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  A Parent Iron Amido Complex in Catalysis of Ammonia Oxidation

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.

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 Creators:
Li, Yongxian1, Author
Chen, Jia-Yi2, Author
Miao, Qiyi3, 4, Author
Yu, Xin1, Author
Feng, Lei1, Author
Liao, Rong-Zhen2, Author
Ye, Shengfa3, 5, Author           
Tung, Chen-Ho1, Author
Wang, Wenguang1, 6, Author
Affiliations:
1School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China, ou_persistent22              
2School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China, ou_persistent22              
3State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China, ou_persistent22              
4University of Chinese Academy of Sciences, Beijing 100049, China, ou_persistent22              
5Research Group Ye, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541708              
6College of Chemistry, Beijing Normal University, Beijing 100875, China, ou_persistent22              

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 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.

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Language(s): eng - English
 Dates: 2021-08-162022-03-022022-03-16
 Publication Status: Published in print
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.1c08609
 Degree: -

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Title: Journal of the American Chemical Society
  Other : JACS
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 144 (10) Sequence Number: - Start / End Page: 4365 - 4375 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870