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(d) Bulk effects. Phase changes are the quintessential examples of cooperative phenomena, in which a material can be more strongly associated with one phase than another. The scientific challenge is to develop materials that can exist in two (or more) phases that possess dramatically different gas capacities. A critical requirement is that the targeted gas be vigorously absorbed or expelled when the material is coaxed from one phase to another by an external stimulus—such as heating, pressure variation, application of a voltage or magnetic field, or irradiation with light (see the PRD “Alternative Driving Forces and Stimuli-Responsive Materials for Carbon Capture”). (e) Rates of gas uptake and release in cooperative systems. Rapid uptake and release of gases, such as CO2 and O2, is a central requirement for their efficient capture and release; therefore, the kinetics for reversible gas sorption in these cooperative systems are as important as the low overall energy budget. Interfaces—between gases and solids and between different solids—are gating factors in determining the rate for any gas sorption process. In these cooperative systems, the energetically-uphill changes in the sorbent that are required to lower the overall energy cost may also severely decrease the rate of uptake. Generally, the speed of gas sorption will be determined by (1) the mechanisms of binding of gases to the external surfaces of the sorbents (adsorption), (2) transport of the sorbent into the bulk of the material (absorption), and (3) the mechanisms and energetics for coupling materials transformations to key the adsorption and absorption steps and their reverse (release). Changes induced by binding of molecular gases can occur on different length scales, from the molecular to the macroscopic, as discussed earlier. Even if a change is energetically favored overall, though, there must be an accessible mechanistic pathway under the conditions of the reactor for that change to occur. A central challenge will be to determine which length scales lead to the fastest rates of sorption and release. There may be an optimal length scale over which the reorganization takes place in the material that leads to a fast rate of uptake (or release) and a low net energy cost. Theoretical models that can be applied self- consistently over a range of length scales will provide important insights into the interplay among kinetics, energetics, and length scale. An exciting opportunity is to test the rapidity of sorption and release of CO2 and oxygen using different types of stimulation. Typically, either temperature or pressure swings are used to release CO2. Alternatively, electrical, magnetic, mechanical, or light stimulation might facilitate transformations that induce either uptake or release of gases (see the PRD “Alternative Driving Forces and Stimuli-Responsive Materials for Carbon Capture”). This approach has the potential for high reversibility with low energy input. The conceptual basis for this focus area is based on the fact that materials transformations are known to be triggered by external stimuli. For example, piezoelectric materials—a special class of metal oxides that expand or contract upon application of an external voltage—have recently been shown to have differential binding energies for CO2 depending on the polarization of the surface.3 This single result provides reason to believe that external stimuli other than heat and pressure changes could drive uptake or release of CO2 and other gases. 66PDF Image | 2020 Carbon Capture
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