Abstract：
:Although the chemistry of uranium-ligand multiple bonding is burgeoning, analogous complexes involving other actinides such as thorium remain rare and there are not yet any terminal thorium nitrides outside of cryogenic matrix isolation conditions. Here, we report evidence that reduction of a thorium-azide produces a transient Th≡N triple bond, but this activates C-H bonds to produce isolable parent imido derivatives or it can be trapped in an N-heterocycle amine. Computational studies on these thorium-nitrogen multiple bonds consistently evidences a σ > π energy ordering. This suggests pushing-from-below for thorium, where 6p-orbitals principally interact with filled f-orbitals raising the σ-bond energy. Previously this was dismissed for thorium, being the preserve of uranium-nitrides or the uranyl dication. Recognising that pushing-from-below perhaps occurs with thorium as well as uranium, and with imido ligands as well as nitrides, suggests this phenomenon may be more widespread than previously thought.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Du J,Alvarez-Lamsfus C,Wildman EP,Wooles AJ,Maron L,Liddle STdoi
10.1038/s41467-019-12206-5subject
Has Abstractpub_date
2019-09-13 00:00:00pages
4203issue
1issn
2041-1723pii
10.1038/s41467-019-12206-5journal_volume
10pub_type
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