Effect of Sintering Temperature on the Magnetic Properties of Fe₃Mn₃Co_60.66Si_33.34

Round 1

Reviewer 1 Report

i)    The manuscript contains several interesting results and may be published after the following revisions:

The synthetic process should be described in detail. The following parameters such as rotation speed and vacuum conditions; "ball to mass" ratio should be clarified.     

ii)            Accuracy of cell parameter determination should be described

iii)           The Mn is known as material which can be easy can evaporate from powders mixture at high temperature. It should be mentioned and the authors should describe how they did control the Mn-concentration in final compounds.

Conclusion: minor revisions

 

no comments

Author Response

1.The synthetic process should be described in detail. The following parameters such as rotation speed and vacuum conditions; "ball to mass" ratio should be clarified.     

Response:Thank you for your valuable comments. We have answered your questions and made the required modifications to the text.Our modifications to the Experimental section are as follows. Commercially available Fe, Mn, Co, and Si powders of 99.9% purity were used to prepare 10 g samples with a molar fraction ratio of 3:3:60.66:33.34 [11]. The weighed powders were mixed and placed in a stainless-steel omnidirectional ball mill (OECO- PBM-AD-6L, Hunan Deke). Stainless steel balls with diameters of 1.5 cm, 1 cm, and 0.3 cm were used, and the total mass was 500 g. To reduce the difference caused by ball milling, we left the number of balls with diameters of 1.5 cm and 1 cm unchanged, and the rest were filled with balls. The ball mill speed was 400 r/min, the ball-to-powder ratio was 50:1, and the ball milling time was 30 h. To prevent the powder from being oxidized during the ball milling process, we vacuumed the ball mill and the vacuum degree was below 5 Pa.

 

 

2.Accuracy of cell parameter determination should be described

 

Response:Thank you very much for your suggestion. While confirming the accuracy of the lattice constant, we detected a major error in the lattice constant through the analysis of JADE6.5 and HRTEM, and made the following corrections:

Table 1 is deleted, and useful data is presented in other ways.

The results of JADE6.5 analysis show that the space group of the crystal is Pbnm, and the lattice constants a, b, and c are 4.9180 Å, 3.7380 Å, and 7.1090 Å, respectively. Fourier and inverse Fourier transforms were performed on different regions of the HRTEM images. Figure 1. Shows the HRTEM images of Fe3Mn3Co60.66Si33.34 sintered at (a) 600 °C, (b) 700 °C, (c) 800 °C, (d) 900 °C, and (e) 950 °C.The results show that amorphous and Co2Si crystals are present in the powder material. After the measurement of the crystal plane spacing, the results show that the actual spacings (0.1864 nm, 0.1859 nm, 0.1857 nm, 0.1865 nm, 0.1867 nm) of the samples at different heat treatment temperatures are less than the theoretical crystal plane spacing (d = 0.1869 nm ) of (020), which is mainly due to the fact that the atomic radii of Fe and Mn are less than that of Co.

 

Figure 1. shows the HRTEM images of Fe3Mn3Co60.66Si33.34 sintered at (a) 600 °C, (b) 700 °C, (c) 800 °C, (d) 900 °C, and (e) 950 °C.

 

We have added a standard PDF card and powder XRD without heat treatment after ball milling to the XRD pattern.Figure 2.XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures.The position of the diffraction peak has a small offset angle from the standard PDF card, mainly because of the ball milling process. After ball milling, the powder has no diffraction peaks of the components and forms a wave packet, which indicates that all the components form solid solutions.

 

Figure 2.XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures

 

3.The Mn is known as material which can be easy can evaporate from powders mixture at high temperature. It should be mentioned and the authors should describe how they did control the Mn-concentration in final compounds.

Response:Thank you for your valuable comments.Mn is volatile at high temperatures and cannot be completely eliminated. Therefore, we introduced the Mn powder into the ball mill tank in proportion during ball milling to dissolve it into a Co-based solid solution, which effectively reduced volatilisation. To determine the difference between the final and actual Mn content, we used an ICP spectrometer to analyse the samples. Table 1 shows the analysis of samples obtained without sintering after ball milling.Table 2 shows the sample analysis after ball milling and sintering.The results show that after heat treatment at 950 °C, the sample is Fe_3.2Mn_2.8Co_60.6Si_33.4 This is not significantly different from the theoretical value. Therefore, we used the theoretical value as the subscript. The Fe content is slightly higher than the theoretical value owing to the influence of the ball-milling medium.

