Exceptional Uranium(VI)-Nitride Triple Bond Covalency from 15N Nuclear Magnetic Resonance Spectroscopy and Quantum Chemical Analysis

Jingzhen Du, John Seed, Victoria Berryman, Nikolas Kaltsoyannis, Ralph Adams, Daniel Lee, Stephen Liddle

Research output: Contribution to journalArticlepeer-review

Abstract

Determining the nature and extent of covalency of early actinide chemical bonding is a fundamentally important challenge. Recently, X-ray absorption, electron paramagnetic, and nuclear magnetic resonance spectroscopic studies have probed actinide-ligand covalency, largely confirming the paradigm of early actinide bonding varying from ionic to polarised-covalent, with this range sitting on the continuum between ionic lanthanide and more covalent d transition metal analogues. Here, we report measurement of the covalency of a terminal uranium(VI)-nitride by 15N nuclear magnetic resonance spectroscopy, and find an exceptional nitride chemical shift and chemical shift anisotropy. This redefines the 15N nuclear magnetic resonance spectroscopy parameter space, and experimentally confirms a prior computational prediction that the uranium(VI)-nitride triple bond is not only highly covalent, but, more so than d transition metal analogues. These results enable construction of general, predictive metal-ligand 15N chemical shift-bond order correlations, and reframe our understanding of actinide chemical bonding to guide future studies.
Original languageEnglish
Pages (from-to)5649
JournalNature Communications
Volume12
DOIs
Publication statusPublished - 24 Sept 2021

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