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Effect of the nature of copper species on methanol synthesis from CO2 hydrogenation reaction over CuO/Ce0.4Zr0.6O2 catalyst
Molecular Catalysis ( IF 3.9 ) Pub Date : 2020-07-07 , DOI: 10.1016/j.mcat.2020.111105
Weiwei Wang , Zhenping Qu , Lixin Song , Qiang Fu

A series of x wt.% CuO/Ce0.4Zr0.6O2 (x = 2, 5, 15, 25, 35 and 40) catalysts obtained by oxalate co-precipitation method are characterized by XRD, BET, SEM, Raman, EPR, H2-TPR, CO2/H2-TPD and high pressure (3 MPa) in situ DRITFS techniques in order to elucidate the effect of CuO loading on the catalytic activity of CO2 hydrogenation to methanol. Catalytic activity results demonstrate that CO2 conversion and methanol selectivity enhance with an increase of the CuO loading until it reaches the maximum values at a CuO loading of 35 wt.%, while further addition of CuO inhibits the catalytic performance. The higher CO2 conversion of 7.0 % (13.2 %) and methanol selectivity of 96.4 % (71.8 %) are obtained over 35 wt.% CuO/Ce0.4Zr0.6O2 catalyst at 220 °C (280 °C) and 3 MPa. The excellent performance of 35 wt.% CuO/Ce0.4Zr0.6O2 is attributed to the presence of adequate copper species with higher copper surface area and larger number of Cu-Ce-Zr solid solution. These two features are benefit to provide larger number of activated hydrogen atom and promote CO2 adsorption, respectively, which are the key to the hydrogenation reaction related to the hydrogen dissociation and the activation of the carbon dioxide.



中文翻译:

铜的性质对CuO / Ce 0.4 Zr 0.6 O 2催化剂上CO 2加氢反应合成甲醇的影响

通过XRD,BET,SEM,Raman,EPR对通过草酸盐共沉淀法获得的一系列x wt。%CuO / Ce 0.4 Zr 0.6 O 2(x = 2、5、15、25、35和40)催化剂进行了表征,H 2 -TPR,CO 2 / H 2 -TPD和高压(3 MPa)原位DRITFS技术,以阐明CuO负载量对CO 2加氢制甲醇的催化活性的影响。催化活性结果表明,CO 2随着CuO负载量的增加,转化率和甲醇选择性增强,直到在35wt。%的CuO负载量下达到最大值,而进一步添加CuO会抑制催化性能。在220°C(280°C)和3 MPa的压力下,在35 wt。%CuO / Ce 0.4 Zr 0.6 O 2催化剂上可获得7.0%(13.2%)的更高的CO 2转化率和96.4%(71.8%)的甲醇选择性。35 wt。%CuO / Ce 0.4 Zr 0.6 O 2的卓越性能这归因于存在具有较高铜表面积和大量Cu-Ce-Zr固溶体的适当铜物种。这两个特征分别有利于提供更多的活化氢原子并促进CO 2吸附,这是与氢离解和二氧化碳活化有关的氢化反应的关键。

更新日期:2020-07-07
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