Zeolites are versatile catalysts and molecular sieves with large topological diversity, but managing phase competition in zeolite synthesis is an empirical, labor-intensive task. Here, 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 over 586,000 zeolite-molecule simulations reproduced the extracted literature and rationalize 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 realizing an intergrowth zeolite through a single bi-selective template. The computation-first approach enabled controlling both zeolite synthesis and structure composition using a priori theoretical descriptors.

中文翻译：

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通过高通量模拟对沸石相竞争和共生的先验控制

沸石是多功能催化剂和分子筛，具有较大的拓扑多样性，但在沸石合成中管理相竞争是一项经验丰富的劳动密集型任务。在这里，我们通过结合高通量原子模拟、文献挖掘、人机交互、合成和表征，从第一原理控制模板化沸石合成中的相选择性。从超过 586,000 个沸石分子模拟中提取的拟议结合指标再现了提取的文献，并使有机结构导向剂设计中的框架竞争合理化。发现模板分子的能量、几何和静电描述符可以调节纯相沸石中的合成可及性窗口和铝分布。此外，这些参数允许通过单个双选择性模板实现共生沸石。计算优先的方法能够使用先验理论描述符控制沸石合成和结构组成。