徐善生
从事元素及金属有机化学和均相烯烃聚合催化剂的研究
个性化签名
- 姓名:徐善生
- 目前身份:
- 担任导师情况:
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学术头衔:
博士生导师
- 职称:-
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学科领域:
有机化学
- 研究兴趣:从事元素及金属有机化学和均相烯烃聚合催化剂的研究
徐善生,南开大学化学系教授,博士生导师。1966年毕业于南开大学化学系,留校工作至今。目前主要从事元素及金属有机化学和均相烯烃聚合催化剂的研究。曾从事防化学武器的研究,前列腺素的全合成研究,中草药的提取与结构改造,有机硅化合物在有机合成中的应用,有机硅氢化反应,二氢茉莉酮酸甲酯、橡苔等香料的合成研究。多项成果分别经国家科技部、解放军参谋部、天津市科委鉴定、验收用于实际生产中。在国内外核心期刊上发表论文100多篇,合著译著、专著各一部,授权中国发明专利7项,获教育部科技进步奖两项,多次被学校评为优秀教师。
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796
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成果数
20
徐善生, Bin Li, Baiquan Wang, * Shansheng Xu, Xiuzhong Zhou, and Haibin Song
Organometallics 2006, 25, 1158-1166,-0001,():
-1年11月30日
Reactions of CpArCHCHArCp [Ar=Ph (1), p-MeOC6H4 (2)] with Ru3(CO)12 in refluxing xylene afforded the unexpected bridgeing C-C cleavage and cyclopentadienyl coupling products: the 2,2'-bisubstituted fulvalene diruthenium complexes (η5:η5-2,2'-ArCH2C5H3C5H3CH2Ar)Ru2(CO)4 [Ar=Ph (5),p-MeOC6H4 (9)] and the partially hydorgented products (η5:η3-ArCH2C5H3C5H6CHAr)Ru2(CO)4 [Ar=Ph(4), p-MeOC6H4 (8)], in addition to the normal bridged bis(cyclopentadienyl) tetracarbonyl diruthenium complexes (ArCHCHAr)[η5-C5H4)Ru(CO)]2(μ-CO)2[Ar=Ph(7),p-MeOC6H4 (10)]. When ligand (tBuC5H4)PhCHCHPh(tBuC5H4) (3) reacted with Ru3(CO)12, the tetrasubstituted fulvalene diruthenium complex (η5:η5-PhCH2tBuC5H2C5H2tBuCH2Ph)Ru2(CO)4 (11) and three normal bridged bis-(cyclopentadienyl) diruthenium complexes (PhCHCHPh)[(η5-tBuC5H3)Ru(CO)]2(μ-CO)2 (12-14) were obtained. The molecular structures of 4, 5, 7-meso, 7-rac, 8, 10-meso, 11, 12, 13, and 14 were determined by X-ray diffraction. The stereochemistry of the reaction was also studied, and the possible mechanism was discussed.
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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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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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【期刊论文】Controlled/"Living" Radical Polymerization of MMA Catalyzed by Cobaltocene
徐善生, Baiquan Wang, *, †, ‡, Yan Zhuang, † Xiongxiong Luo, † Shansheng Xu, † and Xiuzhong Zhou†
Macromolecules 2003, 36, 9684-8686,-0001,():
-1年11月30日
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【期刊论文】Reactions of Doubly Bridged Bis (cylopentadienes) with Iron Pentacarbonyl
徐善生, Baiquan Wang, * Bin Zhu, Jianyong Zhang, Shansheng Xu, Xiuzhong Zhou, and Linhong Weng†
Organometallics 2003, 22, 4842-4852,-0001,():
-1年11月30日
When the doubly bridged bis(cyclopentadiene) ligand (Me2C)(Me2Si)(C5H4)2 (1) reacted with Fe(CO)5 in refluxing toluene, the unusual product [(C5H6)(Me2C)(Me2Si)(η5-C5H3)Fe(CO)]2-(μ-CO)2 (2) with a hydrogenated double bond in one of the cyclopentadiene ligands, the diiron complex (Me2C)(Me2Si)[(η5-C5H3)Fe(CO)2]2 (3), and the desilylation product 4 were obtained. When the reaction was performed in refluxing xylene, the novel complex (Me2C)(η5-C5H3)-(η5:η1-C5H3)[(Me2Si)Fe(CO)2][Fe(CO)2] (5) with and Fe-Si bond, which should be accompanied by the cleavage of a C-Si bond in the ligand, was isolated in addition to the complees 2~4. When bis(cyclopentadienyl) ligands bridged with R2C (R2C=Me2C, (CH2)5C)AND Me2E(E=Si, Ge) groups were used instead of 1, the similar novel complexes (R2C)(η5-C5H3)(η5:η1-C5H3)[(Me2E)Fe(CO)2] (R2C=Me2C, E=Ge (7); R2C=(CH2)5C, E=Si(17), Ge (21)) with and Fe-E bond were obtained in addition to the diiron complexes (R2C)(Me2E)-[(η5-C5H3)Fe(CO)]2[Fe(CO)2](R2C=Me2C, E=Ge (8); R2C=(CH2)5C,E=Si (18), Ge (22)) and the desilylation or degermylation