A near-universal design concept for waterborne high-performance polyimides Daniel Alonso Cerron Infantes 1,2 and Miriam Unterlass1, 2 1 Universität Konstanz, Department of Chemistry, Solid State Chemistry, Konstanz, Germany. 2 CeMM – Research Center for Molecular Medicine of the Austrian Academy of Sciences, Vienna, Austria. Polyimides (PIs) are a class of high-performance polymers that are intensively used in advanced technologies due to their outstanding materials performance. They combine excellent high temperature stability with light weight, high chemical resistance, and high mechanical strength. PIs are used for a variety of high-end engineering applications in various shapes: As flexible films in microelectronics, [1] as foams for thermal insulation, vibration and noise reduction in aeronautics and transportation, [2] or as gas separation and filtration membranes. [3] Recently, they have become highly sought after for battery applications, for the redox-activity of the imide function. [4-5] PI synthesis and production still relies exclusively on reactions performed under high temperatures (e.g., 300 °C), dangerous and polluting solvents (e.g., N-methyl-pyrrolidone, NMP) and carcinogenic catalysts (e.g., isoquinoline). These reactants and reaction conditions are all harmful to the environment and human health, and are discordant with the sustainable development goals. Moreover, hazardous chemicals, such as NMP, are about to be restricted for commercial use according to the REACH regulation. Therefore, alternative pathways towards PI formation are imperative and several strategies have been reported; however, attempts to shape PIs into given forms remains a challenge, since PIs extreme chemical and thermal stability also hampers its processability. Our work focuses on devising general strategies to produce a wide range of PIs using exclusively water as the main reaction and processing solvent. We here present a near-universal molecular design concept for generating processability from aqueous solution. We show that using this concept, PIs can be shaped into various shapes relevant to application, e.g.,microparticles, free-standing films, coatings, and foams. References 1. Liu, Y.-Y., Wang, Y.-K., Wu, D.-Y.: “Synthetic strategies for highly transparent and colorless polyimide film”, J. Appl. Polym. Sci. 2022,139(28), e52604. 2. Weihua Gu, Gehuan Wang, Ming Zhou, Tengze Zhang, and Guangbin Ji*: “Polyimide-Based Foams: Fabrication and Multifunctional Applications”, ACS Appl. Mater. Interfaces 2020, 12, 48246−48258 3. Leblanc, N., Le Cerf, D., Chappey, C., Langevin, D., Métayer, M. and Muller, G.:”Polyimide asymmetric membranes: Elaboration, morphology, and gas permeation performance”, J. Appl. Polym. Sci. 2003, 89, 1838-1848. 4. Haoqi Yang, Shuwu Liu, Lihua Cao, Shaohua Jiang* and Haoqing Hou*: “Superlithiation of non-conductive polyimide toward high-performance lithium-ion batteries”, J. Mater. Chem. A 2018, 6, 21216-21224. 5. N. Goujon, M. Lahnsteiner, D. A. Cerrón-Infantes, H. M. Moura, D. Mention, M. M. Unterlass*, and D. Mecerreyes: “Dual redox-active porous polyimides as high performance and versatile electrode material for next-generation batteries“, Materials Horizons 2023.
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