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resolution. Experimental approaches are needed to enable in situ probing of liquid interfaces, capturing the molecular processes that occur during active transfer of gas across the interface. Understanding of the distribution of absorption phenomena that are primarily molecular versus those that are reactive, and the interplay between the two, will be required to both predict and design better interfacial properties for enhanced gas separation systems. By varying the chemical nature and composition of the liquid, it may be possible to tailor and control the gas– liquid interface so as to improve the overall reversibility and switchability of the sorption reactions. These goals will require strong coupling of experiment and theory, including experimental probing and computer simulation of liquids with greatly improved spatio-temporal resolution. Ideally, these dynamic interfaces could be chemically imaged with atomic- scale spatial resolution on time scales ranging from femtoseconds to minutes. Reactions at solid surfaces are routinely studied today—for example, catalysis on solids is a mainstay of surface science. That level of understanding is not available for liquid–gas interfaces, and reactive processes in these gas capture systems are also critical phenomena. For most CO2 capture processes, the rate of chemical reaction can be the most important determinant of the transfer rate across the interface. Rational design of improved processes can be expected to locate catalytic functions in the interface, both to improve chemical reaction rates and to improve the physical characteristics of the surface through functions like surfactants. Chemically tailored structures that self-organize these functions at the correct interface locations will be required to optimize interface function in capture systems. These tailored systems can become the foundations of facilitated transport mechanisms similar to those prevalent in biological systems. Scientific Questions and Opportunities A key scientific question is to understand the concentration and chemical state of targeted gases and associated materials at liquid interfaces. For CO2, such materials at the interface may include molecular CO2, carbonate/bicarbonate, and stronger complexes such as the carbamates that occur in amine solutions. Further, it is important to understand how this chemistry changes as materials transfer from the surface into the bulk. Such distance- Figure 12. Snapshots (top and side views) of the solution–air interface of 1.2 M aqueous sodium halides from molecular dynamics simulations and number density profiles of water oxygen atoms and ions plotted vs distance from the center of the slabs in the direction normal to the interface, normalized by the bulk water density. Notice the preferential segregation2of the more polarizable anions Br and I to the interface. 40PDF Image | 2020 Carbon Capture
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