The rare combination of In 5p and Zn 3d in the presence of a structure-oriented TDP ligand led to a robust hybrid material of {(MeNH)[InZn(TDP)(OH)]·4DMF·4HO} () with the interlaced hierarchical nanochannels (hexagonal and cylindrical) shaped by six rows of undocumented [InZn(CO)(OH)] clusters, which represented the first 5p-3d nanochannel-based heterometallic metal-organic framework. With respect to the multifarious symbiotic Lewis acid-base and Brønsted acid sites in the high porous framework, the catalytic performance of activated upon CO cycloaddition with styrene oxide was evaluated under solvent-free conditions with 1 atm of CO pressure, which exhibited that the reaction could be well completed at ambient temperature within 48 h or at 60 °C within 4 h with high yield and selectivity. Moreover, because of the acidic function of metal sites and a central free pyridine in the TDP ligand, deacetalization-Knoevenagel condensation of acetals and malononitrile could be efficiently facilitated by an activated sample of under lukewarm conditions.
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