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The accessibility of deeply embedded adsorption sites depends on the macrostructure. Multimodal porous materials with a controlled macroporosity that incorporates mesoporosity and microporosity represent one strategy for achieving the maximum utilization of sorption sites at different length scales. Efficient carbon-capture systems hinge on the synergistic interplay of the hierarchical structures related to the three different length scales. Accordingly, hierarchical synthesis methodologies based on self-assembly are needed to generate capture sites and, ultimately, integrated sorption media.7 Nature has provided an ample number of examples of hierarchal materials that possess precision molecular recognition. The key synthesis strategy underlying the manufacturing of active sites in nature is the “key-and-lock” principle of templating synthesis and compartmentalization. In this context, various 0D, 1D, 2D, and 3D nanostructures can be envisioned for efficient target gas separation. As described previously, recent advances in the synthesis of complex materials, such as MOFs and mesoporous materials, have allowed pore sizes of solid sorbents to be more precisely controlled. Additional attention must be given to tailoring these pores for improved uptake and release of targeted molecules and ions. Further, entirely new classes of molecules are needed to expand the range of architectures that can be accessed. Beyond conventional materials with rigid structures like zeolites or standard activated carbons, the potential exists to identify new materials that use wholly new processes for controlled uptake and release of targeted gases. The understanding of those phenomena, as well as dimensional changes in porous or solid monolithic (e.g., polymer) structures caused by gas uptake or release, will allow the design of new materials with the required architectures. Such materials might incorporate switchable or flexible internal structures to accommodate large amounts of CO2 without a drastic change in the macroscopic size/shape, which usually leads to material degradation. For example, there is a rich opportunity to explore designer structures whose porosity might equal or exceed that of currently known porous materials [Figure 16(a)]. One fundamental question that must be answered is what is the best pore size and shape for the highest CO2 uptake. The answer will require reexamining our current understanding of CO2 sorption mechanisms as applied on the sub-nanoscale level and learning the limits of how far this phenomenon can be extended. The experimental results will have to be coupled with new modeling approaches that specifically consider the interaction of solids with CO2 and the properties (and eventually new ordered structures) of CO2 confined in nanoscale pores. Materials with monodisperse pore size distribution may be very important in future gas sorption schemes, be they oxide, carbon-based, organic, or otherwise. Unfortunately, the availability of such materials is currently limited. Today, high-surface-area activated carbons are prepared using a top-down approach employing chemical or physical activation, but this leads to random pore sizes and distributions. New synthesis routes, most likely incorporating a bottom-up strategy, are needed to achieve tailored-pore-size materials from a variety of materials families. Carbide-derived carbon materials offer a starting point for these studies [Figures 16(b) and 16(c)]. In these materials, the pore size is programmed through the carbide precursor structure and the surface chemistry is determined by the process conditions.6 59PDF Image | 2020 Carbon Capture
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