Data-Driven SDA Design and High-Throughput Experimentation for the Synthesis of High-Silica Small-Pore Zeolites Containing lta-cavities

Zeolites are crystalline microporous materials with diverse topologies used ubiquitously in catalysis and separations. However, the targeted synthesis of specific frameworks remains limited by the complexity of crystallization and competition among phases. Here, we introduce a data-driven strategy that integrates high-throughput simulations and SHapley Additive exPlanations (SHAP) analysis to design both organic and inorganic structure-directing agents (OSDA and ISDAs, respectively) for synthesizing small-pore zeolites containing lta-cages. Guided by this framework, we identified 4,7,13,16,21,24-hexaoxa-1,10-diazabicyclo[8.8.8]hexacosane as an optimal OSDA, and tailored alkali/alkaline-earth metal cations to stabilize specific composite building units. We achieved the phase-selective crystallization of RHO, KFI, LTA, and UFI zeolites with record-high Si/Al ratios under hydroxide-mediated conditions without the use of fluoride. The resulting high-silica materials exhibit exceptional hydrothermal stability, outperforming that of conventional analogues. Our results establish a generalizable framework for computational SDA selection and rational synthesis of zeolites with targeted structure and composition.