Abstract
Carbon capture is necessary to reduce CO2 emissions from burning fossil fuels, which has led to global warming. Molecular simulations offer chemical insights and design principles for new separation media and for understanding the separation process. In this review, we summarize recent applications of simulation methods from ab initio and density functional theory to classical molecular dynamics and Grand canonical Monte Carlo in understanding ionic liquids and porous carbonaceous materials for CO2 separation, especially the postcombustion CO2/N2 separation. We highlight design and simulation of the porous two-dimensional (2D) materials as the highly selective membranes for CO2 separation. Simulated structure–property relationships for the materials are discussed in connection to the corresponding chemisorption, physisorption, or membrane process. In chemisorption, the focus is on reducing the heat of reaction with CO2; in physisorption, the key is to increase the binding strength via CO2-philic groups; in membrane process, the key is to increase solubility for ionic-liquid membranes and to control pore size for 2D materials. Challenges and opportunities for simulating emerging materials are also discussed.
