Department of Materials Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.
Present address: School of Life Science and Technology, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa, 226-8501, Japan.
Angew Chem Int Ed Engl. 2017 Aug 1;56(32):9459-9462. doi: 10.1002/anie.201705277. Epub 2017 Jul 7.
An upper critical solution temperature (UCST)-type self-oscillating polymer was designed that exhibited rhythmic soluble-insoluble changes induced by the Belousov-Zhabotinsky (BZ) reaction. The target polymers were prepared by conjugating Ru(bpy) , a catalyst for the BZ reaction, to ureido-containing poly(allylamine-co-allylurea) (PAU) copolymers. The Ru(bpy) -conjugated PAUs exhibited a UCST-type phase-transition behavior, and the solubility of the polymer changed in response to the alternation in the valency of Ru(bpy) . The ureido content influences the temperature range of self-oscillation, and the oscillation occurred at higher temperatures than conventional LCST-type self-oscillating polymers. Furthermore, the self-oscillating behavior of the Ru-PAU could be regulated by addition of urea, which is a unique tuning strategy. We envision that novel self-oscillating polymers with widely tunable soluble-insoluble behaviors can be rationally designed based these UCST-type polymers.
设计了一种上临界溶解温度（UCST）型自振荡聚合物，该聚合物通过 Belousov-Zhabotinsky（BZ）反应诱导出有节奏的可溶性-不溶性变化。目标聚合物是通过将 Ru(bpy)（BZ 反应的催化剂）接枝到含有脲基的聚（烯丙胺-co-丙烯脲）（PAU）共聚物上制备的。Ru(bpy)-接枝的 PAU 表现出 UCST 型相转变行为，聚合物的溶解度会随着 Ru(bpy)价态的交替而变化。脲基含量影响自振荡的温度范围，并且振荡发生在比传统 LCST 型自振荡聚合物更高的温度下。此外，通过添加尿素可以调节 Ru-PAU 的自振荡行为，这是一种独特的调谐策略。我们设想可以基于这些 UCST 型聚合物合理设计具有广泛可调可溶性-不溶性行为的新型自振荡聚合物。
