In Silico Design of 2D and 3D Covalent Organic Frameworks for Methane Storage Applications

Here, we present a database of 69 840 largely novel covalent organic frameworks assembled in silico from 666 distinct organic linkers and four established synthetic routes. Due to their light weights and high internal surface areas, the frameworks are promising materials for methane storage applications. To assess their methane storage performance, we used grand-canonical Monte Carlo simulations to calculate their deliverable capacities. We demonstrate that the best structure, composed of carbon–carbon bonded triazine linkers in the tbdtopology, has a predicted 65-bar deliverable capacity of 216 v STP/v, better than the best methane storage materials published to date. Using our approach, we also discovered other high-performing materials with 300 structures having calculated deliverable capacities greater than 190 v STP/v and 10% of these outperforming 200 v STP/v. To encourage screening studies of these materials for other applications, all structures and their properties were made available on the Materials Cloud.