期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 30, 页码 8716-8720出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201703695
关键词
ammonia synthesis; clusters; iron catalysts; Li4FeH6; optical spectroscopy
资金
- National Natural Science Funds for Distinguished Young Scholars [51225206]
- National Natural Science Foundation of China [21327901, 21503222, 21603220, 21633011, 21673231]
- Dalian Institute of Chemical Physics [DICP DMTO201504]
- Collaborative Innovation Center of Chemistry for Energy Materials [2011-iChEM]
- State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University [201504]
Lithium hydride (LiH) has a strong effect on iron leading to an approximately 3 orders of magnitude increase in catalytic ammonia synthesis. The existence of lithium-iron ternary hydride species at the surface/interface of the catalyst were identified and characterized for the first time by gas-phase optical spectroscopy coupled with mass spectrometry and quantum chemical calculations. The ternary hydride species may serve as centers that readily activate and hydrogenate dinitrogen, forming Fe-(NH2)-Li and LiNH2 moieties-possibly through a redox reaction of dinitrogen and hydridic hydrogen (LiH) that is mediated by iron-showing distinct differences from ammonia formation mediated by conventional iron or ruthenium-based catalysts. Hydrogen-associated activation and conversion of dinitrogen are discussed.
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