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

Author:  ["Masaaki Kitano","Yasunori Inoue","Youhei Yamazaki","Fumitaka Hayashi","Shinji Kanbara","Satoru Matsuishi","Toshiharu Yokoyama","Sung-Wng Kim","Michikazu Hara","Hideo Hosono"]

Publication:  Nature Chemistry

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Tags:     Chemistry

Abstract

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 N2 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. Methods that fix atmospheric nitrogen to ammonia under mild conditions could offer a more environmentally benign alternative to the Haber–Bosch process. Now, a Ru-loaded electride, [Ca24Al28O64]4+(e−)4, is reported that acts as an efficient electron donor and reversible hydrogen store, and is demonstrated to function as an efficient catalyst for ammonia synthesis.

Cite this article

Kitano, M., Inoue, Y., Yamazaki, Y. et al. Ammonia synthesis using a stable electride as an electron donor and reversible hydrogen store. Nature Chem 4, 934–940 (2012). https://doi.org/10.1038/nchem.1476

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