Bimetallic iron–tin catalyst for N2 to NH3 and a silyldiazenido model intermediate

Michael J. Dorantes; James T. Moore; Eckhard Bill; Bernd Mienert; Connie C. Lu

doi:10.1039/D0CC04563B

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Bimetallic iron–tin catalyst for N₂ to NH₃ and a silyldiazenido model intermediate†

Michael J. Dorantes,

‡^a James T. Moore,

‡^a Eckhard Bill,^b Bernd Mienert^b and Connie C. Lu

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455-0431, USA
E-mail: clu@umn.edu

^b Max Planck Institut für Chemische Energiekonversion, Stiftstraße 34-36, 45470 Mülheim an der Ruhr, Germany

Abstract

A tin-supported iron catalyst produces 5.9 turnovers of NH₃ from N₂, using [Ph₂NH₂]OTf as the acid and CoCp₂* as the reductant. Two redox states of the Fe(N₂) adduct and an Fe silyldiazenido complex were characterized using X-ray crystallography along with NMR and Mössbauer spectroscopies. Density functional theory calculations reveal that the charge on the Sn center correlates strongly with both the polarization of the N₂ moiety and the charge on the distal N atom.

This article is part of the themed collections: Chemical Communications HOT Articles and Bioinspired metal complexes for chemical transformations and catalysis

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Article information

DOI: https://doi.org/10.1039/D0CC04563B
Article type: Communication
Submitted: 02 Jul 2020
Accepted: 04 Aug 2020
First published: 04 Aug 2020

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Chem. Commun., 2020,56, 11030-11033

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Bimetallic iron–tin catalyst for N₂ to NH₃ and a silyldiazenido model intermediate

M. J. Dorantes, J. T. Moore, E. Bill, B. Mienert and C. C. Lu, Chem. Commun., 2020, 56, 11030 DOI: 10.1039/D0CC04563B

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