Journal
INORGANIC CHEMISTRY
Volume 51, Issue 3, Pages 1727-1738Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic2020379
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Funding
- DST [SR/S1/IC-01/2008]
- CSIR, New Delhi, India [01-2235/08/EMR-II]
- IIT Guwahati, India
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A tris(2-aminoethyl)amine-based tris(urea) receptor, L, with electron-withdrawing m-nitrophenyl terminals has been established as a potential system that can efficiently capture and fix atmospheric CO2 as air-stable crystals of a CO32--encapsulated molecular capsule (complex 1), triggered by the presence of n-tetrabutylammonium hydroxide/fluoride in a dimethyl sulfoxide solution of L. Additionally, L in the presence of excess HSO4- has been found to encapsulate a divalent sulfate anion (SO42-) within a dimeric capsular assembly of the receptor (complex 2) via hydrogen-bonding-activated proton transfer between the free and bound HSO4- anions. Crystallographic results show proof of oxyanion encapsulation within the centrosymmetric cage of L via multiple N-H center dot center dot center dot O hydrogen bonds to the six urea functions of two inversion-symmetric molecules. The solution-state binding and encapsulation of oxyanions by N-H center dot center dot center dot O hydrogen bonding has also been confirmed by quantitative H-1 NMR titration experiments, 2D NOESY NMR experiments, and Fourier transform IR analyses of the isolated crystals of the complexes that show huge spectral changes relative to the free receptor.
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