A priori control of zeolite phase competition and intergrowth with high-throughput simulations
Daniel Schwalbe‐Koda, Soonhyoung Kwon, Cecilia Paris, Estefanía Bello‐Jurado, Zach Jensen, Elsa Olivetti, Tom Willhammar, Avelino Corma, Yuriy Román‐Leshkov, Manuel Moliner, Rafael Gómez‐Bombarelli
Abstract
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.