High-throughput transition-state searches in zeolite nanopores

Area of Science:

• Catalysis
• Materials Science
• Computational Chemistry

Background:

• Zeolites are vital catalysts for organic reactions due to their unique nanoporous structures.
• Experimental mechanistic studies are expensive, and traditional simulations are limited by scalability and manual intervention.
• Accurate identification of transition states is crucial for understanding zeolite-catalyzed reactions.

Purpose of the Study:

• To introduce an automated computational pipeline, the pore transition-state finder (PoTS), for locating transition states (TS) within zeolites.
• To overcome the limitations of existing experimental and simulation methods for studying zeolite reaction mechanisms.
• To improve the efficiency and success rate of transition state searches in confined zeolite environments.

Main Methods:

• PoTS identifies gas-phase transition states using density functional theory (DFT).
• Identified transition states are docked near active sites within zeolite pores.
• Reaction modes from gas-phase TS searches seed condensed-phase TS searches using the dimer method.
• The pipeline automates user intervention and bypasses lengthy calculations.

Main Results:

• The PoTS pipeline significantly reduces user intervention and increases the success rate of transition state searches.
• Application of PoTS to a DFT-level dataset of zeolite-confined transition states showed good agreement with experimental data.
• The method successfully bypasses the need for traditional, time-consuming path-following calculations.

Conclusions:

• PoTS offers an efficient and automated approach for determining transition states in zeolites.
• The pipeline enhances the study of zeolite-catalyzed reactions, providing accurate mechanistic insights.
• Future work will address limitations in unsuccessful searches and insufficient theoretical depth for reactions like alkene cracking.