期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 54, 期 32, 页码 9328-9332出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201500942
关键词
borohydride hydrolysis; catalytic activity; hydrogen generation; ammonium ions; metal-free catalysts
资金
- Natural Science Foundation of Hubei Province of China [2015CFC840]
- National Natural Science Foundation of China [51472184, 51472185]
- State Basic Research Development Program of China (973 Program) [2014CB660802]
- fund of State Key Laboratory of Refractories and Metallurgy [G201405]
Development of highly active, low cost, ecologically friendly, and durable homogenous catalysts for hydrogen generation from hydrolysis of borohydride is one of the most desirable pathways for future hydrogen utilization. The unexpected catalytic activities of inorganic ammonium species and the corresponding mechanisms underpinning them are studied. The catalytic activities of the ammonium species are higher than or comparable to those of mostly investigated noble-metal/transition-metal catalysts (such as Pd, Pt, Ni, and Co) but are considerably cheaper, more environmentally friendly, and more readily available. Quantum chemical calculations indicate that the unique ammonium-induced reaction pathway involved with a barrierless elementary reaction at the reaction entrance and the formation of the highly active intermediate BH3 are responsible for the unexpected catalytic activities and the significantly accelerated hydrogen generation.
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