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solids combine well-defined coordination environments surrounding metal centers with bridging organic ligands. The wide range of metals and ligands that can be incorporated in these structures can yield an enormous variety of porous structures.10 The MOFs and ZIFs can separate targeted gases by physisorption or by chemisorption. For example, in a MOF it is possible to bind CO2 in one of at least three ways, which provide progressively stronger binding energy and therefore require more heat to remove the CO2: (1) physisorption onto the internal surface, (2) adsorption onto open metal sites within the backbone of the MOF structure where CO2 binds directly to the metal centers through the oxygen atom, and (3) functionalizing the organic links with amine groups that bind CO2 by chemisorption through the formation of carbamates.11,12 For the latter approach, an energy penalty is associated with the desorption of the CO2, similar to that observed in aqueous amine solutions. Nevertheless, solid sorbents could offer significant advantages over conventional amine-based liquid stripping techniques if the net energy for uptake and release could be optimized and the materials were sufficiently stable upon cycling.13,14 For example, grafting the amine functionalities onto the solids eliminates the energy penalty associated with heating the water, although breaking the covalent bonds between CO2 and the amine groups still requires significant energy.15,16 This problem would be solved if CO2 release could be coupled to an exothermic structural transformation of the MOF or ZIF framework that would compensate for the endothermic CO2 desorption. Here, the use of flexible MOFs, whose structures expand and contract upon CO2 binding and release, may provide an overall thermoneutral process. Because of the large number of possible compositions and structures, there is considerable research potential in the exploration of MOF and ZIF structures and in their evaluation with respect to CO2 uptake and release. There have been recent reports of nonporous sorbents demonstrating improved gas sorption and release. Although the thermochemical behavior of zirconates was studied much earlier,1 the relevence of these systems for high-temperature CO2 capture was only recently appreciated.2 Lithium zirconate (Li2ZrO3) is a particularly promising candidate for CO2 separation at the high temperatures experienced in a precombustion type of reactor.3,4 Although it has been shown that pure Li2ZrO3 absorbs a large quantity of CO2 at high temperatures with a relatively slow sorption rate, addition of potassium carbonate and lithium carbonate was observed to improve the CO2 sorption rate.5 In addition to the compositional tuning and exploration of additives, the strategy of grain size engineering appears to provide significant benefits. For example, nanocrystalline zirconates offer markedly enhanced kinetics6 and point to improvements in total capacity with increased surface adsorption. Understanding the effects of physical and chemical phenomena at the nanoscale may provide important new opportunities to design materials with the composition and grain size for carbon capture applications. Figure 4. Model nanoporous oxygen carriers. Figure 4 displays a model oxygen carrier assembled from two complementary sizes of iron oxide particles that can cycle reversibly between hematite (Fe2O3 and magnetite (Fe3O4). On the left is the result of the reducing cycle, which in the panel on the right has been oxidized on exposure to air. This sample was prepared 21PDF Image | 2020 Carbon Capture
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