Comments on abstract, title, references

This is an interesting manuscript showing the first example of an intrinsically porous trianglamine-based supramolecular organic framework that can be constructed with diverse packing, which allows to tune its guest selectivity. Furthermore, after iodine encapsulation, improvement of CO2 selectivity over CH4 was reported. However, some scientific issues must be addressed in order for this manuscript to be published in JACS:

1) Proper charge-balanced chemical formulas are required before and after the iodine encapsulation. These encompass the TGA, Raman, UV-vis, and EDX studies the authors have described. It is important to address this issue in case charged species such as polyiodide are observed. Especially, the authors claim that all the selectivity of gas adsorption is due to a size effect and it is hard to see the details from the single crystal X-ray diffraction data, since the quality of the cif file provided is inadequate to draw this conclusion (even though I@T-SOF-1 is beam sensitive, this is still hardly acceptable). In this case, characterization of the material should be done more thoroughly.

Comments on introduction/background

Authors present here a well described and innovative piece of work. Porous materials triggers an outstanding level of interest for applications and fundamental research. Sizes and shapes of cavities er of prime importance in respect to applications. The choice of the building blocks is excellent in view of the project. A strong proof of principle was established with solid and complete sets of data. In addition to the ability to create tridimensional porous material taking full advantage of the principles of supramolecular chemistry without using metal ions, I am excited by the perspective offers by the selectivity provided by such material.

Comments on methodology

The authors state as follows. "This reflects the high affinity of this supramolecular framework towards CO2, even at ambient conditions." The use of the word "affinity" suggests a chemical interaction, but the discussion centers on the dynamic or kinetic diameter of the guest molecule. If there is a chemical affinity in the system for CO2 over CH4, it should be explained.

Comments on data and results

Based on the high porosity of the structure outlined in Figure 1, the amount of N2 adsorption found in Figure 2a is too small to claim Type I isotherm only from the low pressure section of the isotherm.

Comments on discussion and conclusions

This is an interesting manuscript showing the first example of an intrinsically porous trianglamine-based supramolecular organic framework that can be constructed with diverse packing, which allows to tune its guest selectivity. Furthermore, after iodine encapsulation, improvement of CO2 selectivity over CH4 was reported.