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Record W1988772002 · doi:10.1021/ja045416h

Allylic Ionization versus Oxidative Addition into Vinyl C−X Bonds by Pd with Polyfunctional Olefin Templates

2004· article· en· W1988772002 on OpenAlexaff
Eamon Comer, Michael G. Organ, Stephen J. Hynes

Bibliographic record

VenueJournal of the American Chemical Society · 2004
Typearticle
Languageen
FieldChemistry
TopicAsymmetric Synthesis and Catalysis
Canadian institutionsYork University
Fundersnot available
KeywordsChemistryNucleophileAllylic rearrangementMalonateOlefin fiberChemoselectivityDimethyl malonateCatalysisMedicinal chemistryAlkeneOrganic chemistryPalladium

Abstract

fetched live from OpenAlex

The chemoselectivity of activation by a (PPh3)4Pd catalyst on a series of small, olefin-based compounds that were substituted with a variety of allylic and vinylic functional groups was studied. Of particular note, the allylic acetate of 1-acetoxy-2-bromo-2-propene (7) was selectively ionized by Pd in the presence of a malonate nucleophile, while oxidative addition of the C-Br bond to Pd occurred exclusively in the presence of a boronic acid nucleophile. When the acetate nucleophile was used, no ionization of the acetate leaving group occurred at all, which was proven by the use of deuterium-labeled substrates (e.g., 11). This report demonstrates that the nucleophile interacts in some way with Pd prior to catalyst activation of the substrate. Certainly in the case of the malonate nucleophile, this is without precedent and contradicts the central dogma of how these proposed catalytic cycles operate.

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)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesnone
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 score0.022
Threshold uncertainty score0.427

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
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)0.0000.000

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 head0.006
GPT teacher head0.216
Teacher spread0.210 · 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.

The models applied no category: nothing in the taxonomy fit this work.
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

Citations15
Published2004
Admission routes1
Has abstractyes

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