samples were repeatedly”
“The X-ray diffraction patterns were recorded on a DRON-3M diffractometerwith attachment for powder diffractionand an X-ray tube BSV21-Cu with a Cu X-ray tube.” -> “The X-ray diffraction patterns were recorded on a DRON-3M diffractometer with attachment for powder diffraction and an X-ray tube BSV21-Cu with a Cu X-ray tube.”
“whereRA and RB are the radii of cations in positions A and B, respectively”
-> “where RA and RB are the radii of cations in positions A and B, respectively;”
“the tolerance coefficient t was calculated takinginto account the”
-> “the tolerance coefficient t was calculated taking into account the”
“Eaisthe activation energy.”
-> “Ea is the activation energy.”
“(x = 0.25, 0.5, 0.75) have different temperature rangesin Fig. 4,”
-> “(x = 0.25, 0.5, 0.75) have different temperature ranges in Fig. 4,”
“where position Ais occupied by Bi3+ ions”
-> “where position A is occupied by Bi3+ ions”
“Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75, 210 1.0)were synthesized by the solid-state method.”
-> “Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75, 210 1.0) were synthesized by the solid-state method.”
Other comments are:
“It was previously studied that the partial replacement of bismuth ions by neodymium cations in the series of perovskite-like Bi-containing oxides Bi3TiNbO9,Bi3TiTaO9 led to a significant decrease in the phase transition temperature (Curie temperature TC) and a change in dielectric properties.”
-> the reference is missing in this sentence.
“the high purity grade (extra pure).”
-> Do the authors have any specific number for the purity, such as 99.9995%?
The inset figure of Figure 2 is too small to be readable.
“electrodes were deposited using an Ag paste annealed at a temperature of 700 °C (for 1 h).”
-> Is Ag paste not oxidized at 700 ⁰C? What was the atmosphere?
The vertical axis label is overlapping the tick labels in the loss tangent plot of Bi2 Nd Ti1.5 W0.5 O9 (Figure 3).
All the atomic ratios need to be subscripts in Figure 3.
The vertical axis labels are wrong in Figure 4.
“For the Bi3-xNdxTi1.5W0.5O9(x = 0.75) the piezoelectric constant d33 could not be 207 measured.”
-> Is x supposed to be 1 in this sentence?
“The temperature and frequency dependences of the 116 dielectric characteristics were measured using an E7-20 immittance meter in the frequency 117 range from 100kHz to 1 MHz and at temperatures in the range from room temperature to 118 900°C.”
-> Was the measurement done under vacuum or inert environment?
Author Response
in this file answers to your comments
Author Response File: 
Author Response.pdf
Reviewer 2 Report
The manuscript entitled “The Structural and Dielectric Properties of Bi3-xNdxTi1.5W0.5O9 (x = 0.25,0.5,0.75,1.0)” submitted by Sergei V. Zubkov and co-workers for consideration for publication in the MDPI journal Electronics presents the investigation of a new series of layered perovskite-like oxides Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5,0.75, 1.0). Presented data needs additional revision. Moreover, I am not sure the manuscript can find an audience in "Electronics", mainly due to no correlation between the presented data and the scope of the journal. Therefore, I cannot recommend the publication of the manuscript in the MDPI journal Electronics. What is more, the following part should be revised before the net submission.
- Line 16, what do you mean with the following sentence: The piezoelectric constantd33was measured for all compounds of the synthesized series?
- The whole manuscript should be checked carefully, I noticed many additional spaces or their lack between particular words.
- Figure 1 is too small
- What is the reason that the spectra in Figure 2 are so thick?
- The experimental XRD pattern should be calculated and presented in the manuscript.
- All figures (especially Figures 3 and 4) are too small and should be revised.
- Description of all symbols and the units should be presented in the text. Partially, the current presentation can lead to the misunderstanding of part of symbols.
- What are the reasons that this article will be of interest and importance to other researchers? How can the other scientists use them?
Author Response
Response to Reviewer Comments
Dear Editor and Reviewer 2：
Thank you for your precious comments and advice. These comments are all valuable and very helpful for revising and improving our manuscript, as well as the important guiding significance to our researches. We have read your comments carefully and have provided explanations and made corrections, which we hope will meet your approval. The revisions made in the manuscript are marked in yellow. Our point-by-point responses are given below:
Point 1: Line 16, what do you mean with the following sentence: The piezoelectric constantd33was measured for all compounds of the synthesized series?
Response 1: should be Response 1: The piezoelectric constant d33 was measured for Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75) compounds of the synthesized series.
Point 2: The whole manuscript should be checked carefully, I noticed many additional spaces or their lack between particular words.
Response 2: we fixed this defect
Point 3: Figure 1 is too small
Response 3: we enlarged figure 1 a little
Point 4: What is the reason that the spectra in Figure 2 are so thick?
