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and postcombustion and oxyfuel separation in particular. The challenges to realizing breakthrough increases are substantial, but the scientific tools are now in place to advance the field from incremental improvements based on limited understanding to true knowledge and insight-driven discovery and optimization. Gas–liquid interfaces are tumultuous places, with molecules in the interfacial region involved in a tug- of-war between attractive solvation forces that pull them into the liquid and entropic forces that drive them out. This conflict results in ceaseless, rapid excursions of individual molecules back and forth across the imaginary line separating the two phases. Understanding these complex, dynamic interfaces requires new analytical techniques with the ability to discriminate between molecules in the interfacial region, typically a few molecules thick at most, and those in the vastly larger bulk liquid region. New nonlinear spectroscopies (second harmonic generation and sum frequency generation) are capable of identifying particular species in the interfacial region, but they do not provide depth resolution. Photoelectron spectroscopy, especially with synchrotron light sources, has allowed species-selective depth profiling of a wide range of atomic and molecular species at gas–liquid interfaces. Complementing experimental techniques, molecular dynamics simulations, based on either empirical force fields or ab initio potentials, can provide a dynamic, molecular-scale view of gas– liquid interfaces. Computational methods assist in interpreting experimental data and inspire the development of new experimental capabilities. In turn, modern experiments are providing a wealth of data that can be used to scrutinize and refine theoretical models.10 Interfacial Reactions Gas–liquid interfaces. Left panel: Snapshots from molecular dynamics simulations depicting air- solution interfaces of aqueous alkali halide solutions. Right panel: Depth profiles of the anion/cation ratios from photoelectron spectroscopy experiments on deliquesced potassium halide crystals. The prediction of the presence of ions at the air–water interface defied conventional wisdom and stimulated the development of new experiments. The increasing enhancement of the population of the anion over the cation with increasing halide mass predicted by the simulations is verified by the experiment. 14PDF Image | 2020 Carbon Capture
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