期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 54, 期 52, 页码 15725-15729出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201508113
关键词
ammonia-borane; heterogeneous catalysis; hydrogen storage; nickel phosphide; reaction mechanisms
资金
- National Key Basic Research Program of China (973 Program) [2013CB834804]
- Ministry of Science and Technology [2012DFH40090]
- 863 Project [2015AA034203]
- National Natural Science Foundation of China [21273257, 21267025, 21471155, 11474292, U1137606]
- Key Research Programme of the Chinese Academy of Science [KGZD-EW-T05]
Ammonia-borane (AB) is a promising chemical hydrogen-storage material. However, the development of real-time, efficient, controllable, and safe methods for hydrogen release under mild conditions is a challenge in the large-scale use of hydrogen as a long-term solution for future energy security. A new class of low-cost catalytic system is presented that uses nanostructured Ni2P as catalyst, which exhibits excellent catalytic activity and high sustainability toward hydrolysis of ammonia-borane with the initial turnover frequency of 40.4 mol((H2)) mol((Ni2P))(-1) min(-1) under air atmosphere and at ambient temperature. This value is higher than those reported for noble-metal-free catalysts, and the obtained Arrhenius activation energy (E-a = 44.6 kJmol(-1)) for the hydrolysis reaction is comparable to Ru-based bimetallic catalysts. A clearly mechanistic analysis of the hydrolytic reaction of AB based on experimental results and a density functional theory calculation is presented.
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