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题名: Titanium and zirconium amido complexes supported by imidazole-containingligands: syntheses, characterization and catalytic activities
作者: Zhao, Yang ;  Lin, Miaoshui ;  Chen, Zhou ;  Pei, Hao ;  Li, Yahong ;  Chen, Yanmei ;  王秀芳 ;  Li, Lei ;  Cao, Yanyuan ;  Zhang, Yong ;  李武
刊名: RSC ADVANCES
出版日期: 2012
卷号: 2, 期号:1, 页码:144-150
英文摘要: A series of new titanium and zirconium amido complexes, incorporating 4,5-diphenyl-2-(2-pyridinyl)-1H-imidazole (HL1), 4,5-bis(4-chlorophenyl)-2-(2-pyridinyl)-1H-imidazole (HL2), 4,5-bis(4-methoxyphenyl)-2-(2-pyridinyl)-1H-imidazole (HL3) and 4,5-bis(2-methoxyphenyl)-2-(2-pyridinyl)-1H-imidazole) (HL4) as the ancillary ligands, have been prepared and are shown to be pre-catalysts for the hydroamination of alkynes. Treatment of Ti(NMe2)(4) with 1 equivalent of HL1, HL2, HL3 and HL4, respectively, results in transamination with one dimethylamide group providing Ti(L1)(NMe2)(3) (1), Ti(L-2)(NMe2)(3) (2), Ti(L3)(NMe2)(3) (3), and Ti(L4)(NMe2)(3)center dot THF (4 center dot THF). Reaction of Ti(NMe2)(4) with 2 equivalents of HL1, HL2, HL3 and HL4, respectively, leads to production of titanium bisamido complexes Ti(L1)(2)(NMe2)(2 center dot)THF(5 center dot THF), Ti(L2)(2)(NMe2)(2)center dot THF (6 center dot THF), Ti(L3)(2)(NMe2)(2)center dot THF (7 center dot THF), and Ti(L-4)(2)(NMe2)(2) (8). Similarly, complexes Zr(L1)(NMe2)(3) (9), Zr(L1)(2)(NMe2)(2)center dot 1.5THF (10 center dot 1.5THF), Zr(L2)(2)(NMe2)(2)center dot 0.5THF (11 center dot 0.5THF), and Zr(L3)(2)(NMe2)(2)center dot 0.5THF (12 center dot 0.5THF) are generated by addition of 1 or 2 equivalents of the corresponding ligands to Zr(NMe2)(4). All compounds have been characterized by elemental and spectroscopic analyses. The solid-state structures of compounds 2 and 6 center dot THF have been further established by single X-ray diffraction analyses. The catalytic activities of 2 and 6 center dot THF towards the hydroamination of alkynes were explored. Complexes 2 and 6 center dot THF were found to be active pre-catalysts for the hydroamination reactions. Complex 2 showed higher catalytic activity and gave highly Markovnikov selective hydroamination of terminal alkynes. A series of new titanium and zirconium amido complexes, incorporating 4,5-diphenyl-2-(2-pyridinyl)-1H-imidazole (HL1), 4,5-bis(4-chlorophenyl)-2-(2-pyridinyl)-1H-imidazole (HL2), 4,5-bis(4-methoxyphenyl)-2-(2-pyridinyl)-1H-imidazole (HL3) and 4,5-bis(2-methoxyphenyl)-2-(2-pyridinyl)-1H-imidazole) (HL4) as the ancillary ligands, have been prepared and are shown to be pre-catalysts for the hydroamination of alkynes. Treatment of Ti(NMe2)(4) with 1 equivalent of HL1, HL2, HL3 and HL4, respectively, results in transamination with one dimethylamide group providing Ti(L1)(NMe2)(3) (1), Ti(L-2)(NMe2)(3) (2), Ti(L3)(NMe2)(3) (3), and Ti(L4)(NMe2)(3)center dot THF (4 center dot THF). Reaction of Ti(NMe2)(4) with 2 equivalents of HL1, HL2, HL3 and HL4, respectively, leads to production of titanium bisamido complexes Ti(L1)(2)(NMe2)(2 center dot)THF(5 center dot THF), Ti(L2)(2)(NMe2)(2)center dot THF (6 center dot THF), Ti(L3)(2)(NMe2)(2)center dot THF (7 center dot THF), and Ti(L-4)(2)(NMe2)(2) (8). Similarly, complexes Zr(L1)(NMe2)(3) (9), Zr(L1)(2)(NMe2)(2)center dot 1.5THF (10 center dot 1.5THF), Zr(L2)(2)(NMe2)(2)center dot 0.5THF (11 center dot 0.5THF), and Zr(L3)(2)(NMe2)(2)center dot 0.5THF (12 center dot 0.5THF) are generated by addition of 1 or 2 equivalents of the corresponding ligands to Zr(NMe2)(4). All compounds have been characterized by elemental and spectroscopic analyses. The solid-state structures of compounds 2 and 6 center dot THF have been further established by single X-ray diffraction analyses. The catalytic activities of 2 and 6 center dot THF towards the hydroamination of alkynes were explored. Complexes 2 and 6 center dot THF were found to be active pre-catalysts for the hydroamination reactions. Complex 2 showed higher catalytic activity and gave highly Markovnikov selective hydroamination of terminal alkynes.
收录类别: SCI
语种: 英语
Citation statistics: 
内容类型: 期刊论文
URI标识: http://ir.isl.ac.cn/handle/363002/2083
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Recommended Citation:
Zhao, Yang,Lin, Miaoshui,Chen, Zhou,et al. Titanium and zirconium amido complexes supported by imidazole-containingligands: syntheses, characterization and catalytic activities[J]. RSC ADVANCES,2012,2(1):144-150.
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