期刊
GREEN CHEMISTRY
卷 17, 期 3, 页码 1692-1701出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4gc02339k
关键词
-
资金
- Shanghai Pujiang Program [14PJ1403500]
- Elite Program of East China Normal University
A highly active catalyst, hierarchical nano-sized Ni/HBEA, is developed for stearic acid and palm oil hydrodeoxygenation (HDO) in dodecane. The TPAOH/NaOH treated hierarchical HBEA sample (crystal size: 15-20 nm) affords more homogeneously dispersed open inter-mesopores (main pore diameter: 25 nm) via controllable base leaching, as evidenced by various microscopy and spectroscopy techniques. By the formation of an aluminum complex on the crystal surface, TPA(+) prevents the specific external structure from deep corrosion. After loading Ni nanoclusters, the modified Ni/HBEA was supported with more loadable and dispersive Ni nanoclusters (d = 7.7 +/- 1.5 nm) in the newly formed inter-crystalline mesopores, which provide higher accessibility towards heavy molecules, as well as restrict the Ni particle growth. This novel catalyst shows a significantly high initial rate of 67 mmol g(-1) h(-1) (equivalent to 19 g g(-1) h(-1)) for producing 85% n-C-17/C-18 and 11% iso-C-17/C-18 alkanes by stearic acid conversion at 260 degrees C and 4 MPa H-2, and the efficiency of this method is far beyond the current techniques using sulfur-metal and reduced-metal catalysts. The HDO route follows the major pathway of sequential hydrogenation and dehydration steps, affording a highly atom-economical process and a suitable diesel oil ingredient (with certain branched alkanes). In addition, high activities are achieved with the improved catalyst after treatment with high concentration stearic acid in dodecane (up to 0.5 g mL(-1)), and the catalyst remains highly active and stable in the four recycling runs of palm oil HDO.
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