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Snapshots of Ce70 Toroid Assembly from Solids and Solution
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    Snapshots of Ce70 Toroid Assembly from Solids and Solution
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 25, 9612–9621
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    https://doi.org/10.1021/jacs.1c04095
    Published June 17, 2021
    Copyright © 2021 American Chemical Society

    Abstract

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    Crystallization at the solid–liquid interface is difficult to spectroscopically observe and therefore challenging to understand and ultimately control at the molecular level. The Ce70-torroid formulated [CeIV70(OH)36(O)64(SO4)60(H2O)10]4–, part of a larger emerging family of MIV70-materials (M = Zr, U, Ce), presents such an opportunity. We elucidated assembly mechanisms by the X-ray scattering (small-angle scattering and total scattering) of solutions and solids as well as crystallizing and identifying fragments of Ce70 by single-crystal X-ray diffraction. Fragments show evidence for templated growth (Ce5, [Ce5(O)3(SO4)12]10-) and modular assembly from hexamer (Ce6) building units (Ce13, [Ce13(OH)6(O)12(SO4)14(H2O)14]6– and Ce62, [Ce62(OH)30(O)58(SO4)58]14-). Ce62, an almost complete ring, precipitates instantaneously in the presence of ammonium cations as two torqued arcs that interlock by hydrogen boding through NH4+, a structural motif not observed before in inorganic systems. The room temperature rapid assemblies of both Ce70 and Ce62, respectively, by the addition of Li+ and NH4+, along with ion-exchange and redox behavior, invite exploitation of this emerging material family in environmental and energy applications.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.1c04095.

    • Details concerning synthesis, instrumentation, crystallography, crystallographic tables, summary of bond lengths and bond valence sum calculations, microscope images of crystals, ion-sorption studies, miscellaneous supplementary images, and table summarizing large cerium-oxo clusters synthesized to date (PDF)

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    CCDC 2057078, 20570852057086, 20570882057091, and 2064990 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

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    This article is cited by 21 publications.

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 25, 9612–9621
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c04095
    Published June 17, 2021
    Copyright © 2021 American Chemical Society

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