Coordination-Driven Assembly of Actinide-Organic Polyrotaxanes Involving Crown Ether Macrocycles
2021
The research on synthesizing new coordination-driven polyrotaxanes as well as regulating structure diversity of them contributes to the prosperity of macrocycle-based supramolecular materials. In this work, we describe the synthesis of a new kind of actinide-organic polyrotaxanes involving crown ether macrocycles for the first time. Crystal structures of two uranyl polyrotaxane compounds, UCER-1 and UCER-2, as well as a third non-polyrotaxane compound UON-1, have been characterized, and the formation mechanism of actinide-organic polyrotaxanes are discussed in terms of factors affecting the assembly process. The comparison of reaction conditions and the corresponding outcomes suggests the necessity of host-guest pseudorotaxane linker for successful construction of targeted actinide-organic polyrotaxanes. The coordination of different coordination atoms, especially bromide ions and uranyl, is analyzed in detail through theoretical calculations. As an extension of cucurbituril-based uranyl-organic polyrotaxanes, the introduction of crown ether macrocycle as a new supramolecular element brings a different kind of actinide polyrotaxanes with intriguing molecular structures and supramolecular assembly behaviours, and will, we believe, expand the research scope of actinide rotaxane coordination polymers.
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