Ammonia Synthesis at Room Temperature and Atmospheric Pressure from N2: A Boron-Radical Approach |
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| Authors: | Dr. Soukaina Bennaamane Barbara Rialland Lhoussain Khrouz Dr. Marie Fustier-Boutignon Dr. Christophe Bucher Dr. Eric Clot Dr. Nicolas Mézailles |
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| Affiliation: | 1. Laboratoire Hétérochimie Fondamentale et Appliquée, Université Paul Sabatier, CNRS, 118 Route de Narbonne, 31062 Toulouse, France;2. Univ Lyon, ENS Lyon, CNRS, Universite Lyon 1, Laboratoire de Chimie, UMR 5182, 46 allée d'Italie, 69364 Lyon, France;3. ICGM, Univ. Montpellier, CNRS, ENSCM, 34000 Montpellier, France |
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| Abstract: | Ammonia, NH3, is an essential molecule, being part of fertilizers. It is currently synthesized via the Haber–Bosch process, from the very stable dinitrogen molecule, N2 and dihydrogen, H2. This process requires high temperatures and pressures, thereby generating ca 1.6 % of the global CO2 emissions. Alternative strategies are needed to realize the functionalization of N2 to NH3 under mild conditions. Here, we show that boron-centered radicals provide a means of activating N2 at room temperature and atmospheric pressure whilst allowing a radical process to occur, leading to the production of borylamines. Subsequent hydrolysis released NH4+, the acidic form of NH3. EPR spectroscopy supported the intermediacy of radicals in the process, corroborated by DFT calculations, which rationalized the mechanism of the N2 functionalization by R2B radicals. |
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| Keywords: | Boron Radical Density-Functional Calculations N2 Fixation Reaction Mechanims Reduction |
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