In Situ Spectroscopic Characterization of Ni1–xZnx/ZnO Catalysts and Their Selectivity for Acetylene Semihydrogenation in Excess Ethylene

Autor: Robert M. Rioux, Richard S. Sim, Bernd Kabius, Nicholas P. Sturgis, Charles S. Spanjers
Rok vydání: 2015
Předmět:
Zdroj: ACS Catalysis. 5:3304-3315
ISSN: 2155-5435
DOI: 10.1021/acscatal.5b00627
Popis: The structures of ZnO-supported Ni catalysts were explored with in situ X-ray absorption spectroscopy, temperature-programmed reduction, X-ray diffraction, high-resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy, and electron energy loss spectroscopy. Calcination of nickel nitrate on a nanoparticulate ZnO support at 450 °C results in the formation of Zn-doped NiO (ca. Ni0.85Zn0.15O) nanoparticles with the rock salt crystal structure. Subsequent in situ reduction monitored by X-ray absorption near-edge structure (XANES) at the Ni K edge reveals a direct transformation of the Zn-doped NiO nanoparticles to a face-centered cubic alloy, Ni1–xZnx, at ∼400 °C with x increasing with increasing temperature. Both in situ XANES and ex situ HRTEM provide evidence for intermetallic β1-NiZn formation at ∼550 °C. In comparison to a Ni/SiO2 catalyst, Ni/ZnO necessitates a higher temperature for the reduction of NiII to Ni0, which highlights the strong interaction between Ni and...
Databáze: OpenAIRE