期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 24, 期 30, 页码 7702-7709出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201800610
关键词
amides; low-valent metals; magnetism; rare-earth metals; reductions
资金
- US National Science Foundation [CHE-1565776, CHE-1464828, CHE-1464841]
- Division Of Chemistry [1464841, 1464828] Funding Source: National Science Foundation
A new series of Ln(2+) complexes has been synthesized that overturns two previous generalizations in rare-earth metal reduction chemistry: that amide ligands do not form isolable complexes of the highly reducing non-traditional Ln(2+) ions, and that yttrium is a good model for the late lanthanides in these reductive reactions. Reduction of Ln(NR2)(3) (R=SiMe3) complexes in THF under Ar with M=K or Rb in the presence of 2.2.2-cryptand (crypt) forms crystallographically characterizable [M(crypt)][Ln(NR2)(3)] complexes not only for the traditional Tm2+ ion and the configurational crossover ions, Nd2+ and Dy2+, but also for the non-traditional Gd2+, Tb2+, Ho2+, and Er2+ ions. Crystallographic data as well as UV/Vis, magnetic susceptibility, and density functional theory studies are consistent with the accessibility of 4f(n)5d(1) configurations for Ln(2+) ions in this tris(silylamide) ligand environment. The Dy2+ complex, [K(crypt)][Dy(NR2)(3)], has a higher magnetic moment than previously observed for any monometallic complex: 11.67 mu(B).
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