Molybdate-intercalated magnesium–aluminum hydrotalcite-like compounds (HTlc) were synthesized by anion-exchange and used as precursor to prepare supported molybdenum nitride catalyst for ammonia decomposition. The as-synthesized precursors and the derived mixed metal oxides and nitride catalysts were characterized by ICP, XRD, Raman spectroscopy, XPS, H2-TPR, and HAADF-STEM-EDX. The characterizations indicated that molybdate was well intercalated into the HTlc interlayer as MoO42– and the Mo content was tunable by altering the intercalation degree of molybdate. Upon calcination, molybdena was dominantly presented as isolated tetrahedrally coordinated MoOx species. Upon nitridation with ammonia at 700 ºC, highly dispersed and composition-uniform molybdenum nitride (Mo2±xN) was formed. The Mo0.5Mg3Al nitride catalyst showed good activity for ammonia decomposition, providing nearly full conversion of ammonia at 625 ºC under a space velocity of 5,000 mL gcat–1 h–1. The optimal catalyst also exhibited high catalytic stability during 100 h operation at 625 ºC, and no obvious aggregation took place, attributable to the strong metal–support interaction between molybdenum nitride and Mg–Al mixed oxide. It is suggested that the hydrotalcite-derived Mg–Al mixed oxide supported highly dispersed Mo2±xN species was active and stable for ammonia decomposition.
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