Tandem catalysis is a process that combines two or more catalysts in a one-pot system that are then used in succession to create a single product. Synthetic tandem systems are of great interest because of their ability to reduce potentially environmentally damaging chemical and material waste, time, and cost while also having the potential to increase activity, selectivity, and durability of many catalytic systems. However, challenges remain in finding a system that supports multiple catalysts in a single pot under mild reaction conditions especially when introducing orthogonal reactions to a single solution.<br/>Herein, tandem systems supported on mesoporous silica nanoparticles (MSNs) is used for the oxidative esterification of an alcohol to form its corresponding ester. The catalytic scaffolds have been designed with Au nanoparticle catalysts embedded into the pore walls of the MSN and palladium (Pd) nanoparticles attached to the functionalized surface of the MSN. By supporting both catalysts on high surface area MSN, stability is increased, less catalyst can be used, and mild reaction conditions are favored. Post synthesis treatments of Au-supported MSN with carbon is also under investigation to extend the lifetime of the catalysts with limiting the negative effects on turn-over number. The ultimate goal of this study is to develop a tandem catalytic system using Au nanoparticles and enzymes for a two-step tandem reaction with cofactor regeneration. This will also be introduced with the enzyme alcohol dehydrogenase (ADH) substituting the Pd nanoparticles on the functionalized surface of the scaffold. In order to increase the recyclability of this system, an <i>in situ</i> cofactor regeneration is under investigation for the ADH catalyzed oxidation.

Oxidative esterification using a tandem catalytic system supported on mesoporous silica nanoparticles

ACS Spring Meeting 2021

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