CeIV70 oxosulfate rings, frameworks, supramolecular assembly and redox activity

Colliard, Ian; Nyman, May

doi:10.1002/anie.202016522

Title: Ce^IV₇₀ oxosulfate rings, frameworks, supramolecular assembly and redox activity

Journal Article · Thu Jan 07 00:00:00 EST 2021 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202016522· OSTI ID:1759989

Colliard, Ian ^[1]; Nyman, May ^[1]

Oregon State Univ., Corvallis, OR (United States)

Abstract M ^IV molecular oxo‐clusters (M=Zr, Hf, Ce, Th, U, Np, Pu) are prolific in bottoms‐up material design, catalysis, and elucidating reaction pathways in nature and in synthesis. Here we introduce Ce ₇₀ , a wheel‐shaped oxo‐cluster, [Ce ^IV ₇₀ (OH) ₃₆ (O) ₆₄ (SO ₄ ) ₆₀ (H ₂ O) ₁₀ ] ⁴⁻ . Ce ₇₀ crystallizes into intricate high pore volume frameworks with divalent transition metals and Ce‐monomer linkers. Eight crystal‐structures feature four framework types in which the Ce ₇₀ ‐rings are linked as propellers, in offset‐stacks, in a tartan pattern, and as isolated rings. Small‐angle X‐ray scattering of Ce ₇₀ dissolved in butylamine, with and without added cations (Ce ^IV , alkaline earths, Mn ^II ), shows the metals‘ differentiating roles in ring linking, leading to supramolecular assemblies. The large acidic pores and abundant terminal sulfates provide ion‐exchange behavior, demonstrated with U ^IV and Nd ^III . Frameworks featuring Ce ^III/IV ‐monomer linkers demonstrate both oxidation and reduction. This study opens the door to mixed‐metal, highly porous framework catalysts, and new clusters for metal‐organic framework design

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Research Organization:: University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003763

OSTI ID:: 1759989

Alternate ID(s):: OSTI ID: 1777610

Journal Information:: Angewandte Chemie (International Edition), Vol. 60, Issue 13; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Cerium
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Supramolecular
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CSD 2016624: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pgdr The current record is supplemented by this dataset	dataset	January 2021
CSD 2016615: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pg3g The current record is supplemented by this dataset	dataset	January 2021
CSD 2016626: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pggt The current record is supplemented by this dataset	dataset	January 2021
CSD 2016629: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pgkx The current record is supplemented by this dataset	dataset	January 2021
CSD 2016618: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pg6k The current record is supplemented by this dataset	dataset	January 2021
CSD 2016617: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pg5j The current record is supplemented by this dataset	dataset	January 2021
CSD 2016621: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pg9n The current record is supplemented by this dataset	dataset	January 2021
CSD 2016616: Experimental Crystal Structure Determination Ian, Colliard,; May, Nyman, https://doi.org/10.25505/fiz.icsd.cc25pg4h The current record is supplemented by this dataset	dataset	January 2021

Title: CeIV70 oxosulfate rings, frameworks, supramolecular assembly and redox activity

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Title: Ce^IV₇₀ oxosulfate rings, frameworks, supramolecular assembly and redox activity