【摘 要】
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A series of Ag-ZrO2/SiO2 catalysts with different metal-support interfaces were synthesized in an effort to elucidate the roles of specific interfaces in contro
【机 构】
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The Gene and Linda Voiland School of Chemical Engineering and Bioengineering,Washington State Univer
论文部分内容阅读
A series of Ag-ZrO2/SiO2 catalysts with different metal-support interfaces were synthesized in an effort to elucidate the roles of specific interfaces in controlling the ethanol to 1,3-butadiene conversion and selectivity.According to the results of detailed characterizations(e.g.CO/pyridine-DRIFTS,XPS,TEM,NH3-TPD,and 1H MAS NMR),it was found that the Ag-O-Si interfaces significantly enhanced the dehy-drogenation of ethanol while the presence of ZrO2 improved the interaction between Ag and ZrO2/SiO2,creating more Agδ+active sites.The high dispersion of ZrO2 on SiO2 generated abundant Zr-O-Si inter-faces with medium and weak Lewis acidity,promoting the condensation of acetaldehyde to crotonalde-hyde.These Zr-O-Si interfaces in close interaction with Agδ+species played a critical role in the enhanced H transfer during the MPV reduction of crotonaldehyde to crotyl alcohol.The synergies among the inter-faces resulted in retarded ethanol dehydration reactivity,balanced ethanol dehydrogenation and conden-sation reactions,and a subsequent high 1,3-butadiene yield.
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