Green chemistry through the solid state: sky is the limit Tomislav Friscic University of Birmingham, UK
This presentation will outline our group’s recent advances in using solid-state reactivity for the development of cleaner, safer synthetic methodologies and materials designs. In particular, it will provide an overview of the emergence of mechanochemistry, i.e. chemical transformations induced by mechanical agitation such as grinding, milling, or extrusion, as a uniquely general solventless synthetic methodology that can also provide access to novel reactivity and molecules. [1] We will show how focusing on the mechanistic aspects of mechanochemical reactions, and in particular the use of methodologies for real-time and in situ monitoring of milling processes, [2] has led to advances in the fundamental understanding and design of metal-organic frameworks (MOFs). [3,4] Specifically, we will show how mechanistic investigations of mechanochemistry led to the discovery of new MOFs, enabled the emergence of a methodology for ab initio crystal structure prediction in this class of materials (MOF-CSP), and also provided the first simple guidelines to design MOFs with controllable stability, based on established or readily accessible descriptors such as Hammett’s constants. [5] Finally, we will show how our studies of MOF stability and energetics became a springboard for the development of a new type of tunable aerospace hypergolic fuels, which can provide a greener alternative for highly toxic and carcinogenic hydrazines. [6] References 1. Friščić et al. Angew. Chem. Int. Ed. 2020, 59, 1018; 2. Friščić et al. Nature Chem. 2013, 5, 66;
3. Akimbekov et al. J. Am. Chem. Soc. 2017, 139, 7952; 4. Arhangelskis et al. Chem. Mater. 2019, 31, 3777; 5. Novendra et al. J. Am. Chem. Soc. 2020, 142, 21720; 6. Titi et al. Sci. Adv. 2019, 5, eaav9044.
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