Table 1.The ICP result of Fe_3.2Mn_2.8Co_60.6Si_33.4 by Thermo Fisher iCAP PRO

Samples	Fe	Mn	Co	Si
Fe3.2Mn2.8Co60.6Si33.4	3.2	2.8	60.6	33.4

Table 2..The ICP result of Fe_3.2Mn_2.8Co_60.6Si_33.4 by Thermo Fisher iCAP PRO

Samples	Fe	Mn	Co	Si
Fe3.2Mn2.8Co60.6Si33.4	3.2	2.8	60.6	33.4

 

Author Response File: Author Response.docx

Reviewer 2 Report

In this work samples of Fe₃Mn₃Co_60.66Si_33.34 were created by sintering at 5 different temperatures: 600, 700, 800, 900, 950 °C. The samples were analyzed by x-ray diffraction, transmission electron microscopy and vibrating sample magnetometry. It was shown how the sintering temperature affects the critical points of the hysteresis loops (coercivity, remanence, saturation strength). Although the samples were all Fe₃Mn₃Co_60.66Si_33.34, the title is more generic as if all possible cases of FeMn co-doped with Co₂Si material system were studied. I find this work very specific, i.e., it is not a systematic study of FeMn co-doped with Co₂Si.The text needs some corrections, e.g., “sintering”, sintering temperature”, “temperature” are used for the same thing (sintering temperature), the three panels of Figure 8 should be in one line, etc. The methods used are standard.

No comments.

Author Response

1. I find this work very specific, i.e., it is not a systematic study of FeMn co-doped with Co₂The text needs some corrections, e.g., “sintering”, sintering temperature”, “temperature” are used for the same thing (sintering temperature), the three panels of Figure 8 should be in one line, etc. The methods used are standard.

 

Response:Thank you for your valuable comments.The effect of the heat treatment temperature on the magnetic properties of Fe3Mn3Co60.66Si33.34 has been studied. This is not a systematic study of FeMn co-doped with Co2Si. As the terms “sintering”, sintering temperature”, and “temperature” were used to refer to the sintering temperature, we consistently used the term “sintering temperature” in the revised article to avoid any ambiguity. In addition, we modified the figure, as shown Figure 1.

 

Figure 1. (a) Relationship between the electrical loss tangent and frequency of all samples at different

sintering temperatures. (b) Relationship between the magnetic loss tangent and frequency for all

samples sintered at different temperatures. (c) Relationship between frequency and loss tangent for

all samples sintered at different temperatures.

Author Response File: Author Response.docx

Reviewer 3 Report

This manuscript presents an interesting proposal to use Fe3Mn3Co60.66Si33.34 nanopowders, prepared via mechanical alloying and sintering, as a possible material for magnetic storage applications due to its suitable properties. Consequently, the effect of different sintering temperatures on the soft magnetic properties of Fe-Mn co-doped Co2Si were investigated by using several techniques. However, there are certain comments and improvements that this reviewer wants to address and have corrected, to help increase the grasp and reason behind this study for a broad audience prior to grant its publication in this journal. Therefore, the work can be accepted after a major revision.

 

- The title is inaccurate.

You should define if you are dealing with Fe3Mn3Co60.66Si33.34 or Fe-Mn co-doped Co2Si.

 1. In the Introduction section:

- The authors should replace the sentence “The results showed that after crystallization treatment, the magnetic saturation strength (Ms)alue of the…” by “The results showed that after crystallization treatment, the magnetic saturation strength (Ms) value of the…”.

 2. In the Experiment section:

- The authors should replace the sentence “Commercially available Fe, Mn, Co, and Si powders of 99.9% purity were to prepare 10 g samples according to the molar fraction ratio…” by “Commercially available Fe, Mn, Co, and Si powders of 99.9% purity were used to prepare 10 g samples according to the molar fraction ratio…”

 - The authors should consider mentioning the milling parameters (i.e., milling media material, milling media shape (diameter), BPR, etc.) and the milling set up.

 3. In the Results and analysis section:

The authors state that “Several diffraction peaks in the XRD pattern are wide because large residual internal stress remained after mechanical alloying, leading to the broadening of diffraction peaks.”.

- Why? How is it possible that after the sintering there were still wide diffraction peaks? The authors should give discussions.

How does the sintering temperatures affect the as-milled powders? The authors should give discussions.

