Synthesis gas (CO + H<sub>2</sub>) conversion is a promising route to converting coal, natural gas, or biomass into synthetic liquid fuels. An effective commercial catalyst for this process has not yet been developed due to the many side reactions that shift selectivity away from the desired products. Experimental and computational studies have shown that rhodium-based catalysts have intrinsic selectivity towards higher oxygenate production, and that the performance can be improved through the addition of metal oxide promoters. However, the interactions between rhodium, the promoter, and adsorbed reaction intermediates are not well understood. In this work, we investigate the intrinsic reactivity and the structure sensitivity of Rh for syngas conversion. We also explore the interactions between promoters and the catalyst. To study the physical and chemical interactions between catalyst materials and reaction intermediates, it is desirable to use method in which the catalyst structure can be controlled at the atomic-level. Atomic layer deposition (ALD) has emerged as a technique for atomic scale catalyst design. In this work, Rh nanoparticles promoted by various metal oxides deposited by ALD were tested in the conversion of syngas to higher oxygenates. The interactions between catalyst and promoter were studied by x-ray photoelectron spectroscopy, temperature programmed reduction, and CO chemisorption experiments. The promoted catalysts show an increase in activity and higher oxygenate selectivity relative to unpromoted Rh nanoparticles.<br/>

Modifying catalysts using atomic layer deposition

253rd National Meeting (2017)

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