Three salen aluminum bromide compounds salen(Bu)AlBr () (salen = ,'-ethylenebis(3,5-di--butylsalicylideneimine)), salpen(Bu)AlBr () (salpen = ,'-propylenebis(3,5-di--butylsalicylideneimine)), and salophen(Bu)AlBr () (salophen = ,'--phenylenenebis(3,5-di--butylsalicylideneimine) were evaluated for their potential use as dealkylation agents with a series of organophosphates. These reactions led to the aluminum phosphate compounds containing six-coordinate aluminum centers and hydrolytically stable P-O-C bonds: = [salen(Bu)AlOP(O)(OMe)], = [salen(Bu)AlOP(O)(OEt)], = [salen(Bu)AlOP(O)(OPh)], = [salophen(Bu)AlOP(O)(OMe)], = [salpen(Bu)AlOP(O)(OPr)], = (salen(Bu)AlO)PO, = (salpen(Bu)AlO)PO, = (salophen(Bu)AlO)PO. All the compounds were characterized by H, C, Al, and P NMR, IR, and mass spectrometry. Furthermore, compounds - were structurally characterized by single-crystal X-ray diffraction. The potential hydrolysis of these compounds was modeled with and demonstrated the unique stability of the final product and ease of isolation.