Facile Synthesis of a Polycatenane Compound Based on Ag-triazole Complexes and Phosphomolybdic Acid for the Catalytic Epoxidation of Olefins with Molecular Oxygen
Round 1
Reviewer 1 Report
I recommend the current manuscript should be considered after two major revisions. The suggested revisions are following:
Although the catalyst showed excellent reactivity, scope of the reactions is limited to only two olefins. I suggest to improve the scope of the reaction. Please, evaluate the scope of the reaction for 5-8 more olefines.
Mechanism of the catalytic activity is unclear. It is suggested to propose a mechanism and show the schematic representation of the catalytic cycle in the manuscript. Please consider additional experiments to support your proposed mechanism.
Author Response
Dear Reviewer,
Attached please find our revised manuscript entitled: “Facile synthesis of a polycatenane compound based on Ag-triazole complexes and phosphomolybdic acid for the catalytic epoxidation of olefins with molecular oxygen” (Manuscript ID: catalysts-527201).
We have carried out the correction of the manuscript according to the reviewers’ comments and suggestions. You will find a list of the major changes in the file of “Response to Reviewers”.
Thank you very much for your kind help!
Author Response File: 
Author Response.pdf
Reviewer 2 Report
This manuscript describes the synthesis of the PMo12 salt with Ag-triazole complex cation, and the application to the oxidation reaction. The heterogeneous nature of the catalysis was confirmed. I feel that the data can be published; however, some important information is missing in this manuscript.
(1) The result of single-crystal X-ray analysis should be posted to CCDC, and the summary should be shown in this manuscript in order for readers to judge the quality of analysis.
(2) Elemental analysis for Ag and Mo is also necessary. The organic elemental analysis result is inconsistent: the formula does not agree with FW 7828 and these C, H and N calculated amount. Water molecules might exist.
(3) The XRD pattern (Figure 8) should be also compared with the calculated pattern from the structure determined by single crystal X-ray analysis.
(4) For oxidation reaction, utilization efficiency of sacrificial reductant ([yield of epoxide]/[consumed aldehyde]) and material balance ([sum of product and unreacted substrate]/[used substrate]) should be shown. Showing a typical GC chart as SI is desirable, because oxidation reaction sometimes produces a number of by-products.
(5) The shape of catalyst (ground powder or unground crystals) in the catalytic use should be described. It is an important point whether the external surface area is sufficiently small or not.
(6) Figure 4 should include the spectrum of the catalyst.
(7) Ref. 47 should be included in the Introduction section.
(8) Abstract: the expression "very high catalytic activity" is exaggerated.
(9) Lines 72-74: Na9[PW9O34] is not a phosphomolybdate but a phosphotungstate.
(10) Experimental section: TBHP is not used in this manuscript.
Author Response
Dear Reviewer,
Attached please find our revised manuscript entitled: “Facile synthesis of a polycatenane compound based on Ag-triazole complexes and phosphomolybdic acid for the catalytic epoxidation of olefins with molecular oxygen” (Manuscript ID: catalysts-527201).
We have carried out the correction of the manuscript according to the reviewers’ comments and suggestions. You will find a list of the major changes in the file of “Response to Reviewers”.
Thank you very much for your kind help!
Author Response File: 
Author Response.docx
Round 2
Reviewer 1 Report
Revised manuscript is significantly improved. Author addressed all my concerns. The new version of the manuscript can be accept in present form.
Author Response
Dear Reviewer,
Thank you very much for your kind help!
Reviewer 2 Report
The added information is still incomplete.
(1) Summary of single crystal X-ray analysis should be added.
The summary should include space group, cell parameters (a, b, c, alpha, beta, gamma, volume), formula and formula weight, Z number, calculated density, R1 and wR2.
ORTEP representations should be added to supporting information.
(2) The GC charts (Figs. S1 and S2) are too small, and the maximum retention time is too short. Enlarge the charts toward the y axis in order to check that the other product peaks are small enough to confirm >99% selectivity. Show longer retention time to include those of other potential products (such as allyl-oxidized product alcohols and isobutyric acid).
(3) Definition of material balance should be described. Does it include isobutyraldehyde?
Author Response
Dear Reviewer,
Attached please find our revised manuscript entitled: “Facile synthesis of a polycatenane compound based on Ag-triazole complexes and phosphomolybdic acid for the catalytic epoxidation of olefins with molecular oxygen” (Manuscript ID: catalysts-527201).
We have carried out the correction of the manuscript according to the reviewers’ comments and suggestions.
Thank you very much for your kind help!
Author Response File: Author Response.pdf
