期刊
CHEMICAL SCIENCE
卷 7, 期 7, 页码 4036-4043出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6sc00767h
关键词
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资金
- Accelerated Innovation Research Initiative Turning Top Science and Ideas into High-Impact Values (ACCEL) program of the Japan Science and Technology Agency (JST)
- Kakenhi from the Japan Society for the Promotion of Science (JSPS) [15H04183]
- Grants-in-Aid for Scientific Research [15H04183] Funding Source: KAKEN
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 degrees C. This catalytic performance is due to [[Ca2N](+)center dot e(1-x)(-)H(x)(-) formed by a reversible reaction of an anionic electron with hydrogen (Ca2N:e(-) + xH -> [Ca2N](+)center dot e(1-x)(-)H(x)(-)) 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 N-2 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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