Enhancing Effect of Fe2+ Doping of Ni/NiO Nanocomposite Films on Catalytic Hydrogen Generation

Highly active and stable non-noble metal catalysts are expected to play a critical role in future hydrogen storage and conversion applications. The design of active sites with composite oxides provides a new approach for developing high-performance catalysts. In this study, an Fe-doped Ni/NiO nanocomposite film was constructed on an ionic liquid/water interface to promote hydrogen generation. The optimized Ni/FeNiO_x-25 catalyst showed excellent catalytic activity toward ammonia borane hydrolysis, with a turnover frequency of 72.3 min^-1. The enhancing effect of Fe²⁺ doping on Ni/NiO films was confirmed by the improved intrinsic activity and theoretical simulations. Fe ion doping stabilized NiO and prevented NiO from becoming Ni. The interfacial Ni-Fe²⁺ dual active sites on the FeNiO_x and Ni interfaces participated in the targeted adsorption and effective activation of water and NH₃BH₃ molecules, respectively. The sufficiently exposed plane surface of the nanofilms provided abundant active sites for catalytic reactions. This significant advance will inspire development in the ambient liquid hydrogen storage field.