摘要
本文使用水热-浸渍的方法合成Cu-Fe/ZrO_(2)催化剂,并用于草酸二甲酯加氢制备乙醇的反应中。研究结果表明,在Fe/ZrO_(2)催化剂中掺杂少量的助剂铜能显著提高草酸二甲酯加氢制乙醇的催化性能。Cu掺杂量1.5 wt%的1.5%Cu-Fe/ZrO_(2)催化剂催化性能最佳,在270℃,2 MPa时,草酸二甲酯转化率100%,乙醇选择性95.7%。通过XRD,XPS,TPR,BET,TEM等表征发现,Cu与Fe之间不仅存在强烈的电子相互作用,而且铜掺杂有效提高了活性组分Fe的分散度。此外,Cu掺杂引起的氢溢流效应提高了催化剂对氢气的解离活化能力,从而增强了草酸二甲酯的加氢程度,提高了乙醇的选择性。研究也发现过量Cu的掺杂会促使Cu颗粒发生团聚,导致催化剂的加氢性能降低。
In this paper, Cu-Fe/ZrO_(2)Catalyst was synthesized by hydrothermal-impregnation method to use in the hydrogenation of dimethyl oxalate to ethanol. The results show that doping a small amount of copper into Fe/ZrO_(2)Catalyst can significantly improve the catalytic performance of dimethyl oxalate hydrogenation to ethanol. The catalytic performance of 1.5% Cu-Fe/ZrO_(2)Catalyst with 1.5 wt% Cu doping is the best. With 270 ℃, 2 MPa, the conversion of dimethyl oxalate is 100% and the selectivity of ethanol is 95.7%. Through XRD, XPS, TPR, BET, TEM and other characterizations, it is found that there is not only a strong electronic interaction between Cu and Fe, but also copper doping effectively promotes the dispersion of active component Fe. In addition, the hydrogen spillover caused by Cu doping improves the dissociation and activation ability of the catalyst for hydrogen, so as to enhance the hydrogenation degree of dimethyl oxalate and improve the selectivity of ethanol. It is also found that excessive Cu doping will promote the agglomeration of Cu particles and reduce the hydrogenation performance of the catalyst.
作者
薛浩东
王雪
秦思乾
张传彩
代斌
XUE Haodong;WANG Xue;QIN Siqian;ZHANG Chuancai;DAI Bin(School of Chemistry and Chemical Engineering,Shihezi University,Shihezi,Xinjiang 832003,China)
出处
《石河子大学学报（自然科学版）》
CAS
北大核心
2022年第3期265-271,共7页
Journal of Shihezi University(Natural Science)
基金
国家自然科学基金项目(21666033)。
关键词
草酸二甲酯
乙醇
氧空位
氢溢流
Fe基催化剂
dimethyl oxalate
ethanol
oxygen vacancy
hydrogen spillover
Fe based catalyst
