Abstract
A meta-phenylenediamine-based disubstituted bis-urea receptor L1 with electron-withdrawing 3-chloro and electron-donating 4-methylphenyl terminals has been established as a potential system to fix and efficiently capture atmospheric CO2 as air-stable entrapment of an unprecedented {CO32--(H2O)2-CO32-} cluster (complex 1a) within its tetrameric long straight pillar-like assembly entirely sealed by n-TBA cations via formation of a barrel-type architecture. L1 and its isomeric 4-bromo-3-methyl disubstituted bis-urea receptor L2 have been found to entrap similar kinds of water-free naked sulfate-sulfate double anion (complexes 1b and 2a) by cooperative binding of urea moieties inside the two pairs of the inversion-symmetric linear tetrameric barrel of L1 and L2, respectively. On the other hand, in the presence of excess halides, L1 self-assembles to form hexa-coordinated fluoride complex 1c and tetra-coordinated bromide complex 1d, while L2 self-assembles to form penta-coordinated fluoride complex 2b in the solid state via semicircular receptor architectures and non-cooperative H-bonding interactions of urea moieties.
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