Okubo Kohei, Yoshino Haruka, Miyasaka Hitoshi, Kasai Hitoshi, Oka Kouki
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan.
Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan.
ACS Appl Mater Interfaces. 2025 Mar 5;17(9):14561-14568. doi: 10.1021/acsami.4c22197. Epub 2025 Feb 21.
Amorphous porous organic polymers (POPs), with high porosity and high chemical and thermal stability, have been investigated for various applications. Most amorphous POPs are synthesized by electropolymerization or chemical polymerization. However, nonhomogeneous film formation in electropolymerization and residual metal-derived impurities in chemical polymerization are challenges. This study developed a novel chemical polymerization method for amorphous POPs using iodine as an oxidant. Specifically, we synthesized a representative amorphous POP, polytriphenylamine (pTPA). The pTPA was obtained as a powder through solution polymerization and as a thin film via vapor-assisted polymerization. Postreaction, ethanol was used to remove iodine completely. Notably, even though pTPA was constructed from rigid structures, the nitrogen-induced gate-opening phenomenon was exhibited for the first time as amorphous POPs. These results demonstrate that impurity-free amorphous POPs exhibit inherent flexibility against their rigid chemical structure. The novel iodine-based chemical polymerization enables us to synthesize neat amorphous POPs and to explore their pure functions.
非晶态多孔有机聚合物（POPs）具有高孔隙率以及高化学和热稳定性，已被研究用于各种应用。大多数非晶态POPs是通过电聚合或化学聚合合成的。然而，电聚合中不均匀的成膜以及化学聚合中残留的金属衍生杂质是挑战。本研究开发了一种以碘为氧化剂的用于非晶态POPs的新型化学聚合方法。具体而言，我们合成了一种代表性的非晶态POP，聚三苯胺（pTPA）。通过溶液聚合得到粉末状的pTPA，通过气相辅助聚合得到薄膜状的pTPA。反应后，使用乙醇完全去除碘。值得注意的是，尽管pTPA由刚性结构构成，但作为非晶态POPs首次表现出氮诱导的门控开启现象。这些结果表明，无杂质的非晶态POPs在其刚性化学结构方面表现出固有的柔韧性。这种新型的基于碘的化学聚合使我们能够合成纯净的非晶态POPs并探索其纯功能。
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