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Record W2767527569 · doi:10.1021/acs.inorgchem.7b01802

Iron(II) Complexes of a Hemilabile SNS Amido Ligand: Synthesis, Characterization, and Reactivity

2017· article· en· W2767527569 on OpenAlexafffund
Uttam Kumar Das, Stephanie L. Daifuku, Theresa E. Iannuzzi, Serge I. Gorelsky, Ilia Korobkov, Bulat Gabidullin, Michael L. Neidig, R. Tom Baker

Bibliographic record

VenueInorganic Chemistry · 2017
Typearticle
Languageen
FieldChemistry
TopicMetal-Catalyzed Oxygenation Mechanisms
Canadian institutionsUniversity of Ottawa
FundersLaboratory Directed Research and DevelopmentDivision of ChemistryNatural Sciences and Engineering Research Council of CanadaCanada Research ChairsAlfred P. Sloan Foundation
KeywordsChemistryReactivity (psychology)Ligand (biochemistry)Characterization (materials science)StereochemistryCombinatorial chemistryNanotechnologyReceptorBiochemistry

Abstract

fetched live from OpenAlex

We report an easily prepared bis(thioether) amine ligand, S Me N H S Me, along with the synthesis, characterization, and reactivity of the paramagnetic iron(II) bis(amido) complex, [Fe(κ 3 -S Me NS Me ) 2 ] ( 1 ). Binding of the two different thioethers to Fe generates both five- and six-membered rings with Fe–S bonds in the five-membered rings (av 2.54 Å) being significantly shorter than those in the six-membered rings (av 2.71 Å), suggesting hemilability of the latter thioethers. Consistent with this hypothesis, magnetic circular dichroism (MCD) and computational (TD-DFT) studies indicate that 1 in solution contains a five-coordinate component [Fe(κ 3 -S Me NS Me )(κ 2 -S Me NS Me )] ( 2 ). This ligand hemilability was demonstrated further by reactivity studies of 1 with 2,2′-bipyridine, 1,2-bis(dimethylphosphino)ethane, and 2,6-dimethylphenyl isonitrile to afford iron(II) complexes [L 2 Fe(κ 2 -S Me NS Me ) 2 ] ( 3 – 5 ). Addition of a Brønsted acid, HNTf 2, to 1 produces the paramagnetic, iron(II) amine–amido cation, [Fe(κ 3 -S Me NS Me )(κ 3 -S Me N H S Me )](NTf 2 ) ( 6; Tf = SO 2 CF 3 ). Cation 6 readily undergoes amine ligand substitution by triphos, affording the 16e – complex [Fe(κ 2 -S Me NS Me )(κ 3 -triphos)](NTf 2 ) ( 7; triphos = bis(2-diphenylphosphinoethyl)phenylphosphine). These complexes are characterized by elemental analysis; 1 H NMR, Mössbauer, IR, and UV–vis spectroscopy; and single-crystal X-ray diffraction. Preliminary results of amine–borane dehydrogenation catalysis show complex 7 to be a selective and particularly robust precatalyst.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Insufficient payload (model declined to judge)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.002
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0020.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.014
GPT teacher head0.233
Teacher spread0.220 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations25
Published2017
Admission routes2
Has abstractyes

Explore more

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