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哈尔滨工程大学材料科学与化学工程学院 高分子材料研究中心,哈尔滨,150001
纸质出版日期:2013-3-20,
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徐晓冬, 朱元棋, 李晗, 冯四伟, 代海存, 沈贤德, 白建伟, 张丽丽, 岡本佳男. 光学活性(甲基)丙烯酰胺的立体定向自由基聚合 立体控制机理探讨[J]. 高分子学报, 2013,(3):286-292.
Xiao-dong Xu, Yuan-qi Zhu, Han Li, Si-wei Feng, Hai-cun Dai, Xian-de Shen, Jian-wei Bai, Li-li Zhang, Yoshio Okamoto. STEREOSPECIFIC RADICAL POLYMERIZATION OF OPTICALLY ACTIVE (METH)ACRYLAMIDE STUDY ON THE MECHANISM OF STEREOCONTROL[J]. Acta Polymerica Sinica, 2013,(3):286-292.
徐晓冬, 朱元棋, 李晗, 冯四伟, 代海存, 沈贤德, 白建伟, 张丽丽, 岡本佳男. 光学活性(甲基)丙烯酰胺的立体定向自由基聚合 立体控制机理探讨[J]. 高分子学报, 2013,(3):286-292. DOI: 10.3724/SP.J.1105.2013.12380.
Xiao-dong Xu, Yuan-qi Zhu, Han Li, Si-wei Feng, Hai-cun Dai, Xian-de Shen, Jian-wei Bai, Li-li Zhang, Yoshio Okamoto. STEREOSPECIFIC RADICAL POLYMERIZATION OF OPTICALLY ACTIVE (METH)ACRYLAMIDE STUDY ON THE MECHANISM OF STEREOCONTROL[J]. Acta Polymerica Sinica, 2013,(3):286-292. DOI: 10.3724/SP.J.1105.2013.12380.
利用Lewis酸三氟甲磺酸镱(Yb(OTf)3)调控(S)-N-(2-羟基-1-苯乙基)甲基丙烯酰胺((S)-HPEMA)和(S)-N-(2-羟基-1-苯乙基)丙烯酰胺((S)-HPEA)的自由基聚合
得到相应的光学活性聚合物;研究了反应条件对聚合物立体结构的影响
发现以甲醇和正丁醇为溶剂时
Yb(OTf)3的存在可显著提高聚合物的mm三元组的含量
而以DMSO为溶剂时
Yb(OTf)3对聚合物的立构规整性没有明显改变;通过1H-NMR研究了Yb(OTf)3与单体之间的相互作用
结果表明单体的酰胺基团与Lewis酸的稀土金属离子间的配位以及单体的羟基与Lewis酸的三氟甲磺酸根间的氢键影响了单体的加成方向和聚合物的立体结构.
Optically active poly(meth)acrylamides were synthesized by the stereospecific radical polymerization of (S)-N-(2-hydroxy-1-phenylethyl)methacrylamide ((S)-HPEMA) and (S)-N-(2-hydroxy-1-phenylethyl)acrylamide ((S)-HPEA) in the absence and presence of Lewis acid ytterbium trifluoromethanesulfonate (Yb(OTf)3).The effect of the Lewis acid on the radical polymerization of (S)-HPEMA and (S)-HPEA was investigated.In the presence of a catalytic amount of the Lewis acid
the isotactic specificity of the polymers remarkably increased when the radical polymerization proceeded in methanol and n-butanol. However
the isotactic selectivity disappeared when the radical polymerization proceeded in DMSO.The interaction between the Lewis acid and monomers (S)-HPEMA and (S)-HPEA was investigated by 1H-NMR.It was found that the monomers strongly interacted with the Lewis acid in methanol-d4
which included the coordination of the amide group to the rare earth metal ion and the hydrogen bond between the hydroxyl group of the monomers and the trifluoromethanesulfonate ion of the Lewis acid.The plausible mechanism of stereocontrol in the radical polymerization of (S)-HPEMA and (S)-HPEA was analyzed.The monomers are activated by the interaction with the Lewis acid
and the activated monomer is preferentially polymerized.Therefore
the Lewis acid is incorporated into the propagating chain end.The Lewis acid could interact with two or more structural units
because of its high coordination numbers and more than one triflate ions
and control the stereochemistry of the polymerization to an isotactic-selective manner.The Lewis acid might weakly interact with the polymer chain to be readily transferred to another monomer and activate it.
立体定向聚合光学活性聚合物甲基丙烯酰胺立构规整性立体控制机理
Stereospecific polymerizationOptically active polymerMethacrylamideTacticityStereoregularity
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