A robust binary hydrogen-bonded supramolecular organic framework (>SOF-7) has been synthesized by solvothermal reaction of 1,4-bis-(4-(3,5-dicyano-2,6-dipyridyl)dihydropyridyl)benzene (>1) and 5,5′-bis-(azanediyl)-oxalyl-diisophthalic acid (>2). Single crystal X-ray diffraction analysis shows that >SOF-7 comprises >2 and 1,4-bis-(4-(3,5-dicyano-2,6-dipyridyl)pyridyl)benzene (>3); the latter formed in situ from the oxidative dehydrogenation of >1. >SOF-7 shows a three-dimensional four-fold interpenetrated structure with complementary O–H···N hydrogen bonds to form channels that are decorated with cyano and amide groups. >SOF-7 exhibits excellent thermal stability and solvent and moisture durability as well as permanent porosity. The activated desolvated material >SOF-7a shows high CO2 adsorption capacity and selectivity compared with other porous organic materials assembled solely through hydrogen bonding.
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