Membrane separation is a high-efficiency, energy-saving, and environment-friendly separation technology. Covalent organic framework (COF)-based mixed-matrix membranes (MMMs) have broad application prospects in gas separation and are expected to provide new solutions for coal-bed methane purification. Herein, a high-throughput screening method is used to calculate and evaluate COF-based MMMs for CH₄/N₂ separation. General design rules are proposed from thermodynamic and kinetic points of view using the computation-ready, experimental COFs. From our database containing 471,671 generated COFs, 5 COF membrane materials were screened with excellent membrane selectivities, which were then used as the filler of MMMs for separation performance evaluation. Among them, BAR-NAP-Benzene_CF₃ combined with polydimethylsiloxane and styrene-b-butadiene-b-styrene show high CH₄ permeability of 4.43 × 10⁻¹³ mol·m·s⁻¹·Pa⁻¹·m⁻² and high CH₄/N₂ selectivity of 9.54, respectively. The obtained results may provide reasonable information for the design of COF-based membranes for the efficient separation of CH₄/N₂.

膜分离是一种高效、节能、环保的分离技术。基于共价有机骨架（COF）的混合基质膜（MMMs）在气体分离中具有广阔的应用前景，有望为煤层气净化提供新的解决方案。本文采用高通量筛选方法计算和评估基于 COF 的 MMM 用于 CH ₄ /N ₂分离。使用可计算的实验 COF 从热力学和动力学的角度提出一般设计规则。从我们包含 471,671 个生成的 COF 的数据库中，筛选出 5 种具有优异膜选择性的 COF 膜材料，然后将其用作 MMM 的填料，用于分离性能评估。其中，BAR-NAP-Benzene_CF₃与聚二甲基硅氧烷和苯乙烯-b-丁二烯-b-苯乙烯结合显示出4.43×10 ^-13 mol·m·s ^-1 ·Pa ^-1 ·m ^-2的高CH ₄渗透率和9.54的高CH ₄ /N ₂选择性， 分别。所得结果可为设计用于高效分离CH ₄ /N ₂的COF基膜提供合理的信息。