The coordinatively unsaturated sites in MIL‐101, Cr3(F,OH)(H2O)2O[(O2C)‐C6H4‐(CO2)]3⋅n H2O (n≈25), having zeotypic giant pores can be selectively functionalized in a way differing from that of mesoporous silica. Metal–organic frameworks, grafted with ethylenediamine or diethylenetriamine on the unsaturated CrIII sites of MIL‐101, exhibit remarkably high activities in the Knoevenagel condensation relative to that of the mesophase.
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