Critical challenges in zeolite synthesis stem from a limited ability to tune the physicochemical properties of crystals a priori and the phenomenological understanding of synthesis parameter influence on crystal growth. Given the widespread use of zeolites as industrial catalysts for many chemical/petrochemical processes and their promise for emerging applications, it is desirable to develop efficient, facile, and economical methods to systematically engineer zeolites with tailored properties. Moreover, fundamental studies that provide molecular-level knowledge of the underlying mechanism(s) of zeolite crystallization can be instrumental in the design of materials with a broad spectrum of properties, thereby establishing the basis for performing systematic studies of catalyst structure-performance relationships. Here, we will discuss the complex mechanisms of zeolite crystallization1,2 and describe new approaches to systematically alter the chemical composition (i.e., Si/Al ratio) of zeolite catalysts via commercially-relevant synthetic routes.3,4 We will also discuss a versatile method to control crystal size, morphology, and surface architecture/acidity.5–8 These methods predominantly rely on the action of crystal growth modifiers, which are molecules (or macromolecules) that possess an affinity for binding to specific crystal faces and alter the anisotropic growth rates of zeolites (with concomitant effects on crystal habit). Using a variety of zeolite framework types with tailored physicochemical properties, we will present the results of catalytic tests that seek to quantify the relationships between catalyst properties (e.g., size, morphology, composition) and their performance in reactions to convert hydrocarbons into chemicals and fuels. References: 1. De Yoreo, J.J. et al., Science 349 (2015) aaa6760-1/9 2. Lupulescu, A.I. and Rimer, J.D., Science 344 (2014) 729-732 3. Conato, M.T., Oleksiak, M.D., McGrail, B.P., Motkuri, R.K., Rimer, J.D. Chem. Commun. 51 (2015) 269-272 4. Maldonado, M., Oleksiak, M.D., Chinta, S., Rimer, J.D., J. Am. Chem. Soc. 135 (2013) 2641-2652 5. Lupulescu, A.I. and Rimer, J.D., Angew. Chem. Int. Ed. 51 (2012) 3345-3349 6. Lupulescu, A.I., Kumar, M., Rimer, J.D., J. Am. Chem. Soc. 135 (2013) 6608-6617 7. Kumar, M., Luo, H., Román-Leshkov, Y., Rimer, J.D., J. Am. Chem. Soc. 137 (2015) 13007-13017 8. Ghorbanpour, A., Gumidyala, A., Grabow, L.C., Crossley, S.P., Rimer, J.D., ACS Nano 9 (2015) 4006-4016

Advanced synthesis methods and structure-performance relationships in zeolite catalysis

251st National Meeting (2016)

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