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Successful integration of this concept into carbon emissions reduction technology also requires that the rates of uptake and release be rapid. Because the coupled materials changes will necessarily be energetically “uphill,” the rates of gas uptake or release could be substantially reduced. Investigating the rates and the mechanisms of gas uptake and release in these systems will enable the development of a predictive framework for coupling materials changes with gas sorption. To fully understand these processes and to develop a rational approach to constructing cooperative systems, new experimental and theoretical methods are needed in conjunction with creative application of existing methods for synthesis, characterization, and modeling. Research Directions Creation of new materials with nonlinear responses to CO2 or O2 binding There are four general approaches to the discovery and exploitation of cooperative effects that will result in an overall low enthalpy for capture and release of CO2 or O2. These approaches can be heuristically organized on the basis of the length-scale of the cooperative interaction: (a) atomically local, (b) molecularly local, (c) nanoscopically and microscopically confined, and (d) macroscopic. (a) Atomically local. Inorganic molecular complexes illustrate that ligands coordinated to the metal center can affect one another’s binding mode and binding energy. As a simple example, the stepwise dissociation of the four CO ligands from Ni(CO)4 to give Ni(CO)3, Ni(CO)2, Ni(CO), and ultimately atomic nickel come with significantly different energy costs. The essential challenge faced in devising strategies for cooperative CO2 capture is whether sorbents can be synthesized in which the local, active sites for CO2 adsorption show similarly nonlinear effects. (b) Molecularly local. There are examples in nature in which the binding of one molecule to an active site in a material increases its affinity for binding of a second molecule. Perhaps the best-known example is hemoglobin, in which the absorption of one molecule of O2 to the previously completely deoxygenated substrate affects the thermodynamics and kinetics of the subsequent oxygen coordination steps. The mechanism of this amplification involves the structural reorganization of the substrate so that the coordination sites are mechanically optimized on the nanoscale for subsequent oxygenation (Figure 18). The materials challenge here is to invent analogous microenvironments for the cooperative absorption of multiple equivalents of CO2 to the same “active area.” (c) Confinement at the nanoscale or micron scale. Three-dimensional environments can be designed and constructed that behave like gas sponges. One way to do this would be to prepare a material that has defined but flexible pores that can facilely expand or contract, but which robustly cycle their structures between the gas-filled or empty states. In an ideal case, the material would be mechanically bistable: one state would be gas-deficient and the other would be gas-rich. As ambient conditions changed (e.g., temperature, pressure) to move from one bistable extreme toward the other, the material’s shape-memory would accelerate the influx and outflow to and from the pores. An example of such a material is nanoporous gold, which has been shown to expand and contract in response to uptake of gases (Figure 19).1 Synthesis of materials for this type of reversible absorption, albeit with CO2, will enable us to test the efficacy of changes on the nanoscale and micron-scale. 64PDF Image | 2020 Carbon Capture
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