Abstract
A biscyclen molecular cabin, synthesized by connecting two cyclen macrocycles with four linkages, entraps a Li+···H2O···Li+ trimer with a water molecule clamped by two Li+ ions. This configuration results in strongly polarized water, characterized by a water proton resonance shift of up to 10.00 ppm. The arrangement facilitates unprecedented O-centered chalcogen bonds between the lone pairs of pyridinyl nitrogen atoms and polarized water oxygen, as confirmed by X-ray crystallography, NMR spectroscopy, and theoretical calculations. Further observation of O-centered chalcogen bonding in a H2O·(LiCl)2 cluster suggests its widespread presence in hydrated salt systems.
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