Response 3: we made the lines thinner
Point 5: All figures (especially Figures 3 and 4) are too small and should be revised
Response 5: we enlarged the pictures a little
Point 6: Description of all symbols and the units should be presented in the text. Partially, the current presentation can lead to the misunderstanding of part of symbols.
Response 6: we tried to describe all parameters and symbols as fully as possible
Point 7: What are the reasons that this article will be of interest and importance to other researchers? How can the other scientists use them?
Response 7: there are several reasons:
- Replacement of Bi3+ ions with Nd3+ ions, which have an ionic radius less than the ionic radius of bismuth, leads to a decrease in the Curie temperature TC. This effect is observed only upon doping with niodymium ions.
- Isovalent substitution of Bi3+ ions by Nd3+ ions leads to a decrease in oxygen vacancies and leakage current and, accordingly, to a decrease in the dielectric loss tangent.
- Elements Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75, 1.0) of the synthesized series can become the basis for creating new lead-free piezo-ferroelectric materials.
- We are the first to assert that the substitution of neodymium ions for bismuth in compounds of the Aurivillius family of phases will lead to a decrease in the phase transition temperature and an improvement in piezoelectric properties.
Once again, we really appreciate your efforts in reviewing our manuscript during these unprecedented and challenging times. We wish good health to you, your family, and community. Your careful review has helped to make our study clearer and more comprehensive. We hope that our revised manuscript meets the publication standards.
We look forward to hearing from you. Sincerely, Zubkov Sergei.
Author Response File: Author Response.pdf
Reviewer 3 Report
The paper by Sergei V. Zubkov et al. reports a new series of layered perovskite-like oxides Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5,0.75, 1.0), a promising perovskite, is successfully synthesized by the method of high-temperature solid-state reaction. In this article, they have studied detailed temperature and frequency dependent dielectric properties, structural properties and piezoelectric constant. However, most of the analyses are not well organized and can be improved to support the proposed aim of this work and the discussions. Overall, this manuscript is probably publishable on this journal, but authors have to address the following issues before accepted:
- Rietveld refinement of the XRD-data are recommended for better crystal structures analysis.
- The FESEM images of these series of samples should be provided.
- In figure 3, author didn’t mention why ε (T) and loss tangent value changes with increase of ‘x’ values and frequencies. Why two curves nature are totally different for x=1.0?
- ‘Figure 4. Dependence of lnσ on 10000/T for the Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75) sample.’ Please check if it is 1000/T or 10000/T.
- Why dielectric constant is high at low frequency?
- What is the grain and grain boundary contribution to the dielectric properties of this samples?
- Cole-Cole plots should be provided for better understanding.
- Which kind of polarization effect contribute to the dielectric constant for this samples?
- The Figures are not clear. The text and graphics in many figures are very blurry. In order to simplify the reader's reading, it is recommended that the author modify the figures.
- The contents in the introduction should be improved carefully. Most of the references are too old. Authors should update the references. Thus, some newly studies would be useful for this study, which could be cited in in the introduction: Journal of Alloys and Compounds 892, 2022, 162216. doi.org/10.1016/j.jallcom.2021.162216; Electron. Mater. Lett. 17, 229–239 (2021); org/10.1016/j.ceramint.2020.02.243; etc.
Author Response
Response to Reviewer Comments
Dear Editor and Reviewer 3：
Thank you for your precious comments and advice. These comments are all valuable and very helpful for revising and improving our manuscript, as well as the important guiding significance to our researches. We have read your comments carefully and have provided explanations and made corrections, which we hope will meet your approval. The revisions made in the manuscript are marked in red. Our point-by-point responses are given below:
Point 1: Rietveld refinement of the XRD-data are recommended for better crystal structures analysis
Response 1: The analysis of the profiles of the diffraction patterns, the determination of the positions of the lines, their indexing (hkl), and refinement of the unit cell parameters were performed by using the PCW 2.4 program [41].
Point 2: The FESEM images of these series of samples should be provided.
Response 2: we will try to apply FESEM images in subsequent studies
Point 3: In figure 3, author didn’t mention why ε (T) and loss tangent value changes with increase of ‘x’ values and frequencies. Why two curves nature are totally different for x=1.0?
Response 3: The temperature dependence of the relative permittivity ε/ε0 for the NPs Bi3-x NdxTi1.5W0.5O9 (x = 1.0) at a frequency from 100 kHz to 1 MHz has a strongly diffuse transition, which is usually typical of ferroelectric relaxors.
Point 3: ‘Figure 4. Dependence of lnσ on 10000/T for the Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75) sample.’ Please check if it is 1000/T or 10000/T.
Response 3: ‘Figure 4. Dependence of lnσ on 1/T for the Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75) sample.’
Point 4: Why dielectric constant is high at low frequency?
Response 4: this is a generally accepted fact and is usually not discussed
Point 5: What is the grain and grain boundary contribution to the dielectric properties of this samples?
