Tuning the Surface Composition of Ni/<italic>meso</italic>‐CeO2 with Iridium as an Efficient Catalyst for Hydrogen Generation from Hydrous Hydrazine.

Abstract: Selective decomposition of hydrous hydrazine (N₂H₄<bold>⋅</bold>H₂O) over metal catalysts provides a promising means for onboard or portable hydrogen source applications. Studies on N₂H₄<bold>⋅</bold>H₂O 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/<italic>meso</italic>‐CeO₂ 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/<italic>meso</italic>‐CeO₂ catalyst shows excellent catalytic performance towards hydrogen generation from N₂H₄<bold>⋅</bold>H₂O, which compares favorably with the Ni−Ir bimetallic catalysts reported to date. [ABSTRACT FROM AUTHOR]