Aminodiphosphine substituted 2Fe2Se complex as new precursor to single and double butterfly Fe/Se models related to FeFe hydrogenase models

Lü, Shuang; Bai, Shu-Fen; Gao, Xin-Ping; Wang, Yan-Lan; Li, Qian‐Li

doi:10.1016/j.molstruc.2023.135939

Journal of Molecular Structure

2023

DOI: 10.1016/j.molstruc.2023.135939

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Aminodiphosphine substituted 2Fe2Se complex as new precursor to single and double butterfly Fe/Se models related to FeFe hydrogenase models

Shuang Lü

Shu-Fen Bai

Xin-Ping Gao

et al.

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2024

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Cited by 3 publications

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The reaction of nonacarbonyldiiron with 8‐alkynyloxyquinolines: Alkynyl activation, cyclization via C‐N bond formation, and C‐H bond cleavage

Luo,

Yu,

Chu

et al. 2024

Applied Organom Chemis

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In this work, the reactions of nonacarbonyldiiron with 8‐alkynyloxyquinoline ligands (L1‐L3) and their resultant iron carbonyl complexes (1a, 1b, 2, and 3) are described. The complexes including the ligands were fully characterized by using a variety of spectroscopic techniques. The four complexes were also crystallographically determined. In the reactions, the quinoline N atom underwent cyclization to form a quinolinium skeleton while the C‐H bond of the quinoline at position 2 or the substituted methyl group was cleaved to form Fe‐C bond(s). Meanwhile, the alkynyl triple bond was reduced to a single bond (1a) or double bonds (1b, 2, and 3) to further coordinate the iron in σ‐bonds or η‐bonds. Particularly, pathways of hydrogenation (1a and 2) and/or dehydrogenation (1b and 3) were accompanied by the reactions. Moreover, the oxidation states of the iron centers in these complexes were identified through analyses of their bond formation, FTIR and NMR spectroscopic signals (1H NMR and DEPT‐135) in combination with their diamagnetic nature, that is, iron (0) for 2 and iron (I) for the rest of the diiron complexes.

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The reaction of nonacarbonyldiiron with 8‐alkynyloxyquinolines: Alkynyl activation, cyclization via C‐N bond formation, and C‐H bond cleavage

Luo,

Yu,

Chu

et al. 2024

Applied Organom Chemis

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Tertiary phosphine‐supported diiron model complexes relevant to [FeFe]‐hydrogenases

Gao,

Jin,

Zhang

et al. 2024

Applied Organom Chemis

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In an effort to better probe the structure–function relationship on the biological [Fe4S4] cluster of [FeFe]‐hydrogenases, a new library of tertiary phosphine‐supported diiron dithiolate complexes [Fe2(μ‐adtNR)(CO)5{P(C6H4X)3}] (1–3) with various substituents (X = F vs. H vs. Me), wherein adtNR is denoted as abbreviation for the (SCH2)2N(C6H4C2H4OC(O)CH2C6H4Me) unit, is prepared as the active site mimics of [FeFe]‐hydrogenases. Notably, the substituent influences of tertiary phosphines on the structures and electrochemical behaviors of 1–3 are studied by spectroscopic and crystallographic techniques as well as cyclic voltammetry. For example, the electronic effect of tertiary phosphines [P(C6H4X)3] is responsible for the electron density around diiron center and the key Fe–Fe as well as Fe–P lengths in 1–3 as revealed by IR spectroscopy and crystallographic analysis. Further, complexes 1–3 show the electrochemical activity for proton reduction into molecular hydrogen (H2) using acetic acid (AcOH) as a proton source. Noticeably, F‐substituent‐containing diiron model complex 1 exhibits greater turnover frequency (i.e., turnover frequency value) and similar overpotential for electrocatalytic H2 evolution relative to H‐ or Me‐substituent‐bearing diiron homologs 2 or 3.

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Crystal structure of bis(μ-benzeneselenolato)-(tetracarbonyl)-{μ-[N-(diphenylphosphanyl)-N-(3-ethynylphenyl)-P,P-diphenylphosphinous amide]} diiron, C₄₈H₃₅Fe₂NO₄P₂Se₂

Lü,

2024

Zeitschrift Für Kristallographie - New Crystal Structures

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Aminodiphosphine substituted 2Fe2Se complex as new precursor to single and double butterfly Fe/Se models related to FeFe hydrogenase models

Cited by 3 publications

References 53 publications

The reaction of nonacarbonyldiiron with 8‐alkynyloxyquinolines: Alkynyl activation, cyclization via C‐N bond formation, and C‐H bond cleavage

The reaction of nonacarbonyldiiron with 8‐alkynyloxyquinolines: Alkynyl activation, cyclization via C‐N bond formation, and C‐H bond cleavage

Tertiary phosphine‐supported diiron model complexes relevant to [FeFe]‐hydrogenases

Crystal structure of bis(μ-benzeneselenolato)-(tetracarbonyl)-{μ-[N-(diphenylphosphanyl)-N-(3-ethynylphenyl)-P,P-diphenylphosphinous amide]} diiron, C₄₈H₃₅Fe₂NO₄P₂Se₂

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Aminodiphosphine substituted 2Fe2Se complex as new precursor to single and double butterfly Fe/Se models related to FeFe hydrogenase models

Cited by 3 publications

References 53 publications

The reaction of nonacarbonyldiiron with 8‐alkynyloxyquinolines: Alkynyl activation, cyclization via C‐N bond formation, and C‐H bond cleavage

The reaction of nonacarbonyldiiron with 8‐alkynyloxyquinolines: Alkynyl activation, cyclization via C‐N bond formation, and C‐H bond cleavage

Tertiary phosphine‐supported diiron model complexes relevant to [FeFe]‐hydrogenases

Crystal structure of bis(μ-benzeneselenolato)-(tetracarbonyl)-{μ-[N-(diphenylphosphanyl)-N-(3-ethynylphenyl)-P,P-diphenylphosphinous amide]} diiron, C48H35Fe2NO4P2Se2

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Crystal structure of bis(μ-benzeneselenolato)-(tetracarbonyl)-{μ-[N-(diphenylphosphanyl)-N-(3-ethynylphenyl)-P,P-diphenylphosphinous amide]} diiron, C₄₈H₃₅Fe₂NO₄P₂Se₂