Response 5: in this study, we do not present the microstructure and therefore do not analyze the effect of the grain and grain boundary on the dielectric properties
Point 6: Cole-Cole plots should be provided for better understanding.
Response 6: unfortunately my Cole-Cole Charts articles don't use this method.
Point 7: The Figures are not clear. The text and graphics in many figures are very blurry. In order to simplify the reader's reading, it is recommended that the author modify the figures.
Response 7: we tried to improve the drawings
Point 8: The contents in the introduction should be improved carefully. Most of the references are too old. Authors should update the references. Thus, some newly studies would be useful for this study, which could be cited in in the introduction: Journal of Alloys and Compounds 892, 2022, 162216. doi.org/10.1016/j.jallcom.2021.162216; Electron. Mater. Lett. 17, 229–239 (2021); org/10.1016/j.ceramint.2020.02.243; etc.
Response 8: we have made a change to the list of references
- Senguptaa, P.; Sadhukhanb, P.; Rayb, A.; Malb, S.; Singhc, Raya, A. R.; Bhattacharyyad, S; Dasb, S. Influence of activation energy on charge conduction mechanism and giant dielectric relaxation of sol-gel derived C3H7NH3PbBr3 perovskite; Act as high performing UV photodetector. Alloys and Compounds. 2021, 892, 162216.
- Zdorovets, M.; A.; Arbuz, A.; Tishkevich, Zubar, D.; T.Trukhanov, A. Phase transformations and changes in the dielectric properties of nanostructured perovskite-like LBZ composites as a result of thermal annealing. Ceramics International. 2020, 46, 14460.
- Sengupta, P.; Sadhukhan, P.; Ray, A.; Ray, R.; Bhattacharyya, S.; Das, S. Temperature and frequency dependent dielectric response of C3H7NH3PbI3: A new hybrid perovskite J. Appl. Phys. 2020, 127, 204103.
- Kozlovskiya, A. L.; Kenzhinab, I. E.; Zdorovetsb, M. V.; Saiymovaa, M.; Tishkeviche, D. I.; Trukhanove , S. V.; Trukhanov, A. V. Synthesis, phase composition and structural and conductive properties of ferroelectric microparticles based on ATiOx (A = Ba, Ca, Sr). Ceramics International. 2019, 45, 17236
Once again, we really appreciate your efforts in reviewing our manuscript during these unprecedented and challenging times. We wish good health to you, your family, and community. Your careful review has helped to make our study clearer and more comprehensive. We hope that our revised manuscript meets the publication standards.
We look forward to hearing from you. Sincerely, Zubkov Sergei.
Author Response File: Author Response.pdf
Round 2
Reviewer 2 Report
The revised manuscript entitled “The Structural and Dielectric Properties of Bi3-xNdxTi1.5W0.5O9 (x = 0.25, 0.5, 0.75, 1.0)” resubmitted by Sergei V. Zubkov and co-workers for reconsideration for publication in the MDPI journal Electronics presents a higher level than the first submission. The Authors have performed the required corrections only partially and added additional explanations. Nevertheless, the modifications are not careless. There are still elements that must be revised. I can recommend a minor revision.
- Figure 1 should be bigger
- All Figures should be presented in the same way, a description of the y and x-axis should be added. All numbers should contain points not commas. The units should be presented in all Figures.
- The references should be revised
Author Response
Response to Reviewer Comments
Dear Editor and Reviewer2：
Thank you for your precious comments and advice. These comments are all valuable and very helpful for revising and improving our manuscript, as well as the important guiding significance to our researches. We have read your comments carefully and have provided explanations and made corrections, which we hope will meet your approval. The revisions made in the manuscript are marked in yellow. Our point-by-point responses are given below:
Point 1: Figure 1 should be bigger
Response 1: we enlarged Figure 1
Point 2: All Figures should be presented in the same way, a description of the
y and x-axis should be added. All numbers should contain points not
commas. The units should be presented in all Figures.
Response 2:
Figure 2.Y-axis is intensity, X-axis is angle in degrees
Figure 3. Left column: Y-axis is relative dielectric constant, X-axis is temperature (degrees Celsius).
Figure 4: Y-axis is the logarithm of conductivity; X-axis is temperature in Kelvin
Figure 5. Y-axis is the crystal lattice parameters in Angstroms. X-X (Ndx)
Point 3: The references should be revised
Response 3: The references revisions made in the manuscript are marked in yellow.
Once again, we really appreciate your efforts in reviewing our manuscript during these unprecedented and challenging times. We wish good health to you, your family, and community. Your careful review has helped to make our study clearer and more comprehensive. We hope that our revised manuscript meets the publication standards.
We look forward to hearing from you. Sincerely, Zubkov Sergei.
Reviewer 3 Report
No more comments. Now the paper can be accepted in present form.
Author Response
We really appreciate your efforts in reviewing our manuscript during these unprecedented and challenging times. We wish good health to you, your family, and community. Your careful review has helped to make our study clearer and more comprehensive.
