Journal
CHEMPHYSCHEM
Volume 18, Issue 19, Pages 2606-2617Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201700665
Keywords
bond dissociation energies; homogeneous catalysis; nitrogen fixation; reaction mechanism; transition metals
Funding
- Agence Nationale pour la Recherche (grant CalixMo) [ANR-14-CE06_0002_01]
- Labex ARCANE [ANR-11-LABX-0003-01]
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Fixation of atmospheric nitrogen is central for the production of ammonia, which is the source of nitrogen fertilizers and is also emerging as a promising renewable fuel. While the development of efficient molecular-based artificial nitrogen fixation systems working under mild conditions is probably a Holy Grail, the catalytic reduction of N-2 by transition-metal complexes isabove allthe main instrument to progress in the mechanistic understanding of N-2 splitting. In this Minireview we first give an overview of molecular-based catalytic systems, including recent breakthroughs, and then we illustrate the alternative pathways for N-2 reduction. We mainly focus on multistep hydrogenation of N-2 by separated proton and electron sources, with a particular attention for the possibility of proton-coupled electron transfer events. Finally, we try to identify the key factors to achieve catalytic reduction of dinitrogen by metal complexes and to enhance their efficiency.
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