Cegłowski Michał, Jerca Valentin Victor, Jerca Florica Adriana, Hoogenboom Richard
Supramolecular Chemistry Group, Center of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281 S4, B-9000 Ghent, Belgium.
Faculty of Chemistry, Adam Mickiewicz University in Poznan, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland.
Pharmaceutics. 2020 Jun 2;12(6):506. doi: 10.3390/pharmaceutics12060506.
Trigger-responsive materials are capable of controlled drug release in the presence of a specific trigger. Reduction induced drug release is especially interesting as the reductive stress is higher inside cells than in the bloodstream, providing a conceptual controlled release mechanism after cellular uptake. In this work, we report the synthesis of 5-fluorouracil (5-FU) molecularly imprinted polymers (MIPs) based on poly(2-isopropenyl-2-oxazoline) (PiPOx) using 3,3'-dithiodipropionic acid (DTDPA) as a reduction-responsive functional cross-linker. The disulfide bond of DTDPA can be cleaved by the addition of tris(2-carboxyethyl)phosphine (TCEP), leading to a reduction-induced 5-FU release. Adsorption isotherms and kinetics for 5-FU indicate that the adsorption kinetics process for imprinted and non-imprinted adsorbents follows two different kinetic models, thus suggesting that different mechanisms are responsible for adsorption. The release kinetics revealed that the addition of TCEP significantly influenced the release of 5-FU from PiPOx-MIP, whereas for non-imprinted PiPOx, no statistically relevant differences were observed. This work provides a conceptual basis for reduction-induced 5-FU release from molecularly imprinted PiPOx, which in future work may be further developed into MIP nanoparticles for the controlled release of therapeutic agents.
触发响应材料能够在特定触发因素存在的情况下实现药物的可控释放。还原诱导的药物释放尤其引人关注,因为细胞内的还原应激高于血液中的还原应激,这为细胞摄取后的概念性控释机制提供了依据。在这项工作中,我们报道了基于聚(2-异丙烯基-2-恶唑啉)(PiPOx),使用3,3'-二硫代二丙酸(DTDPA)作为还原响应功能交联剂合成5-氟尿嘧啶(5-FU)分子印迹聚合物(MIPs)。DTDPA的二硫键可通过添加三(2-羧乙基)膦(TCEP)断裂,从而导致还原诱导的5-FU释放。5-FU的吸附等温线和动力学表明,印迹和非印迹吸附剂的吸附动力学过程遵循两种不同的动力学模型,这表明吸附是由不同机制引起的。释放动力学表明,添加TCEP显著影响了5-FU从PiPOx-MIP中的释放,而对于非印迹的PiPOx,未观察到统计学上的显著差异。这项工作为从分子印迹的PiPOx中还原诱导释放5-FU提供了概念基础,在未来的工作中,这可能会进一步发展为用于治疗剂控释的MIP纳米颗粒。