(84bn) A DFT Analysis of Optimal Solvents for High-Throughput Processing of Imine-Linked Covalent Organic Frameworks

Hydrogen-bonded lamellar solids have shown promise as candidates for next-generation extreme strength materials as they combine the advantages of traditional Kevlar and more recent graphene-like materials. Unfortunately, there has been limited success in finding cheap, non-volatile solvents for high-throughput solution-processing due to the above dual interactions. In this study, we utilize quantum mechanical calculations to understand the nature of the interactions between the 2-D polymer and different solvents (.e.g. water, trifluoroacetic acid etc.) in both vacuum and non-vacuum environments. Specifically, adsorption configurations, binding energies, and charge transfer between the polymer and solvents have been used to evaluate the strength of interactions and eventually, predict optimal solvents for these materials. Our results indicate that polymer-solvent interaction is primarily between the –OH group of the solvent and the imine-linkage of the COF with the strength of the interaction increasing with solvent acidity.