水滑石基 MMgAlOx(M=铜、镍和钴)复合材料上的金纳米颗粒:掺杂剂对 C2H2 半氢化催化活性的影响

Catalysts Pub Date : 2024-05-10 DOI:10.3390/catal14050315
Xun Sun, Wenrui Lv, Yanan Cheng, H. Su, Libo Sun, Lijun Zhao, Zifan Wang, C. Qi
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引用次数: 0

摘要

在金属氧化物支撑的金纳米粒子上将乙炔半氢化为乙烯是一个有趣的课题。在此,通过引入具有独特性质的不同铜、镍和钴掺杂剂,开发了一种基于水滑石的 MMgAlOx(M=Cu、Ni 和 Co)复合氧化物,然后将其用作载体,通过改进的沉积沉淀法获得了 Au/MMgAlOx 催化剂。采用 XRD、BET、ICP-OES、TEM、拉曼、XPS 和 TPD 等方法研究了这些催化剂的物理化学性质以及乙炔半加氢制乙烯的催化性能。总体而言,铜改性 Au/CuMgAlOx 催化剂的催化活性高于其他改性催化剂。Au/CuMgAlOx 的 TOR 为 0.0598 h-1,是 Au/MgAl2O4 的 30 倍。扫描电子显微镜和 XRD 结果表明,引入掺杂剂后,催化剂的结构和形貌没有明显差异。TEM 研究证实,这些掺杂剂对金的粒径有不利影响。因此,所获得的 Au/MMgAlOx 催化剂中 M 掺杂剂对催化性能的影响得到了改善。拉曼、NH3-TPD 和 CO2-TPD 的结果证实,Au/CuMgAlOx 催化剂具有更多的碱性位点,这有利于减少反应后催化剂表面的结焦。XPS 分析表明,金纳米颗粒在 CuMgAlOx 的边缘和表面呈现部分氧化状态。除了 Au/CuMgAlOx 催化剂上碱性位点的比例增加外,纳米金向掺铜基质载体的电荷转移可能在乙炔的选择性氢化过程中发挥了积极作用。此外,还讨论了 Au/CuMgAlOx 催化剂的稳定性和失活问题,并提出了一种可能的反应机制。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Au Nanoparticles Supported on Hydrotalcite-Based MMgAlOx (M=Cu, Ni, and Co) Composite: Influence of Dopants on the Catalytic Activity for Semi-Hydrogenation of C2H2
Semi-hydrogenation of acetylene to ethylene over metal oxide-supported Au nanoparticles is an interesting topic. Here, a hydrotalcite-based MMgAlOx (M=Cu, Ni, and Co) composite oxide was exploited by introducing different Cu, Ni, and Co dopants with unique properties, and then used as support to obtain Au/MMgAlOx catalysts via a modified deposition–precipitation method. XRD, BET, ICP-OES, TEM, Raman, XPS, and TPD were employed to investigate their physic-chemical properties and catalytic performances for the semi-hydrogenation of acetylene to ethylene. Generally, the catalytic activity of the Cu-modified Au/CuMgAlOx catalyst was higher than that of the other modified catalysts. The TOR for Au/CuMgAlOx was 0.0598 h−1, which was 30 times higher than that of Au/MgAl2O4. The SEM and XRD results showed no significant difference in structure or morphology after introducing the dopants. These dopants had an unfavorable effect on the Au particle size, as confirmed by the TEM studies. Accordingly, the effects on catalytic performance of the M dopant of the obtained Au/MMgAlOx catalyst were improved. Results of Raman, NH3-TPD, and CO2-TPD confirmed that the Au/CuMgAlOx catalyst had more basic sites, which is beneficial for less coking on the catalyst surface after the reaction. XPS analysis showed that gold nanoparticles exhibited a partially oxidized state at the edges and surfaces of CuMgAlOx. Besides an increased proportion of basic sites on Au/CuMgAlOx catalysts, the charge transfer from nanogold to the Cu-doped matrix support probably played a positive role in the selective hydrogenation of acetylene. The stability and deactivation of Au/CuMgAlOx catalysts were also discussed and a possible reaction mechanism was proposed.
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