In Silico Discovery of Covalent Organic Frameworks for Carbon Capture

Abstract

We screen a database of more than 69 000 hypothetical covalent organic frameworks (COFs) for carbon capture using parasitic energy as a metric. To compute CO2–framework interactions in molecular simulations, we develop a genetic algorithm to tune the charge equilibration method and derive accurate framework partial charges. Nearly 400 COFs are identified with parasitic energy lower than that of an amine scrubbing process using monoethanolamine; more than 70 are better performers than the best experimental COFs and several perform similarly to Mg-MOF-74. We analyze the effect of pore topology on carbon capture performance to guide the development of improved carbon capture materials.

Predicting the bulk modulus of single-layer covalent organic frameworks with square-lattice topology from molecular building-block properties

“…The underlying combinatorial variety of possible materials, enabled by the previously mentioned bottom-up lego-principle, imposes additional challenges to experimental investigations, so that extensive computational studies are becoming invaluable. For example, in silico methods have been used to study photocatalysis 16 , carbon capture 17,18 , hydrogen storage 19 , gas storage 20 , methane adsorption 21 and drug adsorption 22 in 2D COFs. An especially challenging issue in this context is revealing possible correlations between the chemical and physical properties of COFs and the ones of their molecular constituents.…”

Can COFs replace MOFs in flue gas separation? high-throughput computational screening of COFs for CO2/N2 separation

“…42 Ongari et al 43 recently reported a publicly available clean, uniform and rened with automatic tracking from experimental COF database (CURATED COFs) consisting of 324 optimized COFs with high-quality partial charges. Smit's group 44 predicted CO 2 parasitic energy of the CURATED COFs 43 and hypothetical COFs using molecular simulations and showed that many COFs have lower energy than that of traditional amine scrubbing process. As can be seen from this literature summary, we have limited information on the adsorption and membrane-based CO 2 /N 2 separation performances of COFs and the high-throughput computational screening of COFs is essential to compare their adsorbent and membrane performance evaluation metrics with those of MOFs.…”

Sorption‐induced polymer rearrangement: approaches from molecular modeling

“…Conversely, predictive molecular simulation methods implemented with candidate material screening studies can provide an effective and high-throughput means of identifying promising polymeric adsorbents. Notable studies of this nature have been performed for polymers of intrinsic microporosity (PIMs), 12 metal-organic frameworks, 13 covalent organic frameworks 14 and porous polymer networks. 15 Combining computational and experimental studies has been shown many times over to provide rapid materials prediction, design of adsorbent materials and an increased level of structural understanding.…”