Design and preparation of porous adsorption materials for dealing with environmental issues is attractive and promising, but it remains some challenges such as effective capture of radioactive iodine. Here, two nitrogen-rich porous organic polymers named PAN-B and PAN-T containing triazine and aminal linkages were synthesized through the polycondensation of the triazine-based hexamine (TDATPA) and two aldehyde monomers (benzaldehyde and 2-thenaldehyde) by polycondensation reaction. Fourier transform infrared (FT-IR) and 13C cross polarization/magic angle spinning nuclear magnetic resonance (13C CP/MAS NMR) measurements were performed to characterize their structures. The nitrogen-rich polymers (PAN-B and PAB-T) have hierarchical porous structures, with high Brunauer−Emmett−Teller specific surfaces (SBET) of 1254 m2/g and 1273 m2/g, respectively. And their micropore volume were satisfactory (0.275 cm3/g and 0.279 cm3/g). Moreover, PAN-B and PAN-T behaved very high iodine adsorption efficiency of 237 wt% and 243 wt% in 20 min, respectively, and had high iodine adsorption capacity of above 311 wt%.
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