Harrison Andrew, Tang Christina
Department of Chemical and Life Sciences Engineering, Virginia Commonwealth University, Richmond, VA 23284-3028, USA.
Polymers (Basel). 2021 Jun 18;13(12):1992. doi: 10.3390/polym13121992.
Performing multiple reaction steps in "one pot" to avoid the need to isolate intermediates is a promising approach for reducing solvent waste associated with liquid phase chemical processing. In this work, we incorporated gold nanoparticle catalysts into polymer nanoreactors via amphiphilic block copolymer directed self-assembly. With the polymer nanoreactors dispersed in water as the bulk solvent, we demonstrated the ability to facilitate two reaction steps in one pot with spontaneous precipitation of the product from the reaction mixture. Specifically, we achieved imide synthesis from 4-nitrophenol and benzaldehyde as a model reaction. The reaction occured in water at ambient conditions; the desired 4-benzylideneaminophenol product spontaneously precipitated from the reaction mixture while the nanoreactors remained stable in dispersion. A 65% isolated yield was achieved. In contrast, PEGylated gold nanoparticles and citrate stabilized gold nanoparticles precipitated with the reaction product, which would complicate both the isolation of the product as well as reuse of the catalyst. Thus, amphiphilic nanoreactors dispersed in water are a promising approach for reducing solvent waste associated with liquid phase chemical processing by using water as the bulk solvent, eliminating the need to isolate intermediates, achieving spontaneous product separation to facilitate the recycling of the reaction mixture, and simplifying the isolation of the desired product.
在“一锅法”中进行多个反应步骤以避免分离中间体的需要,是一种减少与液相化学加工相关的溶剂浪费的有前途的方法。在这项工作中,我们通过两亲性嵌段共聚物定向自组装将金纳米颗粒催化剂纳入聚合物纳米反应器中。以分散在水中作为本体溶剂的聚合物纳米反应器为例,我们展示了在一锅法中促进两个反应步骤的能力,产物从反应混合物中自发沉淀出来。具体来说,我们以4-硝基苯酚和苯甲醛的反应作为模型反应实现了酰亚胺的合成。该反应在环境条件下于水中进行;所需的4-苄叉氨基苯酚产物从反应混合物中自发沉淀出来,而纳米反应器在分散体中保持稳定。分离产率达到65%。相比之下,聚乙二醇化金纳米颗粒和柠檬酸盐稳定的金纳米颗粒会与反应产物一起沉淀,这会使产物的分离以及催化剂的再利用都变得复杂。因此,分散在水中的两亲性纳米反应器是一种有前途的方法,可通过使用水作为本体溶剂来减少与液相化学加工相关的溶剂浪费,无需分离中间体,实现产物的自发分离以促进反应混合物的循环利用,并简化所需产物的分离。