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A crystalline tri-thorium cluster with σ-aromatic metal-metal bonding

机译：具有ïƒ芳香金属 - 金属粘合的结晶三钍簇

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摘要

Metal-metal bonding is a widely studied area of chemistry~(1-3), and has become a mature field spanning numerous d transition metal and main group complexes~(4-7). By contrast, actinide-actinide bonding, which is predicted to be weak~(8), is currently restricted to spectroscopically detected gas-phase U_(2)and Th_(2)(refs.~(9,10)), U_(2)H_(2)and U_(2)H_(4)in frozen matrices at 6-7 K (refs.~(11,12)), or fullerene-encapsulated U_(2)(ref.~(13)). Furthermore, attempts to prepare thorium-thorium bonds in frozen matrices have produced only ThH_(n)(n = 1-4)~(14). Thus, there are no isolable actinide-actinide bonds under normal conditions. Computational investigations have explored the probable nature of actinide-actinide bonding~(15), concentrating on localized σ-, π-, and δ-bonding models paralleling d transition metal analogues, but predictions in relativistic regimes are challenging and have remained experimentally unverified. Here, we report thorium-thorium bonding in a crystalline cluster, prepared and isolated under normal experimental conditions. The cluster exhibits a diamagnetic, closed-shell singlet ground state with a valence-delocalized three-centre-two-electron σ-aromatic bond~(16,17)that is counter to the focus of previous theoretical predictions. The experimental discovery of actinide σ-aromatic bonding adds to main group and d transition metal analogues, extending delocalized σ-aromatic bonding to the heaviest elements in the periodic table and to principal quantum number six, and constitutes a new approach to elaborate actinide-actinide bonding.
机译：金属金属粘合是一种广泛研究的化学面积〜（1-3），已成为跨越无数D转化金属和主要组络合物〜（4-7）的成熟场。相反，预测弱〜（8）的滑动术 - 致动键合，目前仅限于光谱检测到的气相U_（2）和TH_（2）（参考文献〜（9,10）），U_（ 2）H_（2）和U_（2）H_（4）在6-7 k的冷冻矩阵（参考文献〜（11,12））或富勒烯 - 封装的U_（2）（参考。〜（13）） 。此外，试图在冷冻矩阵中制备钍键的钍键已经仅产生THH_（n）（n = = 1-4℃）〜（14）。因此，在正常条件下没有可分离的椎酸酯 - 致动粘合剂。计算调查探索了猕猴桃粘结〜（15）的可能性质，集中在局部化的ïƒ - ，ï，和Î'-粘接模型平行于Dâ过渡金属类似物，但相比主义制度的预测是具有挑战性的，并在实验上仍然存在未经证实的。在这里，我们在正常实验条件下报告在结晶簇中的钍 - 钍键合，并在正常的实验条件下分离。该簇具有抗磁性，闭式壳单次晶状体，其具有替补的三中心 - 双电子ïƒ - 芳香键〜（16,17），这与先前理论预测的焦点相反。 Actinideα-芳族键合的实验发现增加了主要基团和Dâ过渡金属类似物，将被截匙α-芳族键合到周期表中最重的元素和主要量子数六，并构成了阐明神奇曲线的新方法粘接。

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  • 来源
    《Nature》 |2021年第7879期|72-75|共4页
  • 作者

    Josef T Boronski; John A Seed; David Hunger; Adam W Woodward; Joris van Slageren; Ashley J Wooles; Louise S Natrajan; Nikolas Kaltsoyannis; Stephen T Liddle;

  • 作者单位

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

    Institute of Physical Chemistry University of Stuttgart;

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

    Institute of Physical Chemistry University of Stuttgart;

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

    Department of Chemistry and Centre for Radiochemistry Research The University of Manchester;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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