Our team at the U.S. Naval Research Laboratory studies the effect on catalytic activity of wiring multiple transport and reactivity functionality into practical, not model, mesoscale architectures. We exploit sol–gel-derived aerogels as a hierarchical platform—structurally complex, but functionally simple in which the mesoporous network (for facile molecular flux to internal sites) is co-continuous with a covalently bonded nanoparticle network (that serves as a long-range electrical conduit). Such a platform offers the means to query how electronic, ionic, and molecular transport within the nanoarchitecture affects the elementary reaction steps that underlie catalytic efficacy. We focus on evaluating energy conversion–relevant catalytic oxidations at gold nanoparticle (Au NP)–modified oxide aerogels and copper nanoparticle (Cu NP)–modified oxide aerogels in the dark and under visible-illumination to stimulate the plasmonic character of the metal NPs. We show that the Au||TiO<sub>2</sub> interfacial design strongly impacts charge carrier (electron and proton) transport over mesoscale distances in catalytic guest–host architecture and affects the presence of electron paramagnetic resonance–visible oxygen vacancies in the oxide network. Hierarchical nanoarchitectures provide a tunable platform with which to develop comprehensive mechanistic understanding that will allow us to design next-generation catalytic architectures with superior performance.

Integrating catalysis-critical transport functions within nanoarchitectured platforms

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.