 - The authors should add the XRD pattern of the raw materials as well as the initial mixture to compare them with the XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures. The authors should give discussions.

 - The XRD results are not deeply analyzed. Diffraction peaks (weak and strong) in Fig. 1 should be indexed and compared among them and with their respective Powder Diffraction File (PDF) or ICDD cards. The authors should give discussions.

 - The data reported in Table 1 are not convincing. The authors used the Scherrer equation to obtain the grain size reported in Table 1. It is worth noticing that such equation has a limit of application for symmetrical diffraction peaks. However, symmetric diffraction peaks are not obvious in the XRD patterns (Fig. 1). Therefore, the authors should use Rietveld refinement, giving the details of the refinement parameters.

 - If the authors are certain of the data in Table 1, they should compare them with HRTEM results.

 - Several groups of as-sintered samples should be set up so that the relationship between sintering temperature and result can be seen more intuitively by analyzing electron microscope photos, in what crystallography parameters are concerned.

 - Fig. 4 shows the image of Fe3Mn3Co60.66Si33.34 sintered at different temperatures, but the contrast difference, in all images, is not obvious. The authors should add other SEM images to enhance the image contrast. Then, the difference of each case should be described in detail.

- The authors should give other SEM images with a scale of 100 nm to corroborate the occurrence of nanopowders.

- It is mentioned, in the manuscript, that nanopowders are present with giving any evidence. According to Figs. 4 and 5, the particles are not in the nanometric scale as the authors supposed. Additionally, the particles are not well dispersed.

Please drop the word "nanopowders" in the manuscript since the proper evidence is not presented in the Results and analysis section.

4. In the Conclusions section:

- The Conclusions are unsatisfactory since the XRD, SEM and TEM results are not convincing.

Author Response

Thank you for your valuable comments. We have answered your questions and modified the text based your suggestions.

 

0.The title is inaccurate.

You should define if you are dealing with Fe₃Mn₃Co_60.66Si_33.34 or Fe-Mn co-doped Co₂Si.

 

Response:Thank you for your valuable comments.We modified the title as “Effect of sintering temperature on the magnetic properties of Fe3Mn3Co60.66Si33.34”

 

1.In the Introduction section:

- The authors should replace the sentence “The results showed that after crystallization treatment, the magnetic saturation strength (Ms)alue of the…” by “The results showed that after crystallization treatment, the magnetic saturation strength (Ms) value of the…”.

Response:Thank you for your valuable comments.The results show that after crystallization treatment, the magnetic saturation strength (Ms) value of the alloy increases from 37.2 A·m2/kg to 58.4 A·m2/kg, and the coercivity (Hc) also increases from 1.25×79.6 A/m to 634.45×79.6 A/m. 

 

2. 2. In the Experimentsection:

The authors should replace the sentence “Commercially available Fe, Mn, Co, and Si powders of 99.9% purity were to prepare 10 g samples according to the molar fraction ratio…” by “Commercially available Fe, Mn, Co, and Si powders of 99.9% purity were used to prepare 10 g samples according to the molar fraction ratio…”

 - The authors should consider mentioning the milling parameters (i.e., milling media material, milling media shape (diameter), BPR, etc.) and the milling set up.

 

Response:Thank you for your valuable comments.Our modifications to the Experimental section are as follows. Commercially available Fe, Mn, Co, and Si powders of 99.9% purity were used to prepare 10 g samples with a molar fraction ratio of 3:3:60.66:33.34 [11]. The weighed powders were mixed and placed in a stainless-steel omnidirectional ball mill (OECO- PBM-AD-6L, Hunan Deke). Stainless steel balls with diameters of 1.5 cm, 1 cm and 0.3 cm were used, and the total mass was 500 g. To reduce the difference caused by ball milling, we left the number of balls with diameters of 1.5 cm and 1 cm unchanged, and the rest were filled with balls. The ball mill speed was 400 r/min, the ball-to-powder ratio was 50:1, and the ball milling time was 30 h. To prevent the powder from being oxidized during the ball milling process, we vacuumed the ball mill, and the vacuum degree was below 5 Pa.

 

 

3. 3. In the Results and analysis section:

The authors state that “Several diffraction peaks in the XRD pattern are wide because large residual internal stress remained after mechanical alloying, leading to the broadening of diffraction peaks.”.

- Why? How is it possible that after the sintering there were still wide diffraction peaks? The authors should give discussions.

