Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, China.
Dalton Trans. 2011 Feb 21;40(7):1610-8. doi: 10.1039/c0dt01225d. Epub 2011 Jan 4.
A series of heteroligated (salicylaldiminato)(β-enaminoketonato)titanium complexes of the general formula [3-Bu(t)-2-OC(6)H(3)CH==N(C(6)F(5))][PhN==C(CF(3))CHC(R)O]TiCl(2) (3a: R==Ph, 3b: R==C(6)H(4)Ph(p), 3c: R==C(6)H(4)Ph(o), 3d: R = 1-naphthyl, 3e: R = C(6)H(4)F2(2,6), 3f: R = C(6)H(4)Cl2(2,5), 3g: R==C(6)F4(2,3,5,6)OMe(4)) were synthesized. The structure of complexes 3d, 3f-g were determined by single crystal X-ray diffraction analysis. The X-ray crystallographic analysis indicated these complexes adopted a distorted octahedral geometry around the titanium center. Upon activation with modified methylaluminoxane, complexes 3a-g exhibited moderate to good catalytic activity for norbornene (NB) vinyl addition polymerization, producing moderate molecular weight polynorbornenes under mild conditions. The introduction of electron-withdrawing groups can greatly enhance the catalytic activity. Significantly, the heteroligated titanium complexes displayed greatly improved activity for vinyl addition polymerization of NB compared to homoligated counterparts, which may stem from the suitable combinations of electronic and steric effects.
一系列异双齿(水杨醛亚胺基)(β-烯胺酮基)钛配合物的通用公式 [3-Bu(t)-2-OC(6)H(3)CH==N(C(6)F(5))][PhN==C(CF(3))CHC(R)O]TiCl(2] (3a: R==Ph, 3b: R==C(6)H(4)Ph(p), 3c: R==C(6)H(4)Ph(o), 3d: R = 1-萘基, 3e: R = C(6)H(4)F2(2,6), 3f: R = C(6)H(4)Cl2(2,5), 3g: R==C(6)F4(2,3,5,6)OMe(4))被合成。配合物 3d、3f-g 的结构通过单晶 X 射线衍射分析确定。X 射线晶体学分析表明,这些配合物在钛中心周围采用了扭曲的八面体几何形状。用改性甲基铝氧烷活化后,配合物 3a-g 对降冰片烯(NB)的乙烯基加成聚合表现出中等至良好的催化活性,在温和条件下生成中等分子量的聚降冰片烯。引入吸电子基团可以大大提高催化活性。值得注意的是,与同双齿配体相比,异双齿钛配合物在 NB 的乙烯基加成聚合中表现出大大提高的活性,这可能源于电子和空间效应的适当组合。