期刊
JOURNAL OF CATALYSIS
卷 368, 期 -, 页码 172-189出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2018.10.002
关键词
Octanol; Ammonia; Direct amination; Borrowing hydrogen; Cyclodextrin; Ni-Pd alumina
资金
- French Agency of Research (ANR, France) through the SHAPes program [13-CDII-0004-06]
- Chevreul Institute (France) [FR 2638]
- Ministere de l'Enseignement Superieur et de la Recherche (France)
- Region Hauts-de-France
- FEDER program
This paper reports the use of beta-cyclodextrin as a pre-shaping agent for the preparation of low-metal xNi-yPd/Al2O3 catalysts (x = 2, 5 wt% and y = 0.2, 0.5, 1.0 wt%) targeting the direct amination of 1-octanol with ammonia. Six different preparation methods were used aiming at tuning the Ni-Pd interaction. The catalysts were finely characterized by XRD, H-2-TPR, CO pulse chemisorption, STEM-EELS/EDS-SDD and XPS, while the elementary interaction between Ni-Pd-cyclodextrin was assessed by marrying ESI-MS experiments with DFT calculations. Among the different methods studied, the most outstanding effect was obtained when beta-cyclodextrin was pre-adsorbed on gamma-Al2O3 before impregnating the Ni and Pd nitrate precursors. At such conditions, the best formulation (5Ni-0.5Pd/Al-CD_M4) afforded 90% conversion and 71% yield to 1-octylamine (TON = 93) in the amination of 1-octanol with ammonia at 160 degrees C for 4 h, which places it among the most active and selective Ni catalysts reported in the literature. (C) 2018 Elsevier Inc. All rights reserved.
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