How does the sintering temperatures affect the as-milled powders? The authors should give discussions.

-The authors should add the XRD pattern of the raw materials as well as the initial mixture to compare them with the XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures. The authors should give discussions.

-The XRD results are not deeply analyzed. Diffraction peaks (weak and strong) in Fig. 1 should be indexed and compared among them and with their respective Powder Diffraction File (PDF) or ICDD cards. The authors should give discussions.

-The data reported in Table 1 are not convincing. The authors used the Scherrer equation to obtain the grain size reported in Table 1. It is worth noticing that such equation has a limit of application for symmetrical diffraction peaks. However, symmetric diffraction peaks are not obvious in the XRD patterns (Fig. 1). Therefore, the authors should use Rietveld refinement, giving the details of the refinement parameters.

-If the authors are certain of the data in Table 1, they should compare them with the HRTEM results.

-Several groups of as-sintered samples should be set up so that the relationship between sintering temperature and result can be seen more intuitively by analyzing electron microscope photos, in what crystallography parameters are concerned.

-Fig. 4 shows the image of Fe3Mn3Co60.66Si33.34 sintered at different temperatures, but the contrast difference, in all images, is not obvious. The authors should add other SEM images to enhance the image contrast. Then, the difference of each case should be described in detail.

-The authors should give other SEM images with a scale of 100 nm to corroborate the occurrence of nanopowders.

-It is mentioned, in the manuscript, that nanopowders are present with giving any evidence. According to Figs. 4 and 5, the particles are not in the nanometric scale as the authors supposed. Additionally, the particles are not well dispersed.

Please drop the word "nanopowders" in the manuscript since the proper evidence is not presented in the Results and analysis section.

 

3.1 The authors state that “Several diffraction peaks in the XRD pattern are wide because large residual internal stress remained after mechanical alloying, leading to the broadening of diffraction peaks.”.

- Why? How is it possible that after the sintering there were still wide diffraction peaks? The authors should give discussions.

How does the sintering temperatures affect the as-milled powders? The authors should give discussions.

-The authors should add the XRD pattern of the raw materials as well as the initial mixture to compare them with the XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures. The authors should give discussions.

-The XRD results are not deeply analyzed. Diffraction peaks (weak and strong) in Fig. 1 should be indexed and compared among them and with their respective Powder Diffraction File (PDF) or ICDD cards. The authors should give discussions.

 

Response:Thank you for your comments on the XRD analysis section. We have reanalysed it and found errors. The following modifications were made:

The peak width is wider than the peak width of 700℃, 800℃, 900℃ and 950℃, because the crystallization is poor at low temperature.

According to the W-H method, grain refinement and increasement in microstrain can cause broadening of the diffraction peak. Therefore, we calculated the grain size and microscopic strain using the W-H method. The results show that the grain size increases and the microscopic strain decreases with increasing temperature, which is consistent with the XRD pattern exhibited by Tupou. The diffraction peaks exhibit broadening behaviour even after heat treatment, which may be due to the short heat treatment time; and the heat treatment temperature is not sufficiently high to completely release the internal stress during heat treatment. The HRTEM image shows that the powder is still amorphous, which may also be the reason for the broadening of the diffraction peaks.

We have added a standard PDF card and powder XRD pattern without heat treatment after ball milling. The position of the diffraction peak has a small offset angle from the standard PDF card, mainly because of the ball milling process. After ball milling, the powder has no diffraction peaks of the components and forms a wave packet, which indicates that all the components form solid solutions.

The XRD pattern of ball milling was added to the original XRD pattern.Figure 1 shows XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures.

 

 

Figure 1.XRD of Fe3Mn3Co60.66Si33.34 at different sintering temperatures

 

The results showed that the diffraction peaks of all group elements disappeared and formed a large wave packet, which indicates the formation of a solid solution. The XRD pattern after heat treatment was fitted by JADE 6.5, and the Co₂Si phase precipitated from the solid solution of the ball-milled powder after different heat treatment temperatures. This is in perfect agreement with the standard PDF#98-005-2281. The crystal structure is an orthorhombic crystal system with space group Pbnm and lattice constants a, b, and c of 4.9180 Å, 3.7380 Å, and 7.1090 Å, respectively. The exposed weaves are (210), (202), (013), (211), (020), and (203) with 100% intensity of the strongest peak and 22.6% intensity of the weakest peak.

