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INTERFACIAL PROCESSES AND KINETICS Abstract Mass transfer across the gas-liquid interface can be the rate-limiting step controlling the uptake and release of carbon dioxide. A key barrier to the development of greatly improved liquid absorption separation processes is the lack of understanding of the nature of gas-liquid interfaces. Once understood, this information could be used to design specific modifications to those interfaces to enhance gas separation systems. Advancing knowledge in this area will require the strong coupling of theory and experiment with the assembly of interdisciplinary expertise in the structures of liquid, physics of interfaces, molecular spectroscopy, and chemical kinetics. In addition, new approaches are needed to characterize dynamic and chemically complex interfaces—examining both the spatial and temporal distribution of solution components and reactants in the interface. Background and Motivation The gas–liquid interface is the gateway to bulk absorption. Transfer across this boundary is well known to limit many CO2 process rates. Therefore, it plays a critical role in any carbon capture process using a liquid. Liquids are intrinsically difficult to study since they are disordered and have a time-varying, dynamic structure. Even less is known about the chemical structure of liquid–gas interfaces. Surface composition is not a simple termination of the bulk structure but rather is dictated by minimization of surface free energy. Mass transfer considerations suggest that kinetic modifications of CO2 absorption processes are best targeted very near the surface to maximize flux into the bulk. Understanding the structure and dynamics of this interface is key to tailoring uptake and release kinetics and will allow controlled design of future sorption materials. Interfaces warrant study to avoid potential kinetic bottlenecks; understand the structure and dynamics of complex liquid–gas interfaces; and understand the linkage among the composition, structure, and chemistry of the interface. Liquids potentially useful for carbon capture, oxygen purification, or other gas separation approaches are likely to be complex systems such as highly concentrated basic solutions, ionic liquids, or exotic multiphase fluids—but we don’t really understand even simple fluids yet. For example, even relatively low-concentration aqueous salt solutions have been predicted to have an asymmetric distribution of anions and cations at the vapor–liquid interface (Figure 12), a result confirmed by recent experiments.1 Research Directions A key barrier to the development of greatly improved liquid absorption separation processes is the lack of understanding of the nature of gas–liquid interfaces. That understanding, once obtained, could be used to design specific modifications to those interfaces to enhance gas separation systems. Advancing knowledge in this area will require the assembly of interdisciplinary expertise in the structures of liquids, the physics of interfaces, molecular spectroscopy, and chemical kinetics. In addition, new approaches are needed to characterize dynamic and chemically complex interfaces—examining both the spatial and temporal distribution of solution components and reactants in the interface. Current experimental tools have shown that the surface composition can be strongly segregated, and additional knowledge needed to understand dynamic separation processes will also require temporal 39PDF Image | 2020 Carbon Capture
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