期刊
CATALYSIS TODAY
卷 364, 期 -, 页码 220-228出版社
ELSEVIER
DOI: 10.1016/j.cattod.2020.04.044
关键词
Dibenzofuran; Hydrodeoxygenation; Pt(111); Density functional theory calculations
资金
- National Natural Science Foundation of China [21808153, U1810113]
- National Key Research and Development Program of China [2016YFB0600305]
- Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi [2019L0293]
This study investigates the mechanism of dibenzofuran hydrodeoxygenation on the Pt(111) surface using density functional theory calculations. The results show that the five-membered-ring opening of tetrahydrodibenzofuran is easier than that of hexahydrodibenzofuran, leading to the formation of 2-cyclohexylphenol through a nonconsecutive hydrogenation pathway and multiple radical species. The investigation suggests that the target product bicyclohexane is most likely formed through a radical intermediate during the hydrodeoxygenation of dibenzofuran on the Pt(111) surface, providing valuable theoretical guidance for designing new catalysts in coal to liquid hydrodeoxygenation.
Catalytic hydrodeoxygenation is an efficient method to upgrade the quality of low-temperature coal tar and coal liquefied oil. However, only limited researches are performed on the mechanism of hydrodeoxygenation and, therefore, innovation of more efficient and stable catalysts is less progressed and still remains a challenging subject. In this study, density functional theory calculations are carried out to get a deeper insight in the mechanism of dibenzofuran hydrodeoxygenation on the Pt(111) surface. Calculated energies and activation barriers indicate that five-membered-ring opening of tetrahydrodibenzofuran is easier than that of hexahydrodibenzofuran. Then, the generated intermediate can be preferentially hydrogenated through a nonconsecutive pathway to 2-cyclohexylphenol, and would result in multiple radical species. The dehydroxylation of that intermediate formed by adding five hydrogen atoms to the phenyl ring of 2-cyclohexylphenol shows a moderate reaction barrier of 1.07 eV; whereas, dehydroxylation of cyclohexylcyclohexanol needs a higher energy barrier of 2.04 eV. For the hydrodeoxygenation of dibenzofuran on the Pt(111) surface, the target product bicyclohexane is most likely to be formed through a radical intermediate. This investigation may provide a potent theoretical guidance to design new catalyst for hydrodeoxygenation of coal to liquid.
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