Insight into hydrogen bonding of uranyl hydroxide layers and capsules by use of 1H magic-angle spinning NMR spectroscopy [Insight into the hydrogen bonding for uranyl hydroxides using 1H MAS NMR spectroscopy]

Alam, Todd M.; Liao, Zuolei; Nyman, May; Yates, Jonathan

doi:10.1021/acs.jpcc.6b02692

Insight into hydrogen bonding of uranyl hydroxide layers and capsules by use of ¹H magic-angle spinning NMR spectroscopy [Insight into the hydrogen bonding for uranyl hydroxides using ¹H MAS NMR spectroscopy]

Journal Article · Wed Apr 27 04:00:00 EDT 2016 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b02692· OSTI ID:1343264

Alam, Todd M. ^[1]; Liao, Zuolei ^[2]; Nyman, May ^[2]; Yates, Jonathan ^[3]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Oregon State Univ., Corvallis, OR (United States)
Univ. of Oxford, Oxford (United Kingdom)

Solid-state ¹H magic-angle spinning (MAS) NMR was used to investigate local proton environments in anhydrous [UO₂(OH)₂] (α-UOH) and hydrated uranyl hydroxide [(UO₂)₄O(OH)₆·5H₂O (metaschoepite). For the metaschoepite material, proton resonances of the μ₂-OH hydroxyl and interlayer waters were resolved, with two-dimensional (2D) double-quantum (DQ) ¹H–¹H NMR correlation experiments revealing strong dipolar interactions between these different proton species. The experimental NMR results were combined with first-principles CASTEP GIPAW (gauge including projector-augmented wave) chemical shift calculations to develop correlations between hydrogen-bond strength and observed ¹H NMR chemical shifts. Furthermore, these NMR correlations allowed characterization of local hydrogen-bond environments in uranyl U₂₄ capsules and of changes in hydrogen bonding that occurred during thermal dehydration of metaschoepite.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; SC0001089

OSTI ID:: 1343264

Report Number(s):: SAND--2015-10774J; 615185

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 19 Vol. 120; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
1H MAS NMR
GIPAW
chemical shift
hydrogen bonding
metaschoepite