Abstract
A specific assembly process, driven by coexisting X-H...O hydrogen bonding and X...O short intermolecular contacts (X = C, N, O) is described, in which the pseudo-Keggin polyoxoanion and two types of molecule...cation pairs (with C1 and Ci symmetries) were assembled to the programmed supramolecular architecture. Cooperation of the positive-charge, resonance effect and the O=C...Oterminal intermolecular contact led to the short and strong symmetrical [O...H...O]+ hydrogen bond (O...O = 2.449(13) A) in one of the molecule...cation pairs [C4H9NO...H...ONC4H9]+ with the H-bonded proton in the center of inversion. The other [C4H9NOH...ONC4H9]+ molecule...cation pair (non-centrosymmetric) was formed through a very strong asymmetric [O.H.O]+ hydrogen bond of 2.431(13) A in length which was created via the synergistic effect between the minor N-H...O secondary interaction, +CAHB (positive-charge-assisted hydrogen bond) and RAHB (resonance assisted hydrogen bond) mechanisms.
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