期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 118, 期 3, 页码 1560-1567出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp408807c
关键词
-
资金
- EPSRC
- Johnson Matthey through CASTech programme
- Dorothy Hodgkin Postgraduate Award (DHPA)
- Johnson Matthey
- EPSRC [EP/G012156/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/G012156/1, 1368768] Funding Source: researchfish
Green oil, which leads to the deactivation of the catalysts used for the selective hydrogenation of acetylene, has long been observed but its formation mechanism is not fully understood. In this work, the formation of 1,3-butadiene, known to be the precursor of green oil, on both Pd(111) and Pd(211) surfaces is examined using density functional theory calculations. The pathways containing C-2 + C-2 coupling reactions as well as the corresponding hydrogenation reactions are studied in detail. Three pathways for 1,3-butadiene production, namely coupling plus hydrogenation and further hydrogenation, hydrogenation plus coupling plus hydrogenation, and a two step hydrogenation followed by coupling, are determined. By comparing the effective barriers, we identify the favored pathway on both surfaces. A general understanding toward the deactivation process of the industrial catalysts is also provided. In addition, the effects of the formation of subsurface carbon atoms as well as the Ag alloying on the 1,3-butadiene formation on Pd-based catalysts are also investigated and compared with experimental results.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据