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Record W4403292282 · doi:10.1021/jacs.4c12203

Experimental Evidence for Zerovalent Pd(NHC) as a Competent Catalyst in C–N Cross-Coupling (NHC = DiMeIHept<sup>Cl</sup>)

2024· article· en· W4403292282 on OpenAlexafffund
Volodymyr Semeniuchenko, Sepideh Sharif, Neha Rana, Nalin Chandrasoma, Wilfried M. Braje, R. Tom Baker, Jeffrey M. Manthorpe, William J. Pietro, Michael G. Organ

Bibliographic record

VenueJournal of the American Chemical Society · 2024
Typearticle
Languageen
FieldChemistry
TopicCatalytic Cross-Coupling Reactions
Canadian institutionsYork UniversityCarleton UniversityUniversity of Ottawa
FundersNatural Sciences and Engineering Research Council of CanadaMitacs
KeywordsCarbeneChemistryCatalysisLigand (biochemistry)Coupling (piping)Medicinal chemistryStereochemistryOrganic chemistryReceptor

Abstract

fetched live from OpenAlex

Use of the branched N-heterocyclic carbene (NHC) ligand 1,3-bis(2,6-bis(3-methyl-1-(2-methylpropyl)butyl)phenyl)-4,5-dichloro-1,3-dihydro-2 H -imidazole-2-ylidene (DiMeIHept Cl ) facilitated the stabilization of several relevant intermediates for Pd(NHC)-catalyzed C–N cross-coupling reactions. Complexes [Pd(DiMeIHept Cl )] 2 (μ-N 2 ), [Pd(DiMeIHept Cl )] 2 (μ–η 2 -1,2-η 2 -4,5-C 6 H 6 ), and Pd(DiMeIHept Cl )(pyridine), representing zerovalent Pd(NHC) bearing labile ligands, were isolated and structurally characterized, along with divalent PdCl(Ph)(DiMeIHept Cl ) and PdCl(Ph)(DiMeIHept Cl )( n -propylamine). The former is a 14-electron Pd complex, which is stable under air and chromatography on silica gel or neutral alumina. One possible reason for this exceptional stability is the numerous dispersion interactions between the NHC alkyl chains and the Pd–Ph group. Detailed investigations of catalyst activation and oxidative addition confirmed that “Pd(NHC)” is formed from many known Pd(II)(NHC) precatalysts and provided activation rates for these different precatalysts.

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)0.001
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow)
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 score0.023
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0010.001
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0010.002
Bibliometrics0.0000.001
Science and technology studies0.0000.001
Scholarly communication0.0000.000
Open science0.0010.000
Research integrity0.0000.001
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 head0.032
GPT teacher head0.355
Teacher spread0.323 · 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

Citations16
Published2024
Admission routes2
Has abstractyes

Explore more

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