Acetylacetone Covalent Triazine Framework: An Efficient Carbon Capture and Storage Material and a Highly Stable Heterogeneous Catalyst

We present, for the first time, covalent triazine frameworks functionalized with acetylacetonate group (acac-CTFs). They are obtained from the polymerization of 4,4′-malonyldibenzonitrile under ionothermal conditions and exhibit BET surface areas up to 1626 m2/g. The materials show excellent CO2 uptake (3.30 mmol/g at 273 K and 1 bar), H2 storage capacity (1.53 wt % at 77 K and 1 bar), and a good CO2/N2 selectivity (up to 46 at 298 K). The enhanced CO2 uptake value and good selectivity are due to the presence of dual polar sites (N and O) throughout the material. In addition, acac-CTF was used to anchor VO(acac)2 as a heterogeneous catalyst. The V@acacCTF showed outstanding reactivity and reusability for the modified Mannich-type reaction with a higher turnover number than the homogeneous catalyst. The higher reactivity and reusability of the catalyst come from the coordination of the vanadyl ions to the acetyl acetonate groups present in the material. The strong metalation is confirmed from Fourier trans...