4.8 Article

Ammonia synthesis using a stable electride as an electron donor and reversible hydrogen store

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NATURE CHEMISTRY
卷 4, 期 11, 页码 934-940

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NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1476

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  1. Japan Society for the Promotion of Science
  2. Ministry of Education, Culture, Sports and Science for Technology in Japan

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Industrially, the artificial fixation of atmospheric nitrogen to ammonia is carried out using the Haber-Bosch process, but this process requires high temperatures and pressures, and consumes more than 1% of the world's power production. Therefore the search is on for a more environmentally benign process that occurs under milder conditions. Here, we report that a Ru-loaded electride [Ca24Al28O64](4+)(e(-))(4) (Ru/C12A7:e(-)), which has high electron-donating power and chemical stability, works as an efficient catalyst for ammonia synthesis. Highly efficient ammonia synthesis is achieved with a catalytic activity that is an order of magnitude greater than those of other previously reported Ru-loaded catalysts and with almost half the reaction activation energy. Kinetic analysis with infrared spectroscopy reveals that C12A7:e(-) markedly enhances N-2 dissociation on Ru by the back donation of electrons and that the poisoning of ruthenium surfaces by hydrogen adatoms can be suppressed effectively because of the ability of C12A7:e(-) to store hydrogen reversibly.

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