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and Langmuir behavior for chemically reacting absorbents. Real absorbents always deviate to some extent from ideality: the absorption of one molecule of gas has some influence on the absorption of the next. The opportunity is to control these interactions. For instance, can we design absorbents that exhibit cooperativity, in which the absorption of one gas molecule promotes the absorption of the next? Cooperativity is accomplished in hemoglobin through the chemical linking of four porphyrin rings; can similar effects be achieved in molecules suitable for industrial gas separations? For an efficient separation system, the adsorbent should have a high capacity and selectivity for the species being separated, which generally translates into a large exothermic heat of absorption, ∆H ̊. However, this enthalpy must be paid back during the regeneration step, when the absorbate is separated from the absorbent, and thus easy regeneration demands low ∆H ̊. For thermodynamically based separations, then, these two objectives would appear to be at odds with each other. However, the absorption entropy provides a separate thermodynamic handle on separations. Can differences in sizes and shapes (entropy) of components to be separated be exploited as an alternative strategy to using differences in interaction energy (enthalpy)? Can strategies be developed to control absorption enthalpy and entropy in as independent a manner as possible? What are the limits on this independent control? These challenges would provide immense improvements in the cost and practicality of large-scale use of liquid absorbents for separation of CO2 and O2 from complex mixtures and would have broad impact on other applications of gas separation. Scientific Questions Absorbent-based gas separations essentially exploit the physical chemistry of gas–liquid equilibrium and reactions. The understanding of these interactions has advanced enormously over the years. CO2 capture (and O2 concentration) elevates these questions to a new level, however: Can they be described, understood, and modeled in the context of a gas mixture as complex as a flue gas, over the wide range of conditions that an absorbent will experience? Even more fundamentally, can they be controlled so as to minimize the energy cost of separations? And finally, can this control be realized in systems that meet all the other practical constraints of a real-world separation? Potential Impact This PRD touches on some of the most fundamental questions of intermolecular interactions and reactivity. This scientific knowledge is imperative if step change improvements in absorption-based separations are to be realized. Further, the evidence suggests that this step change is truly attainable, bringing practical, large-scale carbon capture and separation much closer to reality. The basic questions addressed are not limited to this domain, however. Similar questions emerge in membrane- and adsorbent-based separations, of course. But gas– liquid interactions are also central to biology, to environmental and atmospheric chemistry, to catalysis, to chemical processing, and even to sequestration. The knowledge and associated computational and experimental tools will advance fundamental scientific understanding and ultimately capability in all these domains. 49PDF Image | 2020 Carbon Capture
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