Applied Surface Science ( IF 6.3 ) Pub Date : 2023-06-13 , DOI: 10.1016/j.apsusc.2023.157774
Jiaxin Li , Xiaoyu Niu , Yujun Zhu
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In the selective hydrogenation of furfural (FAL) to furfuryl alcohol (FOL), it is important to develop a simple and cheap non-precious metal catalyst to replace the precious metal catalyst. Therefore, CuxMg3AlOy (x = 0.3, 0.5, 0.7, 0.9, 1.1) composite metal oxide catalysts were prepared by CuMgAl-LDHs as precursor for the selective hydrogenation of FAL to FOL. In this series of catalysts, Cu0.9Mg3AlOy has the best catalytic activity, with 99% FAL conversion and 98.4% selectivity under the mild reaction conditions of 1.6 MPa H2 pressure, 1.5 h and 120 ℃, and good reusability. XRD, TEM, H2-TPR, CO2-TPD, XPS and in-situ DRIFTS characterization were used to investigate the activate species for hydrogenation reaction. It can be proved that Cu2+ and Cu+ on the surface of CuxMg3AlOy can be partially reduced to the Cu0 species in-situ during the reaction, promoting the hydrogenation of FAL. Various studies confirm that Cu0 is mainly responsible for the activation and dissociation of H2, and both Cu0 and Cu+ are used to adsorb the carbonyl group in FAL to improve the selectivity of FOL. Moreover, the appropriate amount of the Cu0 and Cu+ species plays an important role in selective hydrogenation of FAL to FOL through their synergy.
中文翻译:

表面 Cu0 和 Cu+ 物质对水滑石衍生的 CuxMg3Al 氧化物上糠醛选择性加氢至糠醇的协同作用
在糠醛(FAL)选择性加氢制糠醇(FOL)过程中,开发一种简单、廉价的非贵金属催化剂来替代贵金属催化剂具有重要意义。因此,以CuMgAl-LDHs为前驱体制备了Cu x Mg 3 AlO y (x = 0.3,0.5,0.7,0.9,1.1)复合金属氧化物催化剂,用于FAL选择性加氢制备FOL。该系列催化剂中,Cu 0.9 Mg 3 AlO y催化活性最好,在1.6 MPa H 2压力、1.5 h、120 ℃的温和反应条件下,FAL转化率为99%,选择性为98.4%,且重复使用性良好。XRD、TEM、H 2 -TPR、CO 2-TPD、XPS 和原位 DRIFTS 表征用于研究氢化反应的活化物质。证明Cu x Mg 3 AlO y表面的Cu 2+和Cu +在反应过程中可以部分原位还原为Cu 0物种,促进FAL的加氢。各种研究证实Cu 0主要负责H 2的活化和解离,Cu 0和Cu +均用于吸附FAL中的羰基以提高FOL的选择性。另外,适量的Cu 0和Cu +物种通过它们的协同作用在 FAL 选择性氢化为 FOL 中发挥着重要作用。