(461c) A Priori Control of Zeolite Phase Competition with High-Throughput Simulations

Framework diversity makes zeolites versatile materials for catalysis and separations. While this variety of topologies provides multiple pathways to catalyze reactions of interest, it also leads to phase competition between polymorphs. Computer simulations can guide experimental work by predicting organic structure-directing agents (OSDAs) that favor the synthesis of targeted frameworks, but theoretical methods usually overlook phase competition effects when proposing novel templates. Accordingly, computer-designed OSDAs are either unselective towards the desired structures or overly complex to be deployed at an industrial scale. Hence, overcoming phase competition in zeolites requires laborious experimentation and serendipity, even when computer-aided. In this work, we demonstrate an ab initio method to control phase selectivity in zeolites. By developing algorithms to accelerate atomistic simulations of zeolites, we built a computational infrastructure that predicts host-guest interaction energies two orders of magnitude faster than existing approaches. Then, using more than half a million zeolite-molecule simulations, we devised binding affinity metrics that rationalize synthesis outcomes from more than one thousand papers extracted from the literature. The metrics also enable the design of chemically simple OSDAs that simultaneously stabilize the desired topology while destabilizing other phases. To further accelerate the selection of new templates, we developed a web-based platform that provides a visual interface for data exploration by human experts. This human-computer partnership enables researchers to compare templates, obtain information on prior art and literature for zeolite-OSDA pairs, and downselect molecules based on their selectivity, synthetic accessibility, or physical descriptors prior to attempting the synthesis. This work opens a venue for controlling zeolite synthesis and catalytic properties through polymorphism engineering.