Mg/Al Ordering in Layered Double Hydroxides Revealed by Multinuclear NMR Spectroscopy
10.1126/science.1157581
Crossref journal-article
American Association for the Advancement of Science (AAAS)
Science (221)
Abstract

The anion-exchange ability of layered double hydroxides (LDHs) has been exploited to create materials for use in catalysis, drug delivery, and environmental remediation. The specific cation arrangements in the hydroxide layers of hydrotalcite-like LDHs, of general formula Mg 2+ 1– x Al 3+ x OH 2 (Anion n– x / n )· y H 2 O, have, however, remained elusive, and their elucidation could enhance the functional optimization of these materials. We applied rapid (60 kilohertz) magic angle spinning (MAS) to obtain high-resolution hydrogen-1 nuclear magnetic resonance ( 1 H NMR) spectra and characterize the magnesium and aluminum distribution. These data, in combination with 1 H- 27 Al double-resonance and 25 Mg triple-quantum MAS NMR data, show that the cations are fully ordered for magnesium:aluminum ratios of 2:1 and that at lower aluminum content, a nonrandom distribution of cations persists, with no Al 3+ -Al 3+ close contacts. The application of rapid MAS NMR methods to investigate proton distributions in a wide range of materials is readily envisaged.

Bibliography

Sideris, P. J., Nielsen, U. G., Gan, Z., & Grey, C. P. (2008). Mg/Al Ordering in Layered Double Hydroxides Revealed by Multinuclear NMR Spectroscopy. Science, 321(5885), 113–117.

Authors 4
  1. Paul J. Sideris (first)
  2. Ulla Gro Nielsen (additional)
  3. Zhehong Gan (additional)
  4. Clare P. Grey (additional)
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  32. Support was provided by the Center for Environmental Molecular Sciences funded by NSF grant CHE-0021934. Single-pulse 25 Mg MAS NMR was performed in the Environmental Molecular Sciences Laboratory a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The NMR facility at the National High Magnetic Field Laboratory is supported by NSF and the state of Florida (DMR-0084173). P.J.S thanks J. Ford and A. Palmer for helping with data collection and A. Reynolds for the synthesis of related materials. P.J.S acknowledges the Graduate Assistance in Areas of National Need (GAANN) Fellowship for financial assistance. U.G.N. acknowledges the Camille and Henry Dreyfus Postdoctoral Program in Environmental Chemistry for financial support.
Dates
Type When
Created 17 years, 1 month ago (July 3, 2008, 4:53 p.m.)
Deposited 1 year, 7 months ago (Jan. 10, 2024, 4:03 a.m.)
Indexed 4 days, 14 hours ago (Aug. 23, 2025, 1:04 a.m.)
Issued 17 years, 1 month ago (July 4, 2008)
Published 17 years, 1 month ago (July 4, 2008)
Published Print 17 years, 1 month ago (July 4, 2008)
Funders 0

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@article{Sideris_2008, title={Mg/Al Ordering in Layered Double Hydroxides Revealed by Multinuclear NMR Spectroscopy}, volume={321}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1157581}, DOI={10.1126/science.1157581}, number={5885}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Sideris, Paul J. and Nielsen, Ulla Gro and Gan, Zhehong and Grey, Clare P.}, year={2008}, month=jul, pages={113–117} }