471562 Designing Cooperative Interactions to Tune Catalytic Activity and Selectivity for Biomass Conversion

Wednesday, November 16, 2016: 4:15 PM
Imperial B (Hilton San Francisco Union Square)
Nicholas Brunelli1, Nitish Deshpande2, Aamena Parulkar2, Frédéric Perras3 and Marek Pruski3, (1)Chemical & Biomolecular Engineeering, The Ohio State University, Columbus, OH, (2)Chemical and Biomolecular Engineering, The Ohio State University, Columbus, OH, (3)Iowa State University, Ames, IA

Catalytic sites incorporating multiple catalytic units can act cooperatively to achieve higher rates than isolated units. It remains an open question how to design these cooperative interactions. Specific design concepts can be gleaned from enzymes that contain multiple functional groups positioned in close proximity to provide tuned interactions with the substrates. The tuned interactions and precise spatial positioning enable the enzymes to achieve high catalytic rates and high selectivity. Understanding how to incorporate these design concepts into heterogeneous materials would improve catalyst performance.

Previously, we and others have focused on understanding the different aspects of how to tune interactions to achieve cooperative catalysis.[1–5] This work has primarily been for pharmaceutically relevant reactions such as the aldol, nitroaldol, and Knoevenagel reactions. In this presentation, we extend our synthetic approach to control catalytic activity and selectivity for directly relevant biomass production reactions that produce 5-hydroxymethylfurfural. We exploit different elements of cooperative interactions to create a novel design of the catalytic active site. These novel materials are synthesized, characterized, and tested in catalytic reactions. In particular, we utilize advanced spectroscopic techniques to demonstrate formation of the desirable catalytic site. The resulting materials achieve increased catalytic selectivity and activity for these reactions relative to current state-of-the-art materials. Overall, the increased yields and selectivities increase the potential to produce many important commodity chemicals in a sustainable manner.

References

[1] N.A. Brunelli, C.W. Jones, J. Catal. 308 (2013) 60.

[2] N.A. Brunelli, K. Venkatasubbaiah, C.W. Jones, Chem. Mater. 24 (2012) 2433.

[3] N.A. Brunelli, S.A. Didas, K. Venkatasubbaiah, C.W. Jones, J. Am. Chem. Soc. 134 (2012) 13950.

[4] R.K. Zeidan, M.E. Davis, J. Catal. 247 (2007) 379.

[5] J.D. Bass, A. Solovyov, A.J. Pascall, A. Katz, J. Am. Chem. Soc. 128 (2006) 3737.


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