Abstract:We report the synthesis and characterisation of isostructural thorium(IV)- and uranium(IV)-
silanide complexes, providing the first structurally authenticated Th-Si bond and a rare example of a
molecular U-Si bond. These complexes therefore present the first opportunity to directly compare the
chemical bonding of Th-Si and U-Si bonds. Quantum chemical calculations show significant and
surprisingly similar 7s, 6d, and 5f orbital contributions from both actinide (An) elements in polarised
covalent An-Si bonds
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