Materials genomics represents a research mode for materials development, for which reliable methods for efficient materials construction are essential. Here we present a methodology for high-throughput construction of covalent organic frameworks (COFs) based on materials genomics strategy, in which a gene partition method of genetic structural units (GSUs) with reactive sites and quasi-reactive assembly algorithms (QReaxAA) for structure generation were proposed by mimicking the natural growth processes of COFs, leading to a library of 130 GSUs and a database of ~470,000 materials containing structures with 10 unreported topologies as well as the existing COFs. As a proof-of-concept example, two generated 3D-COFs with ffc topology and two 2D-COFs with existing topologies were successfully synthesized. This work not only presents useful genomics methods for developing COFs and largely extended the COF structures, but also will stimulate the switch of materials development mode from trial-and-error to theoretical prediction-experimental validation.

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Membrane based CO 2 /CH 4 separation is an effective and energy saving way for highly demanded natural gas upgrading. Herein, high-throughput computational screening of covalent organic frameworks (COFs) for CO 2 /CH 4 membrane separation is realized by using the 298 COF structures in CoRE COF database. Based on the study of structure−performance relationships, structural features of the outperformed COFs were identified and classified, followed by the structural design by decorating 11 CoRE COFs with 10 kinds of familiar functional groups. By evaluating the 290 designed COFs as membrane materials, the effectiveness and universality of −F and −Cl groups in improving the performance of various COFs were identified. The well-performed COFs were also computationally evaluated as fillers to make COF@polymer mixed matrix membranes, and improved separation performance was obtained.

CH 4 storage associated with adsorbed natural gas technology attracts considerable researches on finding porous materials with remarkable CH 4 delivery performance. In this work, we update the online accessible computation-ready, experimental (CoRE) covalent organic frameworks (COFs) database with 280 COFs in 12 topologies. All framework structures are constructed and compiled from the respective experimental studies and are further evaluated for CH 4 delivery. The highest deliverable capacity (DC) between 65 and 5.8 bar among the CoRE COFs is 190 v(STP)/v at 298 K achieved by 3D PI-COF-4. Structure−property relationships show that large volumetric surface area generally benefits CH 4 delivery. 2D-COFs can also be top performing materials if constructing their pore channels is passable in three dimensions, as the volumetric surface area will be increased accordingly. This idea can be realized by enlarging the interlayer spacings of 2D-COFs. We also evaluate the DC of CoRE COFs under conditions of 233 K, 65 bar (storage) and 358 K, 5.8 bar (discharge). The highest DC obtained from the CoRE COFs and the designed 2D-COFs are 314 and 337 v(STP)/v, respectively.

High-throughput construction of IL/MOF composites and discovery of the synergistic effect in the wire-tube conformation for efficient CO2/CH4 separation.