A priori control of zeolite phase competition and intergrowth with high-throughput simulations
A priori control of zeolite phase competition and intergrowth with high-throughput simulations
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DOI：
10.1126/science.abh3350
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发表时间：
2021-10-15
期刊：
影响因子：
56.9
通讯作者：
Gomez-Bombarelli, Rafael
中科院分区：
文献类型：
--
作者：
Schwalbe-Koda, Daniel;Kwon, Soonhyoung;Gomez-Bombarelli, Rafael
沸石是具有大的拓扑多样性的多用途催化剂和分子筛，但是在沸石合成中管理相竞争是经验性的劳动密集型任务。在这项工作中，我们控制相选择性模板沸石合成从第一原理相结合的高通量原子模拟，文献挖掘，人机交互，合成和表征。从超过586，000个沸石分子模拟中提取的建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，这些参数使我们能够实现共生沸石通过一个单一的双选择性模板剂。计算优先的方法使得能够使用先验理论描述符来控制沸石合成和结构组成。
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.