The Mechanism Responsible for Extraordinary Cs Ion Selectivity in Crystalline Silicotitanate

Combining information from time-resolved X-ray and neutron scattering with theoretical calculations has revealed the elegant mechanism whereby hydrogen crystalline silicotitanate (H-CST; H2Ti2SiO7·1.5H2O) achieves its remarkable ion-exchange selectivity for cesium. Rather than a simple ion-for-ion d...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2008-09, Vol.130 (35), p.11689-11694
Main Authors: Celestian, Aaron J, Kubicki, James D, Hanson, Jonathon, Clearfield, Abraham, Parise, John B
Format: Article
Language:English
Subjects:
08 HYDROGEN
CAPACITY
CESIUM
CONFORMATIONAL CHANGES
HYDROGEN
ION EXCHANGE
national synchrotron light source
NEUTRONS
PROTEINS
SCATTERING
WATER
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Summary:Combining information from time-resolved X-ray and neutron scattering with theoretical calculations has revealed the elegant mechanism whereby hydrogen crystalline silicotitanate (H-CST; H2Ti2SiO7·1.5H2O) achieves its remarkable ion-exchange selectivity for cesium. Rather than a simple ion-for-ion displacement reaction into favorable sites, which has been suggested by static structural studies of ion-exchanged variants of CST, Cs+ exchange proceeds via a two-step process mediated by conformational changes in the framework. Similar to the case of ion channels in proteins, occupancy of the most favorable site does not occur until the first lever, cooperative repulsive interactions between water and the initial Cs-exchange site, repels a hydrogen lever on the silicotitanate framework. Here we show that these interactions induce a subtle conformational rearrangement in CST that unlocks the preferred Cs site and increases the overall capacity and selectivity for ion exchange.
ISSN:0002-7863
1520-5126
DOI:10.1021/ja801134a