Construction the Ni@Carbon nanostructure with dual-reaction surfaces for the selective hydrogenation reaction
2019
Abstract The reduction of the size and modification the surface of Ni 0 are generally used to improve the hydrogenation performances of Ni-based catalysts. In this work, a new method derived Ni 0 @carbon nanostructure was constructed on SiO 2 in order to explore an alternative way to improve the intrinsic activity of Ni 0 in the selective hydrogenation of p-chloronitrobenzene ( p -CNB). The experimental and computational results exhibit that the synergistic effect between Ni 0 core and nitrogen-doped carbon shell (Ni 0 @C-N) can dissociate more hydrogen on larger Ni 0 core (~14 nm) than Ni 0 @C (Ni 0 ≈ 11 nm), while the external surface of carbon shell facilitates the oblique adsorption of p -CNB and the consequent hydrogenation. Such formed dual-reaction surfaces inhibit the dechlorination reaction but increase the active hydrogen species. Consequently, Ni 0 @C-N/SiO 2 catalyst (~14 nm) adversely displays ~2.3-fold higher turnover frequency and ~100% p -chloroaniline selectivity, in contrast to Ni 0 @C/SiO 2 (~11 nm) and the commercial Raney Ni (~6 nm) catalysts.
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