Understanding of Selective H2 Generation from Hydrazine Decomposition on Ni(111) Surface

作者：Yin, Hui; Qiu, Yu-Ping; Dai, Hao; Gan, Li-Yong^*; Dai, Hong-Bin; Wang, Ping^*

来源：Journal of Physical Chemistry C, 2018, 122(10): 5443-5451.

DOI：10.1021/acs.jpcc.7b11293

• CHEMICAL HYDROGEN STORAGE
• HIGHLY EFFICIENT CATALYSTS
• DENSITY-FUNCTIONAL THEORY
• TOTAL-ENERGY CALCULATIONS
• METAL-ORGANIC FRAMEWORKS
• NI-PT NANOPARTICLES
• WAVE BASIS-SET
• ROOM-TEMPERATURE
• ALKALINE-SOLUTION
• HETEROGENEOUS CATALYSIS

Catalytic decomposition of hydrazine monohydrate (N2H4H2O) 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 H-2 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.

• 出版日期2018-3-15
• 单位华南理工大学