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Journal Article

A Parent Iron Amido Complex in Catalysis of Ammonia Oxidation

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Ye,  Shengfa
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences;
Research Group Ye, Max-Planck-Institut für Kohlenforschung, Max Planck Society;

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Citation

Li, Y., Chen, J.-Y., Miao, Q., Yu, X., Feng, L., Liao, R.-Z., et al. (2022). A Parent Iron Amido Complex in Catalysis of Ammonia Oxidation. Journal of the American Chemical Society, 144(10), 4365-4375. doi:10.1021/jacs.1c08609.


Cite as: http://hdl.handle.net/21.11116/0000-000A-70C6-8
Abstract
Parent amido complexes are crucial intermediates in ammonia-based transformations. We report a well-defined ferric ammine system [Cp*Fe(1,2-Ph2PC6H4NH)(NH3)]+ ([1-NH3]+), which processes electrocatalytic ammonia oxidation to N2 and H2 at a mild potential. Through establishing elementary e/H+ conversions with the ferric ammine, a formal Fe(IV)-amido species, [1-NH2]+, together with its conjugated Lewis acid, [1-NH3]2+, was isolated and structurally characterized for the first time. Mechanism studies indicated that further oxidation of [1-NH2]+ induces the reaction of the parent amido unit with NH3. The formation of hydrazine is realized by the non-innocent nature of the phenylamido ligand that facilitates the concerted transfer of one proton and two electrons.