N2 Functionalization using a family of (XCX)M complexes – FuN2

The Haber-Bosch process still stands as one of the most important chemical transformations to mankind. It allows the synthesis of ca 170 million tons/year of ammonia, mostly used as fertilizer, from dinitrogen and dihydrogen using heterogeneous catalyst submitted to drastic conditions, involving high pressures and temperatures (350-550°C, 150-350 atm). This key industrial process is not only the most important, it is also the most expensive one, as it consumes around 1-2% of the world annual energy production. In the current context of climat change and green growth, the development of alternative approaches to decrease the environmental impact of this reaction is of major societal importance. Our goal is thus to explore and discover innovative and sustainable alternatives to the Haber-Bosch process through the development of efficient and selective homogeneous (electro)catalysts capable of transforming N2 into valuable NR3 products. The main driving force behind our initiative comes from the observation that; i) there is currently no clear and reliable rationalization of the “structure/reactivity” relationship in molecular systems able to activate/reduce/functionalize N2 (stoichiometric or catalytic) and that; ii) the very few catalysts investigated so far are limited to titanium, molybdenum, iron or cobalt but that none of them are stable or active enough to stand as viable alternatives. We believe that this unsatisfactory situation is mostly due a lack of specific and systematic studies involving structurally- and electronically-versatile ligands and complexes with group 5-7 metals. We will develop such a family of (OCO)M complexes (OCO = bis arylOxy-Carbene ligand; M = group 5-7); study the functionalization of N2 by various electrophiles at the metal center under reductive conditions to eventually develop more sustainable production of N containing products (NH3, N(SiMe3)3 or NR3) involving chemical or electrochemical activation steps.