We characterized the structure of the aluminosilicate sites by Al MQ/MAS NMR techniques and studied the conditions leading to single-site species. 14 the structures formed should be amorphous and purely statistical, allowing for the use of mean-field concepts, such as average connectivity and Vegard's law. Irreversibility should also result in better decoupling between the chemistries of the precursors used in the sequential cross-linking steps and it would imply that the order of the steps strictly matters. This work aims to answer the question of reversibility for a broader spectrum of interesting metal site precursors using quantum chemistry DFT computational methods.