期刊
JOURNAL OF CATALYSIS
卷 383, 期 -, 页码 13-23出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2019.12.032
关键词
Glycerol; Hydrogenolysis; 1,2-Propanediol; Cu/SBA-15; Interface
资金
- National Natural Science Foundation of China [21878321]
- Natural Science Foundation of Shanxi Province [2016021033]
- Science Foundation for Youth Scholars of the State Key Laboratory of Coal Conversion [2016BWZ002]
- Youth Innovation Promotion Association CAS [2015140]
Metal-support interaction is a hot topic in catalysis, but attention has seldom been drawn to the promotional effect of metal-irreducible SiO2 interfaces. Here, Cu/SBA-15 catalysts with Cu-O-Si-O- interface structures were prepared by simple grinding, and showed high activity and selectivity to 1,2-propanediol above 97% in liquid-phase glycerol hydrogenolysis. Glycerol conversion of ground Cu/SBA-15 with 10% Cu loading was about seven times that of its impregnation counterpart. The linear relationship between turnover frequency and (Cu-O-Si-O- induced Lewis acid sites)/Cu-0 ratio indicated that Cu-O-Si-O- structures were crucial for achieving excellent hydrogenolysis performance. More importantly, in situ Fourier transform infrared spectroscopy of glycerol adsorption and density functional theory calculation results confirmed that Cu-O-Si-O- species were the dominant active dehydration sites of glycerol hydrogenolysis, while the adjacent Cu sites were involved in subsequent hydrogenation of the generated hydroxyacetone. (C) 2019 Elsevier Inc. All rights reserved.
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