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the discovery of carbon capture materials that efficiently separate CO2 at the levels necessary beyond 2020. Protein receptors and enzymes are valued for their abilities to effectively bind substrates, stabilize reactive intermediates or high-energy conformations, and catalyze chemical transformations. Chemists have attempted to develop molecules with these same attributes, but the identification of host structures capable of recognizing a specific guest remains a grand challenge. This challenge can be addressed with a computer-aided design approach in which molecular fragments are assembled to generate candidate Inverse Design of Capture Molecules structures and a variety of computational models are used to rank them. The ability to design chemical structures with predetermined functionality is the key to finding new materials for energy and other new technologies. A particular challenge is developing separation agents for the selective removal of components in complex mixtures, such as those found in carbon capture schemes. The power of using a computational approach to guide experiment was recently demonstrated in the design of a self-assembled cage that binds sulfate with remarkable affinity (right). It is notoriously difficult to remove hydrophilic anions like sulfate from aqueous solutions. Molecular modeling showed that six urea molecules could hydrogen-bond to sulfate, yielding a complex with tetrahedral symmetry. It was reasoned that a self-assembled cage could adopt this arrangement if each urea molecule were the edge of a tetrahedron held together by nickel tris-bipyridine vertices. Starting with this as a basis for the design, the challenge was to identify linkages between the urea and bipyridine groups to generate molecular components that would favor the desired arrangement. This was done using computer-aided molecular design methods in which more than a quarter million possible linkages were evaluated within minutes. After further evaluation with molecular dynamics calculations, a small list of promising candidates was generated. One of these “designer” cage components was synthesized and, when mixed with nickel sulfate, yielded the predicted tetrahedral cage. This result represents the first time that guest binding within the cavity of a self-assembled cage was predetermined. The precise positioning of the binding sites within the cage resulted in a very strong receptor for aqueous sulfate, on a par with sulfate-binding protein. Source: R. Custelcean, J. Bosano, P. V. Bonnesen, V. Kertesz, and B. P. Hay, “Computer-aided design of a sulfate-encapsulating receptor,” Angew. Chem. Int. Ed. 48, 4025–4029 (2009). 102PDF Image | 2020 Carbon Capture
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