After comparison with the standard PDF card, it is evident that there is a slight shift in the peak position of the diffraction peak, and the broadening behaviour of the diffraction peak persists even after the low-temperature heat treatment. According to the W-H method, grain refinement and increasement in microstrain can cause broadening of the diffraction peak. Therefore, we calculated the grain size and microscopic strain using the W-H method. The results show that the grain size increases and the microscopic strain decreases with increasing temperature, which is consistent with the XRD pattern exhibited by Tupou. The diffraction peaks exhibit broadening behaviour even after heat treatment, which may be due to the short heat treatment time; and the heat treatment temperature is not sufficiently high to completely release the internal stress during heat treatment. The HRTEM image shows that the powder is still amorphous, which may also be the reason for the broadening of the diffraction peaks.

 

3.2 -The data reported in Table 1 are not convincing. The authors used the Scherrer equation to obtain the grain size reported in Table 1. It is worth noticing that such equation has a limit of application for symmetrical diffraction peaks. However, symmetric diffraction peaks are not obvious in the XRD patterns (Fig. 1). Therefore, the authors should use Rietveld refinement, giving the details of the refinement parameters.

-If the authors are certain of the data in Table 1, they should compare them with the HRTEM results.

 

Response:Thank you for your comments on Table 1. While confirming the accuracy of the lattice constant, we detected a major error in the lattice constant through the analysis of JADE6.5 and HRTEM, and made the following corrections

 

1.Table 1 is deleted and the useful data is presented in other ways.

2.Instead of calculating the grain size using Scheele's formula, we used only the W-H method to calculate the grain size and microstrain, as shown in Figure 3.

3.The results of JADE6.5 analysis show that the space group of the crystal is Pbnm and the lattice constants a, b, and c are 4.9180 Å, 3.7380 Å, and 7.1090 Å, respectively. Fourier and inverse Fourier transforms were performed on different regions of the HR-TEM images. As show in figure 8.The results show that amorphous and Co2Si crystals are present in the powder material. The measurement of the crystal plane spacings show that the actual spacings (0.1860, 0.1864, 0.1857, 0.1865, 0.1867 nm) at different heat treatment temperatures are less than the theoretical crystal plane spacing (d = 0.1869 nm) of (020), which is mainly due to the fact that the atomic radii of Fe and Mn are less than that of Co.

 

Figure 3Average grain size of Fe3Mn3Co60.66Si33.34 sintered at different temperatures

 

4,We have added a standard PDF card and powder XRD pattern without heat treatment after ball milling. The position of the diffraction peak has a small offset angle from the standard PDF card, mainly because of the ball milling process. After ball milling, the powder has no diffraction peaks of the components and forms a wave packet, which indicates that all the components form solid solutions.

 

3.3 -Several groups of as-sintered samples should be set up so that the relationship between sintering temperature and result can be seen more intuitively by analyzing electron microscope photos, in what crystallography parameters are concerned.

-Fig. 4 shows the image of Fe3Mn3Co60.66Si33.34 sintered at different temperatures, but the contrast difference, in all images, is not obvious. The authors should add other SEM images to enhance the image contrast. Then, the difference of each case should be described in detail.

-The authors should give other SEM images with a scale of 100 nm to corroborate the occurrence of nanopowders.

-It is mentioned, in the manuscript, that nanopowders are present with giving any evidence. According to Figs. 4 and 5, the particles are not in the nanometric scale as the authors supposed. Additionally, the particles are not well dispersed.

Please drop the word "nanopowders" in the manuscript since the proper evidence is not presented in the Results and analysis section.

 

Response:Thank you for your valuable comments.Figure 4 shows the SEM images of Fe₃Mn₃Co_60.66Si_33.34 sintered at (a) 600 °C, (b) 700 °C, (C) 800 °C, (d) 900 °C, and (e) 950 °C, respectively, on a scale of 20 µm. It is observed that the powder is spherical and dispersed in space. One hundred particles were selected from each image, and the size distribution was plotted as shown in Figure 5, which indicates the maximum, minimum, and average sizes. At 600 °C and 700 °C, the powder particle size is mainly distributed in the range of 3–6 µm, and from 800 to 950 °C, the powder particles are mainly distributed in the range of 4–11 µm. As the temperature increases, the average particle size of the powder also increases. Figure 6 shows the SEM images of Fe₃Mn₃Co_60.66Si_33.34 sintered at (a) 600 °C, (b) 700 °C, (c) 800 °C, (d) 900 °C, and (e) 950 °C on a scale of 500 nm. These results indicate that the size of the powder particles should be at the micron level. After heat treatments at different temperatures, only the average size of the powder particles changes, and the morphology does not change significantly.

