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Aluminum complexes containing [RP(O)(2-O-3,5- t Bu 2 C 6 H 2 ) 2 ] 2−  [R =  t Bu ( 3a ), Ph ( 3b )] have been synthesized, structurally characterized, and their reactivity studied in comparison with those of their [RP(2-O-3,5- t Bu 2 C 6 H 2 ) 2 ] 2−  [R =  t Bu ( 2a ), Ph ( 2b )] analogs. Treating AlMe 3  with one equiv of H 2 [ 3a-b ] in THF at 0°C affords quantitatively [ 3a-b ]AlMe, subsequent reactions of which with benzyl alcohol in THF at 25°C generate {[ 3a-b ]Al(μ 2 -OCH 2 Ph)} 2 . The methyl [ 3a-b ]AlMe and the benzyloxide {[ 3a-b ]Al(μ 2 -OCH 2 Ph)} 2  are all active for catalytic ring-opening polymerization (ROP) of ε-caprolactone and  rac -lactide ( rac -LA). Controlled experiments reveal that {[ 3a ]Al(μ 2 -OCH 2 Ph)} 2  is competent in living polymerization. Kinetic studies indicate that [ 3a ]AlMe, in the presence of benzyl alcohol, catalyzes ROP of  rac -LA at a rate faster than [ 3b ]AlMe and [ 2a ]AlMe(THF) by a factor of 1.8 and 23.6, respectively, highlighting the profound reactivity enhancement in ROP catalysis by varying the P-substituents of these biphenolate complexes of aluminum.

Enhanced Reactivity of Aluminum Complexes Containing P-Bridged Biphenolate Ligands in Ring-Opening Polymerization Catalysis