Selective capture of <scp> N ₂ O </scp> using deep eutectic solvents: Mechanistic and molecular thermodynamic insights

Abstract Nitrous oxide (N 2 O) is a potent and long‐lived greenhouse gas that requires effective and selective capture technologies to mitigate its environmental impact. In this study, we systematically investigated the mechanism of selective N 2 O capture using deep eutectic solvents (DESs) from both thermodynamic and molecular perspectives. Three candidate DESs were initially screened using COSMO‐RS predictions in conjunction with physicochemical property analysis. The solubilities of N 2 O and N 2 in these DESs were subsequently evaluated using PC‐SAFT and COSMO‐RS models and validated experimentally. Analysis of thermodynamic parameters, including enthalpy, Gibbs free energy, and entropy, indicated that the capture of N 2 O and N 2 by DESs is a spontaneous and exothermic process. Furthermore, quantum chemical calculations revealed that van der Waals interactions dominate the capture mechanism at the molecular level. This study provides mechanistic insights and establishes a robust, theory‐guided screening framework for the rational design of advanced DESs for efficient N 2 O capture.