This research aims to improve the carbon capture capabilities of nitrogen-doped porous materials, specifically nitrogen-assembly carbons (NACs), for carbon dioxide and methane in gas mixtures. The team will predict the nature and the magnitudes of the interactions between gas molecules and NAC surfaces using scalable quantum mechanical methods combined with Monte Carlo techniques. Building upon the Exascale Computing Project and utilizing Department of Energy computing facilities, the research will determine the role of nitrogen-containing species in NACs that exhibit selectivity for carbon dioxide and methane in environments such as flue gas, biogas, and gaseous products of carbon dioxide conversions. The outcomes of this research will guide the design and synthesis of NACs for carbon capture and storage, as well as chemical transformations. They will foster collaboration between experimental and theoretical scientists at Ames National Laboratory and beyond. The results will advance the development of carbon capture technologies essential for mitigating greenhouse gas emissions impacts on health, the economy, and the environment, aligning with the Department of Energy's mission to address energy and environmental challenges through science and technology.