Seminar
calendar 06/06/2023
clock 12:00 h

Electro- and Photochemical Strategies for N2 Splitting

The direct use of N2 for the synthesis of nitrogenous organic products, such as amines, nitriles or nitro compounds, is a challenging task. Catalytic protocols remain unknown. Reductive splitting of dinitrogen into transition metal nitride complexes represents a potential entry towards N2 fixation beyond ammonia.[1]

 

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.[2] In this seminar, strategies towards reductive N2 splitting will be presented, based on reaction mechanisms and electronic structure/reactivity relationships for key intermediates.

Figure 1. Photoelectrochemically driven N2-fixation to benzonitrile.[2i]

 

Acknowledgements The ERC (CoG 646747 “N2Feed”) and the DFG (SCHN950/7) are acknowledged for generous support.

 

[1] Forrest, S. J. K.; Schluschaß, B.; Yuzik-Klimova, E.; Schneider, S. Chem. Rev., 2021, 121, 6522.

[2] (a) Klopsch, I.; Finger, M.; Würtele, C.; Milde, B.; Werz, D. B.; Schneider, S. J. Am. Chem. Soc. 2014, 136, 6881. (b) Klopsch, I.; Kinauer, M.; Finger, M.; Würtele, C.; Schneider, S. Angew. Chem. Int. Ed. 2016, 55, 4786. (c) Silantyev, G. A.; Förster, M.; Schluschaß, B.; Abbenseth, J.; Würtele, C.; Volkmann, C.; Holthausen, M. C.; Schneider, S. Angew. Chem. Int. Ed. 2017, 56, 5872. (d) Lindley, B. M.; van Alten, R. S.; Finger, M.; Schendzielorz, F.; Würtele, C.; Miller, A. J. M.; Siewert, I.; Schneider S. J. Am. Chem. Soc. 2018, 140, 7922. (e) Schluschaß, B.; Abbenseth, J.; Demeshko, S.; Finger, M.; Franke, A.; Herwig, C.; Würtele, C.; Ivanovic-Burmazovic, I.; Limberg, C.; Telser, J.; Schneider, S. Chem. Sci. 2019, 10, 10275. (f) Schendzielorz, F.; Finger, M.; Abbenseth, J.; Würtele, C.; Krewald, V.; Schneider, S. Angew. Chem. Int. Ed. 2019, 58, 830. (g) Schluschaß, B.; Borter, J.-H.; Rupp, S.; Demeshko, S.; Herwig, C.; Limberg, C.; Maciulis, N.; Schneider, J.; Würtele, C.; Krewald, V.; Schwarzer, D.; Schneider, S. JACS Au 2021, 1, 879. (h) Alig, L.; Eisenlohr, K. A.; Zelenkova, Y.; Rosendahl, S.; Herbst-Irmer, R.; Demeshko, S.; Holthausen, M. C.; Schneider, S. Angew. Chem. Int. Ed. 2022, 61, e202113340. (i) M. Fritz, S. Rupp, C.I. Kiene, S. Kisan, J. Telser, C. Würtele, V. Krewald, S. Schneider, Angew. Chem. Int. Ed. 2022, e202205922.

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