Investigation of BaFe12O19 Hexaferrites Manufactured by Various Synthesis Methods Using a Developed Pulsed Magnetometer
, Viktor A. Zhuravlev 1,*, Olga A. Dotsenko 1 and Roman V. Minin 3Round 1
Reviewer 1 Report
Dmitry V. Wagner and colleagues presented an interesting manuscript that reports on the synthesis of hexaferrite particles by various synthesis methods and the development of a magnetometer to test the magnetic properties of synthesized samples. Although I appreciate the work overall, some corrections must be made before publication.
1) The title should be changed. Now it does not reflect the important part of the work - the development of the pulse magnetometer.
2) Also, the abstract must be improved. In particular, it is necessary to specify what new knowledge has been obtained as a result of this work.
3) The introduction lacks a description of the current state of the art on methods of measuring magnetic properties, and a large part of the work is devoted to this. Please indicate what is the advantage of the device described here compared to the existing ones.
4) Line 25: “Ferrites are simultaneously a ferromagnet and a dielectric…” Please, specify here the kind of ferrites (ferrites is a big family of materials with different chemical composition and structural properties (spinel ferrites, hexaferrites, ferrites with perovskite structure), which have very different, not always ferrimagnetic, properties).
5) Lines 25-26: “… have high values of magnetic properties, such as saturation magnetization, magnetic permeability” -> “… have high values of saturation magnetization and magnetic permeability”. It is not correct to say “high values of magnetic properties”. Alternatively, use the word “quantities”.
6) Lines 34-35: Please explain in more detail what new properties the synthesis methods provide?
7) Please, divide section “2. Materials and Methods” into subsections, e.g., “2.1 Synthesis of samples”; “2.2 Development of pulse magnetometer”; “2.3 Structural and morphological properties of samples”.
8) Please, instead of national standards (“pur.”, “p.a”, “CP” and GOST) use international standards of purity (e.g., >98%) of reagents in the Materials and Methods section.
9) Please, indicate the speed used in the planetary mill.
10) Please, check eq. (3) and eq. (4). There is a disagreement. Also, in eq.(4) is a mistake Ba(NO3)3 -> Ba(NO3)2.
11) Line 168: Please, confirm that the name of this unit “magnetic field pulse forming unit” is correct? I guess this unit forms a pulse of electric current which produces the pulse of the magnetic field in the solenoid.
12) Line 172: This sentence should be at the beginning of the previous paragraph.
13) Please, indicate in the Materials and Methods section the materials and wavelength of the X-ray of the used source.
14) Please, add more details on how the size of particles was analyzed with a laser particle size analyzer. This was done for powder or dissolved samples? Were powders preliminary ground?
15) Table 1: please, correct the caption: this table contains not only results of XRD. Please also indicate errors for CSR and other quantities.
16) Figure 5: Please, show SEM pictures of different samples with the same scale bar. It will make a more easy comparison of morphology between samples.
17) For magnetic properties please indicate of temperature at which they were determined, and put this information on the caption of the corresponding figure and table.
18) Why maximal magnetic field was 26 kOe while in the description of the setup was indicated 100 kOe? It seems that samples are not saturated at the used magnetic field.
19) Lines 334-335: How exactly magnetocrystalline anisotropy fields Ha was determined? Please comment on result of this calculation.
20) Line 352: “weakly magnetic phase” -> “weak ferrimagnetic phase”.
21) Please, check sentence lines 361-364: it is not clear the part “with the magnetic ordering of the easy axis (EA) type”.
22) Lines 376-377: this conclusion is not supported by the results.
23) Lines 389-392: This conclusion is misleading because the sizes indicated were determined by a laser particle size analyzer, not electron microscopy, as stated in the beginning.
Author Response
Response for Reviewer #1
Article title: Investigation of BaFe12O19 hexaferrites manufactured by various synthesis methods using the developed pulsed magnetometer.
Authors: Dmitry V. Wagner*, Katerina V. Kareva, Viktor A. Zhuravlev*, Olga A. Dotsenko, Roman V. Minin.
Manuscript ID: inventions-2155407
Dmitry V. Wagner and colleagues presented an interesting manuscript that reports on the synthesis of hexaferrite particles by various synthesis methods and the development of a magnetometer to test the magnetic properties of synthesized samples. Although I appreciate the work overall, some corrections must be made before publication.
