期刊
CHEMISTRY-AN ASIAN JOURNAL
卷 14, 期 9, 页码 1413-1417出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/asia.201900010
关键词
aromaticity; DFT calculations; dinitrogen activation; frustrated Lewis pairs; reaction mechanism
资金
- National Science Foundation of China [21873079, 21573179]
- Top-Notch Young Talents Program of China
Molecular nitrogen (N-2) is abundant in the atmosphere and, found in many biomolecules, an essential element of life. The Haber-Bosch process, developed over 100years ago, requires relatively harsh conditions to activate N-2 on the iron surface and generate ammonia for use as fertilizer or to produce other chemicals, leading to consumption of more than 2% of the world's annual energy supply. Thus, developing green approaches for N-2 activation under mild conditions is particularly important and urgent. Here we demonstrate that a metal-free N-2 activation could be favorable both thermodynamically and kinetically (with an activation energy as low as 9.1kcalmol(-1)) by using a carbon-boron formal frustrated Lewis pair, which is supported by high-level coupled cluster calculations. Mechanistic studies reveal that aromaticity plays a crucial role in stabilizing both the transition state and the product. Our findings highlight the importance of a combination of an N-heterocyclic carbene with a methyleneborane unit in metal-free N-2 activation, providing conceptual guidance for experimental realization.
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