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徐善生, Baiquan Wang, *[a] Bin Mu, [a] Xiaobin Deng, [a] Huiling Cui, [a] Shansheng Xu, [a] Xiuzhong Zhou, [a] Fenglou Zou, [b] Yang Li, [b] Ling Yang, [c] Yufei Li, [c] and Youliang Hu[c]
Chem. Eur. J. 2005, 11, 669-679,-0001,():
-1年11月30日
合成了一系列亚环烷基桥连环戊二烯基茂金属化合物(CH2)nC(C5H4)2MCI2[M=Ti,n=4(4),5(5),6(6); M=Zr,n=4(10)、5(11)、6(12)],用甲基铝氧烷(MAO)作助催化剂研究了其催化乙烯聚合反应。其中亚环烷基桥连环戊二烯基钛化合物的催化活性远高于相应的锆和铪类似物,且在较高温度显示其最高活性。为进行对比,合成了亚硅杂环戊基桥连环戊二烯基茂金属化合物(CH2)4Si(C5H4)2MCI2(M-Ti,Zr)和亚异丙基桥连环戊二烯基茂金属化合物Me2C(C5H4)2MCI(M=Ti,Zr)并用于催化乙烯聚合。在这两种催化剂中,钛化合物的催化活性都远离于相应的锆类似物,尤其是在较低温度下。用X-射线衍射分析测定了化合物4~9的晶体结构。对催化剂结构与催化活性的关系,特别是桥链的影响进行了讨论。
bridging ligands, metallocenes, structure-activity relationships, titanium, zirconium
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【期刊论文】Diels-Alder Reactions of Benzyne with Indenyl Iron Complexes
徐善生, Baiquan Wang, * Bin Mu, Dafa Chen, Shansheng Xu, and Xiuzhong Zhou
Organometallcs 2004, 23, 6225-6230,-0001,():
-1年11月30日
The indenyl iron compound (η5-C9H7)Fe(η5-C5H5) (1) was found to react with benzyne, generated from o-trimethylsilylphenyl triflate by fluoride-induced 1, 2-elimination, to afford the Diels-Alder adduct 1,2-(1,4-dihydro-naphthalen-1,4-diyl)ferrocene (2). When the bis-(indenyl) iron complexes (η5-R-C9H6)2Fe [R=H(3); 2-Me(6); 1-SiMe3(9)] reacted with benzyne, the bisadducts [R=H(5); 2-Me(8); 1-SiMe3(11)] were obtained along with the corresponding monoadducts [R=H(4); 2-Me(7); 1-SiMe3(10)]. The reaction of teramethyl-dislyene-bridged bis(indenyl) iron (Me2SiSiMe2)(η5-C9H6)2Fe(12) with benzyne gave only the monoadduct (13). Complex 2 was also tested for ring-opening metathesis polymerization (ROMP) in the presence of Grubbs' catalyst [(PCy3)2RuCl2=CHPh] but was found to be inactive under normal conditions. The molecular structures of 2, 5, 8, and 13 have been determinde by X-ray diffraction.
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徐善生, Shansheng Xu, Xuliang Dai, Tao Wu, Baiquan Wang*, Xiuzhong, Zhou, Linhong Weng
Journal of Organometallic Chemistry 645(2002)212-217,-0001,():
-1年11月30日
A series of doubly bridged dinuclear titanium and zirconium complexes (Me2C)(Me2E)(C5H3)2(Cp'MCI2)2 [E=Si,Cp'=C5H5, M=Ti (1), Zr (2); E=Ge, Cp'=C5H5, M=Ti (3), Zr (4); Cp'=C5Me4H, M=Zr, E=Si (5), Ge (6)] and (Me2SiOSiMe2)2(C5H3)2(Cp'MCI2)2[Cp'=C5H5, M=Ti (7), Zr (8); Cp=C5Me4H, M=Zr (9)] were synthesized by the reaction of the lithium compounds of the corresponding doubly bridged cyclopentadienyl ligands with CpTiCl3, CpZrCl3(THF)2 or C5Me4HZrCl3, respectively. These complexes were characterized by 1H-NMR, MS and elemental analysis. The crystal structure of 4 was determined by the X-ray diffraction. Their catalytic properties for ethylene polymerization were also studied in the presence of MAO.
Titanium, Zirconium, Doubly bridged, Dinuclear, Polymerization
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徐善生, Dafa Chen, Ying Li, Baiquan Wang, * Shansheng Xu, and Haibin Song
Organometallics 2006, 25, 307-310,-0001,():
-1年11月30日
Thermal treatment of the prydyl side-chain-func-tionalized cyclopentadiense with Fe(CO)5 and Ru3(CO)12 gave different intramolecular C-H activated products, in addittion to the normal dinuclear metal complexs. Reactions of the dinuclear metal complexs with I2 also gave different metal iodide complexes.
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徐善生, Bin Li a, Baiquan Wang a, b, *, Shansheng Xu a, Xiuzhong Zhou a
Journal of Organometallic Chemistry 690(2005)5309-5317,-0001,():
-1年11月30日
Reductive coupling of phenylfulvene with amalgamated calcium metal followed by hydrolysis yields CpPhCHCHPhCp (1) in high yield. Refluxing ligand 1 and Fe(CO)5 in xylene produces (PhCHCHPh)-coupled bis(cyclopentadienyl) tetracacrbonyl dirron (PhCHCHPh)[(η5-C5H4)Fe(CO2]2 (2) as a mixture of meso (2-meso) and racemis isomers (2-rac). The pure reacmic isomers of the Mo and W analogues (3-rac and 4-rac) have been synthesized by lithiation of ligand 1 and addition of (MeCN)3M(CO)3(M=Mo,W) followed by oxidation with 2 equiv. of ferrocenium tetrafluroborate. All the new complexs have been fully charac-terrized. The meolecular structure of 1-meso, 2-meso, 2-rac, 3-rac, and 4-rac have been determinde by X-ray diffraction analysis.
Metal-metal bond, Cyclopentadienyl, Metal carbonyl
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