Design of Amine-Functionalized Materials for Direct Air Capture Using Integrated High-Throughput Calculations and Machine Learning

Abstract: Direct air capture (DAC) of carbon dioxide is a critical technology for mitigating climate change, but current materials face limitations in efficiency and scalability. We discover novel DAC materials using a combined ML and high-throughput atomistic modeling approach. Our ML model accurately predicts high-quality, density functional theory-computed CO${2}$ binding enthalpies for a wide range of nitrogen-bearing moieties. Leveraging this model, we rapidly screen over 1.6 million binding sites from a comprehensive database of theoretically feasible molecules to identify materials with superior CO${2}$ binding properties. Additionally, we assess the synthesizability and experimental feasibility of these structures using established ML metrics, discovering nearly 2,500 novel materials suitable for integration into DAC devices. Altogether, our high-fidelity database and ML framework represent a significant advancement in the rational development of scalable, cost-effective carbon dioxide capture technologies, offering a promising pathway to meet key targets in the global initiative to combat climate change.