Comment 1
1) The title should be changed. Now it does not reflect the important part of the work - the development of the pulse magnetometer.
Response:
We would like to thank the referee for pointing out the constructive comment that helps us to improve the manuscript. We have changed the title, which is now more in line with the essence of the article: Investigation of BaFe12O19 hexaferrites manufactured by various synthesis methods using the developed pulsed magnetometer.
Comment 2
2) Also, the abstract must be improved. In particular, it is necessary to specify what new knowledge has been obtained as a result of this work.
Response:
We thank the reviewer for the comment and agree with it. In the abstract we added new results obtained in the article.
Comment 3
3) The introduction lacks a description of the current state of the art on methods of measuring magnetic properties, and a large part of the work is devoted to this. Please indicate what is the advantage of the device described here compared to the existing ones.
Response:
Thank the referee for pointing out the constructive and important comment. We added necessary information devoted to development of these methods. In «Materials and Methods» we noted that our installation makes it possible to measure the full cycle of hysteresis loop.
Comment 4
4) Line 25: “Ferrites are simultaneously a ferromagnet and a dielectric…” Please, specify here the kind of ferrites (ferrites is a big family of materials with different chemical composition and structural properties (spinel ferrites, hexaferrites, ferrites with perovskite structure), which have very different, not always ferrimagnetic, properties).
Response:
Thank the reviewer for the comment. We specified in the text that it relates to hexaferrites of all types.
Comment 5
5) Lines 25-26: “… have high values of magnetic properties, such as saturation magnetization, magnetic permeability” -> “… have high values of saturation magnetization and magnetic permeability”. It is not correct to say “high values of magnetic properties”. Alternatively, use the word “quantities”.
Response:
Thank the referee for pointing out the important comment. The grammatical error in the sentence has been corrected.
Comment 6
6) Lines 34-35: Please explain in more detail what new properties the synthesis methods provide?
Response:
We thank the reviewer for the comment. There was an inaccuracy in the sentence, we rephrased and supplemented it.
Comment 7
7) Please, divide section “2. Materials and Methods” into subsections, e.g., “2.1 Synthesis of samples”; “2.2 Development of pulse magnetometer”; “2.3 Structural and morphological properties of samples”.
Response:
We thank the reviewer for the comment and agree with it. The section 2 was separated into 3 subsections for greater readability.
Comment 8
8) Please, instead of national standards (“pur.”, “p.a”, “CP” and GOST) use international standards of purity (e.g., >98%) of reagents in the Materials and Methods section
Response:
Thanks to the reviewer for an important remark that improves the quality of our work. We changed national standards to international standards for the reagents.
Comment 9
9) Please, indicate the speed used in the planetary mill.
Response:
We thank the reviewer for the comment. We added the speed information in the paragraph.
Comment 10
10) Please, check eq. (3) and eq. (4). There is a disagreement. Also, in eq.(4) is a mistake Ba(NO3)3 -> Ba(NO3)2.
Response:
We thank the reviewer for the attention. The typo in the eq.(3) has been corrected. The procedure for carrying out the synthesis in the sol-gel combustion mode is described in [1]. The choice of this ratio is due to previous studies [2], which reported that an excess of barium is necessary to ensure the formation of single-phase BaFe12O19 due to the fact that a small amount of barium volatilizes during combustion and calcination, which leads to a violation of stoichiometry [3]. Relevant explanation and links will be added to the text of the article.
The typo in the eq.(4) has been also corrected.
[1] Bahadur, D.; Rajakumar, S.; Kumar, A. Influence of fuel ratios on auto combustion synthesis of barium ferrite nano particles. J. Chem. Sci., 2006, 118(1), P. 15–21.
[2] Huang, J.; Zhuang, H.; Li, W. Synthesis and characterization of nano crystalline BaFe12O19 powders by low temperature combustion. Mater. Res. Bull., 2003, 38(1), P. 149-159.
[3] Affleck, L.; Auguas, M. D.; Parkin, I. P.; Pankhurst, Q. A.; Kuznetsov, M. V. Microstructural aspects of the self-propagating high temperature synthesis of hexagonal barium ferrites in an external magnetic field. J. Mater. Chem, 2000, 10, P. 1925-1932.
