Highly Flexible Dielectric Films from Solution Processable Covalent Organic Frameworks

Covalent organic frameworks (COFs) are known to be a promising class of materials for a wide range of applications, yet their poor solution processability limits their utility in many areas. Here we report a pore engineering method using hydrophilic side chains to improve the processability of hydrazone and beta-ketoenamine-linked COFs and the production of flexible, crystalline films. Mechanical measurements of the free-standing COF films of COF-PEO-3 (hydrazone-linked) and TFP-PEO-3 (beta-ketoenamine-linked), revealed a Young's modulus of 391.7 MPa and 1034.7 MPa, respectively. The solubility and excellent mechanical properties enabled the use of these COFs in dielectric devices. Specifically, the TFP-PEO-3 film-based dielectric capacitors display simultaneously high dielectric constant and breakdown strength, resulting in a discharged energy density of 11.22 J cm-3. This work offers a general approach for producing solution processable COFs and mechanically flexible COF-based films, which hold great potential for use in energy storage and flexible electronics applications. Porous polymers, like covalent organic frameworks, are promising materials for a wide variety of applications. However, unlike conventional polymers, they are challenging to mold, shape, or process. Here we show how insoluble COFs, functionalized with oligoether sidechains, can be solution cast into high-dielectric films, with excellent flexibility and mechanical strength.**+image