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Issue 7, 2016
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The role of dynamic ligand exchange in the oxidation chemistry of cerium(III)

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Abstract

The CeIII/IV couple is useful for many applications in organic, inorganic, and materials chemistry. However, attaining a general method to access both oxidations states through reversible solution redox chemistry remains challenging. Herein we report the synthesis, characterization, and oxidation chemistry of the novel Ce/Li REMB heterochiral diastereomer, 1-Ce(het). The solution exchange processes of 1-RE(het) (RE = Ce and Yb) were investigated to estimate rates of ligand and cation exchange relevant in homochiral and heterochiral frameworks. A detailed mechanistic investigation following the solution dynamics of 1-Ce(het) revealed reactivity controlled both by ligand reorganization and redistribution processes. Ligand reorganization was responsible for the kinetics associated with the chemical oxidation reaction, whereas ligand redistribution and exchange dictated the isolated products.

Graphical abstract: The role of dynamic ligand exchange in the oxidation chemistry of cerium(iii)

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Publication details

The article was received on 18 Dec 2015, accepted on 22 Mar 2016 and first published on 23 Mar 2016


Article type: Edge Article
DOI: 10.1039/C5SC04897D
Citation: Chem. Sci., 2016,7, 4537-4547
  • Open access: Creative Commons BY-NC license
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    The role of dynamic ligand exchange in the oxidation chemistry of cerium(III)

    J. R. Robinson, Y. Qiao, J. Gu, P. J. Carroll, P. J. Walsh and E. J. Schelter, Chem. Sci., 2016, 7, 4537
    DOI: 10.1039/C5SC04897D

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