Comment 11
11) Line 168: Please, confirm that the name of this unit “magnetic field pulse forming unit” is correct? I guess this unit forms a pulse of electric current which produces the pulse of the magnetic field in the solenoid
Response:
We thank the reviewer and agree that in the previous version we named the unit inaccurately, in the new version it is named an «electric current pulse generation».
Comment 12
12) Line 172: This sentence should be at the beginning of the previous paragraph.
Response:
We thank the reviewer for the remark and agree that it would be more suitable. The sentence devoted to the technique was rearranged.
Comment 13
13) Please, indicate in the Materials and Methods section the materials and wavelength of the X-ray of the used source.
Response:
We thank the referee for attention to detail. The information about the radiation source has been supplemented.
Comment 14
14) Please, add more details on how the size of particles was analyzed with a laser particle size analyzer. This was done for powder or dissolved samples? Were powders preliminary ground?
Response:
We thank the referee for an important remark. Information about performing particle size measurements has been added to the paragraph.
Comment 15
15) Table 1: please, correct the caption: this table contains not only results of XRD. Please also indicate errors for CSR and other quantities.
Response:
We thank the reviewer for the comment and agree that the former name of the table could mislead readers. Table 1 has been renamed. The data given in the table, except for the CSR, were calculated using the Powder Cell 2.4 software. The program fitting produces an error only for the phase composition, not for constant lattices. We did not give the errors for the calculated values, since a review of similar articles (e.g., [4-6]) showed that researchers do not give it for the convenience of table readability, therefore we did not give it either.
[4] Yoshiiri, K.; Wang, K.; Kowalska, E. TiO2/Au/TiO2 Plasmonic Photocatalysts: The influence of Titania Matrix and Gold Properties. Inventions 2022, 7, 54. https://doi.org/10.3390/inventions7030054
[5] Kukartsev, V.A.; Cherepanov, A.I.; Kukartsev, V.V.; Tynchenko, V.S.; Bukhtoyarov, V.V.; Popov, A.M.; Sergienko, R.B.; Tynchenko, S.V. X-ray Diffraction Phase Analysis of Changes in the Lattice of Pervouralsk Quartzite upon Heating. Minerals 2022, 12, 233. https://doi.org/10.3390/min12020233
[6] Giannini, C.; Ladisa, M.; Altamura, D.; Siliqi, D.; Sibillano, T.; De Caro, L. X-ray Diffraction: A Powerful Technique for the Multiple-Length-Scale Structural Analysis of Nanomaterials. Crystals 2016, 6, 87. https://doi.org/10.3390/cryst6080087
Comment 16
16) Figure 5: Please, show SEM pictures of different samples with the same scale bar. It will make a more easy comparison of morphology between samples
Response:
We thank the referee for a valuable suggestion. Unfortunately, we are not able to provide pictures at the same scale, since the measurement was carried out by a third-party organization, and we were provided with images at different scales.
Comment 17
17) For magnetic properties please indicate of temperature at which they were determined, and put this information on the caption of the corresponding figure and table.
Response:
We thank the reviewer for their attention to detail. The measurements were taken at 300 K, the information has been added to the corresponding table and figure.
Comment 18
18) Why maximal magnetic field was 26 kOe while in the description of the setup was indicated 100 kOe? It seems that samples are not saturated at the used magnetic field.
Response:
We thank the reviewer for the comment. According to literature data [Smit, J.; Wijn, H. P. J. Ferrites. Physical properties of ferrimagnetic oxides in relation to their technical applications, Philips Technical Library, Eindhoven, 1959, pp. 232-272.], a field of 26 kOe is sufficient to magnetize Ba-M hexaferrites to saturation. We did not apply the maximum magnetic field, since the destruction of the solenoid may occur with repeated obtainment of high magnetic fields. We try to avoid this whenever possible. The visual increase in the magnetization values is associated with the occurrence of the phenomenon of the paraprocess, which we indicated when describing the results obtained (lines 421 – 427, 429 – 432).
