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A series of ZnMgNiAl layered double hydroxides (LDHs) containing 20 wt.% Ni and different Zn/Mg molar ratios were prepared by a coprecipitation method, and then were introduced with H2PO4− via a microwave-hydrothermal method. With the resulting mixtures as the precursors, Zn/Mg-modified ZnMgNi–P/Al2O3 catalysts were prepared. The Zn/Mg molar ratio affected the formation of Ni2P and Ni12P5 in nickel phosphides. The ZnMgNi–P/Al2O3 catalyst with a Zn/Mg molar ratio of 3:1 exhibits the best dibenzothiophene hydrodesulfurization (HDS) activity. Compared with the Ni–P/Al2O3 catalyst prepared from the impregnation method, the ZnMgNi–P/Al2O3 catalyst shows a higher HDS activity (81.6% vs. 54.3%) and promotes the direct desulfurization of dibenzothiophene

High Active Zn/Mg-Modified Ni–P/Al2O3 Catalysts Derived from ZnMgNiAl Layered Double Hydroxides for Hydrodesulfurization of Dibenzothiophene