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UCN@Cs(6)-C82: An Encapsulated Triangular UCN Cluster with Ambiguous U Oxidation State [U(III) versus U(I)]
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-09-23 , DOI: 10.1021/jacs.1c07519
Qingyu Meng 1 , Laura Abella 2 , Wei Yang 1 , Yang-Rong Yao 3 , Xinye Liu 1 , Jiaxin Zhuang 1 , Xiaomeng Li 1 , Luis Echegoyen 3 , Jochen Autschbach 2 , Ning Chen 1
Affiliation  

Understanding the chemical behavior of actinide elements is essential for the effective management and use of actinide materials. In this study, we report an unprecedented η2 (side-on) coordination of U by a cyanide in a UCN cluster, which was stabilized inside a C82 fullerene cage. UCN@Cs(6)-C82 was successfully synthesized and fully characterized by mass spectrometry, single crystal X-ray crystallography, cyclic voltammetry, spectroscopy, and theoretical calculations. The bonding analysis demonstrates significant donation bonding between CN and uranium, and covalent interactions between uranium and the carbon cage. These effects correlate with an observed elongated cyanide C–N bond, resulting in a rare case where the oxidation state of uranium shows ambiguity between U(III) and U(I). The discovery of this unprecedented triangular configuration of the uranium cyanide cluster provides a new insight in coordination chemistry and highlights the large variety of bonding situations that uranium can have.

中文翻译:

UCN@Cs(6)-C82:具有模糊 U 氧化态的封装三角形 UCN 簇 [U(III) 与 U(I)]

了解锕系元素的化学行为对于锕系材料的有效管理和使用至关重要。在这项研究中,我们报告了 UCN 簇中氰化物对 U 的前所未有的 η 2(侧面)配位,该簇稳定在 C 82富勒烯笼内。成功合成了UCN@ C s (6)-C 82,并通过质谱、单晶 X 射线晶体学、循环伏安法、光谱学和理论计算对其进行了全面表征。结合分析表明 CN 之间存在显着的捐赠结合-和铀,以及铀和碳笼之间的共价相互作用。这些效应与观察到的伸长的氰化物 C-N 键相关,导致铀的氧化态在 U(III) 和 U(I) 之间显示模糊的罕见情况。这种前所未有的氰化铀簇三角形构型的发现为配位化学提供了新的见解,并突出了铀可能具有的多种键合情况。
更新日期:2021-10-06
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