With the intensifying global need for alternative energy and fuels, there is strong interest in the development of efficient catalysts that can drive the chemical conversion of renewable resources into useful products. One promising pathway is to catalytically convert synthesis gas (syngas, CO + H2) to oxygenates. We study the conversion of syngas to synthetic liquid fuels and high-value chemicals using supported metal, heterogeneous catalysts. Two different catalyst systems will be described. First, the promotion of rhodium-based catalysts, which have intrinsic selectivity towards desirable higher oxygenate production, is explored using metal oxides deposited by atomic layer deposition (ALD). In the case of Rh promoted by MoO3, we show that the promoted catalysts exhibit an increase in both activity and oxygenate selectivity relative to unpromoted Rh nanoparticles, and that this is the result of formation of a novel catalyst structure. The second system is cobalt-based catalysts. Recently, interest has risen in Co2C catalysts for oxygenate production. We will describe how introducing a ZnO promoting overlayer on Co/SiO2 by ALD significantly enhances oxygenate selectivity by enabling Co2C formation during syngas reaction. By exploring several different metal oxide supports, we will show that the composition of the support surface strongly controls whether ZnO-promoted Co can transform into the catalytically-selective Co2C. Synchrotron-based studies provide insight into the mechanisms by which the support and promoters change reactivity, while density functional theory (DFT) calculations reveal the reaction pathways on the ALD-modified catalyst surfaces. The outlook for atomic scale surface modification using ALD to synthesize and study catalytic materials will be discussed.

Using atomic-scale surface modification to understand support and promoter effects of syngas conversion catalysts

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.