Hydrogenation Performance of Acetophenone to 1-Phenylethanol on Highly Active Nano Cu/SiO2 Catalyst
Hydrogenation Performance of Acetophenone to 1-Phenylethanol on Highly Active Nano Cu/SiO2 Catalyst
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DOI：
10.1007/s10562-019-02908-2
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发表时间：
2020-01
影响因子：
2.8
通讯作者：
B. Wang;Manman Jin;Hao An;Zhenmei Guo;Z. Lv
中科院分区：
文献类型：
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作者：
B. Wang;Manman Jin;Hao An;Zhenmei Guo;Z. Lv
本文采用尿素均相沉淀法制备了不同铜含量的高活性纳米铜/二氧化硅催化剂。用氮气吸附、X射线衍射仪、氢-TPR、XPS和透射电子显微镜对催化剂进行了表征。结果表明，当铜含量为25wt%时，纳米铜/二氧化硅催化剂对苯乙酮(AP)选择加氢制1-苯乙醇(Phe)表现出良好的催化性能。该催化剂具有铜物种分散性好、粒径小、比表面积高(约540×m~2/g)和丰富的孔结构。讨论了不同反应条件对加氢过程的影响。在最佳反应条件下(温度353K，压力2.0Mpa，空速1.0h−1，H2/AP摩尔比15)，AP转化率和Phe选择性分别达到99.8%和99.08%。此外，该催化剂在500h的运行时间内仍保持了较高的催化性能。Cu+和CuO之间的协同作用提高了催化剂的活性和稳定性。研究表明，该催化剂具有广阔的工业前景。图形摘要：该催化剂对AP加氢具有良好的催化性能。还原后的Cu/SiO_2催化剂中同时含有Cu~+和CuO，与XPS结果一致。Cu2+稳定甲氧基和酰基物种，CuO促进H2分解。AP和Cu中的苯对苯酚具有静电斥力，有利于Phe的解吸。
AbstractIn this work, highly active nano Cu/SiO2catalysts with various copper content were prepared by urea homogeneous precipitation method. The catalysts were characterized by N2adsorption, XRD, H2-TPR, XPS and TEM. It was found that the nano Cu/SiO2catalyst displayed excellent catalytic performance for the selective hydrogenation of acetophenone (AP) to 1-phenylethanol (PhE) when copper content was 25 wt%. The Cu/SiO2catalyst had well dispersed copper species, small particle size, high BET surface area (ca. 540 m2/g) and abundant pore structure. The influence of different reaction conditions on the hydrogenation process were also discussed. AP conversion and the PhE selectivity reached 99.8% and 99.08%, respectively, under the optimal reaction conditions (Temperature: 353 K; Pressure: 2.0 MPa, LHSV: 1.0 h−1and the molar ratio of H2/AP:15). Besides, the above catalyst maintained a high catalytic performance in the duration of 500 h operation. The synergistic effect between Cu+and Cu0improved the activity and stability of Cu/SiO2catalyst. The research indicated that the catalyst had a wide industrial prospect.Graphic AbstractThe Cu/SiO2catalyst showed a good performance for AP hydrogenation. The reduced Cu/SiO2catalyst contains both Cu+and Cu0consistent with XPS. Cu+sties stabilize the methoxy and acyl species and Cu0facilitates the decomposition of H2. Phenyl in AP and Cu had electrostatic repulsion, which was favorable for desorption of PhE.