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论文类型：期刊论文

发表时间：2017-08-01

发表刊物：TOPICS IN CATALYSIS

收录刊物：SCIE、EI、Scopus

卷号：60

期号：12-14

页面范围：987-996

ISSN号：1022-5528

关键字：Nickel phosphide; Hypophosphite; Plasma; Hydrodenitrogenation; Quinoline; Decahydroquinoline

摘要：A series of mixtures of NiCl2, hypophosphites (NaH2PO2 and NH4H2PO2), and additives were used as precursors (denoted as x additive:y hypophosphite:z NiCl2, where x, y, and z represents the molar ratios of the compounds) for the synthesis of Ni2P both in N-2 and H-2 plasma. The catalytic performances of the obtained catalysts were evaluated by the hydrodenitrogenation (HDN) of quinoline (Q) and decahydroquinoline (DHQ). Ni2P was stoichiometrically synthesized by the treatment of 1.0NH(4)H(2)PO(2):2.0NiCl(2) with N-2 plasma at a low total power input of 8 W (40 V x 0.2 A). In H-2 plasma, the precursor was over-reduced to a mixture of Ni and Ni2P, with Ni2P as the minor phase. The over-reduction can be inhibited by the addition of proper amount of alkali-metal chloride (NaCl or KCl) or P2O5 center dot CaCl2 facilitated the reduction of nickel salts to Ni center dot KCl was the best among the additives investigated. Both the surface and bulk over-reduction of 1.0NH(4)H(2)PO(2):2.0NiCl(2) was inhibited by KCl, while P2O5 mainly inhibited the bulk over-reduction. The addition of KCl strongly suppressed the hydrogenation of Q to DHQ, but facilitated the HDN of DHQ. On the other hand, not only the hydrogenation of Q but also the dehydrogenation of DHQ was substantially inhibited by P2O5.