5 years ago

N2-to-NH3 Conversion by a triphos–Iron Catalyst and Enhanced Turnover under Photolysis

N2-to-NH3 Conversion by a triphos–Iron Catalyst and Enhanced Turnover under Photolysis
Paul H. Oyala, Jonas C. Peters, Trixia M. Buscagan
Bridging iron hydrides are proposed to form at the active site of MoFe-nitrogenase during catalytic dinitrogen reduction to ammonia and may be key in the binding and activation of N2 via reductive elimination of H2. This possibility inspires the investigation of well-defined molecular iron hydrides as precursors for catalytic N2-to-NH3 conversion. Herein, we describe the synthesis and characterization of new P2P′PhFe(N2)(H)x systems that are active for catalytic N2-to-NH3 conversion. Most interestingly, we show that the yields of ammonia can be significantly increased if the catalysis is performed in the presence of mercury lamp irradiation. Evidence is provided to suggest that photo-elimination of H2 is one means by which the enhanced activity may arise. Light it up: Light-enhanced N2-to-NH3 conversion catalysis is reported. New triphos-supported Fe(N2)Hx catalysts provide higher ammonia yields for 1 atm N2, and as much as 180 % improvement upon irradiation by a mercury lamp.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201703244

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