Co@C-N with hierarchical pores and highly active sites is synthesized by the pyrolysis of an ionic liquid@metal–organic framework.

A layered metal‐organic framework Zn‐TPN was designed and fabricated by solvothermal reaction. The crystal structure was a lamellar structure, and the unique coordination pattern provided Lewis acid sites that could be employed as efficient catalytic sites. Zn‐TPN displayed a satisfactory catalytic effect for Knoevenagel condensation of malononitrile and benzaldehyde. At 75 °C, the conversion rate reached 96.96 % basing on the acidic sites after 1 hour, and it showed ideal catalytic activities for Knoevenagel condensation containing various aldehydes. Zn‐TPN could be utilized as a promising heterogeneous catalyst for Knoevenagel condensation.