(606i) Highly Stable Two-Dimensional Polyarylene Materials and Interfaces

Despite great strides made in understanding the structural, mechanical, and electronic properties of two-dimensional polymers, there is very little known about their temperature-dependent polymorphs and resiliency. This work is the first comparison of a chemically homologous series of linear and two-dimensional polyarylene polymers at high temperatures. The 2D polymer topology offers a potential to design higher thermal resilience than the 1D polymer topology. First principles DFT molecular mechanics and dynamics methods agree quantitatively with the known behavior of linear poly(p-phenylene terephthalamide), more commonly known as Kevlar®. Additional simulations show that hydrogen-bonded 2D polymers, such as graphamid and covalent organic frameworks, are a unique material topology for providing enhanced structural and thermomechanical stability. These results suggest that hydrogen-bonded 2D polymers offer significant advantages for combined light weight, high strength and high temperature ultra-performance applications.