Axially Symmetric U−O−Ln‐ and U−O−U‐Containing Molecules from the Control of Uranyl Reduction with Simple f‐Block Halides

The reduction of U^VI uranyl halides or amides with simple Ln^II or U^III salts forms highly symmetric, linear, oxo‐bridged trinuclear U^V/Ln^III/U^V, Ln^III/U^IV/Ln^III, and U^IV/U^IV/U^IV complexes or linear Ln^III/U^V polymers depending on the stoichiometry and solvent. The reactions can be tuned to give the products of one‐ or two‐electron uranyl reduction. The reactivity and magnetism of these compounds are discussed in the context of using a series of strongly oxo‐coupled homo‐ and heterometallic poly(f‐block) chains to better understand fundamental electronic structure in the f‐block.