李瑞祥
1. 多齿膦配体及其过渡金属配合物的设计合成;2. 有机膦配合物的选择加氢和不对称加氢反应研究;3. 有机膦配合物的氢甲酰化和不对称氢甲酰化反应研究;4. 负载纳米金属粒子的加氢反应研究。
个性化签名
- 姓名:李瑞祥
- 目前身份:
- 担任导师情况:
- 学位:
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学术头衔:
博士生导师
- 职称:-
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学科领域:
无机化学
- 研究兴趣:1. 多齿膦配体及其过渡金属配合物的设计合成;2. 有机膦配合物的选择加氢和不对称加氢反应研究;3. 有机膦配合物的氢甲酰化和不对称氢甲酰化反应研究;4. 负载纳米金属粒子的加氢反应研究。
李瑞祥,博士,教授、博士生导师。1984 年和 1987 年在兰州大学化学系获学士和硕士学位。1994 年 8 月至 1995 年 1 月香港城市大学访问学者。1999 年 6 月在香港城市大学获得博士学位。1987 年 6 月至今:四川大学化学系任教。
主要研究方向:1. 多齿膦配体及其过渡金属配合物的设计合成;2. 有机膦配合物的选择加氢和不对称加氢反应研究;3. 有机膦配合物的氢甲酰化和不对称氢甲酰化反应研究;4. 负载纳米金属粒子的加氢反应研究。
主要成果:合成新型双齿膦配体及其单金属、双金属配合物,详细考察配体结构与配合物结构和催化性能的关系,研究其催化反应机理 , 取得了一些创新性的研究成果。尤其是最近开展的四齿膦配体以及双金属配合物的设计合成研究,考察双金属的协同催化性能,研究双金属催化的协同作用机理,以制备出有机合成中所需的高活性、高选择性的双金属配合物催化剂,在该领域的研究将显示出非常好的新颖性和研究潜能,为原子经济和绿色化学反应提供一条新途径。在国内外重要学术期刊发表论文 40 余篇,申请发明专利 3 项, 2 项已授权,获省部级科技进步奖 2 项,参编专著 2 部,主持和参加科研项目 10 余项。
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成果数
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李瑞祥, Rui-Xiang Li a, Pu-Ming Cheng a, Dong-Wen Li a, Hua Chen a, Xian-Jun Li a, ), Carl Wessman b, Ning-Bew Wong b, Kam-Chung Tin b
Journal of Molecular Catalysis A: Chemical 159(2000)179-184,-0001,():
-1年11月30日
Acetophenones o-substituted by halogen and methoxyl groups were hydrogenated in the presence of (NH2Et2) Ru2Cl5[(S)-tol-BINAP2] at 358℃ and 85kg/cm2 hydrogen pressure. The results showed that o-bromoacetophenonewas a very active substrate and its asymmetric hydrogenation gave an o-bromo-a-phenylethanol with very highenantioselectivity (97%ee). o-Chloroacetophenone was moderately active and its hydrogenation product o-chloro-a-phenyl-ethanol had a good enantioselectivity (82%ee). o-Fluoroacetophenone exhibited a low reactivity but its hydrogenationproduct o-fluoro-a-phenylethanol showed the highest enantioselectivity (99%ee). among all products. o-Methoxyacetophenoneshowed a low reactivity, and its hydrogenation product o-methoxyl-a-phenylethanol gave a low enantioselectivity (27%ee). The effects of various reaction conditions, such as hydrogen pressure, reaction temperature, solvents, reactiontime, ligand concentration and addition of acid and base, were investigated.
Ruthenium, (, S), -tol-BINAP, o-substituted acetophenone
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李瑞祥, Rui-Xiang Li a, Ning-Bew Wong a, Xian-Jun Li b, Thomas C.W. Mak c, Qing-Chuan Yang c, Kam-Chung Tin a, *
Journal of Organometallic Chemistry 571(1998)223-229,-0001,():
-1年11月30日
A new ligand BDNA [1,8-bis(diphenylphosphinomethyl)naphthalene] and three ruthenium complexes containing the newligand, Ru2Cl4(BDNA)2 1, RuHCl(CO)(PPh3)(BDNA) 2, and RuH2(CO)(PPh3)(BDNA) 3, have been synthesized. Their compositionsand structures were characterized by 31P{1H}-NMR, 1H-NMR, and elemental analysis. Molecular structure of 3 was alsoconfirmed by single-crystal X-ray diffraction. The crystal belonged to the triclinic crystal system, P1( space group, a=10.7450(7),b=12.7100(7), c=18.1390(13) A°, a=89.558(6), b=83.117(2), g=80.859(5)°, V=2428.0(3) A°3, and Z=2. The hydrogenationresults of citral and cinnamaldehyde revealed that complex 2 had good catalytic activity and complex 3 had the high selectivityfor the hydrogenation of C=O bond in a,b-unsaturated aldehydes to form the corresponding allylic alcohols. In the presence ofcomplex 3, very high selectivities of 99.5 and 95.1% were obtained for the hydrogenation of the carbonyl group in citral andcinnamaldehyde, respectively.
