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Record W2314454852 · doi:10.1021/om300182c

Radical Mechanisms in the Reaction of Organic Halides with Diiminepyridine Cobalt Complexes

2012· article· en· W2314454852 on OpenAlexafffund
Di Zhu, Ilia Korobkov, Peter H. M. Budzelaar

Bibliographic record

VenueOrganometallics · 2012
Typearticle
Languageen
FieldChemistry
TopicCatalytic C–H Functionalization Methods
Canadian institutionsUniversity of OttawaUniversity of Manitoba
FundersNatural Sciences and Engineering Research Council of CanadaUniversity of Manitoba
KeywordsChemistryArylHalideHalogenMedicinal chemistryAlkylPyridineRadicalRing (chemistry)HydrogenolysisPhotochemistryOrganic chemistryCatalysis

Abstract

fetched live from OpenAlex

The formally Co(0) complex LCo(N 2 ) (L = 2,6-bis(2,6-dimethylphenyliminoethyl)pyridine) can be prepared via either Na/Hg reduction of LCoCl 2 or hydrogenolysis of LCoCH 2 SiMe 3 . In the latter reaction, LCoH could be trapped by reaction with N≡CC 6 H 4 -4-Cl to give LCoN═CHC 6 H 4 -4-Cl. LCo(N 2 ) reacts with many alkyl and aryl halides RX, including aryl chlorides, to give a mixture of LCoR and LCoX in a halogen atom abstraction mechanism. Intermediacy of free alkyl and aryl radicals is confirmed by the ring-opening of cyclopropylmethyl to crotyl, and the rearrangement of 2,4,6- t Bu 3 C 6 H 2 to 3,5- t Bu 2 C 6 H 3 CMe 2 CH 2, before binding to Co. The organocobalt species generated in this way react further with activated halides R′X (alkyl iodides; allyl and benzyl halides) to give cross-coupling products RR′ in what is most likely again a halogen abstraction mechanism. DFT studies support the proposed radical pathways for both steps. MeI couples smoothly with LCoCH 2 SiMe 3 to give LCoI and CH 3 CH 2 SiMe 3, but the analogous reaction of t BuI leads in part to radical attack at the 3 and 4 positions of the pyridine ring to form ( t Bu 2 -L)CoI and ( t Bu 2 -L)CoI 2 .

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)0.001
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesInsufficient 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 score0.036
Threshold uncertainty score0.997

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.001
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0030.000

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 head0.031
GPT teacher head0.269
Teacher spread0.238 · 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

Citations42
Published2012
Admission routes2
Has abstractyes

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