title: FY17-PDH-EVTest04 GodInput Impact of the Oxygen Defects1FY17-PDH-EVTest04 Reduction Rates of Stearic AcidFY17-PDH-T04.
abstract: Test New Article1 GodEarlyview.Publish-on-load testing.The role of the specific physicochemical properties of ZrO2phases on Ni/ZrO2has been explored with respect to the reduction of stearic acid. Conversion on pure m?ZrO2is 1.3 times more active than on t?ZrO2, whereas Ni/m?ZrO2is three times more active than Ni/t?ZrO2. Although the hydrodeoxygenation of stearic acid can be catalyzed solely by Ni, the synergistic interaction between Ni and the ZrO2support causes the variations in the reaction rates. Adsorption of the carboxylic acid group on an oxygen vacancy of ZrO2and the abstraction of the ??hydrogen atom with the elimination of the oxygen atom to produce a ketene is the key to enhance the overall rate. The hydrogenated intermediate 1?octadecanol is in turn decarbonylated to heptadecane with identical rates on all catalysts. Decarbonylation of 1?octadecanol is concluded to be limited by the competitive adsorption of reactants and intermediate. The substantially higher adsorption of propionic acid demonstrated by IR spectroscopy and the higher reactivity to O2exchange reactions with the more active catalyst indicate that the higher concentration of active oxygen defects on m?ZrO2compared to t?ZrO2causes the higher activity of Ni/m?ZrO2.
authors: Department of Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85747 Garching (Germany).
authors: Sebastian
authors: S
authors: Foraita
authors: Institute for Integrated Catalysis, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, WA 99352 (USA).
authors: John L
authors: JL
authors: Fulton
authors: Institute for Integrated Catalysis, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, WA 99352 (USA).
authors: Zizwe A
authors: ZA
authors: Chase
authors: Institute for Integrated Catalysis, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, WA 99352 (USA).
authors: Aleksei
authors: A
authors: Vjunov
authors: Department of Chemical Engineering and Materials Science, University of California, Davis, 1 Shields Avenue, Davis, CA 95616 (USA).
authors: Pinghong
authors: P
authors: Xu
authors: Department of Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85747 Garching (Germany).
authors: Eszter
authors: E
authors: Baráth
authors: Institute for Integrated Catalysis, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, WA 99352 (USA).
authors: Donald M
authors: DM
authors: Camaioni
authors: Department of Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85747 Garching (Germany).
authors: Chen
authors: C
authors: Zhao
authors: Department of Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstr. 4, 85747 Garching (Germany). johannes.lercher@ch.tum.de.|Institute for Integrated Catalysis, Pacific Northwest National Laboratory, 902 Battelle Boulevard, Richland, WA 99352 (USA). johannes.lercher@ch.tum.de.
authors: Johannes A
authors: JA
authors: Lercher
keywords: EDX?TEM; IR spectroscopy; XAFS; decarbonylation; hydrodeoxygenation; isotopes