Response to Reviewers’ Comments
Thank the reviewers for the constructive suggestions. We have carefully read the insightful comments given by the reviewers, which are very helpful to improve the quality of our paper.
Response to Reviewer #1
(1) General Comment:This paper entitled "Controlled synthesis of Fe3O4@C@manganese oxides (MnO2, Mn3O4and MnO) hierarchical hollow nanospheres and their superior lithium storage properties " deals with enhanced properties of conversion reaction materials through judicious textural organization. I suggest that this paper should be published in Electrochimica Acta after modifications according to comments below-noted.
Reply:reaction paper to metaphor
Thank Reviewer #1 for the appreciation.
(2) Specific Comment No. 1: Graphical abstract's images require better definition. It is meaningful if the authors prove the detached particles are manganese-based. Reply:
Thanks to Reviewer # 1 for the good suggestion.
It has been proven that the nanoparticles formed in the outermost layer of FCMnO2s and FCMnOs are easy to fall off after intensive cycles (see Fig. 8). In TEM images of FCMnO2s and FCMnOs after the 150th cycle at 0.1Ag-1 (Fig. S10), some detached nanoparticles can be observed (white arrows). By analyzing their EDS mappings, Mn and O elements (Fig. S10b, f, j and o) can be observed in the detached particles while no Fe element (Fig. S10c and k) can be found in the detached particles (white arrows), which is also a powerful proof for the fact that the detached nanoparticles are manganese oxides. Moreover, in HRTEM images of the detached nanoparticles (Fig. S10d and l), the stripe spacings of 0.248nm and 0.277nm are assigned to the (211) and (103) plane of Mn3O4, further confirming that the detached nanoparticles are Mn3O4.
However, there are too many figures in the main manuscript. Therefore, Fig. S10 has been added in the revised supplementary information. Accordingly, the corresponding sentence has added in the revised version of the manuscript (see 1 of Changes of the manuscript, 1 of Changes of Supplementary Information).
Fig. S10. TEM, EDS mappings images of Mn, Fe, O, C and N, corresponding STEM and HRTEM images of (a-h) FCMnO2s, (i-p) FCMnOs after the 150th cycle at 0.1Ag-
1. HRTEM images of (d) FCMnO2s and (l) FCMnOs with a rectangular box in (a) and
(i), respectively.
(3) Specific Comment No. 2: Introduction:-What do you mean by "stable circulation"?
Reply:
The expression is not accurate enough. The "stable circulation" has been replaced by “high cycling stability”. Accordingly, the corresponding sentence has amended in the revised version of the manuscript (see 2 of Changes of the manuscript).
(4) Specific Comment No. 3: Conversion reaction (P3 L25) and its electrolyte degradation reaction (p11, L23) need the appropriate reference: Poizot,P.; Laruelle, S.; Grugeon, S.; Dupont, L.; Tarascon, J.-M., Nature 2000, 407, 496-499.
Reply:
The above important reference (Poizot,P.; Laruelle, S.; Grugeon, S.; Dupont, L.;
Tarascon, J.-M., Nature 2000, 407, 496-499) has been cited in revised version of the manuscript. (see 3-5 of Changes of the manuscript).
(5) Specific Comment No. 4: Experimental:-P6 L3: the previous reference (no s). Reply:
“The previous references" has been replaced by“the previous reference”. Accordingly, the corresponding sentence has amended in the revised version of the manuscript (see 6 of Changes of the manuscript).
(6) Specific Comment No. 5: SEM stands for scanning electron microscopy. Reply:
“Scanning electrodes microscopy" has been replaced by “field emission scanning electron microscopy (FESEM)”. Accordingly, the corresponding sentence has amended in the revised version of the manuscript (see 7 of Changes of the manuscript).
(7) Specific Comment No. 6: TG stands for thermogravimetry. Could you write the experimental conditions (rate, gaz)
Reply:
Thank Reviewer # 1 for the good suggestion.
Thermogravimetry (TG) of the samples was carried out on a TG apparatus (Q600) with a heating rate of 10 °C min-1 in air atmosphere. Accordingly, the experimental conditions (rate, gas) have been added in the revised version of the manuscript (see 8 of Changes of the manuscript).
(8) Specific Comment No. 7: What FESEM stands for (P8 L20)?
Reply:
FESEM stands for “Field emission scanning electron microscopy”. Accordingly, the corresponding sentence has amended in the revised version of the manuscript (see 7 of Changes of the manuscript).
(9) Specific Comment No. 8: P7 L15 working electrode instead of anode.
Reply:
In P7 L15, the “anode" has been replaced by “working electrode”. Accordingly, the corresponding sentence has amended in the revised version of the manuscript (see
9 of Changes of the manuscript).
(10) Specific Comment No. 9: P7 L20: electrochemical impedance spectroscopy. Reply:
In P7 L20, the “electrochemical impedance spectrum" has been replaced by “electrochemical impedance spectroscopy”. Accordingly, the corresponding sentence has amended in the revised version of the manuscript (see 9 of Changes of the manuscript).
(11) Specific Comment No. 10: Results and discussion: P8: Could you show the carbon layer. It is not so clear.
Reply:
This is a good suggestion.
TEM images of FCHNs, FCMnO2s, FCMn3O4s and FCMnOs are shown in Fig. S2. The carbon external layer (between two circles) of FCHNs can be observed in Fig. S2a, while the carbon intermediate layer (between two circles) of FCMnO2s, FCMn3O4s and FCMnOs can been also found in Fig. S2b-d, respectively.
In STEM and line scan images of FCMnO2s, FCMn3O4s and FCMnOs(Fig. S3), there are rising carbon peaks, confirming the existence of the carbon layer.
However, the above comment reminds us that the carbon layer of FCHNs, FCMnO2s, FCMn3O4s and FCMnOs should be well shown. Accordingly, the corresponding figures and sentence have been added in the revised version of the manuscript (see 10 of Changes of the manuscript, 2 and 3 of Changes of Supplementary Information).
Fig. S2. TEM images of (a) FCHNs (b) FCMnO2s, (c) FCMn3O4s, (d) FCMnOs.
Fig. S3. STEM image and line scan images of (a-b) FCMnO2s, (c-d) FCMn3O4s, (e-f) FCMnOs.
(12) Specific Comment No. 11: P10: the description of TG after 150°C is not clear. Reply:
In Fig. S4a-d, the TG curve of FCHNs, FCMnO2s, FCMnOs and FCMn3O4s shows that the weight loss at 50-150 ℃ originates from the gradual removal of weakly adsorbed water and other small volatile molecules. In Fig. S4a, c and d, the weight gain of FCHNs (about 1 wt%), FCMnOs and FCMn3O4s at 150-300 ℃ mainly corresponds to the conversion of Fe3O4 to Fe2O3 (ACS Appl. Mater. Interfaces, 4 (2012), 4752−4757, see Fig. R3; Phys Chem. Chem. Phys, 16 (2014) 5284-5294, see Fig. R1), while the

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