Department of Earth and Planetary Sciences and Origin of Life Initiative, Harvard University, 20 Oxford Street, Cambridge, MA, 02138, USA.
Santa Fe Institute, Santa Fe, NM, 87501, USA.
Angew Chem Int Ed Engl. 2017 Sep 25;56(40):12086-12091. doi: 10.1002/anie.201703816. Epub 2017 Jul 24.
We introduce a novel application of an oscillatory chemical reaction to the synthesis of block copolymers. The Belousov-Zhabotinsky (B-Z) reaction is coupled with the polymerization of an amphiphilic block copolymer. Radicals generated in the B-Z reaction initiate the polymerization between a polyethylene glycol (PEG) macroreversible addition-fragmentation chain-transfer agent and butyl acrylate monomers. The attachment of a hydrophobic block on PEG leads to self-assembly and formation of spherical micelles. The nanoscale micelles transform into submicrometer vesicles and grow to giant vesicles as a consequence of the oscillatory behavior of the B-Z reaction. The one-pot synthesis of an amphiphilic di-block copolymer and retention of oscillatory behavior for the B-Z reaction with the formation of giant vesicles bring a new insight into possible pathways for the synthesis of active functional microreactors in the range from hundreds of nanometers to tens of micrometers.
我们介绍了一种新的应用,即将振荡化学反应应用于嵌段共聚物的合成。Belousov-Zhabotinsky(B-Z)反应与两亲嵌段共聚物的聚合反应相结合。B-Z 反应中产生的自由基引发聚乙二醇(PEG)大分子可逆加成-断裂链转移剂与丙烯酸丁酯单体之间的聚合反应。PEG 上接枝疏水嵌段会导致自组装,形成球形胶束。由于 B-Z 反应的振荡行为,纳米级胶束转变为亚微米级囊泡,并进一步生长为巨型囊泡。两亲性二嵌段共聚物的一锅法合成以及 B-Z 反应保留振荡行为并形成巨型囊泡,为从数百纳米到数十微米范围内的活性功能微反应器的合成提供了新的思路。