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DESIGN, SYNTHESIS, AND ASSEMBLY OF NOVEL MATERIAL ARCHITECTURES Abstract To meet the challenge of lowering carbon emissions from combustion processes, new sorbent materials are needed with specifically designed structures that allow them to selectively bind a targeted gas from a complex mixture and release it in a controlled fashion when triggered by external stimuli. Currently, there is a lack of fundamental understanding of gas uptake and release on the nanoscale, which has led to an Edisonian approach to material selection and optimization for gas separations. This lack of understanding continues to hamper the design and development of alternative solid sorbents with improved capacity and lower energy consumption in the sorption/desorption cycle. Armed with this knowledge however, it should be possible to discover and design new material architectures tailored on multiple length scales (molecular, nanoscale, mesoscale, and macroscopic) and incorporating multiple functional domains to further enhance performance. Achieving this goal will require strongly coordinated multiscale modeling, analytical characterization, and synthesis and assembly techniques to achieve new materials with controlled pore structures, tailored pore surface texture and functionality, and nanoscale architecture, all of which will be required for future carbon capture technologies. Background and Motivation Solid sorbents currently used for gas capture include zeolites, activated carbons, calcium oxide, and alkaline and alkaline-earth hydrotalcites.1 More recently, additional materials—including amine-enriched solids, metal-organic-frameworks (MOFs), lithium zirconates, and other natural and synthetic materials—have been explored as potential gas capture materials (Figure 15). Some MOFs have been shown to possess well-defined pore structures and surface areas in excess of 3000 m2/gm and have demonstrated impressive gravimetric uptake.2 However, no material available to date is able to satisfy all the requirements of future carbon capture processes. Furthermore, most of the studies on these materials were done using trial- and-error tests (e.g., testing dozens of commercially available activated carbons). This Edisonian approach cannot provide greatly needed guidance on how to design better solid sorbents; only a fundamental understanding of the sorption mechanisms that occur at the atomic and molecular level will provide the basis for the development of next-generation sorption materials. With this understanding, new strategies for formulating optimized architectures and functionalities can be translated into revolutionary new materials for improved gas uptake and release. Science Research Directions Understanding of the physical and chemical parameters governing solid sorption is a prerequisite for increasing the volumetric and gravimetric uptake of CO2 and other targeted gases associated with carbon emission mitigation. This insight will enable new sorption, transport, and desorption mechanisms that will dramatically increase carbon capture schemes. In designing new sorption materials, one must consider the use of larger pores (tens of nanometers) to facilitate fast transport and gas/surface interactions, and even perhaps tunable nanopores to facilitate both uptake and release of targeted gases. Therefore, research must be directed toward understanding multiple sorption mechanisms that occur at the atomic and molecular level. Once these processes are understood, using new characterization techniques combined with computational modeling, the challenge will lie in the synthesis of these new materials. 57PDF Image | 2020 Carbon Capture
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