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Record W2314182794 · doi:10.1021/ja2085959

Origins of Steric Effects in General-Base-Catalyzed Enolization: Solvation and Electrostatic Attraction

2011· article· en· W2314182794 on OpenAlexaff
Scott O. C. Mundle, Graeme W. Howe, Ronald Kluger

Bibliographic record

VenueJournal of the American Chemical Society · 2011
Typearticle
Languageen
FieldChemistry
TopicChemical Reaction Mechanisms
Canadian institutionsUniversity of Toronto
Fundersnot available
KeywordsChemistryKeto–enol tautomerismSteric effectsSolvationAttractionCatalysisBase (topology)Computational chemistryStereochemistrySolventOrganic chemistry

Abstract

fetched live from OpenAlex

Brønsted plots for general-base-catalyzed enolization of aldehydes and ketones show significant negative deviations for the rates of proton removal by sterically hindered amine bases. The origins of the deviations are not apparent from considerations of interactions at the site of the proton transfer. Contrasting behavior is observed in general-base-catalyzed proton removal from an iminium derivative, N1'-methyl-2-(1-hydroxybenzyl)thiamin (NMHBnT), which shows no deviations from the Brønsted correlation for sterically hindered amine bases. The difference in behavior for these two systems suggests that the steric effects arise from disruption of solvation of the enolate enforced by the electrostatic requirements of the overall process. This interpretation also can account for reduced steric effects for enolization in the presence of metal ions.

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 score0.005
Threshold uncertainty score0.370

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
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 head0.015
GPT teacher head0.246
Teacher spread0.231 · 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

Citations5
Published2011
Admission routes1
Has abstractyes

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