27Al NMR diffusometry of Al13 Keggin nanoclusters

Graham, Trent R.; Chun, Jaehun; Schenter, Gregory K.; Zhang, Xin; Clark, Sue B.; Pearce, Carolyn I.; Rosso, Kevin M.

doi:10.1002/mrc.5218

²⁷Al NMR diffusometry of Al₁₃ Keggin nanoclusters

Journal Article · Sat Sep 18 00:00:00 EDT 2021 · Magnetic Resonance in Chemistry

DOI:https://doi.org/10.1002/mrc.5218· OSTI ID:2474939

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

Although nanometer-sized aluminum hydroxide clusters (i.e., ϵ-Al₁₃, [Al₁₃O₄(OH)₂₄(H₂O)₁₂]⁷⁺) command a central role in aluminum ion speciation and transformations between minerals, measurement of their translational diffusion is often limited to indirect methods. Here, in this work, ²⁷Al pulsed field gradient stimulated echo nuclear magnetic resonance (PFGSTE NMR) spectroscopy has been applied to the AlO₄ core of the ϵ-Al₁₃ cluster with complementary theoretical simulations of the diffusion coefficient and corresponding hydrodynamic radii from a boundary element-based calculation. The tetrahedral AlO₄ center of the ϵ-Al₁₃ cluster is symmetric and exhibits only weak quadrupolar coupling, which results in favorable T₁ and T₂ ²⁷Al NMR relaxation coefficients for ²⁷Al PFGSTE NMR studies. Stokes–Einstein relationship was used to relate the ²⁷Al diffusion coefficient of the ϵ-Al₁₃ cluster to the hydrodynamic radius for comparison with theoretical simulations, dynamic light scattering from literature, and previously published ¹H PFGSTE NMR studies of chelated Keggin clusters. This first-of-its-kind observation proves that ²⁷Al PFGSTE NMR diffusometry can probe symmetric Al environments in polynuclear clusters of greater molecular weight than previously considered.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2474939

Alternate ID(s):: OSTI ID: 1826396

Report Number(s):: PNNL-SA--160471

Journal Information:: Magnetic Resonance in Chemistry, Journal Name: Magnetic Resonance in Chemistry Journal Issue: 2 Vol. 60; ISSN 0749-1581

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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