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  A thiolate-bridged FeIVFeIV μ-nitrido complex and its hydrogenation reactivity toward ammonia formation

Zhang, Y., Zhao, J., Yang, D., Wang, B., Zhou, Y., Wang, J., et al. (2022). A thiolate-bridged FeIVFeIV μ-nitrido complex and its hydrogenation reactivity toward ammonia formation. Nature Chemistry, 14(1), 46-52. doi:10.1038/s41557-021-00852-6.

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 Creators:
Zhang, Yixin1, Author
Zhao, Jinfeng1, Author
Yang, Dawei1, Author
Wang, Baomin1, Author
Zhou, Yuhan1, Author
Wang, Junhu2, Author
Chen, Hui3, Author
Mei, Tao1, Author
Ye, Shengfa4, 5, Author              
Qu, Jingping1, 6, Author
Affiliations:
1State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, People’s Republic of China, ou_persistent22              
2Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, People’s Republic of China, ou_persistent22              
3CAS Key Laboratory of Photochemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, People’s Republic of China, ou_persistent22              
4Research Group Ye, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541708              
5State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, People’s Republic of China, ou_persistent22              
6State Key Laboratory of Bioreactor Engineering, Shanghai Collaborative Innovation Center for Biomanufacturing, Frontiers Science Center for Materiobiology and Dynamic Chemistry, East China University of Science and Technology, Shanghai, People’s Republic of China, ou_persistent22              

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 Abstract: Iron nitrides are key intermediates in biological nitrogen fixation and the industrial Haber–Bosch process, used to form ammonia from dinitrogen. However, the proposed successive conversion of nitride to ammonia remains elusive. In this regard, the search for well-described multi-iron nitrido model complexes and investigations on controlling their reactivity towards ammonia formation have long been of great challenge and importance. Here we report a well-defined thiolate-bridged FeIVFeIV μ-nitrido complex featuring an uncommon bent Fe–N–Fe moiety. Remarkably, this complex shows excellent reactivity toward hydrogenation with H2 at ambient conditions, forming ammonia in high yield. Combined experimental and computational studies demonstrate that a thiolate-bridged FeIIIFeIII μ-amido complex is a key intermediate, which is generated through an unusual two-electron oxidation of H2. Moreover, ammonia production was also realized by treating this diiron μ-nitride with electrons and water as a proton source.

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Language(s): eng - English
 Dates: 2020-12-032021-12-232022-01-01
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41557-021-00852-6
 Degree: -

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Title: Nature Chemistry
  Abbreviation : Nat. Chem.
Source Genre: Journal
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Publ. Info: London, UK : Nature Publishing Group
Pages: - Volume / Issue: 14 (1) Sequence Number: - Start / End Page: 46 - 52 Identifier: ISSN: 1755-4330
CoNE: https://pure.mpg.de/cone/journals/resource/1755-4330