期刊
DALTON TRANSACTIONS
卷 51, 期 22, 页码 8777-8785出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2dt01084d
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资金
- National Natural Science Foundation of China [22071002, 22071122]
- Department of Education, Anhui Province
- Anhui Normal University
Heterobimetallic Ln(iii)-Pd(0) complexes with tetranuclear structures have been synthesized and their properties studied.
Heterobimetallic Ln(iii)-Pd(0) complexes (Ln = Y, Sm, Gd, Yb) featuring tetranuclear structures with COD as bridges were obtained via the metallation of tris(phosphinoamido) rare-earth metal complexes [Ph(2)PNAd](3)Ln (Ad = adamantyl) with (COD)Pd(CH2SiMe3)(2). Notably, the Sc(iii)-Pd(0) complex possesses a C-3-symmetry with a very short Sc-Pd bond length of 2.432(2) angstrom, while the tetranuclear complexes exhibited versatile structures both in solution and in the solid state. Reduction of the trivalent complex (Ph(2)PNAd)(3)Yb with one equivalent of KC8 in the presence of 18-c-6 afforded the divalent complex [(Ph(2)PNAd)(3)Yb][(18-c-6)K(THF)(2)], which was further reacted with (Ph3P)(4)Pd to form the first Yb(ii)-Pd(0) complex. The Pd(0) -> Yb dative interaction weakened significantly from Yb(iii) to Yb(ii) based on computational studies, which was attributed to the attenuated Lewis acidity of the Yb(ii) center. Reactions of Ln(iii)-Pd(0) complexes (Ln = Sc and Yb) with the disulfide PhSSPh showed that the Pd(0) center served as a two-electron donor while the reaction apparently occurred on the Ln(iii) centers to form Ln(iii)-Pd(0) bis-sulfide complexes.
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