An excellent conversions of benzaldehyde was obtained under solvent and solvent free conditions by utilizing Co(im) 2 0.5 DMA as catalyst for the synthesis of benzylidene malononitrile. The catalytic prospect of this crystalline porous framework was extended to oxidation reactions involving ethylene glycol (EG) and ethylbenzene (EB). Unexpectedly, EG was totally oxidized to oxalic acid; which demonstrates the catalyst non-selectivity towards glycolic acid. For EB oxidation under a solvent less condition in the presence of oxygen as oxidant (0.8 Mpa), and a 42% conversion was achieved with 78.4% selectivity for acetophenone at 120°C for a period of 2 h.