High-throughput transition-state searches in zeolite nanopores.

Abstract

Zeolites are essential catalysts for organic transformations owing to their confined nanoporous environments. However, experimental mechanistic studies are costly, and traditional simulations lack scalability, relying on manual structural manipulation. Here we introduce pore transition-state finder (PoTS), an automated pipeline for locating transition states (TS) in zeolites. PoTS identifies gas-phase TSs via density functional theory, docks them near active sites in zeolite pores and uses their reaction modes to seed condensed-phase TS searches with the dimer method. This automation reduces user intervention, improves success rates and bypasses the need for long path-following calculations. We apply PoTS to a density functional theory-level dataset of zeolite-confined TSs, finding good experimental agreement in both cases. Last, we propose a path to address the limitations we observe regarding unsuccessful TS searches and insufficient theory in other reactions, such as alkene cracking.