Data-Driven Design of Biselective Templates for Intergrowth Zeolites

This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpclett.1c03132[EN] Zeolites are inorganic materials with wide industrial applications due to their topological diversity. Tailoring confinement effects in zeolite pores, for instance by crystallizing intergrown frameworks, can improve their catalytic and transport properties, but controlling zeolite crystallization often relies on heuristics. In this work, we use computational simulations and data mining to design organic structure-directing agents (OSDAs) to favor the synthesis of intergrown zeolites. First, we propose design principles to identify OSDAs which are selective toward both end members of the disordered structure. Then, we mine a database of hundreds of thousands of zeoliteOSDA pairs and downselect OSDA candidates to synthesize known intergrowth zeolites such as CHA/AFX, MTT/TON, and BEC/ISV. The computationally designed OSDAs balance phase competition metrics and shape selectivity toward the frameworks, thus bypassing expensive dual-OSDA approaches typically used in the synthesis of intergrowths. Finally, we propose potential OSDAs to obtain hypothesized disordered frameworks such as AEI/SAV. This work may accelerate zeolite discovery through data-driven synthesis optimization and design.This work was supported by the MIT Energy Initiative (MITEI) and MIT International Science and Technology Initiatives (MISTI) Seed Funds. D.S.-K. was additionally funded by the MIT Energy Fellowship. The authors acknowledge CSIC for the support through the I-link+ Program (LINKA20381). Computer calculations were executed at the Massachusetts Green High-Performance Computing Center with support from MIT Research Computing.Schwalbe-Koda, D.; Corma Canós, A.; Román-Leshkov, Y.; Moliner Marin, M.; Gomez-Bombarelli, R. (2021). Data-Driven Design of Biselective Templates for Intergrowth Zeolites. The Journal of Physical Chemistry Letters. 12(43):10689-10694. https://doi.org/10.1021/acs.jpclett.1c031321068910694124