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

Josef T. Boronski, John A. Seed, David Hunger, Adam W. Woodward, Joris Slageren, Ashley J. Wooles, Louise S. Natrajan, Nikolas Kaltsoyannis () and Stephen T. Liddle ()
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Josef T. Boronski: The University of Manchester
John A. Seed: The University of Manchester
David Hunger: University of Stuttgart
Adam W. Woodward: The University of Manchester
Joris Slageren: University of Stuttgart
Ashley J. Wooles: The University of Manchester
Louise S. Natrajan: The University of Manchester
Nikolas Kaltsoyannis: The University of Manchester
Stephen T. Liddle: The University of Manchester

Nature, 2021, vol. 598, issue 7879, 72-75

Abstract: Abstract Metal–metal bonding is a widely studied area of chemistry1–3, and has become a mature field spanning numerous d transition metal and main group complexes4–7. By contrast, actinide–actinide bonding, which is predicted to be weak8, is currently restricted to spectroscopically detected gas-phase U2 and Th2 (refs. 9,10), U2H2 and U2H4 in frozen matrices at 6–7 K (refs. 11,12), or fullerene-encapsulated U2 (ref. 13). Furthermore, attempts to prepare thorium–thorium bonds in frozen matrices have produced only ThHn (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 bonding15, 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 bond16,17 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.

Date: 2021
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DOI: 10.1038/s41586-021-03888-3

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