We next probed the ability of our templated frameworks to catalyze aldol condensation reactions (Scheme 1). We hypothesized that the amine could form a nucleophilic enamine intermediate, while the acid could participate in hydrogen-bonding and electrophilic activation of the aldehyde partner. Similar mechanisms have been shown in other bifunctional acid-base catalysts (Fig. ). To provide unambiguous evidence of acidbase cooperativity, we synthesized four control frameworks: 1) 1-nontemplated, a framework in which the acid and base groups are present in similar concentrations but are randomly distributed throughout the pores; 2) 1-CH2NH2, a framework containing only amine groups; 3) 1-COOH, a framework containing only carboxylic acid groups; and 4) Mg2dotpdc, the bare framework containing no functional groups.