Enzymes often use two or more metal sites to catalyze difficult oxidative, reductive, and redox-neutral transformations. For example, nature uses diiron and dicopper sites to activate O2 and oxygenate substrates, as well as diiron and [NiFe] centers to reversibly form and split H2. Two metal cations can also work jointly to increase the electrophilicity and nucleophilicity of reaction partners, such as in the hydrolysis of phosphate ester and amide bonds. We have been interested in translating these bioinspired concepts to a heterogeneous platform, to leverage the greater stability, recyclability, and unique microenvironments found in porous materials.