Tuning the Surface Composition of Ni/ meso ‐CeO 2 with Iridium as an Efficient Catalyst for Hydrogen Generation from Hydrous Hydrazine

Selective decomposition of hydrous hydrazine (N 2 H 4 ⋅ H 2 O) over metal catalysts provides a promising means for onboard or portable hydrogen source applications. Studies on N 2 H 4 ⋅ H 2 O decomposition catalysts mainly focus on the effects of bulk composition and structure on their performances, instead of the surface‐composition‐dependent properties. Herein, the synthesis of an Ir‐modified Ni/ meso ‐CeO 2 catalyst is reported by using a combination of colloidal solution combustion synthesis and galvanic replacement methods. A combination of structural characterization, control experiments, and DFT calculations reveals that the Ni−Ir alloy resulting from calcination treatment exerts a profound effect on the catalytic properties. The resulting Ni@Ni−Ir/ meso ‐CeO 2 catalyst shows excellent catalytic performance towards hydrogen generation from N 2 H 4 ⋅ H 2 O, which compares favorably with the Ni−Ir bimetallic catalysts reported to date.