LAUSR

Catalytic decomposition of hydrazine monohydrate (N2H4·H2O) over Ni-based catalysts has been extensively investigated as a promising hydrogen generation means for onboard or portable applications. Despite the flourishing experimental development of Ni-based catalysts, the mechanistic study of catalytic decomposition process is still in its infancy. Herein, we report a first-principles study of the elementary steps in N2H4 decomposition over the Ni(111) surface. The calculations show that the decomposition behaviors of N2H4 strongly depend on the surface coverage. At a higher coverage of 0.25 ML, the calculation results are in excellent agreement with the experimental observation. Our calculations, for the first time, presented a complete picture of catalytic selective H2 generation from N2H4 decomposition over Ni surface. Such mechanistic understanding may lay the foundation for the development of high-performance Ni-based catalyst for promoting hydrogen generation from N2H4.