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dependent composition changes also exist in static systems, but they are even more crucial to understanding and predicting mass flux across the interface of an active gas capture system. Addressing these issues will require surface-specific spectroscopies to avoid interference from the bulk. Depth profiling at the very small scale—perhaps as small as a few molecular diameters—is required. Tools are becoming available to probe time-averaged structure and composition (e.g., vibrational sum frequency generation, photoemission from liquids, x-ray and neutron scattering). Ideally, spectroscopic tools and techniques with sufficient temporal resolution would be available to study the kinetics and dynamics of absorption/desorption phenomena. Tools of this quality will require the development of new experimental methods and instrumentation that are capable of working in coexisting gas–liquid environments (moving from high vacuum to high pressure). At the solid–liquid and solid–vapor interfaces, probe microscopies like scanning tunneling microscopy and atomic force microscopy have provided a wealth of information about dynamics and reactivity. The liquid–vapor interface is far more dynamic, so extracting this type of information is presently unfeasible. New approaches are needed to extract comparable information. The combination of theory and experiment has led to an unprecedented level of understanding of how ions are distributed at the aqueous–air interface of salt solutions. Owing to the more complex nature of the liquids envisioned for capture processes, the combination of theory and experiment that will be available with exascale computing suggests that major improvement in theory will be possible within the next decade. The challenge is to describe liquid–vapor interfaces of more complex fluids, incorporating explicit interactions with the vapor phase, capturing static and dynamic features, and especially capturing reactions at the interface. First-principles simulation based on density functional theory has proved invaluable for studying reactions at the solid–gas interface, and only today are methods becoming available for the solid–gas. The liquid–gas interface, because it is disordered on both sides, becomes much more difficult. Exascale computing and new experimental methods will permit the development of the fundamental understanding necessary to allow rational design of novel liquid interfaces for CO2 capture and other separation processes (e.g., O2). With enhanced understanding of the details of interface structure and chemistry, it will be possible to design interface properties that enhance capture rates and eliminate transfer resistances that currently constrain large-scale capture systems. This rational design of interfaces will incorporate the modification of surface physical properties and the catalysis of key chemical reactions responsible for enhancing transport across the interface. It will also improve the handling and environmental characteristics of industrial fluids for which a very large surface area is both an operational requirement and a major limitation because of evaporation, oxidation, and other deleterious side reactions. Potential Impact Advances in this area can be expected to increase the understanding of liquid–gas interfaces and complex solutions. This will be the foundational underpinning of rational design of new materials and processes with enhanced capture capacity and reduced energy demand for regeneration of CO2 and other purified gases. These advances could allow capture device performance near the thermodynamic limit. Understanding gained in these studies could also 41PDF Image | 2020 Carbon Capture
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