27 Al Pulsed Field Gradient, Diffusion–NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions

Graham, Trent R.; Han, Kee Sung; Dembowski, Mateusz; Krzysko, Anthony J.; Zhang, Xin; Hu, Jianzhi; Clark, Sue B.; Clark, Aurora E.; Schenter, Gregory K.; Pearce, Carolyn I.; Rosso, Kevin M.

doi:10.1021/acs.jpcb.8b10145

Title: ²⁷ Al Pulsed Field Gradient, Diffusion–NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions

Journal Article · Wed Oct 24 00:00:00 EDT 2018 · Journal of Physical Chemistry. B

DOI:https://doi.org/10.1021/acs.jpcb.8b10145· OSTI ID:1596368

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Washington State Univ., Pullman, WA (United States)

Here, pulsed field gradient nuclear magnetic resonance (PFG-NMR) measurements were successfully applied to the ²⁷Al (I = 5/2) nucleus in concentrated electrolytes to investigate the diffusion of aluminate ions [Al(OH)₄^–] in simulant high-level nuclear waste (3 M NaOH) between 25 and 85 °C. The temperature-dependent diffusion coefficients obtained from ¹H, ²³Na, and ²⁷Al PFG-NMR were well fit by a Vogel–Fulcher–Tammann model and a power law equation. Comparison of ²⁷Al diffusion coefficients of 0.1 M Al(OH)₄^– in ~3 M MOH (where M = Na⁺, K⁺, (CH₃)₄N⁺) at room temperature varied in agreement with the expected changes in solution viscosity via Stokes–Einstein relationship, confirming that the dominant Al species at these conditions are Al(OH)₄^– monomers. This ²⁷Al PFG-NMR study extends an established methodology to a previously unexplored nucleus enabling this experimental technique to be leverage for exploring ion transport, speciation, and solution structure in concentrated electrolytes.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1596368

Journal Information:: Journal of Physical Chemistry. B, Vol. 122, Issue 48; ISSN 1520-6106

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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