Ab initio Analysis of Membrane Stability in Alkaline Environments: a Joint Density Functional Theory (JDFT) Study

Improving membrane stability in alkaline environments is crucial to the development of alkaline fuel cells (AFCs). Ab initio studies using the nudged elastic band (NEB) method, combined with a detailed transition-state theory analysis, allow us not only to predict quantitative lifetimes of alkali-stable membrane polymers, but also to uncover unexpected mechanisms for improving membrane lifetime. In this later regard, we find that the choice of a first-principles joint-density functional theory (JDFT) description of the solvent and consideration of the impact of the hydrophobic regions of the membrane are critical to understanding the polymer degradation process. This work is foundational to computation-enabled searches for yet more stable AFC membranes.