NiCu single atom alloys catalyze the C H bond activation in the selective non- oxidative ethanol dehydrogenation reaction

By Junjun Shan, Jilei Liu, Mengwei Li, Sylvia Lustig, Sungsik Lee, M. Flytzani-Stephanopoulos. Applied Catalysis B: Environmental, 2018

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Abstract NiCu single atom alloy (SAA) nanoparticles supported on silica are reported to catalyze the non-oxidative dehydrogenation of ethanol, selectively to acetaldehyde and hydrogen products by facilitating the C H bond cleavage. The activity and selectivity of the NiCu SAA catalysts were compared to monometallic copper and to PtCu and PdCu single atom alloys, in a flow reactor at moderate temperatures. In-situ DRIFTS showed that the silica support facilitates the O H bond cleavage of ethanol to form ethoxy intermediates over all the supported alloy catalysts. However, these remain unreactive up to 250 °C for the Cu/SiO2 monometallic nanoparticles, while in the NiCu SAA, acetaldehyde is formed at much lower temperatures, below 150 °C. In situ DRIFTS was also used to identify the C H activation step as the rate determining step of this reaction on all the copper catalysts we examined. The presence of atomically dispersed Ni in Cu significantly lowers the C H bond activation barrier, whereas Pt and Pd atoms were found less effective. This work provides direct evidence that the C H bond cleavage is the rate determining step in ethanol dehydrogenation over this type catalyst.

Subfields: Catalysis, Materials Chemistry, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/e0c8efb1f420588393d32ea6f1202083f4f8de2b