Tandem processes involving catalysts can offer unique and powerful strategies for converting simple starting materials into more complex products in a single reaction vessel. Imines were synthesized directly from alcohols via a tandem catalytic process using manganese octahedral molecular sieves (OMS-2) as catalyst. The synthesis proceeds through two steps: an oxidation of the alcohols to carbonyls followed by the nucleophilic attack by an amine on the carbonyl to form the imine. OMS-2 acts as a bifunctional catalyst and catalyzes two mechanistically distinct processes in a single reaction vessel under the same conditions. Conversions up to 100% were obtained for benzylic alcohols with this efficient, environmentally friendly catalytic reaction. The advantages of this process are that the intermediates need not be isolated and the catalysts can be reused upon simple filtration without loss of activity. (c) 2007 Elsevier Inc. All rights reserved.