Department of Chemical and Biological Engineering, Northwestern University, Evanston, Illinois, 60208.
J Comput Chem. 2019 May 5;40(12):1305-1318. doi: 10.1002/jcc.25787. Epub 2019 Feb 4.
Metal-organic frameworks (MOFs) are a class of nanoporous materials with highly tunable structures in terms of both chemical composition and topology. Due to their tunable nature, high-throughput computational screening is a particularly appealing method to reduce the time-to-discovery of MOFs with desirable physical and chemical properties. In this work, a fully automated, high-throughput periodic density functional theory (DFT) workflow for screening promising MOF candidates was developed and benchmarked, with a specific focus on applications in catalysis. As a proof-of-concept, we use the high-throughput workflow to screen MOFs containing open metal sites (OMSs) from the Computation-Ready, Experimental MOF database for the oxidative C-H bond activation of methane. The results from the screening process suggest that, despite the strong C-H bond strength of methane, the main challenge from a screening standpoint is the identification of MOFs with OMSs that can be readily oxidized at moderate reaction conditions. © 2019 Wiley Periodicals, Inc.
金属-有机骨架（MOFs）是一类纳米多孔材料，其化学组成和拓扑结构具有高度可调节性。由于其可调性质，高通量计算筛选是一种特别有吸引力的方法，可以减少具有理想物理和化学性质的 MOF 的发现时间。在这项工作中，开发并基准测试了一种完全自动化的、高通量的周期性密度泛函理论（DFT）筛选有前途的 MOF 候选物的工作流程，特别关注催化应用。作为概念验证，我们使用高通量工作流程从 Computation-Ready、Experimental MOF 数据库中筛选出含有开放金属位点（OMSs）的 MOFs，用于甲烷的氧化 C-H 键活化。筛选过程的结果表明，尽管甲烷的 C-H 键强度很强，但从筛选的角度来看，主要的挑战是确定具有 OMSs 的 MOFs，这些 MOFs可以在中等反应条件下容易地被氧化。© 2019 Wiley Periodicals, Inc.
