期刊
NATURE ENERGY
卷 3, 期 12, 页码 1067-1075出版社
NATURE PORTFOLIO
DOI: 10.1038/s41560-018-0268-z
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资金
- National Natural Science Foundation of China [21633011, 21603220]
- Sino-Japanese Research Cooperative Program of Ministry of Science and Technology [2016YFE0118300]
- DICP [DICP DMTO201504]
- Youth Innovation Promotion Association CAS [2018213]
- Collaborative Innovation Center of Chemistry for Energy Materials (2011-iChEM)
Ammonia is a promising carbon-free energy carrier, but is currently synthesized industrially under harsh conditions. Synthesizing ammonia using lower temperatures and pressures could therefore improve its prospects as a chemical means to store and transport energy. Here we report that alkali and alkaline earth metal imides function as nitrogen carriers that mediate ammonia production via a two-step chemical looping process operating under mild conditions. Nitrogen is first fixed through the reduction of N-2 by alkali or alkaline earth metal hydrides to form imides and, subsequently, the imides are hydrogenated to produce NH3 and regenerate the metal hydrides. The oxidation state of hydrogen therefore switches between -1 (hydride), O(H-2) and +1 (imide and NH3). Late 3d metals accelerate the reaction rates of both steps. The chemical loop mediated by BaNH and catalysed by Ni produces NH3 at 100 degrees C and atmospheric pressure.
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