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Ultrasmall Cluster Model for Investigating Single Atom Catalysis : Dehydrogenation of 1-Propanamine by Size-Selected Pt<sub>1</sub>Zr<sub>2</sub>O<sub>7</sub> Clusters Supported on HOPG

Ultrasmall Cluster Model for Investigating Single Atom Catalysis : Dehydrogenation of 1-Propanamine by Size-Selected Pt1Zr2O7 Clusters Supported on HOPG

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DENCHY, Michael A., Linjie WANG, Benjamin R. BILIK, Lucas HANSEN, Sandra ALBORNOZ, Francisco LIZANO, Nicolas BLANDO, Zachary HICKS, Gerd GANTEFÖR, Kit H. BOWEN, 2022. Ultrasmall Cluster Model for Investigating Single Atom Catalysis : Dehydrogenation of 1-Propanamine by Size-Selected Pt1Zr2O7 Clusters Supported on HOPG. In: The Journal of Physical Chemistry A. American Chemical Society (ACS). 126(42), pp. 7578-7590. ISSN 1089-5639. eISSN 1520-5215. Available under: doi: 10.1021/acs.jpca.2c03149

@article{Denchy2022-10-27Ultra-59119, title={Ultrasmall Cluster Model for Investigating Single Atom Catalysis : Dehydrogenation of 1-Propanamine by Size-Selected Pt1Zr2O7 Clusters Supported on HOPG}, year={2022}, doi={10.1021/acs.jpca.2c03149}, number={42}, volume={126}, issn={1089-5639}, journal={The Journal of Physical Chemistry A}, pages={7578--7590}, author={Denchy, Michael A. and Wang, Linjie and Bilik, Benjamin R. and Hansen, Lucas and Albornoz, Sandra and Lizano, Francisco and Blando, Nicolas and Hicks, Zachary and Ganteför, Gerd and Bowen, Kit H.} }

Lizano, Francisco Hansen, Lucas Denchy, Michael A. Bilik, Benjamin R. Lizano, Francisco Ganteför, Gerd Hicks, Zachary Wang, Linjie Blando, Nicolas Bowen, Kit H. Denchy, Michael A. Blando, Nicolas 2022-11-11T09:14:21Z Wang, Linjie Hicks, Zachary The selective dehydrogenation of hydrocarbons and their functionalized derivatives is a promising pathway in the realization of endothermic fuel systems for powering important technologies such as hypersonic aircraft. The recent surge in interest in single atom catalysts (SACs) over the past decade offers the opportunity to achieve the ultimate levels of selectivity through the subnanoscale design tailoring of novel catalysts. Experimental techniques capable of investigating the fundamental nature of the active sites of novel SACs in well-controlled model studies offer the chance to reveal promising insights. We report here an approach to accomplish this through the soft landing of mass-selected, ultrasmall metal oxide cluster ions, in which a single noble metal atom bound to a metal oxide moiety serves as a model SAC active site. This method allows the preparation of model catalysts in which monodispersed neutral SAC model active sites are decorated across an inert electrically conductive support at submonolayer surface coverage, in this case, Pt<sub>1</sub>Zr<sub>2</sub>O<sub>7</sub> clusters supported on highly oriented pyrolytic graphite (HOPG). The results contained herein show the characterization of the Pt<sub>1</sub>Zr<sub>2</sub>O<sub>7</sub>/HOPG model catalyst by X-ray photoelectron spectroscopy (XPS), along with an investigation of its reactivity toward the functionalized hydrocarbon molecule, 1-propanamine. Through temperature-programmed desorption/reaction (TPD/R) experiments it was shown that Pt<sub>1</sub>Zr<sub>2</sub>O<sub>7</sub>/HOPG decomposes 1-propanamine exclusively into propionitrile and H<sub>2</sub>, which desorb at 425 and 550 K, respectively. Conversely, clusters without the single platinum atom, that is, Zr<sub>2</sub>O<sub>7</sub>/HOPG, exhibited no reactivity toward 1-propanamine. Hence, the single platinum atom in Pt<sub>1</sub>Zr<sub>2</sub>O<sub>7</sub>/HOPG was found to play a critical role in the observed reactivity. Ganteför, Gerd eng 2022-11-11T09:14:21Z Bilik, Benjamin R. Ultrasmall Cluster Model for Investigating Single Atom Catalysis : Dehydrogenation of 1-Propanamine by Size-Selected Pt<sub>1</sub>Zr<sub>2</sub>O<sub>7</sub> Clusters Supported on HOPG Hansen, Lucas Albornoz, Sandra Bowen, Kit H. Albornoz, Sandra 2022-10-27

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