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A New Thermo-, pH-, and CO2-Responsive Homopolymer of Poly[N-[2-(diethylamino)ethyl]acrylamide]: Is the Diethylamino Group Underestimated?
Macromolecules ( IF 5.1 ) Pub Date : 2015-12-31 00:00:00 , DOI: 10.1021/acs.macromol.5b02458
Zefeng Song 1 , Ke Wang 1 , Chengqiang Gao 1 , Shuang Wang 1 , Wangqing Zhang 1
Affiliation  

A new multi-stimuli-responsive homopolymer of poly[N-[2-(diethylamino)ethyl]acrylamide] (PDEAEAM), which combines the thermoresponsive and pH/CO2-responsive moieties of the diethylamino and acrylamide groups, was proposed and synthesized by RAFT polymerization. Well-defined PDEAEAM was synthesized by solution RAFT polymerization as indicated by the linear increase in the polymer molecular weight with the monomer conversion and the narrow molecular weight distribution. The appending diethylamino group in the polymer backbone was found to be crucial to determine the thermoresponse of PDEAEAM in water. The parameters including the polymerization degree, the polymer concentration, the deuterated solvent, the terminal attached on the polymer backbone, the additives of salt and urea, and pH and bubbling CO2 affecting the thermoresponse of PDEAEAM in aqueous solution at the lower critical solution temperature (LCST) were investigated. The temperature-variable 1H NMR analysis suggests that the dehydration of PDEAEAM at temperature above LCST is ascribed to the weakened hydrogen bonding between the CONHCH2 and/or (CH2N(CH2CH3)2) moieties with the solvent of water. The proposed multi-stimuli-responsive homopolymer of PDEAEAM has two advantages of (1) the convenient and controllable RAFT synthesis and (2) the pH/CO2 tunable LCST at ∼36 °C being very close to body temperature.

中文翻译:

聚[ N- [2-(二乙基氨基)乙基]丙烯酰胺]的新型热,pH和CO 2响应均聚物:二乙基氨基基数被低估了吗?

聚[ N- [2-(二乙氨基)乙基]丙烯酰胺](PDEAEAM)的新型多刺激响应均聚物,结合了热响应和pH / CO 2提出并通过RAFT聚合法合成了二乙氨基和丙烯酰胺基的高反应性部分。通过溶液RAFT聚合合成了定义明确的PDEAEAM,其表现为聚合物分子量随单体转化率和窄分子量分布而线性增加。发现在聚合物主链中附加二乙氨基对确定水中PDEAEAM的热响应至关重要。参数包括聚合度,聚合物浓度,氘代溶剂,连接在聚合物主链上的末端,盐和尿素的添加剂以及pH值和冒泡的CO 2研究了在较低的临界溶液温度(LCST)下对水溶液中PDEAEAM热响应的影响。温度可变的1 H NMR分析表明,在高于LCST的温度下PDEAEAM的脱水归因于CONHCH 2和/或(CH 2 N(CH 2 CH 32)部分与水的溶剂之间的氢键减弱。拟议的PDEAEAM的多刺激响应均聚物具有两个优点:(1)方便且可控制的RAFT合成;(2)pH / CO 2可调LCST在约36°C时非常接近体温。
更新日期:2015-12-31
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