Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.233
Publication date: 18th July 2023
While the fixation of dinitrogen to ammonia at ambient conditions has undergone remarkable advances in recent years, the direct use of dinitrogen for the synthesis of other nitrogenous products, such as amines, nitriles or nitro compounds, is a challenging task. Furthemore, catalytic protocols remain unknown.
The reductive splitting of dinitrogen into transition metal nitride complexes represents a potential entry towards N2 fixation beyond ammonia. Over the past years, we have examined the mechanisms of chemically, photochemically, and electrochemically driven reductive N2 splitting by group 6 and 7 metal complexes as a path for the direct conversion of N2 into several products beyond ammonia, such as nitriles, amides and N2O. In this contribution, the reductive splitting of dinitrogen will be presented. Electro- and photochemically driven pathways are discussed that are based on detailed mechanistic studies and electronic structure/reactivity relationships of key intermediates. Synthetic strategies for selectivity control that are guided by N–H proton-coupled electron transfer thermochemistry of intermediates are presented.
The ERC (CoG 646747 “N2Feed”) and the DFG (SCHN950/7) are acknowledged for generous support.
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