Multiscale Modeling Strategy of 2D Covalent Organic Frameworks Confined at an Air–Water Interface

Two-dimensional covalent organic frameworks (2D COFs) have attracted attention as versatile active materials in many applications. Recent advances demonstrated the synthesis of monolayer 2D COF via an air–water interface. However, interfacial polymerization mechanism has been elusive. In this work, we used a multiscale modeling strategy to study dimethylmethylene-bridged triphenylamine building blocks confined at interface form Schiff-base reaction. A synergy between computational investigations and experiments allowed 2D-COF with one linkers considered. Our simulations complement experimental characterization show preference be favorable orientation for polymerization. The is shown key factor stabilize flat conformation when dimer molecule structural electronic properties COFs based on two monomers are calculated semiconducting nature direct bandgaps. provides first step toward silico interfaces capturing initial steps up prediction material.