Steering of methanol reforming selectivity by zirconia-copper interaction

作者：Mayr Lukas; Kloetzer Bernhard; Zemlyanov Dmitry; Penner Simon^*

来源：Journal of Catalysis, 2015, 321: 123-132.

DOI：10.1016/j.jcat.2014.10.012

• In situ photoelectron spectroscopy
• High-resolution electron-energy-loss spectroscopy
• Methanol steam reforming
• Model catalysts

"Inverse" (ZrO2/ZrOxHy on Cu) and "real" (Cu nanoparticles on ZrO2) ultra-high-vacuum/ambient pressure model catalyst studies were performed using methanol steam reforming as a test reaction. The catalytic profile was correlated with structural and spectroscopic analysis using X-ray photoelectron and Auger electron spectroscopy and high-resolution electron-energy-loss spectroscopy. Access to water-activation-dependent pathways is achieved by special Cu/ZrOxHy phase boundary or interfacial sites formed during reaction, which were studied with respect to surface coverage, island size, and chemical state of Cu/Zr metal/oxide species. In the "real" model system, particle size effects increasing the amount of unwanted CO were observed beyond interfacial selectivity-steering effects. Oxidation of Zr-0 to Zr+4 during reaction forms the most efficient phase boundary with respect to redox-active sites. Ability for reversible hydroxylation of Zr and submonolayer Zr coverage for maximum ZrOxHy/Cu phase boundary dimensions are the most critical parameters in catalyst preparation.

• 出版日期2015-1