کد مقاله | کد نشریه | سال انتشار | مقاله انگلیسی | نسخه تمام متن |
---|---|---|---|---|
60932 | 47554 | 2015 | 10 صفحه PDF | دانلود رایگان |
• Water activation-dependent pathways for methanol steam reforming on ZrOxHy/Cu phase boundary sites.
• Access to full dehydrogenation/total oxidation on Cu/ZrO2 systems by special phase boundary sites.
• CO2 selectivity in methanol steam reforming can be steered by avoiding this type of phase boundary.
• Oxidation of Zr during reaction forms the most active phase boundary regarding redox-active sites.
• Reversible hydroxylation of Zr and a submonolayer Zr coverage are the most critical parameters.
“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 Zr0 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.
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Journal: Journal of Catalysis - Volume 321, January 2015, Pages 123–132