Essential role of hydride ion in ruthenium-based ammonia synthesis catalysts
In: Chemical Science, Jg. 7 (2016), S. 4036-4043
Online
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Zugriff:
The efficient reduction of atmospheric nitrogen to ammonia under low pressure and temperature conditions has been a challenge in meeting the rapidly increasing demand for fertilizers and hydrogen storage. Here, we report that Ca2N:e−, a two-dimensional electride, combined with ruthenium nanoparticles (Ru/Ca2N:e−) exhibits efficient and stable catalytic activity down to 200 °C. This catalytic performance is due to [Ca2N]+·e1−x−Hx− formed by a reversible reaction of an anionic electron with hydrogen (Ca2N:e− + xH ↔ [Ca2N]+·e1−x−Hx−) during ammonia synthesis. The simplest hydride, CaH2, with Ru also exhibits catalytic performance comparable to Ru/Ca2N:e−. The resultant electrons in these hydrides have a low work function of 2.3 eV, which facilitates the cleavage of N2 molecules. The smooth reversible exchangeability between anionic electrons and H− ions in hydrides at low temperatures suppresses hydrogen poisoning of the Ru surfaces. The present work demonstrates the high potential of metal hydrides as efficient promoters for low-temperature ammonia synthesis.
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Essential role of hydride ion in ruthenium-based ammonia synthesis catalysts
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Autor/in / Beteiligte Person: | Kitano, Masaaki ; Yamagata, Kyosuke ; Nakao, Takuya ; Inoue, Yasunori ; Ishikawa, Hiroki ; Hara, Michikazu ; Tada, Tomofumi ; Yokoyama, Toshiharu ; Matsuishi, Satoru ; Hosono, Hideo |
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Zeitschrift: | Chemical Science, Jg. 7 (2016), S. 4036-4043 |
Veröffentlichung: | Royal Society of Chemistry (RSC), 2016 |
Medientyp: | unknown |
ISSN: | 2041-6539 (print) ; 2041-6520 (print) |
DOI: | 10.1039/c6sc00767h |
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