A priori control of zeolite phase competition and intergrowth with high-throughput simulations

[EN] Zeolites are versatile catalysts and molecular sieves with large topological diversity, but managing phase competition in zeolite synthesis is an empirical, labor-intensive task. In this work, we controlled phase selectivity in templated zeolite synthesis from first principles by combining high-throughput atomistic simulations, literature mining, human-computer interaction, synthesis, and characterization. Proposed binding metrics distilled from more than 586,000 zeolite-molecule simulations reproduced the extracted literature and rationalized framework competition in the design of organic structure-directing agents. Energetic, geometric, and electrostatic descriptors of template molecules were found to regulate synthetic accessibility windows and aluminum distributions in pure-phase zeolites. Furthermore, these parameters allowed us to realize an intergrowth zeolite through a single bi-selective template. The computation-first approach enables control of both zeolite synthesis and structure composition using a priori theoretical descriptors. D.S.-K. and R.G.-B. acknowledge the Energy Initiative (MITEI) and MIT International Science and Technology Initiatives (MISTI) Seed Funds. D.S.-K. was also funded by the MIT Energy Fellowship. C.P., E.B.-J., M.M., and A.C. acknowledge financial support by the Spanish government through the "Severo Ochoa" program (SEV-2016-0683, MINECO) and grant RTI2018-101033-B-I00 (MCIU/AEI/FEDER, UE). E.B.-J. acknowledges the Spanish government for an FPI scholarship (PRE2019-088360). Z.J., E.O., S.K., and Y.R.-L. acknowledge partial funding from Designing Materials to Revolutionize and Engineer our Future (DMREF) from the National Science Foundation (NSF); awards 1922311, 1922372, and 1922090; and the Office of Naval Research (ONR) under contract N00014-20-1-2280. S.K. was additionally funded by the Kwanjeong Educational Fellowship. Z.J. was also supported by the Department of Defense (DoD) through the National Defense Science Engineering Graduate (NDSEG) fellowship program. T.W. acknowledges financial support by the Swedish Research Council (grant no. 2019-05465). Computer calculations were executed at the Massachusetts Green HighPerformance Computing Center with support from MIT Research Computing and at the Extreme Science and Engineering Discovery Environment (XSEDE) (53) Expanse through allocation TG-DMR200068. Schwalbe-Koda, D.; Kwon, S.; Paris, C.; Bello-Jurado, E.; Jensen, Z.; Olivetti, E.; Willhammar, T... (2021). A