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首页> 外文期刊>Polyhedron: The International Journal for Inorganic and Organometallic Chemistry >Ni(II) and Cu(II) complexes of phenoxy-ketimine ligands: Synthesis, structures and their utility in bulk ring-opening polymerization (ROP) of L-lactide

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Ni(II) and Cu(II) complexes of phenoxy-ketimine ligands: Synthesis, structures and their utility in bulk ring-opening polymerization (ROP) of L-lactide

机译：苯氧基-酮亚胺配体的Ni（II）和Cu（II）配合物：L-丙交酯的本体开环聚合（ROP）的合成，结构及其实用性

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Synthetic, structural and catalysis studies of Ni(II) and Cu(II) complexes of a series of phenoxy-ketimine ligands with controlled variations of sterics, namely 2-[1-(2,6-diethylphenylimino)ethyl]phenol (1a), 2-[1-(2,6-dimethylphenylimino)ethyl]phenol (1b) and 2-[1(2-methylp henylimino)ethyl]phenol (1c), are reported. Specifically, the ligands la, 1b and 1c were synthesized by the TiCl4 mediated condensation reactions of the respective anilines with o-hydroxyacetophenone in 21-23% yield. The nickel complexes, {2-[1-(2,6-diethylphenylimino)ethyl]phenoxy)(2)Ni(II) (2a) and {2-[1-(2,6-dimethylphenylimino)ethyl]phenoxy}(2)Ni(II) (2b), were synthesized by the reaction of the respective ligands 1a and 1b with Ni(OAC)(2) center dot 4H(2)O in the presence of NEt3 as a base in 71-75% yield. The copper complexes, 12-[1-(2,6-diethylphenylimino)ethyl]phenoxy}(2)Cu(II) (3a), 12-[1-(2,6-dimethylphenylimino)ethyl]phenoxy}(2)Cu(II) (3b) and 12-[1-(2-methylphenylimino)ethyl]phenoxy)2Cu(II) (3c) were synthesized analogously by the reactions of the ligands 1a, 1b and 1c with Cu(OAC)(2) center dot H2O in 70-87% yield. The molecular structures of the nickel and copper complexes 2a, 2b, 3a, 3b and 3c have been determined by X-ray diffraction studies. Structural comparisons revealed that the nickel centers in 2a and 2b are in square planar geometries while the geometry around the copper varied from being square planar in 3a and 3c to distorted square planar in 3b. The catalysis studies revealed that while the copper complexes 3a, 3b and 3c efficiently catalyze ring-opening polymerization (ROP) of L-lactide at elevated temperatures under solvent-free melt conditions, producing polylactide polymers of moderate molecular weights with narrow molecular weight distributions, the nickel counterparts 2a and 2b failed to yield the polylactide polymer. (C) 2007 Elsevier Ltd. All rights reserved.

机译：一系列苯氧基-酮亚胺配体的Ni（II）和Cu（II）配合物的合成，结构和催化研究，所述配合物具有受控的空间变化，即2- [1-（2,6-二乙基苯基亚氨基）乙基]苯酚（1a）报道了2- [1-（1-（2，6-二甲基苯基亚氨基）乙基]苯酚（1b）和2- [1-（2-甲基对苯二甲基亚氨基）乙基]苯酚（1c）。具体地，通过TiCl4介导的各个苯胺与邻羟基苯乙酮的缩合反应合成配体1a，1b和1c，产率为21-23％。镍络合物{2- [1-（2,6-二乙基苯基亚氨基）乙基]苯氧基）（2）Ni（II）（2a）和{2- [1-（2,6-二甲基苯基亚氨基）乙基]苯氧基}（ 2）Ni（II）（2b），是通过在NEt3作为碱的情况下，以71-75％的碱存在下，将各自的配体1a和1b与Ni（OAC）（2）中心点4H（2）O反应来合成的让。铜络合物12- [1-（1-（2,6-二乙基苯基亚氨基）乙基]苯氧基}（2）Cu（II）（3a），12- [1-（2,6-二甲基苯基亚氨基）乙基]苯氧基}（2）通过配体1a，1b和1c与Cu（OAC）（2）的反应类似地合成Cu（II）（3b）和12- [1-（2-（2-甲基苯基亚氨基）乙基]苯氧基）2Cu（II）（3c））中心点H2O的产率为70-87％。镍和铜络合物2a，2b，3a，3b和3c的分子结构已经通过X射线衍射研究确定。结构比较表明，镍2a和2b的中心呈正方形平面几何形状，而铜周围的几何形状则从3a和3c中的正方形平面变为3b中扭曲的正方形平面。催化研究表明，尽管铜络合物3a，3b和3c在无溶剂的熔融条件下，在升高的温度下能有效催化L-丙交酯的开环聚合（ROP），却能生产分子量中等，分子量分布窄的聚丙交酯聚合物，镍对应物2a和2b不能产生聚丙交酯聚合物。（C）2007 Elsevier Ltd.保留所有权利。

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来源
《Polyhedron: The International Journal for Inorganic and Organometallic Chemistry》 |2007年第15期|共12页
作者
John A; Katiyar V; Pang K; Shaikh MM; Nanavati H; Ghosh P;
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正文语种 eng
中图分类化学;
关键词
ring-opening polymerization; phenoxy-ketimine; copper complexes; nickel complexes; L-lactide; IMINE CHELATE LIGANDS; SCHIFF-BASE COMPLEXES; CHAIN-END CONTROL; TITANIUM COMPLEXES; LIVING POLYMERIZATION; COPPER(II) COMPLEXES; METAL-COMPLEXES; ENANTIOSELECTIVE EPOXIDATION; ETHYLENE POLYMERIZATION; EPSILON-CAPROLACTONE;

机译：开环聚合;苯氧基-酮亚胺;铜配合物;镍配合物;L-丙交酯;亚胺螯合配体;席夫夫基配合物;链端控制;钛配合物;活性聚合;铜（II）配合物;金属配合物;对映选择性环氧化;乙烯聚合;ε-己内酯;

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1. Ni(II) and Cu(II) complexes of phenoxy-ketimine ligands: Synthesis, structures and their utility in bulk ring-opening polymerization (ROP) of L-lactide [J] . John A, Katiyar V, Pang K, Polyhedron: The International Journal for Inorganic and Organometallic Chemistry . 2007,第15期

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2. Bulk solvent-free melt ring-opening polymerization of L-lactide catalyzed by Cu(II) and Cu(II)-Nd(III) complexes of the Salen-type Schiff-base ligand [J] . Lei-Lei Chen, Li-Qin Ding, Chu Zeng Applied Organometallic Chemistry . 2011,第4期

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