Figure 8 a1–e1 show the plots of HRTEM at corresponding temperatures after Fourier transform (FFT) and inverse Fourier transform to calculate the crystal plane spacing. The crystal plane spacings are all slightly smaller than the theoretical value of the (020) crystal plane (d = 0.1869 nm). The radius of the Co atom is slightly larger than the radii of Fe and Mn atoms. Therefore, it is inferred that a small amount of Fe and Mn co-doped Co2Si, Fe and Mn replace the Co atoms, such that the actual value is smaller than the theoretical value. Insets (a2)–(e2) show the FFT images in the localised region. All images show the Mann scattering halo, which means that the atoms are arranged in a disordered state in this region, and this amorphous phase exists in all the samples.

We have removed the term 'nanopowder' from the manuscripts, and indeed, no nanopowder was found within the 500nm range (Figure 6). Our previous expression was ambiguous. Instead, what we observed were the formation of nanocrystals within the powder (Figure 8), but it would be inappropriate to label it as nanopowder.

 

 

 

 

Figure 4. Scanning electron microscopy images of Fe3Mn3Co60.66Si33.34 sintered at (a) 600 °C, (b) 700 °C, (c) 800 °C, (d) 900 °C, and (e) 950 °C ,on a scale of 20 µm.

 

Figure 5.The size distribution diagrams in figure 4

 

Figure 6. Scanning electron microscopy images of Fe3Mn3Co60.66Si33.34 sintered at (a) 600 °C, (b) 700 °C, (c) 800 °C, (d) 900 °C, and (e) 950 °C ,on a scale of 500 nm.

 

Figure 8 shows the HRTEM images of Fe3Mn3Co60.66Si33.34 sintered at (a) 600 °C, (b) 700 °C, (c) 800 °C, (d) 900 °C, and (e) 950 °C.

 

 

4.In 结论部分：

-结论不令人满意，因为XRD，SEM和TEM结果不令人信服。

回应：感谢您的宝贵意见。我们将结论中的纳米粉末改为粉末，根据xrd，sem和tem的结果。

 

Author Response File: Author Response.docx

Reviewer 4 Report

Comments to authors

 The manuscript entitled "Effect of sintering temperature on the magnetic properties of Fe–Mn co-doped Co2Si", explores the effect of heat treatment temperature on the microstructure and soft magnetic properties of Fe₃Mn₃Co_60.66Si_33.34. Actually, the magnetic properties are studied for the sintering temperatures of 600 ⁰C, 700 ⁰C, 800 ⁰C, 900 ⁰C and 950 ⁰C. 

Because the material’s Fe₃Mn₃Co_60.66Si_33.34 magnetic properties at sintering temperature of 950 ⁰C, have been studied in a previous Quan Xie paper (Nanomaterials, 2022, 12, 293), this work, in my point of view, is not novel enough. However, the effect of sintering temperature ranged from 600 ⁰C to 950 ⁰C, on Fe₃Mn₃Co_60.66Si_33.34 magnetic properties, has never explored before and this is the strength point of this work.   

There are some points needed to take into consideration by the authors in order the manuscript’s results to be more clarified,

1.      In lines 86-88 authors state, “…peaks in XRD pattern are wide because large residual internal stress remained after mechanical alloying…”. By using the Williamson-Hall method and XRD peaks, the strain induced by residual stress could be evaluated for each sintering temperature, shedding more light on magnetic properties and electromagnetic loss variation.

2.      Following the above comment and according to Figure 3, as the sintering temperature increases the average grain size increases the internal stress reliefs which in turn should be resulted in strain reducing.       

 The comments mentioned above should be taken into consideration in order the manuscript to be published in Inorganics Journal.

Comments for author File: Comments.docx

Author Response

1.In lines 86-88 authors state, “…peaks in XRD pattern are wide because large residual internal stress remained after mechanical alloying…”. By using the Williamson-Hall method and XRD peaks, the strain induced by residual stress could be evaluated for each sintering temperature, shedding more light on magnetic properties and electromagnetic loss variation.