products. When a tert-butyl group was introduced into the cyclopentadienyl rings, or two phenyl groups were introduced at the bridging silicon atom instead of two methyl groups in 1, only the diiron complexes (Me2C)(Me2E)[η5-t-BuC5H2]Fe(CO)2]2 (E=Si(10), Ge (13)) and (Me2C)(Ph2Si)[(η5-C5H3)Fe(CO)2]2 (15) were obtained, in addition to the desilylatin or degermylation products. Whem a methylene bridge was used instead of an isopropylene bridge in 1 and 6, the partially hydrogenated complexes (Me2E)(η3-CHC5H6)(η5-C5H3)Fe(CO)3Fe(CO)2(E=Si(24),Ge (28)), the diiron complexes (CH2)(Me2E)[(η5-C5H3)Fe(CO)]2(μ-CO)2(E=Si (25), Ge (29)), and the desilylation or degermylation products were obtained. The molecular structures of 2, 3, 5, 7, 8, 10, 11t, 15, 17, 18, 21, 24, 25, 28, and 29 were determinde by X-ray diffraction.
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【期刊论文】Reactions of Doubly Bridged Biscylopentadienes with Molybdenum (Tungsten) Carbonyl
徐善生, Baiquan Wang, * Blin Zhu, Shansheng Xu, and Xiuzhong Zhou
Organometallics 2003, 22, 4842-4852,-0001,():
-1年11月30日
Dimolybdenum complexes (X) (Y) [(η5-C5H3)Mo(CO)3]2 [Y=Me2Si, X=Me2C, (CH2)5C, CH2; Y=Ph2Si, X=Me2C] and desilylation products (X)[(η5-C5H4)Mo(CO3)2 were obtained from the reactions of carbon and sliicon doubly bridged biscyclopentadiene ligands (X) (Y) (C5H4)2 with Mo(CO)6 in refluxing xylene. When these ligands reacted with W(CO)6, under similar conditions, in addition to ditungsten complexes (X) (Y) [(η5-C5H3)W(CO)3]2 [X=Me2C; Y=Me2Si, Ph2Si] and desilylation products (X) [(η5-C5H4)W(CO)3]2, a class of structurally novel comolexes (X) (η5-C5H3) [(Y)W(CO)3][W(CO)3][for X=Me2C, (CH2)5C; Y=Me2-Si] with a W-Si bond were also isolated. The reactions of carbon and germanium dobuly bridged biscyclopentadiene ligands (X)(Me2Ge)(C5H4)2[X=Me2C, (CH2)5C] with Mo(CO)6 or W(CO)6 gave similar novel complexes (X)(η5-C5H3)(η5, η1-C5H3)[(Me2Ge)M(CO)3][M(CO)3][X=Me2C, (CH2)5C; M=Mo, W] with a M-Ge bond. The reactions also produced degermylation products. However, the corresponding dimolybdenum or ditungstem complexes were not isolated in these cases. The molecular structures of 2, 6, 8, 10, 11, 13, 14, 15, 19, 21, 22, 25t, and 26t have benn determinde by X-ray diffraction. The M-M distances in complexes 2 [3.4328(12)A], 8 [3.453(2)A], and 11 [3.403(2) A] are conspicuously elongated and are in fact the longest ever reported among the biscyclopentadienyl dimolybdenum or ditungsten complexes. The factors affecting the structures of dimolybdenum or ditungsten complexes are discussed.
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徐善生, Shansheng Xu, Xuliang Dai, Baiquan Wang*, Xiuzhong, Zhou
Journal of Organometallic Chemistry 645(2002)262-267,-0001,():
-1年11月30日
The ansa-metallocene complexes Me2Ge(η5-C5Me4)2MCI2[M=Ti(1), Zr(2)], Me2Ge(η5-C5H3Bu-t)2ZrCl2(3) and Me2Ge(η5-C5H4)(η5-C5H3R)ZrCl2[R=Me(4), t-Bu (5)] were prepared by the reaction of the corresponding ligands with n-BuLi and MCl4 2THF, respectively. The molecular structures of 1 and 2 have benn determinde by the X-ray diffraction method. Complexe 2-5 in combination with MAO were studied as catalysts for ethylene polymerizatiion and all the germyl-bridged zirconocene catalysts show high activities at relative high temperatures. This indicates that the germyl-bridged zirconocene systems show thermally stable catalyst sysstems for polymerization of ethylene.
Titanocene, Zirconocene, Metallocne, Polymerization
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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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