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Titanium and zirconium amido complexes supported by imidazole-containingligands: syntheses, characterization and catalytic activities
Zhao, Yang; Lin, Miaoshui; Chen, Zhou; Pei, Hao; Li, Yahong; Chen, Yanmei; Wang, Xiufang; Li, Lei; Cao, Yanyuan; Zhang, Yong; Li, Wu
2012
发表期刊RSC ADVANCES
ISSN2046-2069
卷号2期号:1页码:144-150
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
文献类型期刊论文
条目标识符http://ir.isl.ac.cn/handle/363002/2083
专题青海盐湖研究所知识仓储
推荐引用方式
GB/T 7714
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.
APA Zhao, Yang.,Lin, Miaoshui.,Chen, Zhou.,Pei, Hao.,Li, Yahong.,...&Li, Wu.(2012).Titanium and zirconium amido complexes supported by imidazole-containingligands: syntheses, characterization and catalytic activities.RSC ADVANCES,2(1),144-150.
MLA Zhao, Yang,et al."Titanium and zirconium amido complexes supported by imidazole-containingligands: syntheses, characterization and catalytic activities".RSC ADVANCES 2.1(2012):144-150.
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