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Synthesis and Reactivity of Fe(II) Complexes Containing Cis Ammonia Ligands

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Download Hi-Res ImageDownload to MS-PowerPointCite This:Inorg. Chem. 2024, 63, 4, 2024-2033
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    Synthesis and Reactivity of Fe(II) Complexes Containing Cis Ammonia Ligands
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2024, 63, 4, 2024–2033
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    https://doi.org/10.1021/acs.inorgchem.3c03757
    Published January 17, 2024
    Copyright © 2024 The Authors. Published by American Chemical Society
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    Abstract

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    The development of earth-abundant transition-metal complexes for electrocatalytic ammonia oxidation is needed to facilitate a renewable energy economy. Important to this goal is a fundamental understanding of how ammonia binds to complexes as a function of ligand geometry and electronic effects. We report the synthesis and characterization of a series of Fe(II)–NH3 complexes supported by tetradentate, facially binding ligands with a combination of pyridine and N-heterocyclic carbene donors. Electronic modification of the supporting ligand led to significant shifts in the FeIII/II potential and variations in NH bond acidities. Finally, investigations of ammonia oxidation by cyclic voltammetry, controlled potential bulk electrolysis, and through addition of stoichiometric organic radicals, TEMPO and tBu3ArO• are reported. No catalytic oxidation of NH3 to N2 was observed, and 15N2 was detected only in reactions with tBu3ArO•.

    Copyright © 2024 The Authors. Published by American Chemical Society

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    CCDC 2271707–2271711, 2292272, 2295151, and 2320328 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2024, 63, 4, 2024–2033
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.3c03757
    Published January 17, 2024
    Copyright © 2024 The Authors. Published by American Chemical Society
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