摘 要
本論文以硫醇、醯胺當作雙成分起始劑活性聚合乙烯係單體，探討其起始反應機制、共聚合反應行為與熱裂解動力等等。在聚合反應過程當中，硫醇、醯胺雙成分起始劑缺一不可，硫醇會經由鏈轉移反應將氫原子轉移到醯胺上形成一過渡狀態錯化合物，在經由適當的重排反應形成thiolamide結構，單體經由這不穩定結構進行活性聚合反應。聚合過程當中，分子量的大小可由單體與硫醇的比例來控制，醯胺在此系統當中扮演著capping agent的功能。由於amide的結構存在於高分子尾端基團上，因此進行聚合反應時會有一定程度的立體效應，不同極性的溶劑會影響capping agent和高分子末端自由基的距離，影響反應速率、分子量分佈係數等等。由於立體效應的存在，所得到的高分子具有較高的玻璃轉移點溫度，高分子末端不存在終止反應造成的不飽和雙鍵，因此具有相當高的熱安定性，搭配不同種類的硫醇、醯胺所得到的末端基團也會影響高分子材料的熱安定性。在共聚合反應時，由於尾端基團的存在會影響共聚單體的反應活性，而產生不同r1、r2的值，加入少量拉電子基團的共單體會加快共聚合反應速率。利用這種活性聚合方法成功地合成團鏈共聚合物高分子。

Abstract
Living radical polymerization of vinyl monomer by thiol and lactam as initiator was investigated in this thesis, including the mechanism, reactivity of copolymerization, and thermal degradation behavior. Proton is transferred from thiol to lactam group and forms the inter-medium structure, thiolamide, as the active specie during the initiation step. Propagation reaction, thereby, occurs via monomer insertion from the terminal group of the polymer chain end. Molecular weight can be controlled by the monomer-to-thiol ratio. Lactam in this system acts as a capping agent, which in terms to control the tactility and the dynamic equilibrium of activation/deactivation process. In addition, polymers prepared by this route have high glassy transition temperatures due to the high proportion of syndiotactic conformation produced. Solvent effects were also examined to reveal the evidence of capping agent on the polymerization rate, tactility, and molecular weight distribution. Since the absence of termination reaction in the system, polymers without vinyl-bond are generated, which causes the high thermal stability. For copolymerization, the polymerization rate enhanced by adding a few mole ratio of comonomer bearing with electron withdraw group, meanwhile the reactivity will also vary accordingly. Finally, well-defined block copolymers were successfully synthesized by this novel approach.

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