Aqueous Polymerization-Induced Self-Assembly for the Synthesis of Ketone-Functionalized Nano-Objects with Low Polydispersity.
Aqueous Polymerization-Induced Self-Assembly for the Synthesis of Ketone-Functionalized Nano-Objects with Low Polydispersity.
复制标题
DOI：
10.1021/acsmacrolett.5b00225
复制
发表时间：
2015-04
影响因子：
5.8
通讯作者：
Wei Zhou;Qingwu Qu;Yuanyuan Xu;Zesheng An
中科院分区：
文献类型：
--
作者：
Wei Zhou;Qingwu Qu;Yuanyuan Xu;Zesheng An
从材料应用和工业放大的角度来看，在具有可控形态的水中一步高效、高浓度地合成功能化、均匀的聚合物纳米对象是非常有吸引力的。在这里，我们报道了一种基于聚合诱导自组装(PISA)的可逆加成-断裂链转移(RAFT)分散聚合的新配方，以合成酮功能化的纳米球和囊泡。值得注意的是，成核块完全由商品单体双丙酮丙烯酰胺(DAAM)中的含酮聚合物组成，导致纳米对象中具有高密度的酮官能团。在PISA和传统的自组装过程中，产生均匀的囊泡是另一个挑战。为了在如此高效的水PISA过程中生成均匀的纳米对象，特别是囊泡，我们设计了策略，允许原位生成的聚合物有足够的时间松弛并重组为多分散度非常低的囊泡。特别是，降低自由基引发剂浓度和降低聚合温度都能有效地改善囊泡的均匀性。这种高效的、水性的PISA能够制备形貌可控的功能化和均匀的纳米对象，固含量高达20%，是该领域的重要进展。
Efficient synthesis of functionalized, uniform polymer nano-objects in water with controlled morphologies in one step and at high concentrations is extremely attractive, from perspectives of both materials applications and industrial scale-up. Herein, we report a novel formulation for aqueous reversible addition-fragmentation chain transfer (RAFT) dispersion polymerization based on polymerization-induced self-assembly (PISA) to synthesize ketone-functionalized nanospheres and vesicles. Significantly, the core-forming block was composed entirely of a ketone-containing polymer from a commodity monomer diacetone acrylamide (DAAM), resulting in a high density of ketone functionality in the nano-objects. Producing uniform vesicles represents another challenge both in PISA and in the traditional self-assembly process. Aiming at producing uniform nano-objects, especially vesicles, in such a highly efficient aqueous PISA process, we devised strategies to allow sufficient time for the in situ generated polymers to relax and reorganize into vesicles with a remarkably low polydispersity. Specifically, both reducing the radical initiator concentration and lowering the polymerization temperature were shown to be effective for improving the uniformity of vesicles. Such an efficient, aqueous PISA to produce functionalized and uniform nano-objects with controlled morphologies at solid contents up to 20% represents important progress in the field.