期刊
DALTON TRANSACTIONS
卷 47, 期 29, 页码 9709-9716出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8dt01834k
关键词
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资金
- National Natural Science Foundation of China [21572205]
- Open Research Fund of State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences [2017-22]
- Key Laboratory of Organic Synthesis of Jiangsu Province [KJS1748]
- K. C. Wong Magna Fund in Ningbo University
An acid-base reaction between the rare-earth tris(o-dimethylaminobenzyl) complexes Ln(CH2C6H4NMe2-o)(3) and the pyrrolyl-functionalized arylamide ligands 2,5-Me2C4H2NCH2SiMe2 NHC6H4R (R = H, (HL1); R = Cl-p, (HL2)) was investigated. Treatment of HL1 and HL2 with 1 equiv. of Ln(CH2C6H4NMe2-o)(3) in toluene at room temperature gave (2,5-Me2C4H2CH2NSiMe2NC6H5) Ln(CH2C6H4NMe2-o)(2) (Ln = Sc (1), La (2), Lu (3)) and (2,5-Me2C4H2NCH2SiMe2NC6H4Cl-p) Ln(CH2 C6H4NMe2-o)(2) (Ln = Sc (4), La (5), Lu (6)) in good isolated yields. These complexes were characterized by elemental analysis and NMR spectroscopy. 2, 4 and 5 were structurally authenticated by single crystal X-ray diffraction. NMR and X-ray diffraction show that there are no interactions between the central metal and the pyrrolyl moiety in small sized metal complexes, while in large lanthanum complexes, besides the coordination of the arylamide moiety to La3+ in eta(1)-bonding mode through a N atom, the pyrrolyl ring also has close contact with La3+ in 2 and 5. The binary systems of 1-6/[Ph3C][B(C6F5)(4)] were employed as catalysts for syndio-specific polymerization of styrene, and the pyrrolyl-ligated lanthanum complexes showed much higher activity than the complexes in which the pyrrolyl moiety had no coordination with the central metal.
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