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Record W2084328567 · doi:10.1021/om1008346

Addition of Enamines or Pyrroles and B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub> “Frustrated Lewis Pairs” to Alkynes

2010· article· en· W2084328567 on OpenAlexaff
M.A. Dureen, Christopher C. Brown, Douglas W. Stephan

Bibliographic record

VenueOrganometallics · 2010
Typearticle
Languageen
FieldChemistry
TopicOrganoboron and organosilicon chemistry
Canadian institutionsUniversity of Toronto
Fundersnot available
KeywordsChemistryPhenylacetyleneDeprotonationMedicinal chemistryArylPyrroleLewis acids and basesBoronStereochemistryOrganic chemistryCatalysisIonAlkyl

Abstract

fetched live from OpenAlex

Reaction of 1-morpholinocyclohexene with B(C 6 F 5 ) 3 and phenylacetylene gave a mixture of two compounds, [C 6 H 10 N(CH 2 CH 2 ) 2 O][PhCCB(C 6 F 5 ) 3 ] ( 1a ) and C 6 H 9 (2-PhC═C(H)B(C 6 F 5 ) 3 )(N(CH 2 CH 2 ) 2 O ( 1b ). The analogous reaction with ethynylferrocene resulted in only the deprotonation product, the alkynyl-borate salt [C 6 H 10 N(CH 2 CH 2 ) 2 O][CpFe(C 5 H 4 )CCB(C 6 F 5 ) 3 ] ( 2 ). The related reactions of pyrrole, phenylacetylene, and B(C 6 F 5 ) 3 led to the vinyl-borate addition product, HNC 4 H 4 (2-PhC═C(H)B(C 6 F 5 ) 3 ) ( 3 ). In a similar fashion, reaction of N -methylpyrrole, phenylacetylene, and B(C 6 F 5 ) 3 gave a 3:2 ratio of the products MeNC 4 H 4 (2-PhC═C(H)B(C 6 F 5 ) 3 ) ( 4a ) and MeNC 4 H 4 (3-PhC═C(H)B(C 6 F 5 ) 3 ) ( 4b ), while the corresponding reaction of N - tert -butylpyrrole with phenylacetylene and B(C 6 F 5 ) 3 provided a single product, t BuNC 4 H 4 (3-PhC═C(H)B(C 6 F 5 ) 3 ) ( 5a ). Variations in the aryl alkynes produced the corresponding addition complexes, t BuNC 4 H 4 (3-ArC═C(H)B(C 6 F 5 ) 3 ) (Ar = p -C 6 H 4 Br 5b, m -C 6 H 4 Cl 5c, p -C 6 H 4 CF 3 5d, CpFe(C 5 H 4 ) 5e ). Similarly MeNC 4 H 2 (2,5-Me 2 )(3-ArC═C(H)B(C 6 F 5 ) 3 ) (Ar = Ph 6a, p -C 6 H 4 Br 6b, m -C 6 H 4 Cl 6c, p -C 6 H 4 CF 3 6d, CpFe(C 5 H 4 ) 6e ) were derived from 1,2,5-trimethylpyrrole. The species 5a and 5b were shown to rearrange to give t BuNC 4 H 3 (3-ArC═C(H)(C 6 F 5 )B(C 6 F 5 ) 2 ) (Ar = Ph 7a, CpFe(C 5 H 4 ) 7b ). The related complexes RNC 4 H 3 (3-PhC═C(H)(C 6 F 5 )B(C 6 F 5 ) 2 ) (R = SiMe 3 8, Ph 9 ) and MeNC 4 H(2,5-Me 2 )(3-PhC═C(H)(C 6 F 5 )B(C 6 F 5 ) 2 ) ( 10 ) were derived directly from the corresponding reactions of the pyrrole, PhCCH, and B(C 6 F 5 ) 3 . In the case of the reaction of N-tert -butylpyrrole, phenylacetylene, and PhB(C 6 F 5 ) 2, phenyl group migration was observed, affording exclusively the species t BuNC 4 H 3 (3-PhC═C(H)(Ph)B(C 6 F 5 ) 2 ) ( 11 ). Reaction of 5a or 4a/4b and t Bu 3 P resulted in deprotonation and formation of the salts [ t Bu 3 PH][RNC 4 H 3 ( X -PhC═C(H)B(C 6 F 5 ) 3 )] (R = t Bu, X = 3 12; R = Me X = 2 13a, 3 13b ). Reaction of 5a − d or 6a − d with one equivalent of Et 3 PO mediated proton transfer to generate a series of vinyl pyrroles t BuNC 4 H 3 (3-ArC═CH 2 ) (Ar = Ph 14a, p -C 6 H 4 Br 14b, m -C 6 H 4 Cl 14c, p- C 6 H 4 CF 3 14d ) and MeNC 4 H 2 (2,5-Me 2 )(3-ArC═CH 3 ) (Ar = Ph 15a, p -C 6 H 4 Br 15b, m -C 6 H 4 Cl 15c, p -C 6 H 4 CF 3 15d ) and the byproduct Et 3 PO·B(C 6 F 5 ) 3 .

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 score0.018
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.001
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.001
Science and technology studies0.0000.001
Scholarly communication0.0000.001
Open science0.0010.000
Research integrity0.0010.001
Insufficient payload (model declined to judge)0.0010.000

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 head0.010
GPT teacher head0.214
Teacher spread0.204 · 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

Citations90
Published2010
Admission routes1
Has abstractyes

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