美国麻省理工学院Rafael Gómez-Bombarelli和Manuel Moliner课题组在研究中取得进展。他们报道了沸石相竞争和共生的先验控制与高通量模拟。相关论文于2021年9月16日发表在《科学》杂志上。

该课题组通过结合高通量原子模拟、文献挖掘、人机交互、合成和表征，从第一性原理控制模板沸石合成的相选择性。提出的结合指标从超过586000沸石-分子模拟再现了提取的文献和合理化的框架竞争在有机结构导向剂中的设计。模板分子的能量、几何和静电描述符可以调节合成的可及性窗口和纯相沸石中的铝分布。

此外，这些参数允许通过单个双选择模板实现共生沸石。计算优先的方法实现使用先验理论描述符控制沸石合成和结构组成。

据介绍，分子筛是一种多用途的催化剂和具有较大拓扑多样性的分子筛，但是管理分子筛合成中的相竞争是一项经验的、劳动密集型的任务。

附：英文原文

Title: A priori control of zeolite phase competition and intergrowth with high-throughput simulations

Author: Daniel Schwalbe-Koda, Soonhyoung Kwon, Cecilia Paris, Estefania Bello-Jurado, Zach Jensen, Elsa Olivetti, Tom Willhammar, Avelino Corma, Yuriy Román-Leshkov, Manuel Moliner, Rafael Gómez-Bombarelli

Issue&Volume: 2021-09-16

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. 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.

DOI: abh3350

Source: https://www.science.org/doi/10.1126/science.abh3350