吕功煊.助剂K对二氧化碳加氢催化剂Cu-Fe-Zn催化活性的影响[J].分子催化,2015,(2):152-163
助剂K对二氧化碳加氢催化剂Cu-Fe-Zn催化活性的影响
The Adjustment of Product Distribution of CO2 Hydrogenation over Cu-Fe-Zn Catalyst while Maintaining its Activity via Potassium Addition
投稿时间:2015-04-09  修订日期:2015-04-17
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吕功煊* 中国科学院兰州化学物理研究所 gxlu@licp.cas.cn 
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中文摘要:
      本文用共沉淀法和浸渍法制备了一系列过渡金属复合物催化剂Kx/Cu-Fe-Zn,通过对催化剂进行了BET,H2-TPR,XRD,XPS,TEM等一系列物理化学性质的表征来探究了助剂K对催化剂的比表面积,还原行为,结构特性以及形貌等方面的影响。在固定床反应器上研究了碱金属助剂K的浸渍量以及温度对二氧化碳加氢反应的催化活性,稳定性以及对产物分布的影响。研究发现,当温度为350℃,助剂K的浸渍量为K0.1/Cu-Fe-Zn时,催化剂的催化活性达到最高,CO2的转化率可以达到68.7%,进一步增加催化剂中K的含量时,催化剂的催化活性出现缓慢下降趋势。研究还发现随着助剂K的浸渍量的增加,二氧化碳加氢反应中大分子量化合物增加,碳链增长,并且有大量高级醇和含氧化合物的形成。本文还讨论了在助剂K存在下催化剂上CO2加氢反应机理。
英文摘要:
      In this paper, the impact of potassium promoter on product distribution for CO2 hydrogenation over Cu-Fe-Zn catalyst was investigated. A series of transition metal Kx/Cu-Fe-Zn catalysts were prepared by a combination co-precipitation and impregnation method. The physiochemical characterizations of these catalysts were performed by BET, H2-TPR, XRD, TEM and XPS techniques to study the effect of potassium on the textural properties, reduction behaviour, structural and morphological change. The effects of addition of potassium promoter on CO2-conversion, product distribution and deactivation were study for CO2 hydrogenation in a fixed bed reactor. The maximum catalytic activity was obtained from K0.1/Cu-Fe-Zn catalyst and its catalytic activity decreased slightly thereafter. The CO2 conversion reached the highest value of 68.7% over K0.1/Cu-Fe-Zn at 350篊. In addition, the results revealed that addition of potassium promoter shifted selectivity to high molecular weight compounds and led to the formation of higher alcohols and oxygen containing compounds in the products. The possible mechanism in the presence of potassium was discussed.
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