Identifying Promising Covalent-Organic Frameworks for Decarburization and Desulfurization from Biogas via Computational Screening

Abstract

Efficient removal of hydrogen sulfide and carbon dioxide is essential for biogas purification, which is still a longstanding challenge economically and environmentally. Recently, covalent-organic frameworks (COFs) have become competitive candidates for acid gases capture. In this study, high-throughput computational screening of a database containing 382 computation-ready experimental COFs were employed to establish structure-performance relationships and to identify the topperforming materials for H 2 S and CO 2 separation from biogas (H 2 S/CO 2 /CH 4 ) under dry operating conditions. By using adsorbent performance score and the sorbent selection parameter as evaluation metrics, the calculated results show that the best material is significantly better than many benchmark materials reported so far. Further, we investigated the adsorption and separation performance of the modified materials in sulfur and carbon capture from ternary gas mixtures. The results indicated that the existence of favorable organic linkers and micro pores played a significant role in promoting the adsorption of H 2 S and CO 2 . This work is anticipated to provide a useful guidance for the design of new materials with high performance for decarburization and desulfurization from biogas.

Functionalized 3D Covalent Organic Frameworks for High‐Performance CO2 Capture and Separation over N2

“…Lennard–Jones (LJ) interactions and Ewald electrostatic interactions were used to calculate gas–gas interactions and gas–COF framework interactions. [ 24 ] Considering CO 2 and N 2 as rigid linear molecules, three charged LJ interaction sites were chosen for CO 2 and N 2 . The LJ potential parameters for CO 2 and N 2 were from the TraPPE model reported by Potoff and Siepmann.…”

Covalent organic frameworks for CO2 capture: from laboratory curiosity to industry implementation

“…Wang et al reported computational screening of COFs for simultaneous desulphurization and decarbonization for biogas production. 277 The results indicated that a limiting cavity diameter (LCD) of 12.5 Å and porosity of 0.65 was quite suitable for simultaneous operation. Aksu et al computationally screened COF materials for removing H 2 S and CO 2 from natural gas mixtures and highlighted the superior performance of several COFs to existing MOFs and zeolites.…”

Combining Interpretable Machine Learning and Molecular Simulation to Advance the Discovery of COF-Based Membranes for Acid Gas Separation

“…38 COF-gas and gas−gas interactions were performed using the Lennard-Jones (LJ) potential description. The Dreiding force field is used to describe the elemental composition of COFs, 39 and the Universal Force Field (UFF) is used to describe other metallic elements, 40 and the work of Wang et al 41 have demonstrated that the "UFF_Dreiding" hybrid force field is in good agreement with experiment. Due to the presence of polar gas molecules, charge equilibrium (Qeq) calculations are used to quickly compute the partial charges of the atomic framework of COFs.…”