Naranjo David, Paulo-Mirasol Sofia, Lanzalaco Sonia, Quan Haoyuan, Armelin Elaine, García-Torres José, Torras Juan
IMEM-BRT Group, Departament d'Enginyeria Química, EEBE, Universitat Politècnica de Catalunya, C/Eduard Maristany, 10-14, Ed. I, Second Floor, 08019 Barcelona, Spain.
Barcelona Research Center in Multiscale Science and Engineering, EEBE, Universitat Politècnica de Catalunya, C/Eduard Maristany, 10-14, Basement S-1, 08019 Barcelona, Spain.
Chem Mater. 2024 Apr 17;36(9):4688-4702. doi: 10.1021/acs.chemmater.4c00433. eCollection 2024 May 14.
Conducting polymers (CPs) play a vital role in imparting electrochemical and photothermal properties to thermosensitive conducting hydrogels (TCH). The application of TCH is expanding not only for biomedical applications but also to address water scarcity. While the volume phase transition (VPT) phenomenon in thermosensitive polymers has been extensively studied, the contribution of CPs to this process and the underlying chemical interactions remain unclear and low explored. In this study, we present a novel conducting polymer hydrogel (CPH) utilizing the thermosensitive polymer poly-(-isopropylacrylamide) (PNIPAAm) enriched with poly-(3,4-ethylenedioxythiophene) (PEDOT) nanoparticles as a model system. This serves as a platform for both experimental and theoretical investigations into the influence of CPs on VPT. Through a comprehensive examination of hydrogel responses to temperature employing Raman spectroscopy, atomistic simulations using advanced hybrid methodologies, and artificial intelligence, we unveil a shielding effect of CP. This effect arises from robust chemical interactions with NIPAAm, inducing a selective dehydration of the hydrogel microenvironment. Remarkably, this mirrors the phenomenon observed during VPT triggered by an increase in the hydrogel temperature. Understanding the intricate interactions between conducting and thermosensitive polymers is imperative for the systematic development and fine-tuning of the performance of future CPHs. This knowledge ensures a more precise adaptation of these materials to their intended end applications.
导电聚合物(CPs)在赋予热敏导电水凝胶(TCH)电化学和光热性能方面发挥着至关重要的作用。TCH的应用不仅在生物医学领域不断拓展,还用于解决水资源短缺问题。虽然热敏聚合物中的体积相变(VPT)现象已得到广泛研究,但CPs对这一过程的贡献以及潜在的化学相互作用仍不清楚且研究较少。在本研究中,我们提出了一种新型导电聚合物水凝胶(CPH),它利用富含聚(3,4-乙撑二氧噻吩)(PEDOT)纳米颗粒的热敏聚合物聚(N-异丙基丙烯酰胺)(PNIPAAm)作为模型系统。这为实验和理论研究CPs对VPT的影响提供了一个平台。通过使用拉曼光谱对水凝胶对温度的响应进行全面研究、采用先进混合方法进行原子模拟以及利用人工智能,我们揭示了CP的屏蔽效应。这种效应源于与NIPAAm的强化学相互作用,导致水凝胶微环境的选择性脱水。值得注意的是,这反映了水凝胶温度升高引发VPT过程中观察到的现象。了解导电聚合物和热敏聚合物之间的复杂相互作用对于未来CPH性能的系统开发和微调至关重要。这些知识可确保这些材料更精确地适应其预期的最终应用。