Abstract

This work reports the synthesis and characterization of Zr(IV)‐based UiO‐67‐(NH2)2 (called 1) metal‐organic framework. Activated 1 (named 1') was shown to be an efficient tandem catalyst in the conversion of benzaldehydedimethyl acetal to benzylidenemalononitrile (4) by reacting with malononitrile in high yield under mild reaction conditions. The catalytic performance of 1' is superior to Zr‐UiO‐67‐NH2, Zr‐UiO‐67 and their respective metal salts and linkers. Catalyst 1' showed wide substrates scope with respect to acetal and active methylene compounds.

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