Ruthenium complex, 1,, 8-Bis(, diphenylphosphinomethyl), naphthalene, Hydrogenation, Citral, Cinnamaldehyde
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李瑞祥, Yulin Huang a, b, *, Li-e Min c, Yaozhong Li b, Ruixiang Li b, Puming Cheng b, Xianjun Li b
Catalysis Communications 3(2002)71-75,-0001,():
-1年11月30日
Not only Na2SO4 has positive effect, but also negative effect on the reaction rate of biphasic hydroformylation ofhexene-1 catalyzed by the complicated catalytic system-RhCleCOTeTPPTST2-TPPTS–CTAB. With the suitableconcentration of Na2SO4 added to the reaction system, the TOF would reach a maximum value. The corresponding optimal [Na2SO4]/[Rh] value for TOF is different with different [Rh]/[TPPTS] ratios in this catalytic system. On thecontrary, no marked effect of Na2SO4 on the selectivity has been found in this system.
Positive effect, Negative effect, Sodium sulfate, Biphasic hydroformylation, TOF
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李瑞祥, Hua Chen, Yaozhong Li, Ruixiang Li, Puming Cheng, Xianjun Li∗
Journal of Molecular Catalysis A: Chemical 198(2003)1-7,-0001,():
-1年11月30日
The hydroformylation of 1-dodecene catalyzed by RhCl(CO)(TPPTS)2-BISBIS [TPPTS: P(m-C6H4SO3Na)3, BISBIS:sulfonated 1,1_-bis(diphenylphosphino methyl)-2,2_-biphenyl] in aqueous/organic two-phase systemwas studied. The additionof cationic surfactant cetyltrimethylamonium bromide (CTAB) greatly accelerated the reaction rate and the high regioselictivityfor linear aldehyde using diphosphine as ligand was attained under two-phase conditions. Both high activity (TOF: 740 h−1)and excellent regioselectivity (96.5% of 1-tridecanal) were obtained at 120℃, 2.0MPa and [BISBIS]/[Rh] ratio of 3 in thepresence of CTAB.
Aqueous two-phase system, 1-Dodecene hydroformylation, Diphosphine, Surfactant
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李瑞祥, Yulin Huanga, Yaozhong Li a, Jiayuan Hua, Puming Chenga, Hua Chena, Ruixiang Li a, Xianjun Li a, ∗, C.W. Yip b, Albert S.C. Chanb
Journal of Molecular Catalysis A: Chemical 189(2002)219-224,-0001,():
-1年11月30日
The enantioselective hydrogenation of ethyl pyruvate catalyzed by finely dispersed oxide supported rhodium nanoclusterwas studied with cinchonidine as chiral modifier. The results indicated that cinchonidine not only exhibited good enantiodifferentiatingability but also could accelerate the reaction by a factor 10. Supports (γ-Al2O3, SiO2, TiO2) played an importantrole in promoting the further increase of catalytic activity and enantioselectivity of polyvinylpyrrolidone-stabilized rhodiumnanoclusters (Rh/PVP). Under the optimum reaction conditions (298 K, 7.0MPa of hydrogen pressure and tetrahydrofuranas solvent), TOF and the enantiomeric excess reached 58.6 min−1 and 65.4% e.e., respectively.
Rhodium, Nanocluster, Cinchonidine, Ethyl pyruvate, Enantioselective hydrogenation
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李瑞祥, Maolin Yuan, Hua Chen, Ruixiang Li, Yaozhong Li, Xianjun Li∗
Applied Catalysis A: General 251(2003)181-185,-0001,():
-1年11月30日
This paper reports the hydroformylation of 1-butene catalyzed by RhCI(CO)(TPPTS)2 (TPPTS: P(m-C6H4SO3Na)3) andBISBIS (sodium salt of sulfonated 2,2-bis(diphenylphosphinomethyl)-1,1-biphenyl) in aqueous/organic two-phase catalyticsystem. The effects of reaction parameters on the catalytic activity and regioselectivity were investigated under the optimum reactionconditions: 130℃, 2.5MPa (syngas pressure), [BISBIS]/[Rh]=5, [1-butene]/[H2]/[CO]=1:1:1, [1-butene]/[Rh]=10 400, TOF and the regioselectivity for n-valeraldehyde were 2987 h−1 and 98%, respectively.
Hydroformylation, 1-Butene, Water-soluble rhodium complex, Two-phase catalysis
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李瑞祥, Yu-Qing Xia, Yuan-You Tang, Zhi-Ming Liang, Chang-Bin Yu, Xiang-Ge Zhou, Rui-Xiang Li ∗, Xian-Jun Li ∗
Journal of Molecular Catalysis A: Chemical 240(2005)132-138,-0001,():
-1年11月30日
Five novel ruthenium complexes, RuCl2(MOTPP)2[(S,S)-DPEN] [MOTPP=tris(4-methoxyphenyl)phosphine] (1), RuCl2(TFTPP)2[(S,S)-DPEN] [TFTPP=tris(4-trifluoromethylphenyl)phosphine] (2), RuCl2(PPh3)2[(S,S)-DPEN] (3), RuCl2(BDPX)[(S,S)-DPEN] [BDPX=1,2-bis(diphenylphosphinomethyl)benzene] (4), RuCl2(BISBI)[(S,S)-DPEN][BISBI=2, 2_-bis((diphenylphosphino)methyl)-1,1_-biphenyl]] (5)were synthesized and used for the hydrogenation of aromatic ketones. The complexes showed high catalytic activities, especially that thecatalytic activity of complex 5 containing the diphosphine with large bite angle and complex 1 containing triarylphosphine with electrondonatinggroup were higher than the other three complexes. The enantioselectivities of products were almost not influenced by the electronfactors of phosphine.
Ruthenium complex, Phosphine, Asymmetric hydrogenation, Diamine, Aromatic ketone
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