کد مقاله | کد نشریه | سال انتشار | مقاله انگلیسی | نسخه تمام متن |
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62126 | 47622 | 2009 | 9 صفحه PDF | دانلود رایگان |

The efficient fixation/utilization of CO2 has been pursued by chemists for decades. In this work, the catalytic kinetics of CO2 fixation to methanol over a binary catalyst Cu/ZrO2 is investigated by first principles kinetic Monte Carlo simulation. A Cu/ZrO2 interface model is first established and the reaction network of CO2 hydrogenation is explored. In the Cu/ZrO2 system two reaction channels to methanol are identified (i) a reverse water–gas shift reaction via CO2 decomposition to CO and (ii) the well-regarded mechanism via a formate intermediate. The theoretical selectivity is determined to be 85% for methanol and 15% for CO. The removal of the oxidative species is kinetically slow. As a result, 87% of the interface sites are covered by these oxidative species, which oxidize the interface Cu. We show that the binding strength of O atom at the interface is a critical parameter determining the activity and selectivity of the catalyst.
DFT based kinetic Monte Carlo simulation of CO2 fixation to methanol over Cu/ZrO2 reveals that hydrolysis is a key step in producing methanol and that the interfacial Cu is partially oxidized during reaction.Figure optionsDownload high-quality image (125 K)Download as PowerPoint slide
Journal: Journal of Catalysis - Volume 263, Issue 1, 1 April 2009, Pages 114–122