Time-Resolved Self-Assembly of a Fullerene-Topology Core鈥揝hell Cluster Containing 68 Uranyl Polyhedra

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• 作者：Jie Qiu ; Jie Ling ; Audrey Sui ; Jennifer E. S. Szymanowski ; Antonio Simonetti ; Peter C. Burns
• 刊名：The Journal of the American Chemical Society
• 出版年：2012
• 出版时间：January 25, 2012
• 年：2012
• 卷：134
• 期：3
• 页码：1810-1816
• 全文大小：512K
• 年卷期：v.134,no.3(January 25, 2012)
• ISSN：1520-5126

文摘

A complex core鈥搒hell cluster consisting of 68 uranyl peroxo polyhedra, 16 nitrate groups, and 44 K⁺ and Na⁺ cations was obtained by self-assembly in alkaline aqueous solution under ambient conditions. Crystals formed after a month and were characterized. The cluster, designated as {U₁U₂₈U_40R}, contains a fullerene-topology cage built from 28 uranyl polyhedra. A ring consisting of 40 uranyl polyhedra linked into five-membered rings and 16 nitrate groups surrounds this cage cluster. Topological pentagons in the cage and ring are aligned, and their corresponding rings of uranyl bipyramids are linked through K⁺ cations located between the two shells. A partially occupied U site is located at the center of the cluster. Time-resolved small-angle X-ray scattering and electrospray ionization mass spectrometry demonstrated that the U₂₈ cage cluster formed in solution within an hour, whereas the U_40R shell formed around the cage cluster after more than several days.