A crystal structure refinement of ITQ-4 including the positions of organic cations and fluoride anions was reported by Bull et al. for a sample synthesized with BQol + as OSDA. The published structure of as-synthesized ITQ-4 is monoclinic (space group 𝐼𝑚), and fluoride anions and hydroxy groups of the BQol + cations are disordered over two positions that are related by a mirror plane (Figure ). A consideration of different possible locations of these atoms leads to six ordered structures that have 𝑃𝑛, 𝐼1, and 𝑃1 symmetries (Figure ). Among these, an arrangement with 𝑃𝑛 symmetry was found to have the lowest energy in preliminary DFT optimizations, which was used as starting point for the following calculations that compared different fluoride positions.