Schwalbe-Koda, DanielKwon, SoonhyoungParis, CeciliaBello-Jurado, EstefaníaJensen, ZachOlivetti, ElsaWillhammar, TomCorma Canós, AvelinoRomán-Leshkov, YuriyMoliner Marin, ManuelGomez-Bombarelli, Rafael2022-07-202022-07-202021-10-150036-8075https://riunet.upv.es/handle/10251/184569[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.Reserva de todos los derechosQUIMICA ORGANICAArtículo10.1126/science.abh3350Abierto34529493