Abstract:
:Despite their importance as mechanistic models for heterogeneous Haber Bosch ammonia synthesis from dinitrogen and dihydrogen, homogeneous molecular terminal metal-nitrides are notoriously unreactive towards dihydrogen, and only a few electron-rich, low-coordinate variants demonstrate any hydrogenolysis chemistry. Here, we report hydrogenolysis of a terminal uranium(V)-nitride under mild conditions even though it is electron-poor and not low-coordinate. Two divergent hydrogenolysis mechanisms are found; direct 1,2-dihydrogen addition across the uranium(V)-nitride then H-atom 1,1-migratory insertion to give a uranium(III)-amide, or with trimesitylborane a Frustrated Lewis Pair (FLP) route that produces a uranium(IV)-amide with sacrificial trimesitylborane radical anion. An isostructural uranium(VI)-nitride is inert to hydrogenolysis, suggesting the 5f1 electron of the uranium(V)-nitride is not purely non-bonding. Further FLP reactivity between the uranium(IV)-amide, dihydrogen, and triphenylborane is suggested by the formation of ammonia-triphenylborane. A reactivity cycle for ammonia synthesis is demonstrated, and this work establishes a unique marriage of actinide and FLP chemistries.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Chatelain L,Louyriac E,Douair I,Lu E,Tuna F,Wooles AJ,Gardner BM,Maron L,Liddle STdoi
10.1038/s41467-019-14221-ysubject
Has Abstractpub_date
2020-01-17 00:00:00pages
337issue
1issn
2041-1723pii
10.1038/s41467-019-14221-yjournal_volume
11pub_type
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