 

Response:Thank you for your valuable comments.The W-H method considers that the broadening of the diffraction peaks is caused by the refinement of the grains and an increase in the microscopic strain. Therefore, we calculated the grain size and microscopic strain using this method, as shown in the figure. With an increase in the heat-treatment temperature, which favours the growth of crystals, the average grain size increases and the internal stress decreases, which leads to a decrease in the microscopic strain. This is consistent with the phenomenon observed in the XRD patterns, where the diffraction peaks sharpen with an increase in the heat-treatment temperature.

 

 

 

Figure 3.Average grain size of Fe3Mn3Co60.66Si33.34 sintered at different temperatures

2.Following the above comment and according to Figure 3, as the sintering temperature increases the average grain size increases the internal stress reliefs which in turn should be resulted in strain reducing.

Response:Thank you for your valuable comments.We have changed this sentence.

 

Author Response File: Author Response.docx

Round 2

Reviewer 2 Report

 

I have read the authors' reply to my comments as well as the comments of the other referees and the reply of the authors to their comments. I have also noticed modifications of the manuscript. All these prove that indeed that was not a systematic work on Fe–Mn co-doped Co2Si, but a premature work on the specific composition Fe₃Mn₃Co_60.66Si_33.34 and that a lot of details had to be addressed. I find the work neither systematic nor novel since standard methods were used. For me, it is not interesting enough, however, if the other referees agree, I have to objection to its publication after all the changes and clarifications the authors made.

 

Moderate syntax check is necessary.

Author Response

1.I have read the authors' reply to my comments as well as the comments of the other referees and the reply of the authors to their comments. I have also noticed modifications of the manuscript. All these prove that indeed that was not a systematic work on Fe–Mn co-doped Co2Si, but a premature work on the specific composition Fe₃Mn₃Co_60.66Si_33.34 and that a lot of details had to be addressed. I find the work neither systematic nor novel since standard methods were used. For me, it is not interesting enough, however, if the other referees agree, I have to objection to its publication after all the changes and clarifications the authors made.

 

Response: Dear reviewer,thank you for your valuable comments. Your question is of great help to us.Since we did not explain it clearly in the previous reply, I would like to apologize again for the confusion caused to you. Our work builds on our last published article in which we investigated 6% Fe doping of Co_60.66Si_33.34(Fe₆Co_60.66Si_33.34), 6% Mn doped with Co_60.66Si_33.34(Mn₆Co_60.66Si_33.34), 3% Fe and 3% Mn co-doped with Co_60.66Si_33.34(Fe₃Mn₃Co_60.66Si_33.34), The results suggest that Fe₃Mn₃Co_60.66Si_33.34 has the best performance. The results are shown in Figure 1: Ms is 36.3emu/g,Hc is 129.73Oe.Therefore, on the basis of the previous article, we chose Fe and Mn co-doped Co_66.6Si_33.4 to study the effect of temperature on its magnetic properties.

While doing the work of Fe₃Mn₃Co_60.66Si_33.34, we also doped in different proportions.Forexample,Fe₂Mn₄Co_60.66Si_33.34,Fe₂Mn₆Co_58.66Si_33.34,Fe₄Mn₂Co_60.66Si_33.34, Fe₆Mn₂Co_60.66Si_33.34.Their performance is not as good as that of Fe₃Mn₃Co_60.66Si_33.34. As shown in Figure 3, the Hc of (b)-(e) is 257.86Oe, 314.86Oe, 476.97Oe and 489.46Oe respectively, and the Ms of (b)-(e) is 21.01emu/g, 23.27emu/g, 22.35emu/g and 22.06emu/g respectively. So we choose Fe₃Mn₃Co_60.66Si_33.34.

While doing the work of Fe₃Mn₃Co_60.66Si_33.34, we also doped in different proportions.Forexample,Fe₂Mn₄Co_60.66Si_33.34,Fe₂Mn₆Co_58.66Si_33.34,Fe₄Mn₂Co_60.66Si_33.34, Fe₆Mn₂Co_60.66Si_33.34.Their performance is not as good as that of Fe₃Mn₃Co_60.66Si_33.34. As shown in Figure 3, the Hc of (b)-(e) is 257.86Oe, 314.86Oe, 476.97Oe and 489.46Oe respectively, and the Ms of (b)-(e) is 21.01emu/g, 23.27emu/g, 22.35emu/g and 22.06emu/g respectively. So we choose Fe₃Mn₃Co_60.66Si_33.34.

Author Response File: Author Response.pdf