Boosting Hydrogen Production from Methanol and Water by in situ Activation of Bimetallic Cu−Zr Species. Issue 10 (29th April 2016)

• Record Type: Journal Article
• Authors: Mayr, Lukas; Klötzer, Bernhard; Schmidmair, Daniela; Köpfle, Norbert; Bernardi, Johannes; Schwarz, Sabine; Armbrüster, Marc; Penner, Simon
• Is Part Of: ChemCatChem. Volume 8:Issue 10(2016)
• Page Start: 1778
• Page End: 1781
• Publication Date: 2016-04-29
• Subjects: copper -- hydrogen -- methanol steam reforming -- water activation -- zirconium; Catalysis -- Periodicals; 541.39505
• DOI: 10.1002/cctc.201600361
• Languages: English
• ISSNs: 1867-3880

Abstract

Abstract: A bimetallic Cu/Cu51 Zr14 precatalyst, activated in situ, for hydrogen generation from methanol and water provides very high CO2 selectivity (>99.9 %) and high H2 yields. Referenced to the geometric surface area of our model surface, higher activity of at least one order of magnitude was observed in comparison to supported Cu/ZrO2 and Cu/ZnO/ZrO2 catalysts. Evolution of structural activation monitored by X‐ray diffraction (XRD), X‐ray photoelectron spectroscopy (XPS), and electron microscopy indicates transformation of the bimetallic Cu/Cu51 Zr14 precatalyst into an active, selective, and self‐stabilizing state with coexistence of dispersed Cu and partially hydroxylated tetragonal ZrO2 . The outstanding performance is assigned to the presence of a high interface‐site concentration following in situ decomposition of the intermetallic compound. These active sites result from the cooperation of Cu, responsible for methanol activation, and tetragonal ZrO2, which activates the water by surface hydroxylation. Abstract : In situ activation : A Cu/Cu51 Zr14 precatalyst, activated in situ, for methanol steam reforming is prepared, and displays an extremely high CO2 selectivity of >99.9 % and an excellent H2 yield. The fully activated catalyst is self‐stabilizing and shows enhancement of the specific activity by at least one order of magnitude compared to supported Cu/Zn catalysts owing to the in situ formed coexistence of disperse Cu and partially hydroxylated tetragonal ZrO2 at the surface.