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首页> 外文期刊>Catalysis science & technology >Copper promoter effect on acid-base and redox sites of Fe/Al2O3 catalysts and their role in ethanol-acetone mixture conversion
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Copper promoter effect on acid-base and redox sites of Fe/Al2O3 catalysts and their role in ethanol-acetone mixture conversion

机译:铜启动子对酸碱的影响和氧化还原网站的Fe /氧化铝催化剂及其作用ethanol-acetone混合物转换

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Active species of copper and iron oxide (Cu-Fe) catalysts supported on alumina were prepared by combining Pechini and wet impregnation methods. The effect of combined acid-base and redox sites of Cu and Fe species on gas-phase ethanol-acetone mixture conversion was investigated. The catalysts were characterized by chemical analyses, XRD, H-2-TPR, Mssbauer spectroscopy, N-2 physisorption, CO2-TPD, SEM-EDS, TG/DTA and pyridine adsorption isotherms. N-2 adsorption/desorption isotherms and SEM-EDS analysis showed that the addition of copper caused an increase of BET surface area and Cu and Fe oxide dispersion. H-2-TPR characterization showed that interactions between Cu and Fe oxides shift the reducibility of Fe3+ species to lower temperature improving the redox properties of the catalyst. The partial reduction of the Cu and Fe oxide species was found to be efficient in inhibiting the side decomposition reactions, improving the catalytic efficiency towards dehydrogenation and hydrogen transfer processes. It was found that acid-base pairs play an important role in the formation of dehydrogenation, dehydration and condensation products from ethanol, while redox sites are decisive for hydrogen transfer reactions with reduction of acetone to isopropanol. H-2-TPR and Mssbauer spectroscopy results for the spent catalysts revealed that the highest catalytic performance of the Cu-FeAl catalysts may be attributed to the good dispersion of the Cu oxide and the site generated by the partial reduction which produces Cu+/Cu-0 and Fe2+ active species. A reaction pathway with the participation of the acid-base and redox sites in the formation of products by consecutive dehydrogenation-condensation or dehydrogenation-hydrogenation reactions has been proposed.
机译:铜和铁的氧化物的活性物种(Cu-Fe)催化剂支持氧化铝所准备的结合Pechini和湿化方法。酸碱和氧化还原网站相结合的效果在气相ethanol-acetone铜和铁物种混合转换进行了研究。催化剂在化学的特征分析、XRD、H-2-TPR Mssbauer光谱,n -物理吸附、CO2-TPD能谱、TG / DTA、吡啶吸附等温线。吸附/解吸等温线和能谱分析表明,添加铜导致增加了表面积和铜打赌铁氧化物分散。表明,铜和铁氧化物之间的相互作用Fe3 +物种的还原能力转移到低温度提高的氧化还原性质催化剂。氧化物种被发现效率抑制分解反应,提高催化效率脱氢和氢转移过程。发现酸碱对发挥形成的重要作用脱氢、脱水和冷凝从乙醇产品,而氧化还原网站决定性的氢转移反应减少异丙醇丙酮。Mssbauer光谱结果催化剂显示最高的催化Cu-FeAl催化剂的性能归功于良好的铜氧化物的色散和减少生成的网站部分生产铜+ / Cu-0和铁+活性物种。反应途径的参与酸碱和氧化还原网站的形成产品连续dehydrogenation-condensation或dehydrogenation-hydrogenation反应已经建议。

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