Indexed by:期刊论文

Date of Publication:2017-08-01

Journal:TOPICS IN CATALYSIS

Included Journals:SCIE、EI、Scopus

Volume:60

Issue:12-14

Page Number:987-996

ISSN No.:1022-5528

Key Words:Nickel phosphide; Hypophosphite; Plasma; Hydrodenitrogenation; Quinoline; Decahydroquinoline

Abstract: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.