Comment 19
19) Lines 334-335: How exactly magnetocrystalline anisotropy fields Ha was determined? Please comment on result of this calculation
Response:
We thank the referee for the important remark. We did not give a detailed description of the calculation of anisotropy fields in the text of the article, so as not to shift its focus from the installation. But for the sake of completeness of information, the lines 350 – 357 indicated the references that contain detailed information that we used when processing the ferromagnetic resonance curves.
Comment 20
20) Line 352: “weakly magnetic phase” -> “weak ferrimagnetic phase”.
Response:
We thank the reviewer for the comment. The previous phrase has been corrected in accordance with the comment.
Comment 21
21) Please, check sentence lines 361-364: it is not clear the part “with the magnetic ordering of the easy axis (EA) type”.
Response:
We thank the reviewer for the remark. The term " magnetic ordering of the easy axis (EA) type" is well-established and widely used in research related to the physics of magnetic phenomena. It means that the magnetic moments in a given material at a given value of the magnetic field will be most easily magnetized to saturation when the external magnetic field is directed along an axis perpendicular to the base plane of the particles. Therefore, it seems to us that this expression is quite appropriate in this context.
Comment 22
22) Lines 376-377: this conclusion is not supported by the results.
Response:
We thank the reviewer for the remark and agree with it. The conclusions regarding the development of the installation have been rewritten in accordance with the main text of the article.
Comment 23
23) Lines 389-392: This conclusion is misleading because the sizes indicated were determined by a laser particle size analyzer, not electron microscopy, as stated in the beginning.
Response:
We thank the reviewer for their attentiveness, we made a mistake in this statement. The sentence has been rewritten.
Thanks again for your careful review.
Reviewer 2 Report
In this manuscript, the author synthesized the M-type hexaferrite by the solid-reaction route, mechanochemical method and sol-gel method, respectively. The phase composition, microstructure, and magnetic properties of the M-type hexaferrite prepared by different methods were compared. However, lack of novelty hinders the publication of this paper. The microstructure and magnetic properties of the M-type hexaferrite prepared by different methods are massively discussed by the previous research. Comparison between different synthesis methods cannot provide enough novelty to this paper.
Author Response
Response for Reviewer #2
Article title: Investigation of BaFe12O19 hexaferrites manufactured by various synthesis methods using the developed pulsed magnetometer.
Authors: Dmitry V. Wagner*, Katerina V. Kareva, Viktor A. Zhuravlev*, Olga A. Dotsenko, Roman V. Minin.
Manuscript ID: inventions-2155407
Referee wrote:
“In this manuscript, the author synthesized the M-type hexaferrite by the solid-reaction route, mechanochemical method and sol-gel method, respectively. The phase composition, microstructure, and magnetic properties of the M-type hexaferrite prepared by different methods were compared. However, lack of novelty hinders the publication of this paper. The microstructure and magnetic properties of the M-type hexaferrite prepared by different methods are massively discussed by the previous research. Comparison between different synthesis methods cannot provide enough novelty to this paper.”
Response:
We would like to comment on your remark. The novelty of the work lies in the development of a pulse magnetometer, which makes it possible to study the magnetic properties of materials, specifically, the measurement of a full cycle of the hysteresis loop. Using the developed installation, measurements in pulsed magnetic fields are carried out up to 100 kOe, therefore we can study both soft and hard magnetic materials.
We would also like to comment on the lack of novelty in the synthesis and study of the structural and magnetic properties of M-type hexaferrites. We agree that this material is being actively investigated, both by us and by other scientific groups. This indicates the relevance of this topic. In addition to studying the properties of hexaferrites, we also carried out the synthesis of materials, which is described in the work. The use of the synthesis methods proposed by us will help other researchers take into account our results when implementing their methods, choose the right synthesis conditions, composition and make their materials better. Comparison of synthesis methods, we believe, will help novice researchers in the field of physics of magnetic phenomena in the choice of materials for research, in the theoretical description of magnetic properties.
We took into account your comments and corrected the article. The title of the article was changed, the introduction was supplemented with a description of the currently used impulse magnets. The conclusions include the results concerning the development of the pulsed magnetometer.
Thanks again for your careful review, it helped us build the intended emphasis of the article more competently.
Round 2
Reviewer 1 Report
The authors addressed all my questions and greatly improved the manuscript. I recommend the paper for publication in its current state.
Reviewer 2 Report
The author has addressed my question. I have no more comments.
